Epitaxy: Programmable Atom Equivalents Versus Atoms
- Mary X. Wang
- ,
- Soyoung E. Seo
- ,
- Paul A. Gabrys
- ,
- Dagny Fleischman
- ,
- Byeongdu Lee
- ,
- Youngeun Kim
- ,
- Harry A. Atwater
- ,
- Robert J. Macfarlane
- , and
- Chad A. Mirkin
Abstract
The programmability of DNA makes it an attractive structure-directing ligand for the assembly of nanoparticle (NP) superlattices in a manner that mimics many aspects of atomic crystallization. However, the synthesis of multilayer single crystals of defined size remains a challenge. Though previous studies considered lattice mismatch as the major limiting factor for multilayer assembly, thin film growth depends on many interlinked variables. Here, a more comprehensive approach is taken to study fundamental elements, such as the growth temperature and the thermodynamics of interfacial energetics, to achieve epitaxial growth of NP thin films. Both surface morphology and internal thin film structure are examined to provide an understanding of particle attachment and reorganization during growth. Under equilibrium conditions, single crystalline, multilayer thin films can be synthesized over 500 × 500 μm2 areas on lithographically patterned templates, whereas deposition under kinetic conditions leads to the rapid growth of glassy films. Importantly, these superlattices follow the same patterns of crystal growth demonstrated in atomic thin film deposition, allowing these processes to be understood in the context of well-studied atomic epitaxy and enabling a nanoscale model to study fundamental crystallization processes. Through understanding the role of epitaxy as a driving force for NP assembly, we are able to realize 3D architectures of arbitrary domain geometry and size.
Results and Discussion
Conclusion
Methods
DNA Functionalization of Gold Nanoparticles
Substrate Preparation and Functionalization
Patterned Template Synthesis
Silanization of Patterned Templates
Unpatterned Substrate Preparation
Substrate DNA Functionalization
Layer-by-Layer DNA–Nanoparticle Superlattice Thin Film Assembly
Determining the Thin Film Annealing Temperature
DNA–NP Superlattice Thin Film Assembly
Silica Embedding
Small-Angle X-ray Scattering
SAXS Experimental Conditions
Grazing Incidence SAXS
Focused Ion Beam-Scanning Electron Microscopy
RMS Roughness and Mean Thickness Calculation
Supporting Information
The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.6b06584.
Oligonucleotide sequences, FIB-SEM and SAXS analysis, and additional figures and tables (PDF)
Terms & Conditions
Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.
Acknowledgment
This work was supported by the following awards: AFOSR FA9550-11-1-0275 and FA9550-12-1-0280; the Department of Defense National Security Science and Engineering Faculty Fellowship N00014-15-1-0043; and the Center for Bio-Inspired Energy Science (CBES), an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences under award DE-SC0000989-0002. This work was also supported by the National Science Foundation’s (NSF) MRSEC program (DMR-1121262) and made use of its Shared Facilities at the Materials Research Center of Northwestern University, specifically the EPIC facility of the NUANCE Center, which also receives support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205). X-ray experiments were carried out at beamline 12-ID-B at the Advanced Photon Source (APS), a U.S. DOE Office of Science User Facility operated by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. EBL was performed at the Kavli Nanoscience Institute’s shared instrumentation center. FIB-SEM was performed at the Shared Experimental Facilities supported in part by the MRSEC Program of the NSF (DMR-1419807). M.X.W. acknowledges support from the National Science Foundation Graduate Research Fellowship, a Ryan Fellowship, and the Northwestern University International Institute for Nanotechnology. S.E.S. acknowledges support from the Center for Bio-Inspired Energy Sciences Fellowship and the Northwestern University International Institute for Nanotechnology. Y.K. acknowledges support from a Ryan Fellowship and the Northwestern University International Institute for Nanotechnology.
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5Hua, F.; Shi, J.; Lvov, Y.; Cui, T. Patterning of Layer-by-Layer Self-Assembled Multiple Types of Nanoparticle Thin Films by Lithographic Technique Nano Lett. 2002, 2, 1219– 1222 DOI: 10.1021/nl0257521Google Scholar5https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD38XntV2ru7o%253D&md5=9d9e2318eaeb5d35370e86a9cc0bc8caPatterning of layer-by-layer self-assembled multiple types of nanoparticle thin films by lithographic techniqueHua, F.; Shi, J.; Lvov, Y.; Cui, T.Nano Letters (2002), 2 (11), 1219-1222CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)A lithog. approach to generate clean patterns of multiple types of nanoparticles on one 4-in. silicon wafer is demonstrated. Each type of nanoparticle is precisely directed to the desired location. The process is mainly based on conventional microelectronic techniques with extremely high reproducibility. This enables the possibility of industrial applications to fabricate devices made of nanocrystals. A thin film of polystyrene spheres, 150 nm in diam., was first coated on the silicon wafer with layer-by-layer self-assembly, followed by a layer of aluminum deposited on the thin film. A layer of pos. photoresist was spun on the surface of aluminum and then patterned by lithog. technique. The unprotected aluminum was removed by wet etching until the polystyrene thin film underneath was exposed to the air. Oxygen plasma was employed to etch the polystyrene thin film all the way to the silicon surface. Subsequently, a thin film of another type of nanoparticle, silica particle 78 nm in diam., was adsorbed onto the surface with layer-by-layer self-assembly. Eventually, aluminum and photoresist were removed and each type of nanoparticle was located next to each other as the pattern was designed. A scanning electron microscope was used to produce the image of the pattern.
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6Rupich, S. M.; Castro, F. C.; Irvine, W. T.; Talapin, D. V. Soft Epitaxy of Nanocrystal Superlattices Nat. Commun. 2014, 5, 5045 DOI: 10.1038/ncomms6045Google Scholar6https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXjvFahsb4%253D&md5=ae591f44726838f9147bfdc325bf2f34Soft epitaxy of nanocrystal superlatticesRupich, Sara M.; Castro, Fernando C.; Irvine, William T. M.; Talapin, Dmitri V.Nature Communications (2014), 5 (), 5045CODEN: NCAOBW; ISSN:2041-1723. (Nature Publishing Group)Epitaxial heterostructures with precise registry between crystal layers play a key role in electronics and optoelectronics. In a close analogy, performance of nanocrystal (NC) based devices depends on the perfection of interfaces formed between NC layers. Here we systematically study the epitaxial growth of NC layers for the first time to enable the fabrication of coherent NC layers. NC epitaxy reveals an exceptional strain tolerance. It follows a universal island size scaling behavior and shows a strain-driven transition from layer-by-layer to Stranski-Krastanov growth with non-trivial island height statistics. Kinetic bottlenecks play an important role in NC epitaxy, esp. in the transition from sub-monolayer to multilayer coverage and the epitaxy of NCs with anisotropic shape. These findings provide a foundation for the rational design of epitaxial structures in a fundamentally and practically important size regime between at. and microscopic systems.
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7Tao, A.; Kim, F.; Hess, C.; Goldberger, J.; He, R.; Sun, Y.; Xia, Y.; Yang, P. Langmuir-Blodgett Silver Nanowire Monolayers for Molecular Sensing Using Surface-Enhanced Raman Spectroscopy Nano Lett. 2003, 3, 1229– 1233 DOI: 10.1021/nl0344209Google Scholar7https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3sXlvFWmtLg%253D&md5=939168fe46bc097210d7c49be90e6c02Langmuir-Blodgett silver nanowire monolayers for molecular sensing using surface-enhanced Raman spectroscopyTao, Andrea; Kim, Franklin; Hess, Christian; Goldberger, Joshua; He, Rongrui; Sun, Yugang; Xia, Younan; Yang, PeidongNano Letters (2003), 3 (9), 1229-1233CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)Langmuir-Blodgett technique was used to assemble monolayers (with areas over 20 cm2) of aligned silver nanowires that are ∼50 nm in diam. and 2-3 μm in length. These nanowires possess pentagonal cross sections and pyramidal tips. They are close-packed and are aligned parallel to each other. The resulting nanowire monolayers serve as excellent substrates for surface-enhanced Raman spectroscopy (SERS) with large electromagnetic field enhancement factors (2 × 105 for thiol and 2,4-dinitrotoluene, and 2 × 109 for Rhodamine 6G) and can readily be used in ultrasensitive, mol.-specific sensing using vibrational signatures.
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8Kotov, N. A.; Dekany, I.; Fendler, J. H. Layer-by-Layer Self-Assembly of Polyelectrolyte-Semiconductor Nanoparticle Composite Films J. Phys. Chem. 1995, 99, 13065– 13069 DOI: 10.1021/j100035a005Google Scholar8https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaK2MXnsVOjs7s%253D&md5=adf646f10c0f369953e3b92950fd4a61Layer-by-Layer Self-Assembly of Polyelectrolyte-Semiconductor Nanoparticle Composite FilmsKotov, Nicholas A.; Dekany, Imre; Fendler, Janos H.Journal of Physical Chemistry (1995), 99 (35), 13065-9CODEN: JPCHAX; ISSN:0022-3654. (American Chemical Society)Spectroscopic (absorption and emission), microscopic (transmission electron and at. force), X-ray diffraction and photocurrent measurements have provided evidence for the formation of stable ultrathin films with regular periodicities, by the layer-by-layer self-assembly of polycations and cadmium sulfide, lead sulfide and titanium dioxide nanoparticles.
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9Park, S. Y.; Lytton-Jean, A. K.; Lee, B.; Weigand, S.; Schatz, G. C.; Mirkin, C. A. DNA-Programmable Nanoparticle Crystallization Nature 2008, 451, 553– 556 DOI: 10.1038/nature06508Google Scholar9https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXhs1ent7g%253D&md5=b5c8c1ab8b7f43d32793560e4869ad2fDNA-programmable nanoparticle crystallizationPark, Sung Yong; Lytton-Jean, Abigail K. R.; Lee, Byeongdu; Weigand, Steven; Schatz, George C.; Mirkin, Chad A.Nature (London, United Kingdom) (2008), 451 (7178), 553-556CODEN: NATUAS; ISSN:0028-0836. (Nature Publishing Group)It was first shown more than ten years ago that DNA oligonucleotides can be attached to gold nanoparticles rationally to direct the formation of larger assemblies. Since then, oligonucleotide-functionalized nanoparticles have been developed into powerful diagnostic tools for nucleic acids and proteins, and into intracellular probess and gene regulators. In contrast, the conceptually simple yet powerful idea that functionalized nanoparticles might serve as basic building blocks that can be rationally assembled through programmable base-pairing interactions into highly ordered macroscopic materials remains poorly developed. So far, the approach has mainly resulted in polymn., with modest control over the placement of, the periodicity in, and the distance between particles within the assembled material. That is, most of the materials obtained thus far are best classified as amorphous polymers, although a few examples of colloidal crystal formation exist. Here, we demonstrate that DNA can be used to control the crystn. of nanoparticle-oligonucleotide conjugates to the extent that different DNA sequences guide the assembly of the same type of inorg. nanoparticle into different cryst. states. We show that the choice of DNA sequences attached to the nanoparticle building blocks, the DNA linking mols. and the absence or presence of a non-bonding single-base flexor can be adjusted so that gold nanoparticles assemble into micrometer-sized face-centered-cubic or body-centered-cubic crystal structures. Our findings thus clearly demonstrate that synthetically programmable colloidal crystn. is possible, and that a single-component system can be directed to form different structures.
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10Macfarlane, R. J.; Lee, B.; Jones, M. R.; Harris, N.; Schatz, G. C.; Mirkin, C. A. Nanoparticle Superlattice Engineering with DNA Science 2011, 334, 204– 208 DOI: 10.1126/science.1210493Google Scholar10https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3MXht1yksbbK&md5=e5902f70c851a5177d4e3b9a28dfbe62Nanoparticle Superlattice Engineering with DNAMacFarlane, Robert J.; Lee, Byeongdu; Jones, Matthew R.; Harris, Nadine; Schatz, George C.; Mirkin, Chad A.Science (Washington, DC, United States) (2011), 334 (6053), 204-208CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)A current limitation in nanoparticle superlattice engineering is that the identities of the particles being assembled often det. the structures that can be synthesized. Therefore, specific crystallog. symmetries or lattice parameters can only be achieved using specific nanoparticles as building blocks (and vice versa). The authors present six design rules that can be used to deliberately prep. nine distinct colloidal crystal structures, with control over lattice parameters on the 25- to 150-nm length scale. These design rules outline a strategy to independently adjust each of the relevant crystallog. parameters, including particle size (5 to 60 nm), periodicity, and interparticle distance. As such, this work represents an advance in synthesizing tailorable macroscale architectures comprising nanoscale materials in a predictable fashion.
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11O’Brien, M. N.; Jones, M. R.; Lee, B.; Mirkin, C. A. Anisotropic Nanoparticle Complementarity in DNA-Mediated Co-Crystallization Nat. Mater. 2015, 14, 833– 839 DOI: 10.1038/nmat4293Google Scholar11https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXhtFeju7jP&md5=8315fd6e146a45ddc2dd3b93458458c2Anisotropic nanoparticle complementarity in DNA-mediated co-crystallizationO'Brien, Matthew N.; Jones, Matthew R.; Lee, Byeongdu; Mirkin, Chad A.Nature Materials (2015), 14 (8), 833-839CODEN: NMAACR; ISSN:1476-1122. (Nature Publishing Group)By using DNA as a surface ligand, mixts. of two different anisotropic nanoparticles were selectively cocrystd., and the effects of nanoparticle size and shape complementarity on the resultant crystal symmetry, microstrain, and effective 'DNA bond' length and strength were investigated. These results were used to understand a more complicated system where both size and shape complementarity change, and where one nanoparticle can participate in multiple types of directional interactions. These findings offer improved control of non-spherical nanoparticles as building blocks for the assembly of sophisticated macroscopic materials, and provide a framework to understand complementarity and directional interactions in DNA-mediated nanoparticle crystn.
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12Senesi, A. J.; Eichelsdoerfer, D. J.; Macfarlane, R. J.; Jones, M. R.; Auyeung, E.; Lee, B.; Mirkin, C. A. Stepwise Evolution of DNA-Programmable Nanoparticle Superlattices Angew. Chem., Int. Ed. 2013, 52, 6624– 6628 DOI: 10.1002/anie.201301936Google Scholar12https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXnvVOitLs%253D&md5=674aaf5fbc8ab183e0420cc85da10081Stepwise Evolution of DNA-Programmable Nanoparticle SuperlatticesSenesi, Andrew J.; Eichelsdoerfer, Daniel J.; Macfarlane, Robert J.; Jones, Matthew R.; Auyeung, Evelyn; Lee, Byeongdu; Mirkin, Chad A.Angewandte Chemie, International Edition (2013), 52 (26), 6624-6628CODEN: ACIEF5; ISSN:1433-7851. (Wiley-VCH Verlag GmbH & Co. KGaA)The authors use a stepwise growth process to systematically study and control the evolution of a bcc. cryst. thin-film comprised of nanoparticle building blocks functionalized with DNA on a complementary DNA substrate. The authors examine crystal growth as a function of temp., no. of layers, and substrate-particle bonding interactions. Importantly, the judicious choice of DNA interconnects allows one to tune the interfacial energy between various crystal planes and the substrate, and thereby control crystal orientation and size in a stepwise fashion using chem. programmable attractive forces.
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13Hellstrom, S. L.; Kim, Y.; Fakonas, J. S.; Senesi, A. J.; Macfarlane, R. J.; Mirkin, C. A.; Atwater, H. A. Epitaxial Growth of DNA-Assembled Nanoparticle Superlattices on Patterned Substrates Nano Lett. 2013, 13, 6084– 6090 DOI: 10.1021/nl4033654Google Scholar13https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXhslersLzM&md5=9ac1c19af28af91f2cfba569fec1f738Epitaxial Growth of DNA-Assembled Nanoparticle Superlattices on Patterned SubstratesHellstrom, Sondra L.; Kim, Youngeun; Fakonas, James S.; Senesi, Andrew J.; MacFarlane, Robert J.; Mirkin, Chad A.; Atwater, Harry A.Nano Letters (2013), 13 (12), 6084-6090CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)Arrays of DNA-functionalized gold nanoparticles have been grown epitaxially on lithog. patterned templates, eliminating grain boundaries and enabling fine control over orientation and size of assemblies up to thousands of square micrometers. This epitaxial growth allowed for orientational control, systematic introduction of strain, and designed defects, which extend the range of structures that can be made using superlattice assembly.
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14Lalander, C. H.; Zheng, Y.; Dhuey, S.; Cabrini, S.; Bach, U. DNA-Directed Self-Assembly of Gold Nanoparticles onto Nanopatterned Surfaces: Controlled Placement of Individual Nanoparticles into Regular Arrays ACS Nano 2010, 4, 6153– 6161 DOI: 10.1021/nn101431kGoogle Scholar14https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3cXht1KhsLnK&md5=7cc8b84ceb08868fdbc94ffb6794af52DNA-Directed Self-Assembly of Gold Nanoparticles onto Nanopatterned Surfaces: Controlled Placement of Individual Nanoparticles into Regular ArraysLalander, Cecilia H.; Zheng, Yuanhui; Dhuey, Scott; Cabrini, Stefano; Bach, UdoACS Nano (2010), 4 (10), 6153-6161CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)A method for the templated DNA-directed self-assembly of individual gold nanoparticles (AuNPs) into discrete nanostructures is described. The templating nanostructures consisted of a linear configuration of six metal dots with a center-to-center dot distance of 55 nm, fabricated by electron beam lithog. The 40 nm DNA-capped AuNPs were immobilized onto this templating nanostructure to produce a linear configuration of six adjacent AuNPs. The geometry of the templating nanostructure is critically important for the successful direction of a single nanoparticle onto individual adsorption sites. For optimized template structures the immobilization efficiency of nanoparticles onto the individual adsorption sites is 80%. The nonspecific assocn. of nanoparticles with specifically adsorbed nanoparticles and the between adsorption of nanoparticles, bridging two individual adsorption sites, were the two main defects obsd. in the immobilized assemblies. Less than 1% of all surface confined AuNPs adsorbed nonspecifically in the areas between the self-assembled regular arrays.
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15Macfarlane, R. J.; Thaner, R. V.; Brown, K. A.; Zhang, J.; Lee, B.; Nguyen, S. T.; Mirkin, C. A. Importance of the DNA “Bond” in Programmable Nanoparticle Crystallization Proc. Natl. Acad. Sci. U. S. A. 2014, 111, 14995– 15000 DOI: 10.1073/pnas.1416489111Google Scholar15https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhslajurjO&md5=79f2b5051b7234646f29404a0fbb4547Importance of the DNA "bond" in programmable nanoparticle crystallizationMacFarlane, Robert J.; Thaner, Ryan V.; Brown, Keith A.; Zhang, Jian; Lee, Byeongdu; Nguyen, Son Binh T.; Mirkin, Chad A.Proceedings of the National Academy of Sciences of the United States of America (2014), 111 (42), 14995-15000CODEN: PNASA6; ISSN:0027-8424. (National Academy of Sciences)If a soln. of DNA-coated nanoparticles is allowed to crystallize, the thermodn. structure can be predicted by a set of structural design rules analogous to Pauling's rules for ionic crystn. The details of the crystn. process, however, have proved more difficult to characterize as they depend on a complex interplay of many factors. Here, we report that this crystn. process is dictated by the individual DNA bonds and that the effect of changing structural or environmental conditions can be understood by considering the effect of these parameters on free oligonucleotides. Specifically, we obsd. the reorganization of nanoparticle superlattices using time-resolved synchrotron small-angle x-ray scattering in systems with different DNA sequences, salt concns., and densities of DNA linkers on the surface of the nanoparticles. The agreement between bulk crystn. and the behavior of free oligonucleotides may bear important consequences for constructing novel classes of crystals and incorporating new interparticle bonds in a rational manner.
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16Zhang, C.; Macfarlane, R. J.; Young, K. L.; Choi, C. H. J.; Hao, L.; Auyeung, E.; Liu, G.; Zhou, X.; Mirkin, C. A. A General Approach to DNA-Programmable Atom Equivalents Nat. Mater. 2013, 12, 741– 746 DOI: 10.1038/nmat3647Google Scholar16https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXnvVSisrc%253D&md5=6c0d26f8c854030efb166a5198e0033aA general approach to DNA-programmable atom equivalentsZhang, Chuan; MacFarlane, Robert J.; Young, Kaylie L.; Choi, Chung Hang J.; Hao, Liangliang; Auyeung, Evelyn; Liu, Guoliang; Zhou, Xiaozhu; Mirkin, Chad A.Nature Materials (2013), 12 (8), 741-746CODEN: NMAACR; ISSN:1476-1122. (Nature Publishing Group)Nanoparticles can be combined with nucleic acids to program the formation of three-dimensional colloidal crystals where the particles' size, shape, compn. and position can be independently controlled. However, the diversity of the types of material that can be used is limited by the lack of a general method for prepg. the basic DNA-functionalized building blocks needed to bond nanoparticles of different chem. compns. into lattices in a controllable manner. By coating nanoparticles protected with aliph. ligands with an azide-bearing amphiphilic polymer, followed by the coupling of DNA to the polymer using strain-promoted azide-alkyne cycloaddn. (also known as copper-free azide-alkyne click chem.), nanoparticles bearing a high-d. shell of nucleic acids can be created regardless of nanoparticle compn. This method provides a route to a virtually endless class of programmable atom equiv. for DNA-based colloidal crystn.
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17Zhang, Y.; Lu, F.; Yager, K. G.; van der Lelie, D.; Gang, O. A General Strategy for the DNA-Mediated Self-Assembly of Functional Nanoparticles into Heterogeneous Systems Nat. Nanotechnol. 2013, 8, 865– 872 DOI: 10.1038/nnano.2013.209Google Scholar17https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXhs1ChsrrP&md5=e403c85b29f0525227164c548be3d3ffA general strategy for the DNA-mediated self-assembly of functional nanoparticles into heterogeneous systemsZhang, Yugang; Lu, Fang; Yager, Kevin G.; van der Lelie, Daniel; Gang, OlegNature Nanotechnology (2013), 8 (11), 865-872CODEN: NNAABX; ISSN:1748-3387. (Nature Publishing Group)Nanoparticles coated with DNA mols. can be programmed to self-assemble into three-dimensional superlattices. Such superlattices can be made from nanoparticles with different functionalities and could potentially exploit the synergetic properties of the nanoscale components. However, the approach has so far been used primarily with single-component systems. Here, the authors report a general strategy for the creation of heterogeneous nanoparticle superlattices using DNA and carboxylic-based conjugation. Nanoparticles with all major types of functionality-plasmonic (gold), magnetic (Fe2O3), catalytic (palladium) and luminescent (CdSe/Te@ZnS and CdS@ZnS)-can be incorporated into binary systems in a rational manner. The authors also examine the effect of nanoparticle characteristics (including size, shape, no. of DNA per particle and DNA flexibility) on the phase behavior of the heterosystems, and demonstrate that the assembled materials can have novel optical and field-responsive properties.
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18Lee, J.-S.; Lytton-Jean, A. K.; Hurst, S. J.; Mirkin, C. A. Silver Nanoparticle-Oligonucleotide Conjugates Based on DNA with Triple Cyclic Disulfide Moieties Nano Lett. 2007, 7, 2112– 2115 DOI: 10.1021/nl071108gGoogle Scholar18https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXmsV2ltbc%253D&md5=2df3f75517d010058d7127788753dd69Silver Nanoparticle-Oligonucleotide Conjugates Based on DNA with Triple Cyclic Disulfide MoietiesLee, Jae-Seung; Lytton-Jean, Abigail K. R.; Hurst, Sarah J.; Mirkin, Chad A.Nano Letters (2007), 7 (7), 2112-2115CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)The authors report a new strategy for prepg. silver nanoparticle-oligonucleotide conjugates that are based upon DNA with cyclic disulfide-anchoring groups. These particles are extremely stable and can withstand NaCl concns. up to 1.0 M. When silver nanoparticles functionalized with complementary sequences are combined, they assemble to form DNA-linked nanoparticle networks. This assembly process is reversible with heating and is assocd. with a red shifting of the particle surface plasmon resonance and a concomitant color change from yellow to pale red. Analogous to the oligonucleotide-functionalized gold nanoparticles, these particles also exhibit highly cooperative binding properties with extremely sharp melting transitions. This work is an important step toward using silver nanoparticle-oligonucleotide conjugates for a variety of purposes, including mol. diagnostic labels, synthons in programmable materials synthesis approaches, and functional components for nanoelectronic and plasmonic devices.
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19Brodin, J. D.; Auyeung, E.; Mirkin, C. A. DNA-Mediated Engineering of Multicomponent Enzyme Crystals Proc. Natl. Acad. Sci. U. S. A. 2015, 112, 4564– 4569 DOI: 10.1073/pnas.1503533112Google Scholar19https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXkvFejs7o%253D&md5=681d247aaedba6b20d9fae1ad94e6f44DNA-mediated engineering of multicomponent enzyme crystalsBrodin, Jeffrey D.; Auyeung, Evelyn; Mirkin, Chad A.Proceedings of the National Academy of Sciences of the United States of America (2015), 112 (15), 4564-4569CODEN: PNASA6; ISSN:0027-8424. (National Academy of Sciences)The ability to predictably control the coassembly of multiple nanoscale building blocks, esp. those with disparate chem. and phys. properties such as biomols. and inorg. nanoparticles, has far-reaching implications in catalysis, sensing, and photonics, but a generalizable strategy for engineering specific contacts between these particles is an outstanding challenge. This is esp. true in the case of proteins, where the types of possible interparticle interactions are numerous, diverse, and complex. Herein, the authors explore the concept of trading protein-protein interactions for DNA-DNA interactions to direct the assembly of two nucleic-acid-functionalized proteins with distinct surface chemistries into six unique lattices composed of catalytically active proteins, or of a combination of proteins and DNA-modified gold nanoparticles. The programmable nature of DNA-DNA interactions used in this strategy allows the authors to control the lattice symmetries and unit cell consts., as well as the compns. and habit, of the resulting crystals. This study provides a potentially generalizable strategy for constructing a unique class of materials that take advantage of the diverse morphologies, surface chemistries, and functionalities of proteins for assembling functional cryst. materials.
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20Evanoff, D. D.; Chumanov, G. Synthesis and Optical Properties of Silver Nanoparticles and Arrays ChemPhysChem 2005, 6, 1221– 1231 DOI: 10.1002/cphc.200500113Google Scholar20https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2MXmsVKgtb8%253D&md5=4a805855aead6232bb364c5e05a49e8fSynthesis and optical properties of silver nanoparticles and arraysEvanoff, David D., Jr.; Chumanov, GeorgeChemPhysChem (2005), 6 (7), 1221-1231CODEN: CPCHFT; ISSN:1439-4235. (Wiley-VCH Verlag GmbH & Co. KGaA)A review. This Minireview systematically examines optical properties of Ag nanoparticles as a function of size. Extinction, scattering, and absorption cross sections and distance dependence of the local electromagnetic field, as well as the quadrupolar coupling of 2-dimensional assemblies of such particles are exptl. measured for a wide range of particle sizes. Such measurements were possible because of the development of a novel synthetic method for the size-controlled synthesis of chem. clean, highly cryst. Ag nanoparticles of narrow size distribution. The method and its unique advantages are compared to other methods for synthesis of metal nanoparticles. Synthesis and properties of nanocomposite materials using these and other nanoparticles are also described. Important highlights in the history of the field of metal nanoparticles as well as an examn. of the basic principles of plasmon resonances are included.
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21Kelly, K. L.; Coronado, E.; Zhao, L. L.; Schatz, G. C. The Optical Properties of Metal Nanoparticles: The Influence of Size, Shape, and Dielectric Environment J. Phys. Chem. B 2003, 107, 668– 677 DOI: 10.1021/jp026731yGoogle Scholar21https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD38Xps1Ghur0%253D&md5=f7be29b07a5f0d8311d7f0042f359274The Optical Properties of Metal Nanoparticles: The Influence of Size, Shape, and Dielectric EnvironmentKelly, K. Lance; Coronado, Eduardo; Zhao, Lin Lin; Schatz, George C.Journal of Physical Chemistry B (2003), 107 (3), 668-677CODEN: JPCBFK; ISSN:1520-6106. (American Chemical Society)The optical properties of metal nanoparticles have long been of interest in phys. chem., starting with Faraday's studies of colloidal Au in the middle 1800s. More recently, new lithog. techniques as well as improvements to classical wet chem. methods have made it possible to synthesize noble metal nanoparticles with a wide range of sizes, shapes, and dielec. environments. In this feature article, the authors describe recent progress in the theory of nanoparticle optical properties, particularly methods for solving Maxwell's equations for light scattering from particles of arbitrary shape in a complex environment. Included is a description of the qual. features of dipole and quadrupole plasmon resonances for spherical particles; a discussion of anal. and numerical methods for calcg. extinction and scattering cross sections, local fields, and other optical properties for nonspherical particles; and a survey of applications to problems of recent interest involving triangular Ag particles and related shapes.
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22Storhoff, J. J.; Lazarides, A. A.; Mucic, R. C.; Mirkin, C. A.; Letsinger, R. L.; Schatz, G. C. What Controls the Optical Properties of DNA-Linked Gold Nanoparticle Assemblies? J. Am. Chem. Soc. 2000, 122, 4640– 4650 DOI: 10.1021/ja993825lGoogle Scholar22https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3cXis1GntbY%253D&md5=c62e6e197b0b08079c1f4483230503a7What Controls the Optical Properties of DNA-Linked Gold Nanoparticle Assemblies?Storhoff, James J.; Lazarides, Anne A.; Mucic, Robert C.; Mirkin, Chad A.; Letsinger, Robert L.; Schatz, George C.Journal of the American Chemical Society (2000), 122 (19), 4640-4650CODEN: JACSAT; ISSN:0002-7863. (American Chemical Society)A study aimed at understanding the factors that control the optical properties of DNA-linked gold nanoparticle aggregates contg. oligonucleotide linkers of varying length (24-72 base pairs) is described. In this system, ∼15 nm diam. Au particles modified with (alkanethiol)-12 base oligomers are hybridized to a series of oligonucleotide linkers ranging from 24 to 72 base pairs (∼80-240 Å) in length. Aggregated at room temp., the various macroscopic nanoparticle assemblies have plasmon frequency changes that are inversely dependent on the oligonucleotide linker length. Upon annealing at temps. close to the melting temp. of the DNA, the optical properties of the DNA-linked assemblies contg. the longer linkers (48 and 72 base pairs) red-shift until they are similar to the assemblies contg. the shorter linkers (24 base pairs). The pre- and post-annealed DNA-linked assemblies were characterized by sedimentation rate, transmission electron microscopy, dynamic light scattering, and UV-vis spectroscopy which show that the oligonucleotide linker length kinetically controls the size of the aggregates that are formed under the pre-annealed conditions, thereby controlling the optical properties. Through the use of small-angle X-ray scattering and electrodynamic modeling in conjunction with the techniques mentioned above, we have detd. that the temp.-dependent optical changes obsd. upon annealing of the aggregates contg. the longer oligonucleotides (48 and 72 base pairs) can be attributed to aggregate growth through an "Ostwald ripening" mechanism (where larger aggregates grow at the expense of smaller aggregates). This type of aggregate growth leads to the red-shift in plasmon frequency obsd. for the aggregates. Significantly, these expts. provide evidence that the optical properties of these DNA-linked nanoparticle assemblies are governed by aggregate size, regardless of oligonucleotide linker length, which has important implications for the development of colorimetric detection methods based on these nanoparticle materials.
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23Choi, J.-H.; Wang, H.; Oh, S. J.; Paik, T.; Sung, P.; Sung, J.; Ye, X.; Zhao, T.; Diroll, B. T.; Murray, C. B. Exploiting the Colloidal Nanocrystal Library to Construct Electronic Devices Science 2016, 352, 205– 208 DOI: 10.1126/science.aad0371Google Scholar23https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XlsFSmtbg%253D&md5=37a791816e5a2a43bc6d6070cd0533c8Exploiting the colloidal nanocrystal library to construct electronic devicesChoi, Ji-Hyuk; Wang, Han; Oh, Soong Ju; Paik, Taejong; Sung, Pil; Sung, Jinwoo; Ye, Xingchen; Zhao, Tianshuo; Diroll, Benjamin T.; Murray, Christopher B.; Kagan, Cherie R.Science (Washington, DC, United States) (2016), 352 (6282), 205-208CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)Synthetic methods produce libraries of colloidal nanocrystals with tunable phys. properties by tailoring the nanocrystal size, shape, and compn. Here, the authors exploit colloidal nanocrystal diversity and design the materials, interfaces, and processes to construct all-nanocrystal electronic devices using soln.-based processes. Metallic silver and semiconducting cadmium selenide nanocrystals are deposited to form high-cond. and high-mobility thin-film electrodes and channel layers of field-effect transistors. Insulating aluminum oxide nanocrystals are assembled layer by layer with polyelectrolytes to form high-dielec. const. gate insulator layers for low-voltage device operation. Metallic indium nanocrystals are codispersed with silver nanocrystals to integrate an indium supply in the deposited electrodes that serves to passivate and dope the cadmium selenide nanocrystal channel layer. The authors fabricate all-nanocrystal field-effect transistors on flexible plastics with electron mobilities of 21.7 square centimeters per V-second.
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24Jonsson, P. E. Superparamagnetism and Spin Glass Dynamics of Interacting Magnetic Nanoparticle Systems Adv. Chem. Phys. 2003, 128, 191– 248 DOI: 10.1002/0471484237.ch3Google ScholarThere is no corresponding record for this reference.
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25Li, T.; Senesi, A. J.; Lee, B. Small Angle X-Ray Scattering for Nanoparticle Research Chem. Rev. 2016, 116, 11128 DOI: 10.1021/acs.chemrev.5b00690Google Scholar25https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XlsF2qsrw%253D&md5=659565f88b80ce6994bb98c07f034eb2Small Angle X-ray Scattering for Nanoparticle ResearchLi, Tao; Senesi, Andrew J.; Lee, ByeongduChemical Reviews (Washington, DC, United States) (2016), 116 (18), 11128-11180CODEN: CHREAY; ISSN:0009-2665. (American Chemical Society)X-ray scattering is a structural characterization tool that has impacted diverse fields of study. It is unique in its ability to examine materials in real time and under realistic sample environments, enabling researchers to understand morphol. at nanometer and angstrom length scales using complementary small and wide angle X-ray scattering (SAXS, WAXS), resp. Herein, we focus on the use of SAXS to examine nanoscale particulate systems. We provide a theor. foundation for X-ray scattering, considering both form factor and structure factor, as well as the use of correlation functions, which may be used to det. a particle's size, size distribution, shape, and organization into hierarchical structures. The theory is expanded upon with contemporary use cases. Both transmission and reflection (grazing incidence) geometries are addressed, as well as the combination of SAXS with other X-ray and non-X-ray characterization tools. We conclude with an examn. of several key areas of research where X-ray scattering has played a pivotal role, including in situ nanoparticle synthesis, nanoparticle assembly, and operando studies of catalysts and energy storage materials. Throughout this review we highlight the unique capabilities of X-ray scattering for structural characterization of materials in their native environment.
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26Meyers, S. T.; Anderson, J. T.; Hung, C. M.; Thompson, J.; Wager, J. F.; Keszler, D. A. Aqueous Inorganic Inks for Low-Temperature Fabrication of ZnO TFTs J. Am. Chem. Soc. 2008, 130, 17603– 17609 DOI: 10.1021/ja808243kGoogle Scholar26https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXhsVOjsLbM&md5=aa4a4cd305f8cf5ca4496836f5efb6eeAqueous Inorganic Inks for Low-Temperature Fabrication of ZnO TFTsMeyers, Stephen T.; Anderson, Jeremy T.; Hung, Celia M.; Thompson, John; Wager, John F.; Keszler, Douglas A.Journal of the American Chemical Society (2008), 130 (51), 17603-17609CODEN: JACSAT; ISSN:0002-7863. (American Chemical Society)A simple, low-cost, and nontoxic aq. ink chem. is described for digital printing of ZnO films. Selective design through controlled pptn., purifn., and dissoln. affords an aq. Zn(OH)x(NH3)y(2-x)+ soln. that is stable in storage, yet promptly decomps. at temps. <150° to form wurtzite ZnO. Dense, high-quality, polycryst. ZnO films are deposited by ink-jet printing and spin-coating, and film structure is elucidated via x-ray diffraction and electron microscopy. Semiconductor film functionality and quality were examd. through integration in bottom-gate thin-film transistors. Enhancement-mode TFTs with ink-jet printed ZnO channels annealed at 300° exhibit strong field effect and excellent current satn. in tandem with incremental mobilities from 4-6 cm2 V-1 s-1. Spin-coated ZnO semiconductors processed at 150° are integrated with soln.-deposited aluminum oxide phosphate dielecs. in functional transistors, demonstrating both high performance, i.e., mobilities up to 1.8 cm2 V-1 s-1, and the potential for low-temp. soln. processing of all-oxide electronics.
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27Seo, S. E.; Wang, M. X.; Shade, C. M.; Rouge, J. L.; Brown, K. A.; Mirkin, C. A. Modulating the Bond Strength of DNA–Nanoparticle Superlattices ACS Nano 2016, 10, 1771– 1779 DOI: 10.1021/acsnano.5b07103Google Scholar27https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhtVGgsrY%253D&md5=328033b90f7c203f49f7667cb9bd7466Modulating the Bond Strength of DNA-Nanoparticle SuperlatticesSeo, Soyoung E.; Wang, Mary X.; Shade, Chad M.; Rouge, Jessica L.; Brown, Keith A.; Mirkin, Chad A.ACS Nano (2016), 10 (2), 1771-1779CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)A method for modulating the bond strength in DNA-programmable nanoparticle (NP) superlattice crystals utilizes noncovalent interactions between a family of [Ru(dipyrido[2,3-a:3',2'-c]phenazine)(N-N)2]2+-based small mol. intercalators and DNA duplexes to postsynthetically modify DNA-NP superlattices. This increases the strength of the DNA bonds that hold the nanoparticles together, making the superlattices more resistant to thermal degrdn. The authors investigate the relationship between the structure of the intercalator and its binding affinity for DNA duplexes and det. how this translates to the increased thermal stability of the intercalated superlattices. The authors find that intercalator charge and steric profile give us a wide range of tunability and control over DNA-NP bond strength, with the resulting crystal lattices retaining their structure at temps. greater than 50°C above nonintercalated structures. This allows the authors to subject DNA-NP superlattice crystals to conditions under which they would normally melt, enabling the construction of a core-shell (gold NP-quantum dot NP) superlattice crystal.
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28Pal, S.; Zhang, Y.; Kumar, S. K.; Gang, O. Dynamic Tuning of DNA-Nanoparticle Superlattices by Molecular Intercalation of Double Helix J. Am. Chem. Soc. 2015, 137, 4030– 4033 DOI: 10.1021/ja512799dGoogle Scholar28https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXktVGksro%253D&md5=97bcbd513a7426d143786a5a98b65a46Dynamic tuning of DNA-nanoparticle superlattices by molecular intercalation of double helixPal, Suchetan; Zhang, Yugang; Kumar, Sanat K.; Gang, OlegJournal of the American Chemical Society (2015), 137 (12), 4030-4033CODEN: JACSAT; ISSN:0002-7863. (American Chemical Society)Nanoparticle (NP) assembly using DNA recognition has emerged as a powerful tool for the fabrication of 3D superlattices. In addn. to the vast structural diversity, this approach provides an avenue for dynamic 3D NP assembly, which is promising for the modulation of interparticle distances and, hence, for example, for in situ tuning of optical properties. While several approaches have been explored for changing NP sepns. in the lattices using responsiveness of single-stranded DNA (ss-DNA), far less work has been done for the manipulation of most abundant double-stranded DNA (ds-DNA) motifs. Here, we present a novel strategy for modulation of interparticle distances in DNA linked 3D self-assembled NP lattices by mol. intercalator. We utilize ethidium bromide (EtBr) as a model intercalator to demonstrate selective and isotropic lattice expansion for three superlattice types (bcc, fcc, and AlB2) due to the intercalation of ds-DNA linking NPs. We further show the reversibility of the lattice parameter using n-butanol as a retrieving agent as well as an increased lattice thermal stability by 12-14 °C due to the inclusion of EtBr. The proposed intercalator-based strategy permits the creation of reconfigurable and thermally stable superlattices, which could lead to tunable and functionally responsive materials.
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29Shade, C. M.; Kennedy, R. D.; Rouge, J. L.; Rosen, M. S.; Wang, M. X.; Seo, S. E.; Clingerman, D. J.; Mirkin, C. A. Duplex-Selective Ruthenium-Based DNA Intercalators Chem. - Eur. J. 2015, 21, 10983– 10987 DOI: 10.1002/chem.201502095Google Scholar29https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXhtVOlsrrN&md5=d13f15beca0381da6af91821e35e96b9Duplex-Selective Ruthenium-Based DNA IntercalatorsShade, Chad M.; Kennedy, Robert D.; Rouge, Jessica L.; Rosen, Mari S.; Wang, Mary X.; Seo, Soyoung E.; Clingerman, Daniel J.; Mirkin, Chad A.Chemistry - A European Journal (2015), 21 (31), 10983-10987CODEN: CEUJED; ISSN:0947-6539. (Wiley-VCH Verlag GmbH & Co. KGaA)We report the design and synthesis of small mols. that exhibit enhanced luminescence in the presence of duplex rather than single-stranded DNA. The local environment presented by a well-known [Ru(dipyrido[3,2-a:2',3'-c]phenazine)L2]2+-based DNA intercalator was modified by functionalizing the bipyridine ligands with esters and carboxylic acids. By systematically varying the no. and charge of the pendant groups, it was detd. that decreasing the electrostatic interaction between the intercalator and the anionic DNA backbone reduced single-strand interactions and translated to better duplex specificity. In studying this class of complexes, a single RuII complex emerged that selectively luminesces in the presence of duplex DNA with little to no background from interacting with single-stranded DNA. This complex shows promise as a new dye capable of selectively staining double- vs. single-stranded DNA in gel electrophoresis, which cannot be done with conventional SYBR dyes.
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30Auyeung, E.; Macfarlane, R. J.; Choi, C. H. J.; Cutler, J. I.; Mirkin, C. A. Transitioning DNA-Engineered Nanoparticle Superlattices from Solution to the Solid State Adv. Mater. 2012, 24, 5181– 5186 DOI: 10.1002/adma.201202069Google Scholar30https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC38XhtVGgt77L&md5=683eb55258a822fea064ac10d21f4be9Transitioning DNA-Engineered Nanoparticle Superlattices from Solution to the Solid StateAuyeung, Evelyn; MacFarlane, Robert J.; Choi, Chung Hang J.; Cutler, Joshua I.; Mirkin, Chad A.Advanced Materials (Weinheim, Germany) (2012), 24 (38), 5181-5186, S5181/1-S5181/12CODEN: ADVMEW; ISSN:0935-9648. (Wiley-VCH Verlag GmbH & Co. KGaA)The authors report a method for stabilizing DNA-assembled three-dimensional superlattices in the solid state by silica encapsulation, where both the symmetries and lattice spacings of the soln.-phase lattices are preserved. Once encapsulated, superlattice morphologies are no longer dictated by DNA interactions, and as such remain stable against distortion, collapse, or dissocn. under many previously inaccessible conditions.
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- Jinghan Zhu, Haixin Lin, Youngeun Kim, Muwen Yang, Kacper Skakuj, Jingshan S. Du, Byeongdu Lee, George C. Schatz, Richard P. Van Duyne, Chad A. Mirkin. Light‐Responsive Colloidal Crystals Engineered with DNA. Advanced Materials 2020, 32 (8) https://doi.org/10.1002/adma.201906600
- Paul A. Gabrys, Leonardo Z. Zornberg, Robert J. Macfarlane. Programmable Atom Equivalents: Atomic Crystallization as a Framework for Synthesizing Nanoparticle Superlattices. Small 2019, 15 (26) https://doi.org/10.1002/smll.201805424
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- Christine R. Laramy, Matthew N. O’Brien, Chad A. Mirkin. Crystal engineering with DNA. Nature Reviews Materials 2019, 4 (3) , 201-224. https://doi.org/10.1038/s41578-019-0087-2
- Qing-Yuan Lin, Jarad A. Mason, Zhongyang Li, Wenjie Zhou, Matthew N. O’Brien, Keith A. Brown, Matthew R. Jones, Serkan Butun, Byeongdu Lee, Vinayak P. Dravid, Koray Aydin, Chad A. Mirkin. Building superlattices from individual nanoparticles via template-confined DNA-mediated assembly. Science 2018, 359 (6376) , 669-672. https://doi.org/10.1126/science.aaq0591
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References
ARTICLE SECTIONS
This article references 30 other publications.
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1Zhang, Z.; Lagally, M. G. Atomistic Processes in the Early Stages of Thin-Film Growth Science 1997, 276, 377– 383 DOI: 10.1126/science.276.5311.3771https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaK2sXis1Gktrc%253D&md5=9e9f2887ebbe59053b44d097fc5fb4fcAtomistic processes in the early stages of thin-film growthZhang, Zhenyu; Lagally, Max G.Science (Washington, D. C.) (1997), 276 (5311), 377-383CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)Growth of thin films from atoms deposited from the gas phase is intrinsically a non-equil. phenomenon governed by a competition between kinetics and thermodn. Precise control of the growth and thus of the properties of deposited films becomes possible only after an understanding of this competition is achieved. Here, the at. nature of the most important kinetic mechanisms of film growth is explored. These mechanisms include adatom diffusion on terraces, along steps, and around island corners; nucleation and dynamics of the stable nucleus; atom attachment to and detachment from terraces and islands; and interlayer mass transport. Ways to manipulate the growth kinetics in order to select a desired growth mode are briefly addressed. 64 Refs.
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2Bartelt, M.; Evans, J. W. Transition to Multilayer Kinetic Roughening for Metal (100) Homoepitaxy Phys. Rev. Lett. 1995, 75, 4250– 4253 DOI: 10.1103/PhysRevLett.75.4250There is no corresponding record for this reference.
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3Venables, J.; Spiller, G.; Hanbucken, M. Nucleation and Growth of Thin Films Rep. Prog. Phys. 1984, 47, 399– 459 DOI: 10.1088/0034-4885/47/4/0023https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaL2cXltVWgsbk%253D&md5=667b1964c3b792ce01f041e3b09fef2fNucleation and growth of thin filmsVenables, J. A.; Spiller, G. D. T.; Hanbuecken, M.Reports on Progress in Physics (1984), 47 (4), 399-459CODEN: RPPHAG; ISSN:0034-4885.A review with many refs.
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4Shevchenko, E. V.; Talapin, D. V.; Kotov, N. A.; O’Brien, S.; Murray, C. B. Structural Diversity in Binary Nanoparticle Superlattices Nature 2006, 439, 55– 59 DOI: 10.1038/nature044144https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD28Xht1aqsQ%253D%253D&md5=430839319981045e9982a364f99b3a76Structural diversity in binary nanoparticle superlatticesShevchenko, Elena V.; Talapin, Dmitri V.; Kotov, Nicholas A.; O'Brien, Stephen; Murray, Christopher B.Nature (London, United Kingdom) (2006), 439 (7072), 55-59CODEN: NATUAS; ISSN:0028-0836. (Nature Publishing Group)Assembly of small building blocks such as atoms, mols. and nanoparticles into macroscopic structures-i.e., 'bottom up' assembly-is a theme that runs through chem., biol. and material science. Bacteria, macromols. and nanoparticles can self-assemble, generating ordered structures with a precision that challenges current lithog. techniques. The assembly of nanoparticles of two different materials into a binary nanoparticle superlattice (BNSL) can provide a general and inexpensive path to a large variety of materials (metamaterials) with precisely controlled chem. compn. and tight placement of the components. Maximization of the nanoparticle packing d. is proposed as the driving force for BNSL formation, and only a few BNSL structures were predicted to be thermodynamically stable. Recently, colloidal crystals with micrometre-scale lattice spacings were grown from oppositely charged polymethyl methacrylate spheres. Here the authors demonstrate formation of >15 different BNSL structures, using combinations of semiconducting, metallic and magnetic nanoparticle building blocks. At least ten of these colloidal cryst. structures were not reported previously. Elec. charges on sterically stabilized nanoparticles det. BNSL stoichiometry; addnl. contributions from entropic, van der Waals, steric and dipolar forces stabilize the variety of BNSL structures.
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5Hua, F.; Shi, J.; Lvov, Y.; Cui, T. Patterning of Layer-by-Layer Self-Assembled Multiple Types of Nanoparticle Thin Films by Lithographic Technique Nano Lett. 2002, 2, 1219– 1222 DOI: 10.1021/nl02575215https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD38XntV2ru7o%253D&md5=9d9e2318eaeb5d35370e86a9cc0bc8caPatterning of layer-by-layer self-assembled multiple types of nanoparticle thin films by lithographic techniqueHua, F.; Shi, J.; Lvov, Y.; Cui, T.Nano Letters (2002), 2 (11), 1219-1222CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)A lithog. approach to generate clean patterns of multiple types of nanoparticles on one 4-in. silicon wafer is demonstrated. Each type of nanoparticle is precisely directed to the desired location. The process is mainly based on conventional microelectronic techniques with extremely high reproducibility. This enables the possibility of industrial applications to fabricate devices made of nanocrystals. A thin film of polystyrene spheres, 150 nm in diam., was first coated on the silicon wafer with layer-by-layer self-assembly, followed by a layer of aluminum deposited on the thin film. A layer of pos. photoresist was spun on the surface of aluminum and then patterned by lithog. technique. The unprotected aluminum was removed by wet etching until the polystyrene thin film underneath was exposed to the air. Oxygen plasma was employed to etch the polystyrene thin film all the way to the silicon surface. Subsequently, a thin film of another type of nanoparticle, silica particle 78 nm in diam., was adsorbed onto the surface with layer-by-layer self-assembly. Eventually, aluminum and photoresist were removed and each type of nanoparticle was located next to each other as the pattern was designed. A scanning electron microscope was used to produce the image of the pattern.
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6Rupich, S. M.; Castro, F. C.; Irvine, W. T.; Talapin, D. V. Soft Epitaxy of Nanocrystal Superlattices Nat. Commun. 2014, 5, 5045 DOI: 10.1038/ncomms60456https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXjvFahsb4%253D&md5=ae591f44726838f9147bfdc325bf2f34Soft epitaxy of nanocrystal superlatticesRupich, Sara M.; Castro, Fernando C.; Irvine, William T. M.; Talapin, Dmitri V.Nature Communications (2014), 5 (), 5045CODEN: NCAOBW; ISSN:2041-1723. (Nature Publishing Group)Epitaxial heterostructures with precise registry between crystal layers play a key role in electronics and optoelectronics. In a close analogy, performance of nanocrystal (NC) based devices depends on the perfection of interfaces formed between NC layers. Here we systematically study the epitaxial growth of NC layers for the first time to enable the fabrication of coherent NC layers. NC epitaxy reveals an exceptional strain tolerance. It follows a universal island size scaling behavior and shows a strain-driven transition from layer-by-layer to Stranski-Krastanov growth with non-trivial island height statistics. Kinetic bottlenecks play an important role in NC epitaxy, esp. in the transition from sub-monolayer to multilayer coverage and the epitaxy of NCs with anisotropic shape. These findings provide a foundation for the rational design of epitaxial structures in a fundamentally and practically important size regime between at. and microscopic systems.
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7Tao, A.; Kim, F.; Hess, C.; Goldberger, J.; He, R.; Sun, Y.; Xia, Y.; Yang, P. Langmuir-Blodgett Silver Nanowire Monolayers for Molecular Sensing Using Surface-Enhanced Raman Spectroscopy Nano Lett. 2003, 3, 1229– 1233 DOI: 10.1021/nl03442097https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3sXlvFWmtLg%253D&md5=939168fe46bc097210d7c49be90e6c02Langmuir-Blodgett silver nanowire monolayers for molecular sensing using surface-enhanced Raman spectroscopyTao, Andrea; Kim, Franklin; Hess, Christian; Goldberger, Joshua; He, Rongrui; Sun, Yugang; Xia, Younan; Yang, PeidongNano Letters (2003), 3 (9), 1229-1233CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)Langmuir-Blodgett technique was used to assemble monolayers (with areas over 20 cm2) of aligned silver nanowires that are ∼50 nm in diam. and 2-3 μm in length. These nanowires possess pentagonal cross sections and pyramidal tips. They are close-packed and are aligned parallel to each other. The resulting nanowire monolayers serve as excellent substrates for surface-enhanced Raman spectroscopy (SERS) with large electromagnetic field enhancement factors (2 × 105 for thiol and 2,4-dinitrotoluene, and 2 × 109 for Rhodamine 6G) and can readily be used in ultrasensitive, mol.-specific sensing using vibrational signatures.
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8Kotov, N. A.; Dekany, I.; Fendler, J. H. Layer-by-Layer Self-Assembly of Polyelectrolyte-Semiconductor Nanoparticle Composite Films J. Phys. Chem. 1995, 99, 13065– 13069 DOI: 10.1021/j100035a0058https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaK2MXnsVOjs7s%253D&md5=adf646f10c0f369953e3b92950fd4a61Layer-by-Layer Self-Assembly of Polyelectrolyte-Semiconductor Nanoparticle Composite FilmsKotov, Nicholas A.; Dekany, Imre; Fendler, Janos H.Journal of Physical Chemistry (1995), 99 (35), 13065-9CODEN: JPCHAX; ISSN:0022-3654. (American Chemical Society)Spectroscopic (absorption and emission), microscopic (transmission electron and at. force), X-ray diffraction and photocurrent measurements have provided evidence for the formation of stable ultrathin films with regular periodicities, by the layer-by-layer self-assembly of polycations and cadmium sulfide, lead sulfide and titanium dioxide nanoparticles.
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9Park, S. Y.; Lytton-Jean, A. K.; Lee, B.; Weigand, S.; Schatz, G. C.; Mirkin, C. A. DNA-Programmable Nanoparticle Crystallization Nature 2008, 451, 553– 556 DOI: 10.1038/nature065089https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXhs1ent7g%253D&md5=b5c8c1ab8b7f43d32793560e4869ad2fDNA-programmable nanoparticle crystallizationPark, Sung Yong; Lytton-Jean, Abigail K. R.; Lee, Byeongdu; Weigand, Steven; Schatz, George C.; Mirkin, Chad A.Nature (London, United Kingdom) (2008), 451 (7178), 553-556CODEN: NATUAS; ISSN:0028-0836. (Nature Publishing Group)It was first shown more than ten years ago that DNA oligonucleotides can be attached to gold nanoparticles rationally to direct the formation of larger assemblies. Since then, oligonucleotide-functionalized nanoparticles have been developed into powerful diagnostic tools for nucleic acids and proteins, and into intracellular probess and gene regulators. In contrast, the conceptually simple yet powerful idea that functionalized nanoparticles might serve as basic building blocks that can be rationally assembled through programmable base-pairing interactions into highly ordered macroscopic materials remains poorly developed. So far, the approach has mainly resulted in polymn., with modest control over the placement of, the periodicity in, and the distance between particles within the assembled material. That is, most of the materials obtained thus far are best classified as amorphous polymers, although a few examples of colloidal crystal formation exist. Here, we demonstrate that DNA can be used to control the crystn. of nanoparticle-oligonucleotide conjugates to the extent that different DNA sequences guide the assembly of the same type of inorg. nanoparticle into different cryst. states. We show that the choice of DNA sequences attached to the nanoparticle building blocks, the DNA linking mols. and the absence or presence of a non-bonding single-base flexor can be adjusted so that gold nanoparticles assemble into micrometer-sized face-centered-cubic or body-centered-cubic crystal structures. Our findings thus clearly demonstrate that synthetically programmable colloidal crystn. is possible, and that a single-component system can be directed to form different structures.
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10Macfarlane, R. J.; Lee, B.; Jones, M. R.; Harris, N.; Schatz, G. C.; Mirkin, C. A. Nanoparticle Superlattice Engineering with DNA Science 2011, 334, 204– 208 DOI: 10.1126/science.121049310https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3MXht1yksbbK&md5=e5902f70c851a5177d4e3b9a28dfbe62Nanoparticle Superlattice Engineering with DNAMacFarlane, Robert J.; Lee, Byeongdu; Jones, Matthew R.; Harris, Nadine; Schatz, George C.; Mirkin, Chad A.Science (Washington, DC, United States) (2011), 334 (6053), 204-208CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)A current limitation in nanoparticle superlattice engineering is that the identities of the particles being assembled often det. the structures that can be synthesized. Therefore, specific crystallog. symmetries or lattice parameters can only be achieved using specific nanoparticles as building blocks (and vice versa). The authors present six design rules that can be used to deliberately prep. nine distinct colloidal crystal structures, with control over lattice parameters on the 25- to 150-nm length scale. These design rules outline a strategy to independently adjust each of the relevant crystallog. parameters, including particle size (5 to 60 nm), periodicity, and interparticle distance. As such, this work represents an advance in synthesizing tailorable macroscale architectures comprising nanoscale materials in a predictable fashion.
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11O’Brien, M. N.; Jones, M. R.; Lee, B.; Mirkin, C. A. Anisotropic Nanoparticle Complementarity in DNA-Mediated Co-Crystallization Nat. Mater. 2015, 14, 833– 839 DOI: 10.1038/nmat429311https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXhtFeju7jP&md5=8315fd6e146a45ddc2dd3b93458458c2Anisotropic nanoparticle complementarity in DNA-mediated co-crystallizationO'Brien, Matthew N.; Jones, Matthew R.; Lee, Byeongdu; Mirkin, Chad A.Nature Materials (2015), 14 (8), 833-839CODEN: NMAACR; ISSN:1476-1122. (Nature Publishing Group)By using DNA as a surface ligand, mixts. of two different anisotropic nanoparticles were selectively cocrystd., and the effects of nanoparticle size and shape complementarity on the resultant crystal symmetry, microstrain, and effective 'DNA bond' length and strength were investigated. These results were used to understand a more complicated system where both size and shape complementarity change, and where one nanoparticle can participate in multiple types of directional interactions. These findings offer improved control of non-spherical nanoparticles as building blocks for the assembly of sophisticated macroscopic materials, and provide a framework to understand complementarity and directional interactions in DNA-mediated nanoparticle crystn.
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12Senesi, A. J.; Eichelsdoerfer, D. J.; Macfarlane, R. J.; Jones, M. R.; Auyeung, E.; Lee, B.; Mirkin, C. A. Stepwise Evolution of DNA-Programmable Nanoparticle Superlattices Angew. Chem., Int. Ed. 2013, 52, 6624– 6628 DOI: 10.1002/anie.20130193612https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXnvVOitLs%253D&md5=674aaf5fbc8ab183e0420cc85da10081Stepwise Evolution of DNA-Programmable Nanoparticle SuperlatticesSenesi, Andrew J.; Eichelsdoerfer, Daniel J.; Macfarlane, Robert J.; Jones, Matthew R.; Auyeung, Evelyn; Lee, Byeongdu; Mirkin, Chad A.Angewandte Chemie, International Edition (2013), 52 (26), 6624-6628CODEN: ACIEF5; ISSN:1433-7851. (Wiley-VCH Verlag GmbH & Co. KGaA)The authors use a stepwise growth process to systematically study and control the evolution of a bcc. cryst. thin-film comprised of nanoparticle building blocks functionalized with DNA on a complementary DNA substrate. The authors examine crystal growth as a function of temp., no. of layers, and substrate-particle bonding interactions. Importantly, the judicious choice of DNA interconnects allows one to tune the interfacial energy between various crystal planes and the substrate, and thereby control crystal orientation and size in a stepwise fashion using chem. programmable attractive forces.
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13Hellstrom, S. L.; Kim, Y.; Fakonas, J. S.; Senesi, A. J.; Macfarlane, R. J.; Mirkin, C. A.; Atwater, H. A. Epitaxial Growth of DNA-Assembled Nanoparticle Superlattices on Patterned Substrates Nano Lett. 2013, 13, 6084– 6090 DOI: 10.1021/nl403365413https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXhslersLzM&md5=9ac1c19af28af91f2cfba569fec1f738Epitaxial Growth of DNA-Assembled Nanoparticle Superlattices on Patterned SubstratesHellstrom, Sondra L.; Kim, Youngeun; Fakonas, James S.; Senesi, Andrew J.; MacFarlane, Robert J.; Mirkin, Chad A.; Atwater, Harry A.Nano Letters (2013), 13 (12), 6084-6090CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)Arrays of DNA-functionalized gold nanoparticles have been grown epitaxially on lithog. patterned templates, eliminating grain boundaries and enabling fine control over orientation and size of assemblies up to thousands of square micrometers. This epitaxial growth allowed for orientational control, systematic introduction of strain, and designed defects, which extend the range of structures that can be made using superlattice assembly.
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14Lalander, C. H.; Zheng, Y.; Dhuey, S.; Cabrini, S.; Bach, U. DNA-Directed Self-Assembly of Gold Nanoparticles onto Nanopatterned Surfaces: Controlled Placement of Individual Nanoparticles into Regular Arrays ACS Nano 2010, 4, 6153– 6161 DOI: 10.1021/nn101431k14https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3cXht1KhsLnK&md5=7cc8b84ceb08868fdbc94ffb6794af52DNA-Directed Self-Assembly of Gold Nanoparticles onto Nanopatterned Surfaces: Controlled Placement of Individual Nanoparticles into Regular ArraysLalander, Cecilia H.; Zheng, Yuanhui; Dhuey, Scott; Cabrini, Stefano; Bach, UdoACS Nano (2010), 4 (10), 6153-6161CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)A method for the templated DNA-directed self-assembly of individual gold nanoparticles (AuNPs) into discrete nanostructures is described. The templating nanostructures consisted of a linear configuration of six metal dots with a center-to-center dot distance of 55 nm, fabricated by electron beam lithog. The 40 nm DNA-capped AuNPs were immobilized onto this templating nanostructure to produce a linear configuration of six adjacent AuNPs. The geometry of the templating nanostructure is critically important for the successful direction of a single nanoparticle onto individual adsorption sites. For optimized template structures the immobilization efficiency of nanoparticles onto the individual adsorption sites is 80%. The nonspecific assocn. of nanoparticles with specifically adsorbed nanoparticles and the between adsorption of nanoparticles, bridging two individual adsorption sites, were the two main defects obsd. in the immobilized assemblies. Less than 1% of all surface confined AuNPs adsorbed nonspecifically in the areas between the self-assembled regular arrays.
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15Macfarlane, R. J.; Thaner, R. V.; Brown, K. A.; Zhang, J.; Lee, B.; Nguyen, S. T.; Mirkin, C. A. Importance of the DNA “Bond” in Programmable Nanoparticle Crystallization Proc. Natl. Acad. Sci. U. S. A. 2014, 111, 14995– 15000 DOI: 10.1073/pnas.141648911115https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhslajurjO&md5=79f2b5051b7234646f29404a0fbb4547Importance of the DNA "bond" in programmable nanoparticle crystallizationMacFarlane, Robert J.; Thaner, Ryan V.; Brown, Keith A.; Zhang, Jian; Lee, Byeongdu; Nguyen, Son Binh T.; Mirkin, Chad A.Proceedings of the National Academy of Sciences of the United States of America (2014), 111 (42), 14995-15000CODEN: PNASA6; ISSN:0027-8424. (National Academy of Sciences)If a soln. of DNA-coated nanoparticles is allowed to crystallize, the thermodn. structure can be predicted by a set of structural design rules analogous to Pauling's rules for ionic crystn. The details of the crystn. process, however, have proved more difficult to characterize as they depend on a complex interplay of many factors. Here, we report that this crystn. process is dictated by the individual DNA bonds and that the effect of changing structural or environmental conditions can be understood by considering the effect of these parameters on free oligonucleotides. Specifically, we obsd. the reorganization of nanoparticle superlattices using time-resolved synchrotron small-angle x-ray scattering in systems with different DNA sequences, salt concns., and densities of DNA linkers on the surface of the nanoparticles. The agreement between bulk crystn. and the behavior of free oligonucleotides may bear important consequences for constructing novel classes of crystals and incorporating new interparticle bonds in a rational manner.
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16Zhang, C.; Macfarlane, R. J.; Young, K. L.; Choi, C. H. J.; Hao, L.; Auyeung, E.; Liu, G.; Zhou, X.; Mirkin, C. A. A General Approach to DNA-Programmable Atom Equivalents Nat. Mater. 2013, 12, 741– 746 DOI: 10.1038/nmat364716https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXnvVSisrc%253D&md5=6c0d26f8c854030efb166a5198e0033aA general approach to DNA-programmable atom equivalentsZhang, Chuan; MacFarlane, Robert J.; Young, Kaylie L.; Choi, Chung Hang J.; Hao, Liangliang; Auyeung, Evelyn; Liu, Guoliang; Zhou, Xiaozhu; Mirkin, Chad A.Nature Materials (2013), 12 (8), 741-746CODEN: NMAACR; ISSN:1476-1122. (Nature Publishing Group)Nanoparticles can be combined with nucleic acids to program the formation of three-dimensional colloidal crystals where the particles' size, shape, compn. and position can be independently controlled. However, the diversity of the types of material that can be used is limited by the lack of a general method for prepg. the basic DNA-functionalized building blocks needed to bond nanoparticles of different chem. compns. into lattices in a controllable manner. By coating nanoparticles protected with aliph. ligands with an azide-bearing amphiphilic polymer, followed by the coupling of DNA to the polymer using strain-promoted azide-alkyne cycloaddn. (also known as copper-free azide-alkyne click chem.), nanoparticles bearing a high-d. shell of nucleic acids can be created regardless of nanoparticle compn. This method provides a route to a virtually endless class of programmable atom equiv. for DNA-based colloidal crystn.
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17Zhang, Y.; Lu, F.; Yager, K. G.; van der Lelie, D.; Gang, O. A General Strategy for the DNA-Mediated Self-Assembly of Functional Nanoparticles into Heterogeneous Systems Nat. Nanotechnol. 2013, 8, 865– 872 DOI: 10.1038/nnano.2013.20917https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXhs1ChsrrP&md5=e403c85b29f0525227164c548be3d3ffA general strategy for the DNA-mediated self-assembly of functional nanoparticles into heterogeneous systemsZhang, Yugang; Lu, Fang; Yager, Kevin G.; van der Lelie, Daniel; Gang, OlegNature Nanotechnology (2013), 8 (11), 865-872CODEN: NNAABX; ISSN:1748-3387. (Nature Publishing Group)Nanoparticles coated with DNA mols. can be programmed to self-assemble into three-dimensional superlattices. Such superlattices can be made from nanoparticles with different functionalities and could potentially exploit the synergetic properties of the nanoscale components. However, the approach has so far been used primarily with single-component systems. Here, the authors report a general strategy for the creation of heterogeneous nanoparticle superlattices using DNA and carboxylic-based conjugation. Nanoparticles with all major types of functionality-plasmonic (gold), magnetic (Fe2O3), catalytic (palladium) and luminescent (CdSe/Te@ZnS and CdS@ZnS)-can be incorporated into binary systems in a rational manner. The authors also examine the effect of nanoparticle characteristics (including size, shape, no. of DNA per particle and DNA flexibility) on the phase behavior of the heterosystems, and demonstrate that the assembled materials can have novel optical and field-responsive properties.
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18Lee, J.-S.; Lytton-Jean, A. K.; Hurst, S. J.; Mirkin, C. A. Silver Nanoparticle-Oligonucleotide Conjugates Based on DNA with Triple Cyclic Disulfide Moieties Nano Lett. 2007, 7, 2112– 2115 DOI: 10.1021/nl071108g18https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXmsV2ltbc%253D&md5=2df3f75517d010058d7127788753dd69Silver Nanoparticle-Oligonucleotide Conjugates Based on DNA with Triple Cyclic Disulfide MoietiesLee, Jae-Seung; Lytton-Jean, Abigail K. R.; Hurst, Sarah J.; Mirkin, Chad A.Nano Letters (2007), 7 (7), 2112-2115CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)The authors report a new strategy for prepg. silver nanoparticle-oligonucleotide conjugates that are based upon DNA with cyclic disulfide-anchoring groups. These particles are extremely stable and can withstand NaCl concns. up to 1.0 M. When silver nanoparticles functionalized with complementary sequences are combined, they assemble to form DNA-linked nanoparticle networks. This assembly process is reversible with heating and is assocd. with a red shifting of the particle surface plasmon resonance and a concomitant color change from yellow to pale red. Analogous to the oligonucleotide-functionalized gold nanoparticles, these particles also exhibit highly cooperative binding properties with extremely sharp melting transitions. This work is an important step toward using silver nanoparticle-oligonucleotide conjugates for a variety of purposes, including mol. diagnostic labels, synthons in programmable materials synthesis approaches, and functional components for nanoelectronic and plasmonic devices.
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19Brodin, J. D.; Auyeung, E.; Mirkin, C. A. DNA-Mediated Engineering of Multicomponent Enzyme Crystals Proc. Natl. Acad. Sci. U. S. A. 2015, 112, 4564– 4569 DOI: 10.1073/pnas.150353311219https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXkvFejs7o%253D&md5=681d247aaedba6b20d9fae1ad94e6f44DNA-mediated engineering of multicomponent enzyme crystalsBrodin, Jeffrey D.; Auyeung, Evelyn; Mirkin, Chad A.Proceedings of the National Academy of Sciences of the United States of America (2015), 112 (15), 4564-4569CODEN: PNASA6; ISSN:0027-8424. (National Academy of Sciences)The ability to predictably control the coassembly of multiple nanoscale building blocks, esp. those with disparate chem. and phys. properties such as biomols. and inorg. nanoparticles, has far-reaching implications in catalysis, sensing, and photonics, but a generalizable strategy for engineering specific contacts between these particles is an outstanding challenge. This is esp. true in the case of proteins, where the types of possible interparticle interactions are numerous, diverse, and complex. Herein, the authors explore the concept of trading protein-protein interactions for DNA-DNA interactions to direct the assembly of two nucleic-acid-functionalized proteins with distinct surface chemistries into six unique lattices composed of catalytically active proteins, or of a combination of proteins and DNA-modified gold nanoparticles. The programmable nature of DNA-DNA interactions used in this strategy allows the authors to control the lattice symmetries and unit cell consts., as well as the compns. and habit, of the resulting crystals. This study provides a potentially generalizable strategy for constructing a unique class of materials that take advantage of the diverse morphologies, surface chemistries, and functionalities of proteins for assembling functional cryst. materials.
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20Evanoff, D. D.; Chumanov, G. Synthesis and Optical Properties of Silver Nanoparticles and Arrays ChemPhysChem 2005, 6, 1221– 1231 DOI: 10.1002/cphc.20050011320https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2MXmsVKgtb8%253D&md5=4a805855aead6232bb364c5e05a49e8fSynthesis and optical properties of silver nanoparticles and arraysEvanoff, David D., Jr.; Chumanov, GeorgeChemPhysChem (2005), 6 (7), 1221-1231CODEN: CPCHFT; ISSN:1439-4235. (Wiley-VCH Verlag GmbH & Co. KGaA)A review. This Minireview systematically examines optical properties of Ag nanoparticles as a function of size. Extinction, scattering, and absorption cross sections and distance dependence of the local electromagnetic field, as well as the quadrupolar coupling of 2-dimensional assemblies of such particles are exptl. measured for a wide range of particle sizes. Such measurements were possible because of the development of a novel synthetic method for the size-controlled synthesis of chem. clean, highly cryst. Ag nanoparticles of narrow size distribution. The method and its unique advantages are compared to other methods for synthesis of metal nanoparticles. Synthesis and properties of nanocomposite materials using these and other nanoparticles are also described. Important highlights in the history of the field of metal nanoparticles as well as an examn. of the basic principles of plasmon resonances are included.
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21Kelly, K. L.; Coronado, E.; Zhao, L. L.; Schatz, G. C. The Optical Properties of Metal Nanoparticles: The Influence of Size, Shape, and Dielectric Environment J. Phys. Chem. B 2003, 107, 668– 677 DOI: 10.1021/jp026731y21https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD38Xps1Ghur0%253D&md5=f7be29b07a5f0d8311d7f0042f359274The Optical Properties of Metal Nanoparticles: The Influence of Size, Shape, and Dielectric EnvironmentKelly, K. Lance; Coronado, Eduardo; Zhao, Lin Lin; Schatz, George C.Journal of Physical Chemistry B (2003), 107 (3), 668-677CODEN: JPCBFK; ISSN:1520-6106. (American Chemical Society)The optical properties of metal nanoparticles have long been of interest in phys. chem., starting with Faraday's studies of colloidal Au in the middle 1800s. More recently, new lithog. techniques as well as improvements to classical wet chem. methods have made it possible to synthesize noble metal nanoparticles with a wide range of sizes, shapes, and dielec. environments. In this feature article, the authors describe recent progress in the theory of nanoparticle optical properties, particularly methods for solving Maxwell's equations for light scattering from particles of arbitrary shape in a complex environment. Included is a description of the qual. features of dipole and quadrupole plasmon resonances for spherical particles; a discussion of anal. and numerical methods for calcg. extinction and scattering cross sections, local fields, and other optical properties for nonspherical particles; and a survey of applications to problems of recent interest involving triangular Ag particles and related shapes.
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22Storhoff, J. J.; Lazarides, A. A.; Mucic, R. C.; Mirkin, C. A.; Letsinger, R. L.; Schatz, G. C. What Controls the Optical Properties of DNA-Linked Gold Nanoparticle Assemblies? J. Am. Chem. Soc. 2000, 122, 4640– 4650 DOI: 10.1021/ja993825l22https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3cXis1GntbY%253D&md5=c62e6e197b0b08079c1f4483230503a7What Controls the Optical Properties of DNA-Linked Gold Nanoparticle Assemblies?Storhoff, James J.; Lazarides, Anne A.; Mucic, Robert C.; Mirkin, Chad A.; Letsinger, Robert L.; Schatz, George C.Journal of the American Chemical Society (2000), 122 (19), 4640-4650CODEN: JACSAT; ISSN:0002-7863. (American Chemical Society)A study aimed at understanding the factors that control the optical properties of DNA-linked gold nanoparticle aggregates contg. oligonucleotide linkers of varying length (24-72 base pairs) is described. In this system, ∼15 nm diam. Au particles modified with (alkanethiol)-12 base oligomers are hybridized to a series of oligonucleotide linkers ranging from 24 to 72 base pairs (∼80-240 Å) in length. Aggregated at room temp., the various macroscopic nanoparticle assemblies have plasmon frequency changes that are inversely dependent on the oligonucleotide linker length. Upon annealing at temps. close to the melting temp. of the DNA, the optical properties of the DNA-linked assemblies contg. the longer linkers (48 and 72 base pairs) red-shift until they are similar to the assemblies contg. the shorter linkers (24 base pairs). The pre- and post-annealed DNA-linked assemblies were characterized by sedimentation rate, transmission electron microscopy, dynamic light scattering, and UV-vis spectroscopy which show that the oligonucleotide linker length kinetically controls the size of the aggregates that are formed under the pre-annealed conditions, thereby controlling the optical properties. Through the use of small-angle X-ray scattering and electrodynamic modeling in conjunction with the techniques mentioned above, we have detd. that the temp.-dependent optical changes obsd. upon annealing of the aggregates contg. the longer oligonucleotides (48 and 72 base pairs) can be attributed to aggregate growth through an "Ostwald ripening" mechanism (where larger aggregates grow at the expense of smaller aggregates). This type of aggregate growth leads to the red-shift in plasmon frequency obsd. for the aggregates. Significantly, these expts. provide evidence that the optical properties of these DNA-linked nanoparticle assemblies are governed by aggregate size, regardless of oligonucleotide linker length, which has important implications for the development of colorimetric detection methods based on these nanoparticle materials.
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23Choi, J.-H.; Wang, H.; Oh, S. J.; Paik, T.; Sung, P.; Sung, J.; Ye, X.; Zhao, T.; Diroll, B. T.; Murray, C. B. Exploiting the Colloidal Nanocrystal Library to Construct Electronic Devices Science 2016, 352, 205– 208 DOI: 10.1126/science.aad037123https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XlsFSmtbg%253D&md5=37a791816e5a2a43bc6d6070cd0533c8Exploiting the colloidal nanocrystal library to construct electronic devicesChoi, Ji-Hyuk; Wang, Han; Oh, Soong Ju; Paik, Taejong; Sung, Pil; Sung, Jinwoo; Ye, Xingchen; Zhao, Tianshuo; Diroll, Benjamin T.; Murray, Christopher B.; Kagan, Cherie R.Science (Washington, DC, United States) (2016), 352 (6282), 205-208CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)Synthetic methods produce libraries of colloidal nanocrystals with tunable phys. properties by tailoring the nanocrystal size, shape, and compn. Here, the authors exploit colloidal nanocrystal diversity and design the materials, interfaces, and processes to construct all-nanocrystal electronic devices using soln.-based processes. Metallic silver and semiconducting cadmium selenide nanocrystals are deposited to form high-cond. and high-mobility thin-film electrodes and channel layers of field-effect transistors. Insulating aluminum oxide nanocrystals are assembled layer by layer with polyelectrolytes to form high-dielec. const. gate insulator layers for low-voltage device operation. Metallic indium nanocrystals are codispersed with silver nanocrystals to integrate an indium supply in the deposited electrodes that serves to passivate and dope the cadmium selenide nanocrystal channel layer. The authors fabricate all-nanocrystal field-effect transistors on flexible plastics with electron mobilities of 21.7 square centimeters per V-second.
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24Jonsson, P. E. Superparamagnetism and Spin Glass Dynamics of Interacting Magnetic Nanoparticle Systems Adv. Chem. Phys. 2003, 128, 191– 248 DOI: 10.1002/0471484237.ch3There is no corresponding record for this reference.
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25Li, T.; Senesi, A. J.; Lee, B. Small Angle X-Ray Scattering for Nanoparticle Research Chem. Rev. 2016, 116, 11128 DOI: 10.1021/acs.chemrev.5b0069025https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XlsF2qsrw%253D&md5=659565f88b80ce6994bb98c07f034eb2Small Angle X-ray Scattering for Nanoparticle ResearchLi, Tao; Senesi, Andrew J.; Lee, ByeongduChemical Reviews (Washington, DC, United States) (2016), 116 (18), 11128-11180CODEN: CHREAY; ISSN:0009-2665. (American Chemical Society)X-ray scattering is a structural characterization tool that has impacted diverse fields of study. It is unique in its ability to examine materials in real time and under realistic sample environments, enabling researchers to understand morphol. at nanometer and angstrom length scales using complementary small and wide angle X-ray scattering (SAXS, WAXS), resp. Herein, we focus on the use of SAXS to examine nanoscale particulate systems. We provide a theor. foundation for X-ray scattering, considering both form factor and structure factor, as well as the use of correlation functions, which may be used to det. a particle's size, size distribution, shape, and organization into hierarchical structures. The theory is expanded upon with contemporary use cases. Both transmission and reflection (grazing incidence) geometries are addressed, as well as the combination of SAXS with other X-ray and non-X-ray characterization tools. We conclude with an examn. of several key areas of research where X-ray scattering has played a pivotal role, including in situ nanoparticle synthesis, nanoparticle assembly, and operando studies of catalysts and energy storage materials. Throughout this review we highlight the unique capabilities of X-ray scattering for structural characterization of materials in their native environment.
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26Meyers, S. T.; Anderson, J. T.; Hung, C. M.; Thompson, J.; Wager, J. F.; Keszler, D. A. Aqueous Inorganic Inks for Low-Temperature Fabrication of ZnO TFTs J. Am. Chem. Soc. 2008, 130, 17603– 17609 DOI: 10.1021/ja808243k26https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXhsVOjsLbM&md5=aa4a4cd305f8cf5ca4496836f5efb6eeAqueous Inorganic Inks for Low-Temperature Fabrication of ZnO TFTsMeyers, Stephen T.; Anderson, Jeremy T.; Hung, Celia M.; Thompson, John; Wager, John F.; Keszler, Douglas A.Journal of the American Chemical Society (2008), 130 (51), 17603-17609CODEN: JACSAT; ISSN:0002-7863. (American Chemical Society)A simple, low-cost, and nontoxic aq. ink chem. is described for digital printing of ZnO films. Selective design through controlled pptn., purifn., and dissoln. affords an aq. Zn(OH)x(NH3)y(2-x)+ soln. that is stable in storage, yet promptly decomps. at temps. <150° to form wurtzite ZnO. Dense, high-quality, polycryst. ZnO films are deposited by ink-jet printing and spin-coating, and film structure is elucidated via x-ray diffraction and electron microscopy. Semiconductor film functionality and quality were examd. through integration in bottom-gate thin-film transistors. Enhancement-mode TFTs with ink-jet printed ZnO channels annealed at 300° exhibit strong field effect and excellent current satn. in tandem with incremental mobilities from 4-6 cm2 V-1 s-1. Spin-coated ZnO semiconductors processed at 150° are integrated with soln.-deposited aluminum oxide phosphate dielecs. in functional transistors, demonstrating both high performance, i.e., mobilities up to 1.8 cm2 V-1 s-1, and the potential for low-temp. soln. processing of all-oxide electronics.
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27Seo, S. E.; Wang, M. X.; Shade, C. M.; Rouge, J. L.; Brown, K. A.; Mirkin, C. A. Modulating the Bond Strength of DNA–Nanoparticle Superlattices ACS Nano 2016, 10, 1771– 1779 DOI: 10.1021/acsnano.5b0710327https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhtVGgsrY%253D&md5=328033b90f7c203f49f7667cb9bd7466Modulating the Bond Strength of DNA-Nanoparticle SuperlatticesSeo, Soyoung E.; Wang, Mary X.; Shade, Chad M.; Rouge, Jessica L.; Brown, Keith A.; Mirkin, Chad A.ACS Nano (2016), 10 (2), 1771-1779CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)A method for modulating the bond strength in DNA-programmable nanoparticle (NP) superlattice crystals utilizes noncovalent interactions between a family of [Ru(dipyrido[2,3-a:3',2'-c]phenazine)(N-N)2]2+-based small mol. intercalators and DNA duplexes to postsynthetically modify DNA-NP superlattices. This increases the strength of the DNA bonds that hold the nanoparticles together, making the superlattices more resistant to thermal degrdn. The authors investigate the relationship between the structure of the intercalator and its binding affinity for DNA duplexes and det. how this translates to the increased thermal stability of the intercalated superlattices. The authors find that intercalator charge and steric profile give us a wide range of tunability and control over DNA-NP bond strength, with the resulting crystal lattices retaining their structure at temps. greater than 50°C above nonintercalated structures. This allows the authors to subject DNA-NP superlattice crystals to conditions under which they would normally melt, enabling the construction of a core-shell (gold NP-quantum dot NP) superlattice crystal.
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28Pal, S.; Zhang, Y.; Kumar, S. K.; Gang, O. Dynamic Tuning of DNA-Nanoparticle Superlattices by Molecular Intercalation of Double Helix J. Am. Chem. Soc. 2015, 137, 4030– 4033 DOI: 10.1021/ja512799d28https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXktVGksro%253D&md5=97bcbd513a7426d143786a5a98b65a46Dynamic tuning of DNA-nanoparticle superlattices by molecular intercalation of double helixPal, Suchetan; Zhang, Yugang; Kumar, Sanat K.; Gang, OlegJournal of the American Chemical Society (2015), 137 (12), 4030-4033CODEN: JACSAT; ISSN:0002-7863. (American Chemical Society)Nanoparticle (NP) assembly using DNA recognition has emerged as a powerful tool for the fabrication of 3D superlattices. In addn. to the vast structural diversity, this approach provides an avenue for dynamic 3D NP assembly, which is promising for the modulation of interparticle distances and, hence, for example, for in situ tuning of optical properties. While several approaches have been explored for changing NP sepns. in the lattices using responsiveness of single-stranded DNA (ss-DNA), far less work has been done for the manipulation of most abundant double-stranded DNA (ds-DNA) motifs. Here, we present a novel strategy for modulation of interparticle distances in DNA linked 3D self-assembled NP lattices by mol. intercalator. We utilize ethidium bromide (EtBr) as a model intercalator to demonstrate selective and isotropic lattice expansion for three superlattice types (bcc, fcc, and AlB2) due to the intercalation of ds-DNA linking NPs. We further show the reversibility of the lattice parameter using n-butanol as a retrieving agent as well as an increased lattice thermal stability by 12-14 °C due to the inclusion of EtBr. The proposed intercalator-based strategy permits the creation of reconfigurable and thermally stable superlattices, which could lead to tunable and functionally responsive materials.
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29Shade, C. M.; Kennedy, R. D.; Rouge, J. L.; Rosen, M. S.; Wang, M. X.; Seo, S. E.; Clingerman, D. J.; Mirkin, C. A. Duplex-Selective Ruthenium-Based DNA Intercalators Chem. - Eur. J. 2015, 21, 10983– 10987 DOI: 10.1002/chem.20150209529https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXhtVOlsrrN&md5=d13f15beca0381da6af91821e35e96b9Duplex-Selective Ruthenium-Based DNA IntercalatorsShade, Chad M.; Kennedy, Robert D.; Rouge, Jessica L.; Rosen, Mari S.; Wang, Mary X.; Seo, Soyoung E.; Clingerman, Daniel J.; Mirkin, Chad A.Chemistry - A European Journal (2015), 21 (31), 10983-10987CODEN: CEUJED; ISSN:0947-6539. (Wiley-VCH Verlag GmbH & Co. KGaA)We report the design and synthesis of small mols. that exhibit enhanced luminescence in the presence of duplex rather than single-stranded DNA. The local environment presented by a well-known [Ru(dipyrido[3,2-a:2',3'-c]phenazine)L2]2+-based DNA intercalator was modified by functionalizing the bipyridine ligands with esters and carboxylic acids. By systematically varying the no. and charge of the pendant groups, it was detd. that decreasing the electrostatic interaction between the intercalator and the anionic DNA backbone reduced single-strand interactions and translated to better duplex specificity. In studying this class of complexes, a single RuII complex emerged that selectively luminesces in the presence of duplex DNA with little to no background from interacting with single-stranded DNA. This complex shows promise as a new dye capable of selectively staining double- vs. single-stranded DNA in gel electrophoresis, which cannot be done with conventional SYBR dyes.
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30Auyeung, E.; Macfarlane, R. J.; Choi, C. H. J.; Cutler, J. I.; Mirkin, C. A. Transitioning DNA-Engineered Nanoparticle Superlattices from Solution to the Solid State Adv. Mater. 2012, 24, 5181– 5186 DOI: 10.1002/adma.20120206930https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC38XhtVGgt77L&md5=683eb55258a822fea064ac10d21f4be9Transitioning DNA-Engineered Nanoparticle Superlattices from Solution to the Solid StateAuyeung, Evelyn; MacFarlane, Robert J.; Choi, Chung Hang J.; Cutler, Joshua I.; Mirkin, Chad A.Advanced Materials (Weinheim, Germany) (2012), 24 (38), 5181-5186, S5181/1-S5181/12CODEN: ADVMEW; ISSN:0935-9648. (Wiley-VCH Verlag GmbH & Co. KGaA)The authors report a method for stabilizing DNA-assembled three-dimensional superlattices in the solid state by silica encapsulation, where both the symmetries and lattice spacings of the soln.-phase lattices are preserved. Once encapsulated, superlattice morphologies are no longer dictated by DNA interactions, and as such remain stable against distortion, collapse, or dissocn. under many previously inaccessible conditions.
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Supporting Information
Supporting Information
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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.6b06584.
Oligonucleotide sequences, FIB-SEM and SAXS analysis, and additional figures and tables (PDF)
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