Herein, we investigate the use of proteins with tunable DNA modification distributions to modulate nanoparticle superlattice structure. Using beta-galactosidase (βgal) as a model system, we have employed the orthogonal chemical reactivities of surface amines and thiols to synthesize protein-DNA conjugates with 36 evenly distributed or 8 specifically positioned oligonucleotides. When these are assembled into crystalline superlattices with gold nanoparticles, we find that the distribution of DNA modifications modulates the favored structure: βgal with uniformly distributed DNA bonding elements results in body-centered cubic crystals, whereas DNA functionalization of cysteines results in AB packing. We probe the role of protein oligonucleotide number and conjugate size on this observation, which revealed the importance of oligonucleotide distribution in this observed assembly behavior. These results indicate that proteins with defined DNA modification patterns are powerful tools for controlling nanoparticle superlattices architecture, and establish the importance of oligonucleotide distribution in the assembly behavior of protein-DNA conjugates.
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http://dx.doi.org/10.1021/jacs.6b11893 | DOI Listing |
Phys Chem Chem Phys
January 2025
College of Materials and Textile Engineering, Jiaxing University, Jiaxing 314001, China.
Programmable organization of uniform organic/inorganic functional building blocks into large-scale ordered superlattices has attracted considerable attention since the bottom-up self-organization strategy opens up a robust and universal route for designing novel and multifunctional materials with advanced applications in memory storage devices, catalysis, photonic crystals, and biotherapy. Despite making great efforts in the construction of superlattice materials, there still remains a challenge in the preparation of organic/inorganic hybrid superlattices with tunable dimensions and exotic configurations. Here, we report the spontaneous self-organization of polystyrene-tethered gold nanoparticles (AuNPs@PS) into freestanding organic/inorganic hybrid superlattices templated at the diethylene glycol-air interface.
View Article and Find Full Text PDFNano Lett
January 2025
State Key Laboratory of Solidification Processing, Center of Advanced Lubrication and Seal Materials, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi'an 710072, P.R. China.
Plasmonic superlattices enable the precise manipulation of electromagnetic fields at the nanoscale. However, the optical properties of static lattices are dictated by their geometry and cannot be reconfigured. Here, we present a surface-interface engineered plasmonic superlattice with confined polyelectrolyte-functionalized metal-organic framework (MOF) hybrid layers to tune plasmon resonance for ultrafast chemical sensing.
View Article and Find Full Text PDFNano Lett
January 2025
University of Science & Technology of China, Hefei, Anhui 230026, China.
Metallic oxide can induce localized surface plasmon resonance (LSPR) through creating vacancies, which effectively achieve high carrier concentrations and offer advantages such as versatility and tunability. However, vacancies are typically created by altering the stoichiometric ratio of elements through doping, and it is challenging to achieve LSPR enhancement in the visible spectral range. Here, we have assembled CuO-superlattices to induce a high concentration of oxygen vacancies, resulting in LSPR within the visible spectrum.
View Article and Find Full Text PDFSoft Matter
January 2025
Department of Nuclear and Quantum Engineering, Korea Advanced Institute of Science and Technology, Daejeon, 34141, Republic of Korea.
Synthesizing nanoparticle superlattices (NPSLs) with different symmetries is of great interest due to their impact on the collective emergent properties and potential applications. While several parameters have been identified as determinants for forming different symmetries of NPSLs, the high core dispersity, softness, and ligand interpenetration were proposed to drive the formation of the C14 Frank-Kasper (C14) structure like MgZn-type. Here, we report that the C14 phase can be formed in highly monodisperse one-size spherical nanoparticles (NPs) by controlling the interplay among their softness and ligand grafting density.
View Article and Find Full Text PDFNano Lett
December 2024
Department of Nuclear and Quantum Engineering, Korea Advanced Institute of Science and Technology, Daejeon, 34141, Republic of Korea.
Interparticle ligand exchange can occur during the formation of nanoparticle superlattices (NPSLs), affecting the symmetry of the NPSLs. Here, we report time-resolved small-angle neutron scattering (TR-SANS) measurements of the interparticle exchange kinetics of thiolate ligands among gold nanoparticles (AuNPs) at different temperatures. To track the ligand exchange among AuNPs, two groups of AuNPs were functionalized with hydrogenated and deuterated dodecanethiol, respectively, and then mixed in a solvent mixture of toluene and deuterated toluene for shell contrast.
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