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  1. Article ; Online: Colorimetric quantification of linking in thermoreversible nanocrystal gel assemblies.

    Kang, Jiho / Valenzuela, Stephanie A / Lin, Emily Y / Dominguez, Manuel N / Sherman, Zachary M / Truskett, Thomas M / Anslyn, Eric V / Milliron, Delia J

    Science advances

    2022  Volume 8, Issue 7, Page(s) eabm7364

    Abstract: Nanocrystal gels can be responsive, tunable materials, but designing their structure and properties is challenging. By using reversibly bonded molecular linkers, gelation can be realized under conditions predicted by thermodynamics. However, simulations ... ...

    Abstract Nanocrystal gels can be responsive, tunable materials, but designing their structure and properties is challenging. By using reversibly bonded molecular linkers, gelation can be realized under conditions predicted by thermodynamics. However, simulations have offered the only microscopic insights, with no experimental means to monitor linking leading to gelation. We introduce a metal coordination linkage with a distinct optical signature allowing us to quantify linking in situ and establish structural and thermodynamic bases for assembly. Because of coupling between linked indium tin oxide nanocrystals, their infrared absorption shifts abruptly at a chemically tunable gelation temperature. We quantify bonding spectroscopically and use molecular simulation to understand temperature-dependent bonding motifs, revealing that gel formation is governed by reaching a critical number of effective links that extend the nanocrystal network. Microscopic insights from our colorimetric linking chemistry enable switchable gels based on thermodynamic principles, opening the door to rational design of programmable nanocrystal networks.
    Language English
    Publishing date 2022-02-18
    Publishing country United States
    Document type Journal Article
    ZDB-ID 2810933-8
    ISSN 2375-2548 ; 2375-2548
    ISSN (online) 2375-2548
    ISSN 2375-2548
    DOI 10.1126/sciadv.abm7364
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article ; Online: Plasmonic Response of Complex Nanoparticle Assemblies.

    Sherman, Zachary M / Kim, Kihoon / Kang, Jiho / Roman, Benjamin J / Crory, Hannah S N / Conrad, Diana L / Valenzuela, Stephanie A / Lin, Emily / Dominguez, Manuel N / Gibbs, Stephen L / Anslyn, Eric V / Milliron, Delia J / Truskett, Thomas M

    Nano letters

    2023  Volume 23, Issue 7, Page(s) 3030–3037

    Abstract: Optical properties of nanoparticle assemblies reflect distinctive characteristics of their building blocks and spatial organization, giving rise to emergent phenomena. Integrated experimental and computational studies have established design principles ... ...

    Abstract Optical properties of nanoparticle assemblies reflect distinctive characteristics of their building blocks and spatial organization, giving rise to emergent phenomena. Integrated experimental and computational studies have established design principles connecting the structure to properties for assembled clusters and superlattices. However, conventional electromagnetic simulations are too computationally expensive to treat more complex assemblies. Here we establish a fast, materials agnostic method to simulate the optical response of large nanoparticle assemblies incorporating both structural and compositional complexity. This many-bodied, mutual polarization method resolves limitations of established approaches, achieving rapid, accurate convergence for configurations including thousands of nanoparticles, with some overlapping. We demonstrate these capabilities by reproducing experimental trends and uncovering far- and near-field mechanisms governing the optical response of plasmonic semiconductor nanocrystal assemblies including structurally complex gel networks and compositionally complex mixed binary superlattices. This broadly applicable framework will facilitate the design of complex, hierarchically structured, and dynamic assemblies for desired optical characteristics.
    Language English
    Publishing date 2023-03-29
    Publishing country United States
    Document type Journal Article
    ISSN 1530-6992
    ISSN (online) 1530-6992
    DOI 10.1021/acs.nanolett.3c00429
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  3. Article ; Online: Structural Control of Plasmon Resonance in Molecularly Linked Metal Oxide Nanocrystal Gel Assemblies.

    Kang, Jiho / Sherman, Zachary M / Conrad, Diana L / Crory, Hannah S N / Dominguez, Manuel N / Valenzuela, Stephanie A / Anslyn, Eric V / Truskett, Thomas M / Milliron, Delia J

    ACS nano

    2023  Volume 17, Issue 23, Page(s) 24218–24226

    Abstract: Nanocrystal gels exhibit collective optical phenomena based on interactions among their constituent building blocks. However, their inherently disordered structures have made it challenging to understand, predict, or design properties such as optical ... ...

    Abstract Nanocrystal gels exhibit collective optical phenomena based on interactions among their constituent building blocks. However, their inherently disordered structures have made it challenging to understand, predict, or design properties such as optical absorption spectra that are sensitive to the coupling between the plasmon resonances of the individual nanocrystals. Here, we bring indium tin oxide nanocrystal gels under chemical control and show that their infrared absorption can be predicted and systematically tuned by selecting the nanocrystal sizes and compositions and molecular structures of the link-mediating surface ligands. Thermoreversible assemblies with metal-terpyridine links form reproducible gel architectures, enabling us to derive a plasmon ruler that governs the spectral shifts upon gelation, predicated on the nanocrystal and ligand compositions. This empirical guide is validated using large-scale, many-bodied simulations to compute the optical spectra of gels with varied structural parameters. Based on the derived plasmon ruler, we design and demonstrate a nanocrystal mixture whose spectrum exhibits distinctive line narrowing upon assembly.
    Language English
    Publishing date 2023-11-27
    Publishing country United States
    Document type Journal Article
    ISSN 1936-086X
    ISSN (online) 1936-086X
    DOI 10.1021/acsnano.3c09515
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  4. Article ; Online: A self-degradable hydrogel sensor for a nerve agent tabun surrogate through a self-propagating cascade.

    Lee, Doo-Hee / Valenzuela, Stephanie A / Dominguez, Manuel N / Otsuka, Mai / Milliron, Delia J / Anslyn, Eric V

    Cell reports. Physical science

    2021  Volume 2, Issue 9

    Abstract: Nerve agents that irreversibly deactivate the enzyme acetylcholinesterase are extremely toxic weapons of mass destruction. Thus, developing methods to detect these lethal agents is important. To create an optical sensor for a surrogate of the nerve agent ...

    Abstract Nerve agents that irreversibly deactivate the enzyme acetylcholinesterase are extremely toxic weapons of mass destruction. Thus, developing methods to detect these lethal agents is important. To create an optical sensor for a surrogate of the nerve agent tabun, as well as a physical barrier that dissolves in response to this analyte, we devise a network hydrogel that decomposes via a self-propagating cascade. A Meldrums acid-derived linker is incorporated into a hydrogel that undergoes a declick reaction in response to thiols, thereby breaking network connections, which releases more thiols, propagating the response throughout the gel. A combination of chemical reactions triggered by the addition of the tabun mimic initiates the cascade. The dissolving barrier is used to release dyes, as well as nanocrystals that undergo a spontaneous aggregation. Thus, this sensing system for tabun generates a physical response and the delivery of chemical agents in response to an initial trigger.
    Language English
    Publishing date 2021-08-25
    Publishing country United States
    Document type Journal Article
    ISSN 2666-3864
    ISSN (online) 2666-3864
    DOI 10.1016/j.xcrp.2021.100552
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  5. Article ; Online: Universal Gelation of Metal Oxide Nanocrystals via Depletion Attractions.

    Saez Cabezas, Camila A / Sherman, Zachary M / Howard, Michael P / Dominguez, Manuel N / Cho, Shin Hum / Ong, Gary K / Green, Allison M / Truskett, Thomas M / Milliron, Delia J

    Nano letters

    2020  Volume 20, Issue 5, Page(s) 4007–4013

    Abstract: Nanocrystal gelation provides a powerful framework to translate nanoscale properties into bulk materials and to engineer emergent properties through the assembled microstructure. However, many established gelation strategies rely on chemical reactions ... ...

    Abstract Nanocrystal gelation provides a powerful framework to translate nanoscale properties into bulk materials and to engineer emergent properties through the assembled microstructure. However, many established gelation strategies rely on chemical reactions and specific interactions, e.g., stabilizing ligands or ions on the nanocrystals' surfaces, and are therefore not easily transferable. Here, we report a general gelation strategy via nonspecific and purely entropic depletion attractions applied to three types of metal oxide nanocrystals. The gelation thresholds of two compositionally distinct spherical nanocrystals agree quantitatively, demonstrating the adaptability of the approach for different chemistries. Consistent with theoretical phase behavior predictions, nanocrystal cubes form gels at a lower polymer concentration than nanocrystal spheres, allowing shape to serve as a handle to control gelation. These results suggest that the fundamental underpinnings of depletion-driven assembly, traditionally associated with larger colloidal particles, are also applicable at the nanoscale.
    Language English
    Publishing date 2020-05-01
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
    ISSN 1530-6992
    ISSN (online) 1530-6992
    DOI 10.1021/acs.nanolett.0c01311
    Database MEDical Literature Analysis and Retrieval System OnLINE

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