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Plasmonic catalysis is uniquely positioned between photo/electrochemistry and thermal chemistry such that multiple factors may compete to dominate the reaction enhancement mechanism. The adoption of norms originating in both photochemistry and thermal chemistry has resulted in the use of language and methods of data analysis, which, in the context of plasmonic catalysis, may be implicitly contradictory. This article tracks several years of research towards understanding thermal and nonthermal effects in plasmonic catalysis and culminates with a discussion on how the choice of language and presentation of data can be tuned to avoid subtle yet significant contradictory implications.more » « lessFree, publicly-accessible full text available December 11, 2024
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Plasmonic photocatalysis presents a promising method for light-to-matter conversion. However, most current studies focused on understanding the relative importance of thermal and nonthermal effects while their synergistic effects remained less studied. Here, we propose an index, termed Overall Light Effectiveness (OLE), to capture the combined impact of these light effects on reactions. By systematically varying the thickness of catalyst layers, we isolated thermal and nonthermal contributions and optimized them to achieve maximum light enhancement. We demonstrate the approach using carbon dioxide hydrogenation reaction on titania-supported rhodium nanoparticles as a model reaction system. It shows a generalizable potential in designing catalyst systems with optimum combinations of heating and light illumination, especially with broadband light illumination such as sunlight, for achieving the most economical light-to-matter conversion in plasmonic catalysis.more » « lessFree, publicly-accessible full text available December 1, 2024
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Plasmonic photocatalysis is an emerging research field that holds promise for sustainable energy applications, particularly in solar energy conversion. In this study, we focus on the enhancement of broadband light absorption capabilities for plasmonic photocatalyst under white light illumination. By replacing parts of the catalyst with solar absorber, we can significantly improve the total reaction rate under mild heating conditions with less catalyst. Through careful comparison of reaction conditions and systematic optimization of the contributions from photothermal and non-thermal effects, we demonstrate a substantial enhancement in broadband light absorption capacity and overall light effectiveness, paving the way for advanced plasmonic photocatalysts with greater efficiency and practical applicability using solar light as the energy source.more » « less
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Toward One‐Way Smoke: Synthesis of Copper‐Based Microclubs with Asymmetric Scattering and Absorption
Abstract The ultimate goal of this work is to create an engineered aerosol that acts as one‐way smoke, i.e. it creates an asymmetric vision environment in which the ability to image objects depends on the viewing direction. To this end, a rapid, one‐pot synthesis of copper‐based microclubs is developed that consists of a Cu2O octahedron attached to a Cu2O@Cu shaft. Millions of synthesized particles are analyzed in minutes with a FlowCam to provide a robust statistical analysis of their geometry, and rapidly elucidate the roles of the reaction constituents on the particle shape and yield. The combination of asymmetry in both shape and composition introduces a 30% difference in scattering of light propagating parallel to the microclub axis from opposing directions. This work represents a first step toward the creation of an asymmetric imaging environment with an aerosol consisting of acoustically aligned microclubs.
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Abstract Migrating cells must deform their stiff cell nucleus to move through pores and fibers in tissue. Lamin A/C is known to hinder cell migration by limiting nuclear deformation and passage through confining channels, but its role in nuclear deformation and passage through fibrous environments is less clear. Cell and nuclear migration through discrete, closely spaced, slender obstacles which mimic the mechanical properties of collagen fibers are studied. Nuclei bypass slender obstacles while preserving their overall morphology by deforming around them with deep local invaginations of little resisting force. The obstacles do not impede the nuclear trajectory and do not cause rupture of the nuclear envelope. Nuclei likewise deform around single collagen fibers in cells migrating in 3D collagen gels. In contrast to its limiting role in nuclear passage through confining channels, lamin A/C facilitates nuclear deformation and passage through fibrous environments; nuclei in lamin‐null (
Lmna−/− ) cells lose their overall morphology and become entangled on the obstacles. Analogous to surface tension‐mediated deformation of a liquid drop, lamin A/C imparts a surface tension on the nucleus that allows nuclear invaginations with little mechanical resistance, preventing nuclear entanglement and allowing nuclear passage through fibrous environments.