A5080023418- Quantum Information and Cryptography
- Quantum and electron transport phenomena
- Quantum Computing Algorithms and Architecture
- Graphene research and applications
- 2D Materials and Applications
- Topological Materials and Phenomena
- Mechanical and Optical Resonators
- Plasmonic and Surface Plasmon Research
- Strong Light-Matter Interactions
- Electronic and Structural Properties of Oxides
- Physics of Superconductivity and Magnetism
- Gold and Silver Nanoparticles Synthesis and Applications
- Diamond and Carbon-based Materials Research
- Quantum Mechanics and Applications
- Thermal Radiation and Cooling Technologies
- Photonic and Optical Devices
- Cold Atom Physics and Bose-Einstein Condensates
- Advanced Condensed Matter Physics
- Quantum optics and atomic interactions
- Neural Networks and Reservoir Computing
- Magnetic properties of thin films
- Semiconductor materials and devices
- Machine Learning in Materials Science
- Molecular Junctions and Nanostructures
- Quantum Dots Synthesis And Properties
University of California, Los Angeles
2022-2025
Physical Sciences (United States)
2022-2025
University of California System
2025
Harvard University
2016-2023
Harvard University Press
2018-2021
National Institute for Materials Science
2021
Universidade de Vigo
2021
Imperial College London
2021
University of Tsukuba
2021
ORCID
2021
Abstract Decay of surface plasmons to hot carriers finds a wide variety applications in energy conversion, photocatalysis and photodetection. However, detailed theoretical description plasmonic hot-carrier generation real materials has remained incomplete. Here we report predictions for the prompt distributions excited ‘hot’ electrons holes generated by plasmon decay, before inelastic relaxation, using quantized model with electronic structure. We find that carrier are sensitive band...
The behavior of metals across a broad frequency range from microwave to ultraviolet frequencies is interest in plasmonics, nanophotonics, and metamaterials. Depending on the frequency, losses collective excitations can be predominantly classical resistive effects or Landau damping. In this context, we present first-principles calculations that capture all significant microscopic mechanisms underlying surface plasmon decay predict initial excited carrier distributions so generated....
Abstract Nanoscale localization of electromagnetic fields near metallic nanostructures underpins the fundamentals and applications plasmonics. The unavoidable energy loss from plasmon decay, initially seen as a detriment, has now expanded scope plasmonic to exploit generated hot carriers. However, quantitative understanding spatial these carriers, akin near-field maps, been elusive. Here we spatially map hot-electron-driven reduction chemistry with 15 nm resolution function time field...
Abstract Surface plasmons provide a pathway to efficiently absorb and confine light in metallic nanostructures, thereby bridging photonics the nano scale. The decay of surface generates energetic ‘hot’ carriers, which can drive chemical reactions or be injected into semiconductors for nano-scale photochemical photovoltaic energy conversion. Novel plasmonic hot carrier devices architectures continue demonstrated, but complexity underlying processes make complete microscopic understanding all...
Abstract In this article, we review strong light-matter coupling at the interface of materials science, quantum chemistry, and photonics. The control light heat thermodynamic limits enables exciting new opportunities for rapidly converging fields polaritonic chemistry optics atomic scale from a theoretical computational perspective. Our follows remarkable experimental demonstrations that now routinely achieve limit matter. many molecules couple collectively to single-photon mode, whereas, in...
Objects around us constantly emit and absorb thermal radiation. The emission absorption processes are governed by two fundamental radiative properties: emissivity absorptivity. For reciprocal systems, the absorptivity restricted to be equal Kirchhoff's law of This restriction limits degree freedom control radiation contributes an intrinsic loss mechanism in photonic energy harvesting systems. Existing approaches violate typically utilize magneto-optical effects with external magnetic field....
Abstract Harnessing photoexcited “hot” carriers in metallic nanostructures could define a new phase of non-equilibrium optoelectronics for photodetection and photocatalysis. Surface plasmons are considered pivotal enabling efficient operation hot carrier devices. Clarifying the fundamental role plasmon excitation is therefore critical exploiting their full potential. Here, we measure internal quantum efficiency gold (Au)–gallium nitride (GaN) Schottky diodes to elucidate quantify distinct...
Strong light-matter interaction in cavity environments is emerging as a promising approach to control chemical reactions non-intrusive and efficient manner. The underlying mechanism that distinguishes between steering, accelerating, or decelerating reaction has, however, remained unclear, hampering progress this frontier area of research. We leverage quantum-electrodynamical density-functional theory unveil the microscopic behind experimentally observed reduced rate under induced resonant...
<italic xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">Contribution:</i> A roadmap is provided for building a quantum engineering education program to satisfy U.S. national and international workforce needs. xmlns:xlink="http://www.w3.org/1999/xlink">Background:</i> The rapidly growing information science (QISE) industry will require both quantum-aware quantum-proficient engineers at the bachelor's level....
Correlated quantum phenomena in one-dimensional (1D) systems that exhibit competing electronic and magnetic order are of strong interest for the study fundamental interactions excitations, such as Tomonaga-Luttinger liquids topological orders defects with properties completely different from quasiparticles expected their higher-dimensional counterparts. However, clean 1D difficult to realize experimentally, particularly magnetically ordered systems. Here, we show van der Waals layered...
Abstract In quantum materials, degeneracies and frustrated interactions can have a profound impact on the emergence of long-range order, often driving strong fluctuations that suppress functionally relevant electronic or magnetic phases 1–7 . Engineering atomic structure in bulk at heterointerfaces has been an important research strategy to lift these degeneracies, but equilibrium methods are limited by thermodynamic, elastic chemical constraints 8 Here we show all-optical, mode-selective...
Ultrafast laser measurements probe the nonequilibrium dynamics of excited electrons in metals with increasing temporal resolution. Electronic structure calculations can provide a detailed microscopic understanding hot electron dynamics, but parameter-free description pump-probe has not yet been possible, despite intensive research, because phenomenological treatment electron-phonon interactions. We present ab initio predictions electron-temperature dependent heat capacities and coupling...
Collection of hot electrons generated by the efficient absorption light in metallic nanostructures, contact with semiconductor substrates can provide a basis for construction solar energy-conversion devices. Herein, we evaluate theoretically efficiency systems that rely on internal photoemission processes at metal-semiconductor Schottky-barrier diodes. In this theory, current-voltage characteristics are given yield as well thermionic dark current over varied-energy barrier height. The Fowler...
The mechanism by which light is emitted from plasmonic metals such as gold and silver has been contentious, particularly at photon energies below direct interband transitions. Using nanoscale cavities, blue-pumped emission found to directly track dark-field scattering on individual nanoconstructs. By exploiting slow atomic-scale restructuring of the nanocavity facets spectrally tune dominant gap plasmons, this correlation can be measured 600 900 nm in gold, silver, mixed constructs ranging...
Ultrafast pump-probe measurements of plasmonic nanostructures probe the nonequilibrium behavior excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present nanoparticles along with a complete theoretical description based on first-principles calculations carrier dynamics and optical response, free any fitting parameters. We account for detailed electronic-structure density states, distributions, electron-phonon coupling, dielectric...
Nanoparticles attached just above a flat metallic surface can trap optical fields in the nanoscale gap. This enables local spectroscopy of few molecules within each coupled plasmonic hotspot, with near thousand-fold enhancement incident fields. As result non-radiative relaxation pathways, plasmons such sub-nanometre cavities generate hot charge carriers, which catalyse chemical reactions or induce redox processes located hotspots. Here, surface-enhanced Raman allows us to track these...