Transport of hot carriers in plasmonic nanostructures
Abstract
Plasmonic hot carrier devices extract excited carriers from metal nanostructures before equilibration and have the potential to surpass semiconductor light absorbers. However their efficiencies have so far remained well below theoretical limits, which necessitates quantitative prediction of carrier transport and energy loss in plasmonic structures to identify and overcome bottlenecks in carrier harvesting. Here, we present a theoretical and computational framework, nonequilibrium scattering in space and energy (NESSE), to predict the spatial evolution of carrier energy distributions that combines the best features of phase-space (Boltzmann) and particle-based (Monte Carlo) methods. Within the NESSE framework, we bridge first-principles electronic structure predictions of plasmon decay and carrier collision integrals at the atomic scale, with electromagnetic field simulations at the nano- to mesoscale. Finally, we apply NESSE to predict spatially-resolved energy distributions of photoexcited carriers that impact the surface of experimentally realizable plasmonic nanostructures at length scales ranging from tens to several hundreds of nanometers, enabling first-principles design of hot carrier devices.
Additional Information
© 2019 American Physical Society. Received 6 March 2019; published 8 July 2019. This material is based upon work performed at the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231, as well as the Center for Computational Innovations at Rensselaer Polytechnic Institute. A.S.J. thanks the UK Marshall Commission and the US Goldwater Scholarship for financial support. G.T. acknowledges support from the Swiss National Science Foundation, Early Postdoctoral Mobility Fellowship No. P2EZP2-159101. P.N. acknowledges start-up funding from the Harvard John A. Paulson School of Engineering and Applied Sciences and partial support from the Harvard University Center for the Environment (HUCE). R.S. acknowledges start-up funding from the Department of Materials Science and Engineering at Rensselaer Polytechnic Institute.Attached Files
Published - PhysRevMaterials.3.075201.pdf
Submitted - 1707.07060.pdf
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Additional details
- Alternative title
- Far-from-equilibrium transport of excited carriers in nanostructures
- Eprint ID
- 96792
- Resolver ID
- CaltechAUTHORS:20190627-130903657
- Department of Energy (DOE)
- DE-SC0004993
- Department of Energy (DOE)
- DE-AC02-05CH11231
- UK Marshall Commission
- Barry M. Goldwater Scholarship
- Swiss National Science Foundation (SNSF)
- P2EZP2-159101
- Harvard University
- Rensselaer Polytechnic Institute
- Created
-
2019-06-27Created from EPrint's datestamp field
- Updated
-
2021-11-16Created from EPrint's last_modified field
- Caltech groups
- JCAP
- Other Numbering System Name
- WAG
- Other Numbering System Identifier
- 1343