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Ab Initio Study of Hot Carriers in the First Picosecond after Sunlight Absorption in Silicon

Bernardi, Marco and Vigil-Fowler, Derek and Lischner, Johannes and Neaton, Jeffrey B. and Louie, Steven G. (2014) Ab Initio Study of Hot Carriers in the First Picosecond after Sunlight Absorption in Silicon. Physical Review Letters, 112 (25). Art. No. 257402. ISSN 0031-9007. doi:10.1103/PhysRevLett.112.257402.

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Hot carrier thermalization is a major source of efficiency loss in solar cells. Because of the subpicosecond time scale and complex physics involved, a microscopic characterization of hot carriers is challenging even for the simplest materials. We develop and apply an ab initio approach based on density functional theory and many-body perturbation theory to investigate hot carriers in semiconductors. Our calculations include electron-electron and electron-phonon interactions, and require no experimental input other than the structure of the material. We apply our approach to study the relaxation time and mean free path of hot carriers in Si, and map the band and k dependence of these quantities. We demonstrate that a hot carrier distribution characteristic of Si under solar illumination thermalizes within 350 fs, in excellent agreement with pump-probe experiments. Our work sheds light on the subpicosecond time scale after sunlight absorption in Si, and constitutes a first step towards ab initio quantification of hot carrier dynamics in materials.

Item Type:Article
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URLURL TypeDescription
Bernardi, Marco0000-0001-7289-9666
Neaton, Jeffrey B.0000-0001-7585-6135
Additional Information:© 2014 American Physical Society. Received 21 January 2014; published 26 June 2014. M. B. thanks Sinisa Coh for discussion. This research was supported by the SciDAC Program on Excited State Phenomena in Energy Materials funded by the U.S. Department of Energy, Office of Basic Energy Sciences and of Advanced Scientific Computing Research, under Contract No. DE-AC02-05CH11231 at Lawrence Berkeley National Laboratory, which provided for algorithm and code developments and simulations; and by the National Science Foundation under Grant No. DMR 10-1006184 which provided for basic theory and formalism. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. S. G. L. acknowledges support of a Simons Foundation Fellowship in Theoretical Physics. This research used resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. Department of Energy.
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC02-05CH11231
NSFDMR 10-1006184
Simons FoundationUNSPECIFIED
Issue or Number:25
Classification Code:PACS numbers: 78.56.-a, 71.20.Mq, 78.47.db, 88.40.H-
Record Number:CaltechAUTHORS:20150924-101329607
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:60476
Deposited By: Tony Diaz
Deposited On:24 Sep 2015 20:42
Last Modified:10 Nov 2021 22:34

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