A Caltech Library Service

Ab initio study of hot electrons in GaAs

Bernardi, Marco and Vigil-Fowler, Derek and Ong, Chin Shen and Neaton, Jeffrey B. and Louie, Steven G. (2015) Ab initio study of hot electrons in GaAs. Proceedings of the National Academy of Sciences of the United States of America, 112 (17). pp. 5291-5296. ISSN 0027-8424. PMCID PMC4418885. doi:10.1073/pnas.1419446112.

[img] PDF - Published Version
See Usage Policy.

[img] PDF - Supplemental Material
See Usage Policy.


Use this Persistent URL to link to this item:


Hot carrier dynamics critically impacts the performance of electronic, optoelectronic, photovoltaic, and plasmonic devices. Hot carriers lose energy over nanometer lengths and picosecond timescales and thus are challenging to study experimentally, whereas calculations of hot carrier dynamics are cumbersome and dominated by empirical approaches. In this work, we present ab initio calculations of hot electrons in gallium arsenide (GaAs) using density functional theory and many-body perturbation theory. Our computed electron–phonon relaxation times at the onset of the Γ, L, and X valleys are in excellent agreement with ultrafast optical experiments and show that the ultrafast (tens of femtoseconds) hot electron decay times observed experimentally arise from electron–phonon scattering. This result is an important advance to resolve a controversy on hot electron cooling in GaAs. We further find that, contrary to common notions, all optical and acoustic modes contribute substantially to electron–phonon scattering, with a dominant contribution from transverse acoustic modes. This work provides definitive microscopic insight into hot electrons in GaAs and enables accurate ab initio computation of hot carriers in advanced materials.

Item Type:Article
Related URLs:
URLURL TypeDescription Information CentralArticle
Bernardi, Marco0000-0001-7289-9666
Neaton, Jeffrey B.0000-0001-7585-6135
Additional Information:© 2015 National Academy of Sciences. Edited by Allan H. MacDonald, The University of Texas at Austin, Austin, TX, and approved March 16, 2015 (received for review October 9, 2014). Published ahead of print April 13, 2015. This research was supported by the Scientific Discovery through Advanced Computing (SciDAC) Program on Excited State Phenomena in Energy Materials funded by US Department of Energy, Offices of Basic Energy Sciences and Advanced Scientific Computing Research Contract DE-AC02-05CH11231 at Lawrence Berkeley National Laboratory, which provided for algorithm and code developments and simulations, and National Science Foundation Grant 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, US Department of Energy Contract DE-AC02-05CH11231. This research used resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science, US Department of Energy. Author contributions: M.B., D.V.-F., J.B.N., and S.G.L. designed research; M.B., D.V.-F., and C.S.O. performed calculations; M.B., D.V.-F., J.B.N., and S.G.L. analyzed data; M.B., D.V.-F., J.B.N., and S.G.L. wrote the paper; and C.S.O. contributed to code development. The authors declare no conflict of interest. This article is a PNAS Direct Submission. This article contains supporting information online at
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC02-05CH11231
NSFDMR 10-1006184
Subject Keywords:hot carriers; semiconductors; GaAs; ultrafast; electron–phonon scattering
Issue or Number:17
PubMed Central ID:PMC4418885
Record Number:CaltechAUTHORS:20150923-133149273
Persistent URL:
Official Citation:Marco Bernardi, Derek Vigil-Fowler, Chin Shen Ong, Jeffrey B. Neaton, and Steven G. Louie Ab initio study of hot electrons in GaAs PNAS 2015 112 (17) 5291-5296; published ahead of print April 13, 2015, doi:10.1073/pnas.1419446112
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:60442
Deposited By: Tony Diaz
Deposited On:23 Sep 2015 20:46
Last Modified:10 Nov 2021 22:34

Repository Staff Only: item control page