Title: Ab initio phonon coupling and optical response of hot electrons in plasmonic metals

Abstract

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 of hot electron dynamics, but a parameter-free description of pump-probe measurements has not yet been possible, despite intensive research, because of the phenomenological treatment of electron-phonon interactions. As such, we present ab initio predictions of the electron-temperature dependent heat capacities and electron-phonon coupling coefficients of plasmonic metals. We find substantial differences from free-electron and semiempirical estimates, especially in noble metals above transient electron temperatures of 2000 K, because of the previously neglected strong dependence of electron-phonon matrix elements on electron energy. We also present first-principles calculations of the electron-temperature dependent dielectric response of hot electrons in plasmonic metals, including direct interband and phonon-assisted intraband transitions, facilitating complete theoretical predictions of the time-resolved optical probe signatures in ultrafast laser experiments.

Authors:

Brown, Ana M. ^[1]; Sundararaman, Ravishankar ^[1]; Narang, Prineha ^[2]; Goddard, William A. ^[1]; Atwater, Harry A. ^[1]

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+ Show Author Affiliations

1. California Inst. of Technology (CalTech), Pasadena, CA (United States)
2. California Inst. of Technology (CalTech), Pasadena, CA (United States); 3NG NEXT, Redondo Beach, CA (United States)

Publication Date:

Thu Aug 11 00:00:00 EDT 2016

Research Org.:

Energy Frontier Research Centers (EFRC) (United States). Light-Material Interactions in Energy Conversion (LMI); : Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF)

OSTI Identifier:

1388843

Alternate Identifier(s):

OSTI ID: 1290315

Grant/Contract Number:  

SC0001293; SC0004993; AC02-05CH11231

Resource Type:

Accepted Manuscript

Journal Name:

Physical Review B

Additional Journal Information:

Journal Volume: 94; Journal Issue: 7; Related Information: LMI partners with California Institute of Technology (lead); Harvard University; University of Illinois, Urbana-Champaign; Lawrence Berkeley National Laboratory; Journal ID: ISSN 2469-9950

Publisher:

American Physical Society (APS)

Country of Publication:

United States

Language:

English

Subject:

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; solar (photovoltaic); solid state lighting; phonons; thermal conductivity; electrodes - solar; materials and chemistry by design; optics; synthesis (novel materials); synthesis (self-assembly)