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. 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.
Additional Information
© 2016 American Physical Society. Received 1 February 2016; revised manuscript received 26 July 2016; published 11 August 2016. This material is based upon work performed by 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 No. 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. P.N. and W.A.G. acknowledge financial support from NG NEXT for this project. P.N. is supported by a National Science Foundation Graduate Research Fellowship and by the Resnick Sustainability Institute. A.B. is supported by a National Science Foundation Graduate Research Fellowship, a Link Foundation Energy Fellowship, and the DOE "Light-Material Interactions in Energy Conversion" Energy Frontier Research Center (Grant No. DE-SC0001293).Attached Files
Published - PhysRevB.94.075120.pdf
Submitted - 1602.00625v1.pdf
Supplemental Material - Ag_ImEpsilon.dat
Supplemental Material - Ag_ReEpsilon.dat
Supplemental Material - Al_ImEpsilon.dat
Supplemental Material - Al_ReEpsilon.dat
Supplemental Material - Au_ImEpsilon.dat
Supplemental Material - Au_ReEpsilon.dat
Supplemental Material - Cu_ImEpsilon.dat
Supplemental Material - Cu_ReEpsilon.dat
Supplemental Material - SI.pdf
Files
Name | Size | Download all |
---|---|---|
md5:f7eb463fd4f2cc59cb53d91e472925f2
|
980.5 kB | Preview Download |
md5:e4d6717e9b4d7887d417ed33585cbb30
|
729.1 kB | Download |
md5:5efbe0a2728dc68914c2c46fad097bc6
|
720.1 kB | Download |
md5:c80b7a2b83bb95514b6dd2f0505794d3
|
747.1 kB | Download |
md5:ae31d7aaaf5f8c110264ae3c03772829
|
705.4 kB | Download |
md5:7a9ec17629d22fc51baa1ea91d593f89
|
743.6 kB | Download |
md5:eb475e4e221018883a57328ee52fdf86
|
702.2 kB | Download |
md5:4fb7aa3b28eeb6542b67ca05ebfe929a
|
702.1 kB | Download |
md5:3e3a686c41d4b552b8e06af06365627a
|
1.3 MB | Preview Download |
md5:4f33e10c2cfdbe898158f5785694edde
|
226.9 kB | Preview Download |
md5:e94e2751ff624f2cc06c6d10175e95c9
|
731.1 kB | Download |
Additional details
- Eprint ID
- 67884
- Resolver ID
- CaltechAUTHORS:20160613-140325024
- Department of Energy (DOE)
- DE-SC0004993
- Department of Energy (DOE)
- DE-AC02-05CH11231
- NSF Graduate Research Fellowship
- Resnick Sustainability Institute
- Link Foundation
- Department of Energy (DOE)
- DE-SC0001293
- Created
-
2016-06-13Created from EPrint's datestamp field
- Updated
-
2021-11-11Created from EPrint's last_modified field
- Caltech groups
- JCAP, Resnick Sustainability Institute
- Other Numbering System Name
- WAG
- Other Numbering System Identifier
- 1175