Journal
PHYSICAL REVIEW LETTERS
Volume 118, Issue 8, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.118.087401
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Funding
- Office of Science of the U.S. Department of Energy [DE-SC0004993, DE-AC02-05CH11231]
- Office of Science, Office of Basic Energy Sciences of the U.S. Department of Energy [DE-AC02-05CH11231]
- NG NEXT at Northrop Grumman Corporation
- National Science Foundation Graduate Research Fellowship
- Resnick Sustainability Institute
- Link Foundation Energy Fellowship
- DOE Light-Material Interactions in Energy Conversion Energy Frontier Research Center [DE-SC0001293]
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Ultrafast pump-probe measurements of plasmonic nanostructures probe the nonequilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements of plasmonic nanoparticles along with a complete theoretical description based on first-principles calculations of carrier dynamics and optical response, free of any fitting parameters. We account for detailed electronic-structure effects in the density of states, excited carrier distributions, electron-phonon coupling, and dielectric functions that allow us to avoid effective electron temperature approximations. Using this calculation method, we obtain excellent quantitative agreement with spectral and temporal features in transient-absorption measurements. In both our experiments and calculations, we identify the two major contributions of the initial response with distinct signatures: short-lived highly nonthermal excited carriers and longer-lived thermalizing carriers.
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