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Published on: July 21, 2018
Experimental and Ab Initio Ultrafast Carrier Dynamics in Plasmonic Nanoparticles
Ana M Brown1, Ravishankar Sundararaman2,3, Prineha Narang1,2,4
1Thomas J. Watson Laboratories of Applied Physics, California Institute of Technology, 1200 East California Boulevard, Pasadena, California 91125, USA.
This study uses ultrafast pump-probe measurements and first-principles calculations to analyze excited carriers in plasmonic nanoparticles. Researchers identified distinct signatures of short-lived nonthermal and longer-lived thermalizing carriers, advancing our understanding of plasmonic nanostructure dynamics.
Area of Science:
- Condensed matter physics
- Materials science
- Nanophotonics
Background:
- Ultrafast pump-probe measurements reveal nonequilibrium carrier behavior in plasmonic nanostructures.
- Conventional analyses often obscure competing effects, limiting understanding of excited carrier dynamics.
Purpose of the Study:
- To provide a comprehensive theoretical description of carrier dynamics and optical response in plasmonic nanoparticles.
- To achieve quantitative agreement with experimental transient-absorption measurements without fitting parameters.
Main Methods:
- Utilizing ultrafast pump-probe spectroscopy on plasmonic nanoparticles.
- Performing first-principles calculations of carrier dynamics, including electronic structure, electron-phonon coupling, and dielectric functions.
- Avoiding effective electron temperature approximations by detailed electronic considerations.
Main Results:
- Excellent quantitative agreement was achieved between theoretical calculations and experimental spectral and temporal features.
- Two distinct contributions to the initial response were identified: highly nonthermal excited carriers and thermalizing carriers.
- The distinct signatures of these carrier populations were characterized.
Conclusions:
- The developed theoretical framework accurately describes ultrafast carrier dynamics in plasmonic nanostructures.
- The study successfully differentiates and characterizes short-lived nonthermal and longer-lived thermalizing carrier populations.
- This work offers a parameter-free approach for analyzing complex carrier behavior in plasmonic systems.
