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arXiv · 1608.03309

Experimental and ab initio ultrafast carrier dynamics in plasmonic nanoparticles

Ana M. Brown·Ravishankar Sundararaman·Prineha Narang·Adam M. Schwartzberg·William A. Goddard III·Harry A. Atwater
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Abstract

Ultrafast pump-probe measurements of plasmonic nanostructures probe the non-equilibrium 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 which 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 non-thermal excited carriers and longer-lived thermalizing carriers.

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Ana M. Brown, Ravishankar Sundararaman, Prineha Narang, Adam M. Schwartzberg, William A. Goddard III, Harry A. Atwater. 2016-12-24. Experimental and ab initio ultrafast carrier dynamics in plasmonic nanoparticles. https://doi.org/10.1103/physrevlett.118.087401

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