Ultrafast relaxation dynamics of excited carriers in metals: Simplifying the intertwined dependencies upon scattering strengths, phonon temperature, photon energy, and excitation level

D. M. RiffeRichard B. Wilson

D. M. RiffeRichard B. Wilson

Jan 2024

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摘要原文

Using the Boltzmann transport equation (BTE), we study the evolution of nonequilibrium carrier distributions in simple ($sp$) metals, assumed to have been instantaneously excited by an ultrafast laser pulse with photon energy $h \nu$. The mathematical structure of the BTE scattering integrals reveals that $h \nu$ is a natural energy scale for describing the dynamics. Normalizing all energy quantities by $h \nu$ leads to a set of three unitless parameters -- $\beta / \delta$, $\gamma$, and $\alpha$ -- that control the relaxation dynamics: $\beta / \delta$ is the normalized ratio of electron-phonon to electron-electron scattering strengths, $\gamma$ is the normalized phonon (lattice) temperature, and $\alpha$ is the normalized absorbed energy density. Using this theory, we systematically investigate relaxation times for the high-energy part of the distribution ($\tau_H$), energy transfer to the phonon subsystem ($\tau_E$), and intracarrier thermalization ($\tau_{th}$). In the linear region of response (valid when $\alpha$ is sufficiently small), we offer heuristic descriptions of each of these relaxation times as functions of $\beta / \delta$ and $\gamma$. Our results as a function of excitation level $\alpha$ show that many ultrafast experimental investigations lie in a transition region between low excitation (where the relaxation times are independent of $\alpha$) and high excitation (where the two-temperature model of carrier dynamics is valid). Approximate boundaries that separate these three regions are described by simple expressions involving the normalized parameters of our model.