Efficient hot carrier dynamics in near-infrared photocatalytic metals

Abstract

Photoexcited metals can produce highly-energetic hot carriers whose controlled generation and extraction is a promising avenue for technological applications. While hot carrier dynamics in Au-group metals have been widely investigated, a microscopic description of the dynamics of photoexcited carriers in the mid-infrared and near-infrared Pt-group metals range is still scarce. Since these materials are widely used in catalysis and, more recently, in plasmonic catalysis, their microscopic carrier dynamics characterization is crucial. We employ \emph{ab initio} many-body perturbation theory to investigate the hot carrier generation, relaxation times, and mean free path in bulk Pd and Pt. We show that the direct optical transitions of photoexcited carriers in this metals are mainly generated in the near-infrared range. We also find that the electron-phonon mass enhancement parameter for Pt is 16 $\%$ higher than Pd, a result that help explains several experimental results showing diverse trends. Moreover, we predict that Pd (Pt) hot electrons possess total relaxation times of up to 35 fs (24 fs), taking place at approximately 0.5 eV (1.0 eV) above the Fermi energy. Finally, an efficient hot electron generation and extraction can be achieved in nanofilms of Pd (110) and Pd (100) when subject to excitation energies ranging from 0.4 to 1.6 eV.

arXiv commentAccepted for publication in Physical Review B

References in corpus (14)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Phonons and related properties of extended systems from density-functional perturbation theory
• EPW: Electron-phonon coupling, transport and superconducting properties using maximally localized Wannier functions
• Electron-phonon interactions and related physical properties of metals from linear-response theory
• Many-body perturbation theory calculations using the yambo code
• Challenges in Plasmonic Catalysis
• Ab initio calculations of ultra-short carrier dynamics in 2D materials: valley depolarization in single-layer WSe${}_2$
• Verification of first-principles codes: comparison of total energies, phonon frequencies, electron-phonon coupling and zero-point motion correction to the gap between ABINIT and QE/Yambo
• First--principles calculation of the plasmon resonance and of the reflectance spectrum of Silver in the GW approximation
• Dielectric constants of Ir, Ru, Pt, and IrO2: Contributions from bound charges
• Competition between the electronic and phonon-mediated scattering channels in the out-of-equilibrium carrier dynamics of semiconductors: an ab-initio approach
• Parametric dependence of hot electron relaxation timescales on electron-electron and electron-phonon interaction strengths
• Phase Transition and Electronic Structure Investigation of MoS${}_2$-rGO Nanocomposite Decorated with AuNPs
• The electronic structure of palladium in the presence of many-body effects

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