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Main Authors: Inoue, Soshun, Inaoka, Takeshi, Ishihara, Hajime
Format: Preprint
Published: 2025
Subjects:
Online Access:https://arxiv.org/abs/2505.19444
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author Inoue, Soshun
Inaoka, Takeshi
Ishihara, Hajime
author_facet Inoue, Soshun
Inaoka, Takeshi
Ishihara, Hajime
contents Hot carrier generation in metals, where high-energy electron-hole pairs are produced via plasmon excitation, has emerged as a promising mechanism for photoelectric conversion and photocatalysis. However, conventional theories often describe this process through phenomenological relaxation via Landau damping, which fails to account for the microscopic origin of the frequency-dependent internal quantum efficiency (IQE) observed in experiments. To address this gap, we develop an extended Bohm-Pines theory for a metallic thin film that explicitly incorporates light-matter interactions within a non-local response framework. Our approach treats collective (plasmonic) and individual (electron-hole) excitations on equal footing and includes their coupling mediated by both longitudinal and transverse electromagnetic fields. This results in a self-consistent theory of the optical response of metallic films. The derived total Hamiltonian includes radiative corrections that recover the known dispersion of surface plasmon polaritons and, importantly, predict a frequency-dependent radiative coupling between collective and individual modes. This previously neglected transverse coupling naturally explains the IQE peak near the plasmon resonance and reveals a new mechanism of hot carrier generation distinct from conventional Landau damping. Our results provide a unified theoretical foundation for understanding plasmon-induced hot carrier dynamics and offer guidance for resonance-based photonic design strategies to enhance energy conversion efficiency in metal nanostructures.
format Preprint
id arxiv_https___arxiv_org_abs_2505_19444
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Radiative coupling between plasmon and electron-hole pairs in a metallic film based on extended Bohm-Pines theory
Inoue, Soshun
Inaoka, Takeshi
Ishihara, Hajime
Optics
Hot carrier generation in metals, where high-energy electron-hole pairs are produced via plasmon excitation, has emerged as a promising mechanism for photoelectric conversion and photocatalysis. However, conventional theories often describe this process through phenomenological relaxation via Landau damping, which fails to account for the microscopic origin of the frequency-dependent internal quantum efficiency (IQE) observed in experiments. To address this gap, we develop an extended Bohm-Pines theory for a metallic thin film that explicitly incorporates light-matter interactions within a non-local response framework. Our approach treats collective (plasmonic) and individual (electron-hole) excitations on equal footing and includes their coupling mediated by both longitudinal and transverse electromagnetic fields. This results in a self-consistent theory of the optical response of metallic films. The derived total Hamiltonian includes radiative corrections that recover the known dispersion of surface plasmon polaritons and, importantly, predict a frequency-dependent radiative coupling between collective and individual modes. This previously neglected transverse coupling naturally explains the IQE peak near the plasmon resonance and reveals a new mechanism of hot carrier generation distinct from conventional Landau damping. Our results provide a unified theoretical foundation for understanding plasmon-induced hot carrier dynamics and offer guidance for resonance-based photonic design strategies to enhance energy conversion efficiency in metal nanostructures.
title Radiative coupling between plasmon and electron-hole pairs in a metallic film based on extended Bohm-Pines theory
topic Optics
url https://arxiv.org/abs/2505.19444