Role of ultrafast electron-optical-phonon interactions in high harmonic generation from graphene

TL;DR

This study reveals how optical phonons in graphene suppress high harmonic generation, influence temperature dependence, and cause rapid decoherence, providing insights into electron-phonon interactions on attosecond timescales.

Contribution

The paper introduces a static-limit formalism including optical phonons to analyze their impact on HHG in graphene, highlighting phonon-induced suppression and decoherence effects.

Findings

Optical phonons strongly suppress HHG yields in graphene.

HHG yields are weakly temperature-dependent due to zero-point motion.

Phonons cause rapid interband coherence dephasing (~5.7 fs).

Abstract

High harmonic generation (HHG) is a widely explored process in solids, where intense lasers drive attosecond-to-femtosecond electron dynamics within bands, causing high-energy emission. While electrons and photons are considered the main players in HHG, solids also host ubiquitous phonons that are typically assumed negligible in HHG due to their longer timescales. We theoretically study HHG in graphene with a formalism including optical phonons in the static limit, where the lattice is frozen on the electronic timescale and HHG is computed by sampling thermally-occupied phonons and ensemble-averaging. We show that in graphene: (i) Optical phonons strongly suppress HHG yields by coupling to interband currents and causing harmonic phase scrambling (destructive interference), explaining the lack of experimental HHG above ~3 eV. (ii) HHG yields become temperature-dependent due to phonon occupations, though in graphene this dependence is weak since phonon energy scales are dominated by zero-point motion. (iii) Optical phonons dephase interband coherences at a rate equivalent to T2~5.7 fs, substantially faster than e-e scattering, suggesting thermal phonons dominate electronic decoherence in strong fields. (iv) Phonons smoothen HHG ellipticity-dependent curves, yielding better agreement with experiments. Remarkably, all effects are timescale-independent, arising in the static picture of electron-phonon interactions, making results transferable to attosecond phenomena. Our results shed light on the dephasing time problem in HHG and the role of phonons on attosecond timescales, with implications for other systems and processes such as Floquet gaps and photocurrents in graphene.