Probing quantum nonlinear phononics in multilayer graphene with time-resolved Raman scattering
Abstract
Coherently driven phonons are conventionally described classically. Nonlinear phonon-phonon interactions, however, allow an infrared drive to reshape the fluctuation spectrum and generate substantial nonthermal enhancement of phonon fluctuations, motivating a description beyond the coherent displacement alone. We benchmark classical and semiclassical approximations against the full quantum theory and find that the semiclassical treatment substantially improves agreement with the quantum dynamics. We propose nonequilibrium spontaneous Raman scattering as a sensitive probe of these effects and apply our framework to recent experiments suggesting quantum nonlinear phononics involving the E1u and E2g modes in multilayer graphene. At very strong pump fields, driving the E1u mode significantly modifies the E2g Raman spectrum; however, reproducing the reported response at experimental field strengths requires accounting for pump-induced Raman matrix element dynamics or alternative energy pathways into the E2g mode. Our findings extend nonlinear phononics beyond average atomic displacements to the dynamics of lattice fluctuations, highlighting the interplay between coherent motion and quantum correlations in driven materials.
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BibTeX
@misc{dolgner2026probing,
title = {{Probing quantum nonlinear phononics in multilayer graphene with time-resolved Raman scattering}},
author = {Jakob Dolgner and Michael Rübhausen and Dirk Manske},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.16566},
eprint = {2610.16566},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.16566},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Probing quantum nonlinear phononics in multilayer graphene with time-resolved Raman scattering
AU - Jakob Dolgner
AU - Michael Rübhausen
AU - Dirk Manske
PY - 2026
DA - 2026/10/12
PB - arXiv
DO - 10.48550/arxiv.2610.16566
UR - https://arxiv.org/abs/2610.16566
AB - Coherently driven phonons are conventionally described classically. Nonlinear phonon-phonon interactions, however, allow an infrared drive to reshape the fluctuation spectrum and generate substantial nonthermal enhancement of phonon fluctuations, motivating a description beyond the coherent displacement alone. We benchmark classical and semiclassical approximations against the full quantum theory and find that the semiclassical treatment substantially improves agreement with the quantum dynamics. We propose nonequilibrium spontaneous Raman scattering as a sensitive probe of these effects and apply our framework to recent experiments suggesting quantum nonlinear phononics involving the E_1u and E_2g modes in multilayer graphene. At very strong pump fields, driving the E_1u mode significantly modifies the E_2g Raman spectrum; however, reproducing the reported response at experimental field strengths requires accounting for pump-induced Raman matrix element dynamics or alternative energy pathways into the E_2g mode. Our findings extend nonlinear phononics beyond average atomic displacements to the dynamics of lattice fluctuations, highlighting the interplay between coherent motion and quantum correlations in driven materials.
ER -