Temperature-Dependent nonlinear optics from first-principles: Second-Harmonic Generation in few-layers MoS2
Abstract
We present a first-principles real-time approach to study non-linear response of solids at finite temperature. Finite temperature effects are included as renormalization of the quasiparticle energies and a dephasing term proportional to the quasiparticle lifetimes. We evaluate electron-phonon matrix elements from Density-Functional Perturbation Theory for lattice dynamics and then calculate quasiparticles renormalization and lifetime from the Fan and Debye-Waller terms of the electron self-energy. Electron excitations are treated at the independent particle level of approximation. We apply the approach to the second-harmonic generation (SHG) in monolayer and trilayer MoS2. We observe a nontrivial temperature-dependence of the SHG due to a strong crystal-momentum dependent quasiparticle renormalization. From the phonon-mode analysis we find that the coupling with acoustic and shear modes determines the overall crystal-momentum dependence respectively in monolayer and trilayer MoS2. The nontrivial temperature-dependence of the SHG can help rationalize the increase of SHG intensity with increasing temperature observed in monolayer MoS2 at a given laser energy [Adv. Optical Mater. 8, 2000441 (2020)].
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BibTeX
@misc{romani2026temperaturedependent,
title = {{Temperature-Dependent nonlinear optics from first-principles: Second-Harmonic Generation in few-layers MoS$_2$}},
author = {Anna Romani and Claudio Attaccalite and Myrta Grüning},
howpublished = {HAL},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.07796},
eprint = {2609.07796},
archivePrefix = {arXiv},
url = {https://hal.science/hal-05744834v1},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Temperature-Dependent nonlinear optics from first-principles: Second-Harmonic Generation in few-layers MoS_2
AU - Anna Romani
AU - Claudio Attaccalite
AU - Myrta Grüning
PY - 2026
DA - 2026/09/07
PB - HAL
DO - 10.48550/arxiv.2609.07796
UR - https://hal.science/hal-05744834v1
AB - We present a first-principles real-time approach to study non-linear response of solids at finite temperature. Finite temperature effects are included as renormalization of the quasiparticle energies and a dephasing term proportional to the quasiparticle lifetimes. We evaluate electron-phonon matrix elements from Density-Functional Perturbation Theory for lattice dynamics and then calculate quasiparticles renormalization and lifetime from the Fan and Debye-Waller terms of the electron self-energy. Electron excitations are treated at the independent particle level of approximation. We apply the approach to the second-harmonic generation (SHG) in monolayer and trilayer MoS_2. We observe a nontrivial temperature-dependence of the SHG due to a strong crystal-momentum dependent quasiparticle renormalization. From the phonon-mode analysis we find that the coupling with acoustic and shear modes determines the overall crystal-momentum dependence respectively in monolayer and trilayer MoS_2. The nontrivial temperature-dependence of the SHG can help rationalize the increase of SHG intensity with increasing temperature observed in monolayer MoS_2 at a given laser energy [Adv. Optical Mater. 8, 2000441 (2020)].
ER -