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arXiv · 2609.07796

Temperature-Dependent nonlinear optics from first-principles: Second-Harmonic Generation in few-layers MoS$_2$

Anna Romani·Claudio Attaccalite·Myrta Grüning
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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 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)].

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Anna Romani, Claudio Attaccalite, Myrta Grüning. 2026-09-07. Temperature-Dependent nonlinear optics from first-principles: Second-Harmonic Generation in few-layers MoS$_2$. https://arxiv.org/abs/2609.07796

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