Non-Resonant Impulsively Stimulated Raman Scattering by a Terahertz Field: a Case Study of 1T-TaS2

Abstract

Time-domain ultrafast and nonlinear terahertz spectroscopy techniques are recently applied to many condensed matter systems for investigating their collective excitations. In centrosymmetric systems, these collective modes are typically Raman-active and therefore do not couple directly to the terahertz electric field. The mechanism by which light-matter interaction realizes in these studies has not been explicitly discussed in detail. In this work, we perform terahertz pump - optical probe and terahertz third harmonic generation investigations on 1T-TaS2, a material exhibiting a rich charge-density-wave (CDW) phase diagram including the commensurate, nearly-commensurate and incommensurate CDW phases. The transition between these distinct states leaves a clear signature on the dynamical Raman response. We investigate how the Raman-active phonons couple to a broadband monocycle terahertz field as well as a narrowband multicycle terahertz field. Our results indicate that a modified impulsively stimulated Raman scattering mechanism involving two-photon absorption, also known as non-resonant Raman scattering, underlies the coherent excitation and observation of the lattice modes. These results are relevant for future spectroscopy investigation and coherent control of collective modes using low-energy terahertz field as well as cavity electrodynamical dressing of solids.

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BibTeX RIS

BibTeX

@misc{zhang2026nonresonant,
  title = {{Non-Resonant Impulsively Stimulated Raman Scattering by a Terahertz Field: a Case Study of 1T-TaS2}},
  author = {Haotian Zhang and Yuheng Guo and Zidu Yu and Yongbo Lv and Yiting Wang and Liwen Feng and Jiaying Xu and Tianlong Xia and Xinbo Wang and Hao Chu},
  howpublished = {arXiv},
  year = {2026},
  month = sep,
  doi = {10.48550/arxiv.2609.03519},
  eprint = {2609.03519},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2609.03519},
}

RIS

TY  - UNPB
TI  - Non-Resonant Impulsively Stimulated Raman Scattering by a Terahertz Field: a Case Study of 1T-TaS2
AU  - Haotian Zhang
AU  - Yuheng Guo
AU  - Zidu Yu
AU  - Yongbo Lv
AU  - Yiting Wang
AU  - Liwen Feng
AU  - Jiaying Xu
AU  - Tianlong Xia
AU  - Xinbo Wang
AU  - Hao Chu
PY  - 2026
DA  - 2026/09/03
PB  - arXiv
DO  - 10.48550/arxiv.2609.03519
UR  - https://arxiv.org/abs/2609.03519
AB  - Time-domain ultrafast and nonlinear terahertz spectroscopy techniques are recently applied to many condensed matter systems for investigating their collective excitations. In centrosymmetric systems, these collective modes are typically Raman-active and therefore do not couple directly to the terahertz electric field. The mechanism by which light-matter interaction realizes in these studies has not been explicitly discussed in detail. In this work, we perform terahertz pump - optical probe and terahertz third harmonic generation investigations on 1T-TaS2, a material exhibiting a rich charge-density-wave (CDW) phase diagram including the commensurate, nearly-commensurate and incommensurate CDW phases. The transition between these distinct states leaves a clear signature on the dynamical Raman response. We investigate how the Raman-active phonons couple to a broadband monocycle terahertz field as well as a narrowband multicycle terahertz field. Our results indicate that a modified impulsively stimulated Raman scattering mechanism involving two-photon absorption, also known as non-resonant Raman scattering, underlies the coherent excitation and observation of the lattice modes. These results are relevant for future spectroscopy investigation and coherent control of collective modes using low-energy terahertz field as well as cavity electrodynamical dressing of solids.
ER  -

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