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PreprintCC BY 4.0arXiv

All-Optical Control of Interfacial Polarization in MoS2/WSe2 Heterobilayers

  • Muhammad Sufyan Ramzan
  • Giancarlo Soavi
  • Caterina Cocchi
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Abstract

All-optical tuning of van der Waals heterostructures with coherent radiation offers a promising path toward ultrafast memory and optoelectronic devices. In the first-principles framework of real-time time-dependent density functional theory, we predict the induction of a persistent, long-lived out-of-plane polarization in MoS2/WSe2 heterobilayers, resonantly driven by intense ultrafast pulses. While weak fields preserve the intrinsic type-II band alignment, intermediate intensities trigger a four-fold enhancement of interlayer charge transfer. By analyzing the high-harmonic generation spectrum, we identify a transition from the perturbative to the strong-field regime inducing photoinduced interfacial polarity. We additionally show that lattice strain, ubiquitously present in heterobilayers, can be used as additional knob to adjust the resonant condition without compromising the permanent dipole induction. Our findings provide a theoretical blueprint for the all-optical manipulation of polar phases in low-dimensional heterostructures at the femtosecond scale.

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Cite

BibTeXRIS
BibTeX
@misc{ramzan2026alloptical,
  title = {{All-Optical Control of Interfacial Polarization in MoS$_2$/WSe$_2$ Heterobilayers}},
  author = {Muhammad Sufyan Ramzan and Giancarlo Soavi and Caterina Cocchi},
  howpublished = {arXiv},
  year = {2026},
  month = sep,
  doi = {10.48550/arxiv.2608.21493},
  eprint = {2608.21493},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2608.21493},
  note = {CC BY 4.0},
}
RIS
TY  - UNPB
TI  - All-Optical Control of Interfacial Polarization in MoS_2/WSe_2 Heterobilayers
AU  - Muhammad Sufyan Ramzan
AU  - Giancarlo Soavi
AU  - Caterina Cocchi
PY  - 2026
DA  - 2026/09/14
PB  - arXiv
DO  - 10.48550/arxiv.2608.21493
UR  - https://arxiv.org/abs/2608.21493
AB  - All-optical tuning of van der Waals heterostructures with coherent radiation offers a promising path toward ultrafast memory and optoelectronic devices. In the first-principles framework of real-time time-dependent density functional theory, we predict the induction of a persistent, long-lived out-of-plane polarization in MoS_2/WSe_2 heterobilayers, resonantly driven by intense ultrafast pulses. While weak fields preserve the intrinsic type-II band alignment, intermediate intensities trigger a four-fold enhancement of interlayer charge transfer. By analyzing the high-harmonic generation spectrum, we identify a transition from the perturbative to the strong-field regime inducing photoinduced interfacial polarity. We additionally show that lattice strain, ubiquitously present in heterobilayers, can be used as additional knob to adjust the resonant condition without compromising the permanent dipole induction. Our findings provide a theoretical blueprint for the all-optical manipulation of polar phases in low-dimensional heterostructures at the femtosecond scale.
ER  -