Published June 18, 2025 | Version Published
Journal Article Open

Phonon-Driven Multipolar Dynamics in a Spin-Orbit Coupled Mott Insulator

  • 1. ROR icon University of Toronto
  • 2. ROR icon California Institute of Technology

Abstract

Motivated by advances in pump-probe experiments and light-driven phenomena, we theoretically study the impact of pumped and driven phonons in Mott insulators which host multipole moments, thus going beyond conventional dipolar magnetism. As a case study, we examine pseudospin-1/2 Mott insulators hosting quadrupolar and octupolar moments, and investigate the effect of resonantly exciting ℰ𝑔 phonon modes which couple linearly to the quadrupoles. We show that this leads to multipolar precession, with the backaction resulting in pseudochiral phonon dynamics in the octupolar ordered phase. We further study the impact of a short-time two-phonon drive, showing that it can induce the buildup of octupolar order or even switch its sign on picosecond timescales. Our results are obtained using a Monte Carlo code incorporating phonons, molecular dynamics simulations to numerically integrate the coupled spin-phonon equations of motion, and analytical Floquet theory. Our work shows how driven phonons can probe and control hidden orders in solids.

Copyright and License

© 2025 American Physical Society.

Acknowledgement

This research was funded by Discovery Grant RGPIN-2021-03214 from the Natural Sciences and Engineering Research Council (NSERC) of Canada (A. P.), an Ontario Graduate Scholarship (K. H.), and an NSERC CGS-D fellowship (R. S.). We thank Sreekar Voleti, David Hsieh, Prashant Padmanabhan, Emily Zhang, William Bateman-Hemphill, and Cristian Batista for extremely helpful discussions. Numerical computations were performed on the Niagara supercomputer at the SciNet HPC Consortium and the Digital Research Alliance of Canada.

Data Availability

The data that support the findings of this Letter are openly available [86].

Supplemental Material

Supplemental Material contains details of (i) Short-time phonon dynamics in the pump-probe regime, (ii) Mean field model of pseudospin-phonon dynamics, (iii) Floquet-Magnus expansion, (iv) Mean field model of octupolar switching, (v) Damping dependence of octupolar and phonon dynamics, and (vi) Octupolar switching for low damping and continuous drive.

Multipolar_SM.pdf

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Additional details

Related works

Is new version of
Discussion Paper: arXiv:2404.17633 (arXiv)
Is supplemented by
Supplemental Material: https://journals.aps.org/prl/supplemental/10.1103/1rmw-pd6n/Multipolar_SM.pdf (URL)
Dataset: https://github.com/khart9/DataMultipolarPRL2025.git (URL)

Funding

Natural Sciences and Engineering Research Council
RGPIN-2021-03214
Government of Ontario
Ontario Graduate Scholarship -

Dates

Accepted
2025-05-12

Caltech Custom Metadata

Caltech groups
Institute for Quantum Information and Matter, Division of Physics, Mathematics and Astronomy (PMA)
Publication Status
Published