Ultrafast Frustration-Breaking and Magnetophononic Driving of Singlet Excitations in a Quantum Magnet

TL;DR

This paper demonstrates a nonlinear magnetophononic technique using terahertz pulses to coherently drive phonons, breaking magnetic frustration in a quantum magnet and enabling ultrafast control of singlet excitations.

Contribution

It introduces a novel method to manipulate quantum spin states via simultaneous optical phonon excitation, enabling ultrafast control of magnetic interactions in frustrated magnets.

Findings

Resonant phonon driving populates singlet two-triplon states.

Breaking of magnetic frustration enables forbidden quantum phenomena.

Ultrafast manipulation of quantum many-body states achieved.

Abstract

Ideal magnetic frustration forms the basis for the emergence of exotic quantum spin states that are entirely nonmagnetic. Such singlet spin states are the defining feature of the Shastry-Sutherland model, and of its faithful materials realization in the quantum antiferromagnet SrCu$_2$(BO$_3$)$_2$. To address these states on ultrafast timescales, despite their lack of any microscopic order parameter, we introduce a nonlinear magnetophononic mechanism to alter the quantum spin dynamics by driving multiple optical phonon modes coherently and simultaneously. We apply intense terahertz pulses to create a nonequilibrium modulation of the magnetic interactions that breaks the ideal frustration of SrCu$_2$(BO$_3$)$_2$, such that previously forbidden physics can be driven in a coherent manner. Specifically, this driving populates a purely magnetic excitation, the singlet branch of the two-triplon bound state, by resonance with the difference frequency of two pumped phonons. Our results demonstrate how light-driven phonons can be used for the ultrafast and selective manipulation of interactions in condensed matter, even at frequencies far from those of the pump spectrum, offering valuable additional capabilities for the dynamical control of quantum many-body phenomena.