Revealing Quadrupolar Excitations with Non-Linear Spectroscopy

TL;DR

This paper demonstrates that two-dimensional coherent spectroscopy can detect quadrupolar excitations in spin-1 quantum magnets, overcoming limitations of linear response methods and providing new insights into multipolar quasiparticles.

Contribution

It introduces the use of non-linear spectroscopy, specifically 2DCS, to observe quadrupolar excitations in spin-1 systems, a feat difficult with traditional linear probes.

Findings

2DCS reveals quadrupolar excitations in spin-1 ferromagnets.

2DCS provides access to quadrupolar spectral weight.

The method combines exact diagonalization and spin wave theory.

Abstract

Local moments with a spin $S>1/2$ can exhibit a rich variety of elementary quasiparticle excitations, such as quadrupolar excitations, that go beyond the dipolar magnons of conventional spin-$1/2$ systems. However, the experimental observation of such quadrupolar excitations is often challenging due to the dipolar selection rules of many linear response probes, rendering them invisible. Here we show that non-linear spectroscopy, in the form of two-dimensional coherent spectroscopy (2DCS), can be used to reveal quadrupolar excitations. Considering a family of spin-1 Heisenberg ferromagnets with single-ion easy-axis anisotropy as an example, we explicitly calculate their 2DCS signature by combining exact diagonalization and generalized spin wave theory. We further demonstrate that 2DCS can provide access to the quadrupolar weight of an excitation, analogous to how linear response provides access to the dipolar weight. Our work highlights the potential of non-linear spectroscopy as a powerful tool to diagnose multipolar excitations in quantum magnets.