Unambiguous identification of fractionalized excitations in quantum spin liquids has been a long-standing issue in correlated topological phases. Conventional spectroscopic probes, such as the dynamical spin structure factor, can only detect composites of fractionalized excitations, leading to a broad continuum in energy. Lacking a clear signature in conventional probes has been the biggest obstacle in the field. In this work, we theoretically investigate what kinds of distinctive signatures of fractionalized excitations can be probed in two-dimensional nonlinear spectroscopy by considering the exactly solvable Kitaev spin liquids. We demonstrate the existence of a number of salient features of the Majorana fermions and fluxes in two-dimensional nonlinear spectroscopy, which provide crucial information about such excitations.Unambiguous identification of fractionalized excitations in quantum spin liquids has been a long-standing issue in correlated topological phases. Conventional spectroscopic probes, such as the dynamical spin structure factor, can only detect composites of fractionalized excitations, leading to a broad continuum in energy. Lacking a clear signature in conventional probes has been the biggest obstacle in the field. In this work, we theoretically investigate what kinds of distinctive signatures of fractionalized excitations can be probed in two-dimensional nonlinear spectroscopy by considering the exactly solvable Kitaev spin liquids. We demonstrate the existence of a number of salient features of the Majorana fermions and fluxes in two-dimensional nonlinear spectroscopy, which provide crucial information about such excitations.

arXiv:1911.07138Physical Review LettersMar 20, 202067 citations

Quantum Spin Liquids: Signatures of Fractionalization

Nandini Trivedi

Nov 1, 20190 citations

Probing signatures of fractionalization in the candidate quantum spin liquid Cu2IrO3 via anomalous Raman scattering

Srishti Pal, Arnab Seth, Piyush Sakrikar +5 more

Long-range entanglement in quantum spin liquids (QSLs) leads to novel low-energy excitations with fractionalized quantum numbers and (in two dimensions) statistics. Experimental detection and manipulation of these excitations present a challenge particularly in view of diverse candidate magnets. A promising probe of fractionalization is their coupling to phonons. Here, we present Raman scattering results for the $S=1/2$ honeycomb iridate ${\mathrm{Cu}}_{2}{\mathrm{IrO}}_{3}$ , a candidate Kitaev QSL with fractionalized Majorana fermions and Ising flux excitations. We observe anomalous low-temperature frequency shift and linewidth broadening of the Raman intensities in addition to a broad magnetic continuum, both of which, as we derive, are naturally attributed to the phonon decaying into itinerant Majoranas. The dynamic Raman susceptibility marks a crossover from the QSL to a thermal paramagnet at $\ensuremath{\sim}120$ K. The phonon anomalies below this temperature demonstrate a strong phonon-Majorana coupling. These results provide evidence of spin fractionalization in ${\mathrm{Cu}}_{2}{\mathrm{IrO}}_{3}$ .Long-range entanglement in quantum spin liquids (QSLs) leads to novel low-energy excitations with fractionalized quantum numbers and (in two dimensions) statistics. Experimental detection and manipulation of these excitations present a challenge particularly in view of diverse candidate magnets. A promising probe of fractionalization is their coupling to phonons. Here, we present Raman scattering results for the $S=1/2$ honeycomb iridate ${\mathrm{Cu}}_{2}{\mathrm{IrO}}_{3}$, a candidate Kitaev QSL with fractionalized Majorana fermions and Ising flux excitations. We observe anomalous low-temperature frequency shift and linewidth broadening of the Raman intensities in addition to a broad magnetic continuum, both of which, as we derive, are naturally attributed to the phonon decaying into itinerant Majoranas. The dynamic Raman susceptibility marks a crossover from the QSL to a thermal paramagnet at $\ensuremath{\sim}120$ K. The phonon anomalies below this temperature demonstrate a strong phonon-Majorana coupling. These results provide evidence of spin fractionalization in ${\mathrm{Cu}}_{2}{\mathrm{IrO}}_{3}$.

arXiv:2011.00606Physical review. B./Physical review. BNov 17, 202123 citations

Probing Majorana wavefunctions in Kitaev honeycomb spin liquids with second-order two-dimensional spectroscopy

Yihua Qiang, Victor L. Quito, Thaís V. Trevisan +1 more

Two-dimensional coherent terahertz spectroscopy (2DCS) emerges as a valuable tool to probe the nature, couplings, and lifetimes of excitations in quantum materials. It thus promises to identify unique signatures of spin liquid states in quantum magnets by directly probing properties of their exotic fractionalized excitations. Here, we calculate the second-order 2DCS of the Kitaev honeycomb model and demonstrate that distinct spin liquid fingerprints appear already in this lowest-order nonlinear response $χ^{(2)}_{yzx}(ω_1, ω_2)$ when using crossed light polarizations. We further relate the off-diagonal 2DCS peaks to the localized nature of the matter Majorana excitations trapped by $\mathbb{Z}_2$ flux excitations and show that 2DCS thus directly probes the inverse participation ratio of Majorana wavefunctions. By providing experimentally observable features of spin liquid states in the 2D spectrum, our work can guide future 2DCS experiments on Kitaev magnets.Two-dimensional coherent terahertz spectroscopy (2DCS) emerges as a valuable tool to probe the nature, couplings, and lifetimes of excitations in quantum materials. It thus promises to identify unique signatures of spin liquid states in quantum magnets by directly probing properties of their exotic fractionalized excitations. Here, we calculate the second-order 2DCS of the Kitaev honeycomb model and demonstrate that distinct spin liquid fingerprints appear already in this lowest-order nonlinear response $χ^{(2)}_{yzx}(ω_1, ω_2)$ when using crossed light polarizations. We further relate the off-diagonal 2DCS peaks to the localized nature of the matter Majorana excitations trapped by $\mathbb{Z}_2$ flux excitations and show that 2DCS thus directly probes the inverse participation ratio of Majorana wavefunctions. By providing experimentally observable features of spin liquid states in the 2D spectrum, our work can guide future 2DCS experiments on Kitaev magnets.

arXiv:2301.11243Jan 26, 20233 citations

Highly Mobile Gapless Excitations in a Two-Dimensional Candidate Quantum Spin Liquid

穣山下

ScienceJan 1, 20100 citations

S=1/2

honeycomb iridate

{\mathrm{Cu}}_{2}{\mathrm{IrO}}_{3}

, a candidate Kitaev QSL with fractionalized Majorana fermions and Ising flux excitations. We observe anomalous low-temperature frequency shift and linewidth broadening of the Raman intensities in addition to a broad magnetic continuum, both of which, as we derive, are naturally attributed to the phonon decaying into itinerant Majoranas. The dynamic Raman susceptibility marks a crossover from the QSL to a thermal paramagnet at $\ensuremath{\sim}120$ K. The phonon anomalies below this temperature demonstrate a strong phonon-Majorana coupling. These results provide evidence of spin fractionalization in

{\mathrm{Cu}}_{2}{\mathrm{IrO}}_{3}

χ^{(2)}_{yzx}(ω_1, ω_2)

when using crossed light polarizations. We further relate the off-diagonal 2DCS peaks to the localized nature of the matter Majorana excitations trapped by

\mathbb{Z}_2

flux excitations and show that 2DCS thus directly probes the inverse participation ratio of Majorana wavefunctions. By providing experimentally observable features of spin liquid states in the 2D spectrum, our work can guide future 2DCS experiments on Kitaev magnets.