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arXiv:2407.03691 · Physical review. B./Physical review. B

Triplons, triplon pairs, and dynamical symmetries in laser-driven Shastry-Sutherland magnets

Mina Udono, Masahiro Sato

Published Nov 21, 2024• 3 citations
arXivHTMLPDF

Abstract

In frustrated magnets, a variety of novel phenomena arise due to their peculiar magnetic states, whose excitations usually reside in the GHz to THz range. Intense THz lasers, therefore, lead to examining nonlinear optical effects in such magnets. Employing an unbiased numerical method, we calculate the laser-pulse driven harmonic spectra of the Shastry-Sutherland magnets, which are well known as the model of a quantum frustrated magnet $\mathrm{SrCu}{}_{2}$($\mathrm{BO}{}_{3}$)${}_{2}$. As a result, nonlinear responses of triplons and a two-triplon bound state are numerically shown to emerge through the Zeeman or magnetoelectric couplings between the laser and the electron spin. Furthermore, the dynamical symmetries and selection rules of harmonic spectra for the Shastry-Sutherland model realized in $\mathrm{SrCu}{}_{2}$($\mathrm{BO}{}_{3}$)${}_{2}$, are derived. The selection rules tell us that one can obtain information on magnetic anisotropy and symmetry from the spectra by manipulating external fields or two-color lasers. Our results indicate that laser-driven harmonic spectra are useful as a probe of less-detectable quantum many-body states in frustrated magnets.

DOI
10.1103/physrevb.110.l201112

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Abstract The Shastry–Sutherland compound SrCu2(BO3)2constituting orthogonally coupled dimers harbors anS = 0 singlet ground state. The confluence of strong interdimer interaction and frustration engenders a spectrum of low-energy excitations including localized triplons as well as singlet and triplet bound states. Their dynamics are controlled by an external magnetic field and temperature. Here, we employ high-field Raman spectroscopy to map the field and temperature evolution of such bosonic composite quasiparticles on approaching the 1/8 magnetization plateau. Our study unveils that the magnetic field and thermal fluctuations show remarkably similar effects in melting the singlet bound states, but are disparate in their effects on the fine spectral shapes. This, together with the anti-crossing of two singlet bound states in the intermediate fieldB = 10 − 16 T, is discussed in terms of the correlated dynamics of frustrated, interacting bosons.
The temperature dependence of the gapped triplet excitations (triplons) in the 2D Shastry-Sutherland quantum magnet SrCu(2)(BO(3))(2) is studied by means of inelastic neutron scattering. The excitation amplitude rapidly decreases as a function of temperature, while the integrated spectral weight can be explained by an isolated dimer model up to 10 K. Analyzing this anomalous spectral line shape in terms of damped harmonic oscillators shows that the observed damping is due to a two-component process: one component remains sharp and resolution limited while the second broadens. We explain the underlying mechanism through a simple yet quantitatively accurate model of correlated decay of triplons: an excited triplon is long lived if no thermally populated triplons are nearby but decays quickly if there are. The phenomenon is a direct consequence of frustration induced triplon localization in the Shastry-Sutherland lattice.
In the quantum magnet SrCu2(BO3)2, an anomalous thermal broadening of the triplon modes has been measured at relatively low temperatures compared to the triplon gap A using both inelastic neutron scattering and Raman spectroscopy. Given how accurately a broad variety of physical phenomena in SrCu2(BO3)2 are captured by the spin S = 1/2 Shastry-Sutherland model, it remains an open question whether the anomalous thermal broadening is also an intrinsic feature of this minimal model. However, few techniques are available for computing the finite-temperature dynamics of strongly interacting many-body systems. To address this problem, we have developed a broadly applicable numerical simulation method based on matrix-product states to simulate dynamical spectral functions at nonzero temperatures accurately, detailed in a companion paper [Phys. Rev. B 113, 024406 (2026)]. Using this technique, we demonstrate that the experimentally observed broadening is captured by the Shastry-Sutherland model. Perturbative calculations identify the origin of this phenomenon as singlet bound two-triplon states being thermally excited at an energy scale small compared to the gap A to the single triplon excitations at the experimentally relevant model parameters.
Frustrated magnets host rich emergent behavior because competing interactions generate dense manifolds of low-energy states. The Ising Shastry-Sutherland model is a paradigmatic setting, motivated experimentally by Ising-like rare-earth tetraborides such as TmB4_44​ and ErB4_44​, whose field-induced magnetization plateaus have motivated extensive microscopic modeling. Yet how tunable quantum fluctuations reorganize this material-motivated phase diagram remains largely unexplored. Here, we realize a transverse- and longitudinal-field Ising model on the Shastry-Sutherland lattice using a programmable Rydberg-atom array. We map its quantum phase diagram using density matrix renormalization group calculations and probe corresponding signatures experimentally in arrays containing more than 110 atoms. Beyond the established classical phases, the calculations identify two regimes absent in the classical limit and stabilized at finite transverse field: a 2/52/52/5 filling plateau whose finite stability region emerges from a classically degenerate phase boundary and a symmetry-preserving quantum-dimer regime replacing classically selected collinear order. Experiments on finite open arrays reveal signatures consistent with these regimes across three boundary-pinning conditions, with the resulting response maps agreeing qualitatively with the calculated phase diagram. Our results establish programmable Rydberg-atom arrays as tools for exploring frustrated, material-motivated Hamiltonians and motivate searches for new, quantum-driven magnetization plateaus and quantum-dimer behavior in ErB4_44​ under a transverse field or in strain-tuned TmB4_44​.