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arXiv:1010.4476 · Physical Review B

Effect of Dzyaloshinskii-Moriya interactions on the phase diagram and magnetic excitations of SrCu 2 (BO 3 ) 2

Judit Romhányi, Keisuke Totsuka, Karlo Penc

Published Jan 26, 2011• 47 citations
arXivHTMLPDF

Abstract

The orthogonal dimer structure of the SrCu${}_{2}$(BO${}_{3}$)${}_{2}$ spin-1/2 magnet provides a realization of the Shastry--Sutherland model. Using a dimer-product variational wave function, we map out the phase diagram of the Shastry--Sutherland model including anisotropies. Based on the variational solution, we construct a bond-wave approach to obtain the excitation spectra as a function of the magnetic field. The characteristic features of the experimentally measured neutron and ESR spectra are reproduced, like the anisotropy-induced zero-field splittings and the persistent gap at higher fields.

DOI
10.1103/physrevb.83.024413

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The orthogonal dimer structure of the SrCu2{}_{2}2​(BO3{}_{3}3​)2{}_{2}2​ spin-1/2 magnet provides a realization of the Shastry--Sutherland model. Using a dimer-product variational wave function, we map out the phase diagram of the Shastry--Sutherland model including anisotropies. Based on the variational solution, we construct a bond-wave approach to obtain the excitation spectra as a function of the magnetic field. The characteristic features of the experimentally measured neutron and ESR spectra are reproduced, like the anisotropy-induced zero-field splittings and the persistent gap at higher fields.
The magnetic properties of SrCu 2 (BO 3 ) 2 are reviewed from a theoretical point of view. SrCu 2 (BO 3 ) 2 is a new two-dimensional spin gap system and its magnetic properties are well described by a spin-1/2 antiferromagnetic Heisenberg model of the orthogonal dimer lattice. The model has a dimer singlet ground state whose exactness was proven by Shastry and Sutherland for a topologically equivalent model more than 20 years ago. The exactness of the ground state is maintained even if interlayer couplings are introduced for SrCu 2 (BO 3 ) 2 . In the two-dimensional model, quantum phase transitions take place between different ground states for which three phases are expected: a gapped dimer singlet state, a plaquette resonating valence bond state and a gapless magnetic ordered state. Analysis of the experimental data shows that the dimer singlet ground state is realized in SrCu 2 (BO 3 ) 2 . The orthogonality of the dimer bonds, which is the underlying symmetry of the exactness of the ground state, also leads to an unusual property of elementary excitations, namely the almost localized nature of the triplet excitations. Application of an external magnetic field changes the density of the triplet excitations. In general, there is competition between kinetic energies and interaction energies between triplets. The almost localized nature of the triplets makes it easy to form regular lattices. In fact, at certain densities, where the commensurability energy is significant, the triplet excitations form superstructures and plateaux appear at 1/2, 1/3, 1/4 and 1/8 in the magnetization curve. In high-magnetic-field experiments, magnetic plateaux at magnetizations of 1/3, 1/4 and 1/8 have been observed. Translational symmetry of the lattice is spontaneously broken at the plateaux, except for the 1/2 plateau. The 1/3 and 1/4 plateaux are expected to have magnetic superstructures of stripe form while the 1/2 plateau has a square unit cell and the 1/8 plateau a rhomboid cell. Especially at the 1/8 plateau, nuclear magnetic resonance experiments indicate the presence of at least 11 distinct Cu sites with different spin polarizations, which is the first evidence of breaking of the translational symmetry at the plateau phase. The spin texture calculated on the basis of a Heisenberg model with adiabatic spin–phonon coupling is consistent with the experimental results.
The recent ESR measurement on the Shastry-Sutherland compound SrCu 2 (BO 3 ) 2 detected the pressure-induced phase transition that is expected to correspond to the quantum phase transition from the orthogonal dimer to the plaquette singlet phases.In this experiment the pressure dependence of the spin gap was observed by ESR.The ESR transition of the spin gap is forbidden due to the spin conservation law, but the Dzyaloshinsky-Moriya interaction of this compound enables the observation.Then the selection rule of the ESR transition of the spin gap in the presence ot the Dzyaloshinsky-Moriya interaction is investigated using the numerical diagonalization of the Shastry-Sutherland model.As a result, it is found that the selection rule changes at the quantum phase transition between the dimer and the plaquette singlet phases.
We have studied spin excitation spectra in the Shastry-Sutherland model compound SrCu2(BO3)2\mathrm{Sr}{\mathrm{Cu}}_{2}{(\mathrm{B}{\mathrm{O}}_{3})}_{2}SrCu2​(BO3​)2​ in magnetic fields using far-infrared Fourier spectroscopy. The transitions from the ground singlet state to the triplet state at $24\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ and to several bound triplet states are induced by the electric field component of the far-infrared light. To explain the light absorption in the spin system we invoke a dynamic Dzyaloshinskii-Moriya (DM) mechanism where light couples to a phonon mode, allowing the DM interaction. Two optical phonons couple light to the singlet to triplet transition in SrCu2(BO3)2\mathrm{Sr}{\mathrm{Cu}}_{2}{(\mathrm{B}{\mathrm{O}}_{3})}_{2}SrCu2​(BO3​)2​. One is aaa-polarized and creates an intradimer dynamic DM along the ccc axis. The other is ccc-polarized and creates an intradimer dynamic DM interaction, it is in the (ab)(ab)(ab) plane and perpendicular to the dimer axis. Singlet levels at 21.5 and $28.6\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ anticross with the first triplet as is seen in far-infrared spectra. We used a cluster of two dimers with a periodic boundary condition to perform a model calculation with scaled intra- and interdimer exchange interactions. Two static DM interactions are sufficient to describe the observed triplet state spectra. The static interdimer DM in the ccc-direction ${d}_{1}=0.7\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ splits the triplet state sublevels in zero field [C\'epas et al., Phys. Rev. Lett. 87, 167205 (2001)]. The static intradimer DM in the (ab)(ab)(ab) plane (perpendicular to the dimer axis) ${d}_{2}=1.8\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$, allowed by the buckling of CuBO3\mathrm{Cu}\mathrm{B}{\mathrm{O}}_{3}CuBO3​ planes, couples the triplet state to the $28.6\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ singlet as is seen from the avoided crossing.
Anomalous thermal broadening in the Shastry-Sutherland model and SrCu2(_2(2​(BO3)2_3)_23​)2​
The quantum magnet SrCu2(_2(2​(BO3)2_3)_23​)2​ and its remarkably accurate theoretical description, the spin-1/21/21/2 Shastry-Sutherland model, host a variety of intriguing phenomena such as a dimer ground state with a nearly flat band of triplon excitations, a series of magnetization plateaux, and a possible pressure-induced deconfined quantum critical point. One open puzzle originating from inelastic neutron scattering and Raman experiments is the anomalous broadening of the triplon modes at relatively low temperatures compared to the triplon gap ΔΔΔ. We demonstrate that the experimentally observed broadening is captured by the Shastry-Sutherland model. To this end, we develop a numerical simulation method based on matrix-product states to simulate dynamical spectral functions at nonzero temperatures accurately. Perturbative calculations identify the origin of this phenomenon as a small energy scale compared to ΔΔΔ between single triplon and bound triplon states at the experimentally relevant model parameters.
By using the perturbation expansion up to the fifth order, we study the two-triplet-dimer excitation spectra in the Shastry-Sutherland model, where the localized nature of a triplet-dimer, the propagation of a triplet-dimer pair by the correlated hopping and the long-range interactions between triplet-dimers play an essential role. It is found that the dispersion relations for first-neighbor triplet-dimer pair excitations with S=1 and p-type symmetry qualitatively explain the second-lowest branch observed in the neutron inelastic scattering experiment. It is also predicted that the second-lowest branch consists of two components, p_x- and p_y-states, with slightly different excitation energies. The origin of the singlet mode at 3.7meV observed in the Raman scattering experiment is also discussed.
We calculate the electron spin resonance (ESR) spectra of the quasi-two-dimensional dimer spin liquid SrCu2(BO3)2\mathrm{Sr}{\mathrm{Cu}}_{2}{(\mathrm{B}{\mathrm{O}}_{3})}_{2}SrCu2​(BO3​)2​ as a function of magnetic field BBB. Using the standard Lanczos method, we solve a Shastry-Sutherland Hamiltonian with additional Dzyaloshinsky-Moriya (DM) terms which are crucial to explain different qualitative aspects of the ESR spectra. In particular, a nearest-neighbor DM interaction with a nonzero Dz{D}_{z}Dz​ component is required to explain the low frequency ESR lines for $B\ensuremath{\Vert}c$. This suggests that crystal symmetry is lowered at low temperatures due to a structural phase transition.