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Physical review. B./Physical review. B

Optical selection rules of the magnetic excitation in the S=12 one-dimensional Ising-like antiferromagnet BaCo2V2O8

Shojiro Kimura, Hiroaki Onishi, Akira Okutani, Mitsuru Akaki, Yasuo Narumi, Masayuki Hagiwara, Kouichi Okunishi, Koichi Kindo, Zhangzhen He, Tomoyasu Taniyama, Mitsuru Itoh

Published Jan 18, 2022• 6 citations
Publisher

Abstract

In this study, we clarify the selection rules of optical transitions from the ground state to the magnetic excited states in the quasi-one-dimensional quantum Ising-like antiferromagnet ${\mathrm{BaCo}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}$ with spin $S=\frac{1}{2}$ using the high-field electron spin resonance measurement with illuminating polarized electromagnetic waves. We demonstrate that the unconventional magnetic excitation via the pair creation of quasipaticles at wave numbers ${q}_{z}$ = $\ensuremath{\pi}/2$ and $\ensuremath{\pi}$ in the field-induced quantum critical state can couple with both oscillating magnetic and electric fields. Our density matrix renormalization group calculations indicate that the observed selection rules can be explained by two- and four-fold periodical spin interactions, originating from the screw chain structure in ${\mathrm{BaCo}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}$, in addition to the magnetoelectric coupling between spins and electric dipoles.

DOI
10.1103/physrevb.105.014417

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In this study, we clarify the selection rules of optical transitions from the ground state to the magnetic excited states in the quasi-one-dimensional quantum Ising-like antiferromagnet BaCo2V2O8{\mathrm{BaCo}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}BaCo2​V2​O8​ with spin S=12S=\frac{1}{2}S=21​ using the high-field electron spin resonance measurement with illuminating polarized electromagnetic waves. We demonstrate that the unconventional magnetic excitation via the pair creation of quasipaticles at wave numbers qz{q}_{z}qz​ = \ensuremathπ/2\ensuremath{\pi}/2\ensuremathπ/2 and \ensuremathπ\ensuremath{\pi}\ensuremathπ in the field-induced quantum critical state can couple with both oscillating magnetic and electric fields. Our density matrix renormalization group calculations indicate that the observed selection rules can be explained by two- and four-fold periodical spin interactions, originating from the screw chain structure in BaCo2V2O8{\mathrm{BaCo}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}BaCo2​V2​O8​, in addition to the magnetoelectric coupling between spins and electric dipoles.
In this study, we clarify the selection rules of optical transitions from the ground state to the magnetic excited states in the quasi-one-dimensional quantum Ising-like antiferromagnet BaCo2V2O8 with spin S = 1 2 using the high-field electron spin resonance measurement with illuminating polarized electromagnetic waves.We demonstrate that the unconventional magnetic excitation via the pair creation of quasipaticles at wave numbers qz = π/2 and π in the field-induced quantum critical state can couple with both oscillating magnetic and electric fields. Our density matrix renormalization group calculations indicate that the observed selection rules can be explained by two- and four-fold periodical spin interactions, originating from the screw chain structure in BaCo2V2O8, in addition to the magnetoelectric coupling between spins and electric dipoles.
The high-field multifrequency electron spin resonance (ESR), the magnetization, and the specific heat of single crystals of BaCo2V2O8 (a quasi-one-dimensional Ising-like antiferromagnet with S = 1/2) were measured in two different transverse magnetic fields: H || [100] and H || [110]. A softening of the lowest ESR mode was observed near the saturation field of the magnetization around 40 T in H || [110], whereas it occurs around 10 T in H || [100], far below the saturation field. These observations were reproduced by numerical calculations using the density-matrix renormalization group methods, including the staggered magnetic fields induced by a uniform external magnetic field and the interchain magnetic exchange interaction. We found that the directional dependence of the lowest mode originates mainly from the remarkable angular dependence of the induced magnetic field. The interchain interaction is also quantitatively important for reproducing the experimental results. The directional dependence of the lowest mode is demonstrated by the particle–hole excitation of spinons using the Jordan–Wigner transformation.
By combining inelastic neutron scattering and numerical simulations, we study the quasi-one-dimensional Ising-like quantum antiferromagnet BaCo2V2O8{\mathrm{BaCo}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}BaCo2​V2​O8​ in a longitudinal magnetic field applied along the Ising anisotropy, which is also the chain direction. The external field closes the excitation gap due to the magnetic anisotropy, inducing a transition from the N\'eel ordered state to an incommensurate longitudinal spin density wave phase. If the field is increased further, another transition into a transverse antiferromagnetic phase takes place at 9 T due to the competition between longitudinal and transverse correlations. We numerically and experimentally show that the model of XXZ chains connected by a weak interchain interaction well reproduces this transition. We also calculate the dynamical susceptibility and demonstrate that it agrees quantitatively with inelastic neutron scattering measurements. In contrast to the abrupt change of magnetic ordering, the spectra do not change much at the transition at 9 T, and the spin dynamics can be described as a Tomonaga-Luttinger liquid. We also refine the modeling of BaCo2V2O8{\mathrm{BaCo}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}BaCo2​V2​O8​ by including a four-site periodic term arising from the crystal structure which enables one to account for an anomaly of the magnetic susceptibility appearing at 19.5 T, as well as for the anticrossing observed in the inelastic neutron scattering spectra.
We study the dynamics of the quasi-one-dimensional Ising-Heisenberg antiferromagnet BaCo2V2O8{\mathrm{BaCo}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}BaCo2​V2​O8​ under a transverse magnetic field. Combining inelastic neutron scattering experiments and theoretical analyses by field theories and numerical simulations, we mainly elucidate the structure of the spin excitation spectrum in the high-field phase, appearing above the quantum phase transition point ${\ensuremath{\mu}}_{0}{H}_{c}\ensuremath{\approx}10\phantom{\rule{0.28em}{0ex}}\mathrm{T}$. We find that it is characterized by collective solitonic excitations superimposed on a continuum. These solitons are strongly bound in pairs due to the effective staggered field induced by the nondiagonal ggg tensor of the compound and are topologically different from the fractionalized spinons in the weak-field region. The dynamical susceptibility numerically calculated with the infinite time-evolving block decimation method shows an excellent agreement with the measured spectra, which enables us to identify the dispersion branches with elementary excitations. The lowest-energy dispersion has an incommensurate nature and has a local minimum at an irrational wave number due to the applied transverse field.
Near the transverse-field-induced quantum critical point of the Ising chain, an exotic dynamic spectrum consisting of exactly eight particles was predicted, which is uniquely described by an emergent quantum integrable field theory with the symmetry of the E8{E}_{8}E8​ Lie algebra, but rarely explored experimentally. Here we use high-resolution terahertz spectroscopy to resolve quantum spin dynamics of the quasi-one-dimensional Ising antiferromagnet BaCo2V2O8\mathrm{BaC}{\mathrm{o}}_{2}{\mathrm{V}}_{2}{\mathrm{O}}_{8}BaCo2​V2​O8​ in an applied transverse field. By comparing to an analytical calculation of the dynamical spin correlations, we identify E8{E}_{8}E8​ particles as well as their two-particle excitations.
Abstract We report on high-resolution terahertz spectroscopic studies of quantum spin dynamics in the quasi-one-dimensional Ising-like ferromagnet CoNb2O6 and antiferromagnet BaCo2V2O8 as a function of an applied transverse magnetic field. In the ordered phases stabilized by inter-chain couplings, we reveal characteristics for confined spinon excitations, E 8 dynamical spectrum, and field-induced quantum phase transitions. The connections between these characteristic dynamical features are found in the field-dependent evolution of the excitation spectra.