In this work, we investigate the evolution and settling of magnon condensation in the spin-1/2 dimer system Sr$_{3}$Cr$_{2}$O$_{8}$ using a combination of magnetostriction in pulsed fields and inelastic neutron scattering in a continuous magnetic field. The magnetic structure in the Bose-Einstein condensation (BEC) phase was probed by neutron diffraction in pulsed magnetic fields up to 39~T. The magnetic structure in this phase was confirmed to be an XY-antiferromagnetic structure validated by irreducible representational analysis. The magnetic phase diagram as a function of an applied magnetic field for this system is presented. Furthermore, zero-field neutron diffraction results indicate that dimerization plays an important role in stabilizing the low-temperature crystal structure.
Sr$_{3}$Cr$_{2}$O$_{8}$ consist of a lattice of spin-1/2 Cr$^{5+}$ ions, which form hexagonal bilayers and which are paired into dimers by the dominant antiferromagnetic intrabilayer coupling. The dimers are coupled three-dimensionally by frustrated interdimer interactions. A structural distortion from hexagonal to monoclinic leads to orbital order and lifts the frustration giving rise to spatially anisotropic exchange interactions. We have grown large single crystals of Sr$_{3}$Cr$_{2}$O$_{8}$ and have performed DC susceptibility, high field magnetisation and inelastic neutron scattering measurements. The neutron scattering experiments reveal three gapped and dispersive singlet to triplet modes arising from the three twinned domains that form below the transition thus confirming the picture of orbital ordering. The exchange interactions are extracted by comparing the data to a Random Phase Approximation model and the dimer coupling is found to be $J_{0}=5.55$ meV, while the ratio of interdimer to intradimer exchange constants is $J/J_{0}=0.64$. The results are compared to those for other gapped magnets.
Bose-Einstein condensation (BEC) of triplet excitations triggered by a magnetic field, sometimes called magnon BEC, in dimerized antiferromagnets gives rise to a long-range antiferromagnetic order in the plane perpendicular to the applied magnetic field. To explore the effects of spin-orbit coupling on magnon condensation, we study the spin model on the distorted honeycomb lattice with dimerized Heisenberg exchange ($J$ terms) and uniform off-diagonal exchange ($Gamma$ terms) interactions. By using variational Monte Carlo method and spin wave theory, we find that an out-of-plane magnetic field can induce different types of long-range magnetic orders, no matter if the ground state is a non-magnetic dimerized state or an antiferromagnetically ordered N{e}el state. Furthermore, the critical properties of field-driven phase transitions in systems with spin-orbit coupling can be different from the conventional magnon BEC. Our study is helpful to understand the rich phases of spin-orbit coupled antiferromagnets in an external magnetic field.
In $A_{3}$Cr$_{2}$O$_{8}$, where $A$ = Sr or Ba, the Cr$^{5+}$ ions surrounded by oxygen ions in a tetrahedral coordination are Jahn-Teller active. The Jahn-Teller distortion leads to a structural transition and a related emergence of three twinned monoclinic domains below the structural phase transition. This transition is highly dynamic over an extended temperature range for $A$ = Sr. We have investigated mixed compounds Ba$_{3-x}$Sr$_{x}$Cr$_{2}$O$_{8}$ with $x=2.9$ and $x=2.8$ by means of X-ray and neutron diffraction, Raman scattering and calorimetry. Based on the obtained evolution of the phonon frequencies, we find a distinct suppression of the orbital-lattice fluctuation regime with increasing Ba content. This stands in contrast to the linear behaviour exhibited by unit cell volumes, atomic positions and intradimer spin-spin exchange interactions.
Using single crystal inelastic neutron scattering with and without application of an external magnetic field and powder neutron diffraction, we have characterized magnetic interactions in Ba$_3$Cr$_2$O$_8$. Even without field, we found that there exist three singlet-to-triplet excitation modes in $(h,h,l)$ scattering plane. Our complete analysis shows that the three modes are due to spatially anisotropic interdimer interactions that are induced by local distortions of the tetrahedron of oxygens surrounding the Jahn-Teller active Cr$^{5+} (3d^1)$. The strong intradimer coupling of $J_0 = 2.38(2)$ meV and weak interdimer interactions ($|J_{rm inter}| leq 0.52(2)$ meV) makes Ba$_3$Cr$_2$O$_8$ a good model system for weakly-coupled $s = 1/2$ quantum spin dimers.
We explore the spin states in the quantum spin chain compound SrCo$_{2}$V$_{2}$O$_{8}$ up to 14.9 T and down to 50 mK, using single-crystal neutron diffraction. Upon cooling in zero-field, antiferromagnetic (AFM) order of Neel type develops at $T_mathrm{{N}}$ $simeq$ 5.0 K. Applying an external magnetic field ($H$ $parallel$ $c$-axis) destabilizes the Neel order, leading to an order-disorder transition when applying a field between $T_mathrm{{N}}$ and $sim$ 1.5 K. Below 1.5 K, we observe a Neel to longitudinal spin density wave (LSDW) order transition at 3.9 T, and a LSDW to emergent AFM order transition at 7.0 T. Our results also reveal several unique signatures for the states of the spins that are not present in the isostructural counterpart BaCo$_{2}$V$_{2}$O$_{8}$.