Spin-spin correlations of the spin-ladder compound (C$_5$H$_{12}$N)$_2$CuBr$_4$ measured by magnetostriction and comparison to Quantum Monte Carlo results
Fabrizio Anfuso, Markus Garst, Achim Rosch, Oliver Heyer, Thomas Lorenz, Christian Ruegg, Karl Kraemer
Magnetostriction and thermal expansion of the spin-ladder compound piperidinium copper bromide (C$_5$H$_{12}$N)$_2$CuBr$_4$ are analyzed in detail. We find perfect agreement between experiments and the theory of a two-leg spin ladder Hamiltonian for more than a decade in temperature and in a wide range of magnetic fields. Relating the magnetostriction along different crystallographic directions to two static spin-spin correlation functions, which we compute with Quantum Monte Carlo, allows us to reconstruct the magnetoelastic couplings of (C$_5$H$_{12}$N)$_2$CuBr$_4$. We especially focus on the quantum critical behavior near the two critical magnetic fields $H_{c1}$ and $H_{c2}$, which is characterized by strong singularities rooted in the low dimensionality of the critical spin-system. Extending our discussion in Lorenz et al [Phys. Rev. Lett., 100, 067208 (2008)], we show explicitly that the thermal expansion near the upper critical field $H_{c2}$ is quantitatively described by a parameter-free theory of one-dimensional, non-relativistic Fermions. We also point out that there exists a singular quantum critical correction to the elastic moduli. This correction is proportional to the magnetic susceptibility $χ$ which diverges as $χ\sim 1/\sqrt{T}$ at the critical fields and thus leads to a strong softening of the crystal.
Inelastic neutron scattering is used to measure spin excitations in fully deuterated single crystal samples of the strong-leg antiferromagnetic S=1/2 spin ladder compound (C$_7$H$_{10}$N)$_2$CuBr$_4$. Sharp resolution-limited magnons are observed across the entire one-dimensional Brillouin zone. The results validate the previously proposed {\it symmetric} spin ladder model and provide a reliable estimate of the relevant exchange interactions.
The thermodynamic behavior of the spin $S=1/2$ antiferromagnetic two-leg ladder compound $(C_{5}H_{12}N)_{2} CuBr_{4}$ in a uniform magnetic field is studied using numerical and analytical approaches. The entropy $S(H,T)$ and specific heat $C(H,T)$ are calculated. The specific heat shows various behaviors in different regions of the magnetic field. The field-dependence of the specific heat is almost symmetric about the average of quantum critical fields in complete agreement with experimental results. In addition, it is found that during an adiabatic demagnetization process, temperature drops …
Polarized inelastic neutron scattering experiments recently identified the amplitude (Higgs) mode in C$_9$H$_{18}$N$_2$CuBr$_4$, a two-dimensional near-quantum-critical spin-1/2 two-leg ladder compound, which exhibits a weak easy-axis exchange anisotropy. Here, we theoretically examine the dynamic spin structure factor of such planar coupled spin-ladder systems using large-scale quantum Monte Carlo simulations. This allows us to provide a quantitative account of the experimental neutron scattering data within a consistent quantum spin model. Moreover, we trance the details of the continuous ev…
Inelastic neutron scattering was used to determine the spin Hamiltonian for the singlet ground state system of fully deuterated BPCB, (C$_{5}$D$_{12}$N)$_{2}$CuBr$_{4}$. A 2-leg spin-1/2 ladder model, with $J_\bot = (1.09 \pm 0.01)$ meV and $J_\| = (0.296 \pm 0.005)$ meV, accurately describes the data. The experimental limit on the effective inter-ladder exchange constant is $|J_{\rm int}^{\rm eff}|\lesssim 0.006$ meV, and the limit on total diagonal, intra-ladder exchange is $|J_F+J_{F'}|\leq 0.1$ meV. Including the effects of copper to bromide covalent spin transfer on the magnetic form-fact…
We present experiments on the magnetic field-dependent thermal transport in the spin-1/2 ladder system (C$_5$H$_{12}$N)$_2$CuBr$_4$. The thermal conductivity $κ(B)$ is only weakly affected by the field-induced transitions between the gapless Luttinger-liquid state realized for $B_{c1}< B < B_{c2}$ and the gapped states, suggesting the absence of a direct contribution of the spin excitations to the heat transport. We observe, however, that the thermal conductivity is strongly suppressed by the magnetic field deeply within the Luttinger-liquid state. These surprising observations are discussed i…
The $S=1/2$ spin ladder compound (C$_5$H$_{12}$N)$_2$CuBr$_4$ (BPCB) is studied by means of high-resolution inelastic neutron scattering. In agreement with previous studies we find a band of triplet excitations with a spin gap of $\sim0.8$~meV and a bandwidth of $\sim0.6$~meV. In addition, we observe a distinct splitting of the triplet band of $50(1)$~$μ$eV or $40(2)$~$μ$eV at the band minimum or maximum, respectively. By comparison to a strong coupling expansion calculation of the triplet dispersion for a spin ladder with anisotropic exchange, weakly anisotropic leg interactions are identifie…
Magnetic excitations in the spin-ladder material (C$_5$H$_{12}$N)$_2$CuBr$_4$ [BPCB] are probed by high-resolution multi-frequency electron spin resonance (ESR) spectroscopy. Our experiments provide a direct evidence for a biaxial anisotropy ($\sim 5\%$ of the dominant exchange interaction), that is in contrast to a fully isotropic spin-ladder model employed for this system previously. It is argued that this anisotropy in BPCB is caused by spin-orbit coupling, which appears to be important for describing magnetic properties of this compound. The zero-field zone-center gap in the excitation spe…
We present high-resolution measurements of the $c^\star$-axis thermal expansion and magnetostriction of piperidinium copper bromide \hp. The experimental data at low temperatures is well accounted for by a two-leg spin-ladder Hamiltonian. The thermal expansion shows a complex behaviour with various sign changes and approaches a $1/\sqrt{T}$ divergence at the critical fields. All low-temperature features are semi-quantitatively explained within a free fermion model; full quantitative agreement is obtained with Quantum Monte Carlo simulations.
The magnetization, $M(H \leq 30$ T, 0.7 K $\leq T \leq 300$ K), from single crystals and powder samples of (C$_{5}$H$_{12}$N)$_{2}$CuBr$_{4}$ has been used to identify this system as an $S=1/2$ Heisenberg two-leg ladder in the strong coupling limit, $J_{\perp} = 13.3$ K and $J_{\parallel} = 3.8$ K, with $H_{c1} = 6.6$ T and $H_{c2} = 14.6$ T. An inflection point in $M(H, T = 0.7$ K) at half-saturation, $M_{s}/2$, is described by an effective \emph{XXZ} chain. The data exhibit universal scaling behavior in the vicinity of $H_{c1}$ and $H_{c2}$, indicating the system is near a quantum critical p…
We present the results of muon-spin spectroscopy ($μ^{+}$SR) measurements on the molecular spin ladder system (Hpip)$_{2}$CuBr$_{4(1-x)}$Cl$_{4x}$, [Hpip=(C$_{5}$H$_{12}$N)]. Using transverse field $μ^{+}$SR we are able to identify characteristic behaviour in each of the regions of the phase diagram of the $x=0$ strong-rung spin ladder system (Hpip)$_{2}$CuBr$_4$. Comparison of our results to those of the dimer-based molecular magnet Cu(pyz)(gly)(ClO$_{4}$) shows several common features. We locate the crossovers in partially disordered (Hpip)$_{2}$CuBr$_{4(1-x)}$Cl$_{4x}$ ($x=0.05$), where a r…
We present specific-heat and neutron-scattering results for the \emph{S}=1/2 quantum antiferromagnet (dimethylammonium)(3,5-dimethylpyridinium)CuBr$_4$. The material orders magnetically at \emph{T}$_N$=1.99(2)\,K, and magnetic excitations are accompanied by an energy gap of 0.30(2) meV due to spin anisotropy. The system is best described as coupled two-leg spin-1/2 ladders with the leg exchange $J_{\rm leg}$=0.60(2)~meV, rung exchange $J_{\rm rung}$=0.64(9)~meV, interladder exchange $J_{\rm int}$=0.19(2)~meV, and an interaction-anisotropy parameter $λ$=0.93(2), according to inelastic neutron-s…
We report low temperature electron spin resonance experimental and theoretical studies of an archetype $S=1/2$ strong-rung spin ladder material (C$_{5}$H$_{12}$N)$_{2}$CuBr$_{4}$. Unexpected dynamics is detected deep in the Tomonaga-Luttinger spin liquid regime. Close to the point where the system is half-magnetized (and believed to be equivalent to a gapless easy plane chain in zero field) we observed orientation-dependent spin gap and anomalous $g$-factor values. Field theoretical analysis demonstrates that the observed low-energy excitation modes in magnetized (C$_{5}$H$_{12}$N)$_{2}$CuBr$_…
Quantum phase transitions in quantum matter occur at zero temperature between distinct ground states by tuning a nonthermal control parameter. Often, they can be accurately described within the Landau theory of phase transitions, similarly to conventional thermal phase transitions. However, this picture can break down under certain circumstances. Here, we present a comprehensive study of the effect of hydrostatic pressure on the magnetic structure and spin dynamics of the spin-1/2 ladder compound C$_9$H$_{18}$N$_2$CuBr$_4$. Single-crystal heat capacity and neutron diffraction measurements reve…
Inelastic neutron scattering is used to measure the spin excitation spectrum of the Heisenberg $S=1/2$ ladder material (C$_7$H$_10$N)$_2$CuBr$_4$ in its entirety, both in the gapped spin-liquid and the magnetic field induced Tomonaga-Luttinger spin liquid regimes. A fundamental change of the spin dynamics is observed between these two regimes. DMRG calculations quantitatively reproduce and help understand the observed commensurate and incommensurate excitations. The results validate long-standing quantum field theoretical predictions, but also test the limits of that approach.
Magnetic insulators have proven to be usable as quantum simulators for itinerant interacting quantum systems. In particular the compound (C$_{5}$H$_{12}$N)$_{2}$CuBr$_{4}$ (short (Hpip)$_{2}$CuBr$_{4}$) was shown to be a remarkable realization of a Tomonaga-Luttinger liquid (TLL) and allowed to quantitatively test the TLL theory. Substitution weakly disorders this class of compounds and allows thus to use them to tackle questions pertaining to the effect of disorder in TLL as well, such as the formation of the Bose glass. As a first step in this direction we present in this paper a study of th…
The zero-field excitation spectrum of the strong-leg spin ladder (C$_7$H$_10$N)$_2$CuBr$_4$ (DIMPY) is studied with a neutron time-of-flight technique. The spectrum is decomposed into its symmetric and asymmetric parts with respect to the rung momentum and compared with theoretical results obtained by the density matrix renormalization group method. Additionally, the calculated dynamical correlations are shown for a wide range of rung and leg coupling ratios in order to point out the evolution of arising excitations, as e.g. of the two-magnon bound state from the strong to the weak coupling li…
Motivated by the intriguing mode splittings in a magnetic field recently observed with inelastic neutron scattering in the spin ladder compound (C$_5$H$_{12}$N)$_2$CuBr$_4$ (BPCB), we investigate the nature of the spin ladder excitations using DMRG and analytical arguments. Starting from the fully frustrated ladder, for which we derive the low-energy spectrum, we show that bound states are generically present close to $k=0$ in the dynamical structure factor of spin ladders above $H_{c 1}$, and that they are characterized by a field-independent binding energy and an intensity that grows with $H…
By means of inelastic neutron scattering we investigate finite temperature dynamics in the quantum spin ladder compound (C$_5$H$_{12}$N)$_2$CuBr$_4$ (BPCB) near the magnetic field induced quantum critical point with dynamical exponent $z=2$. We observe universal finite-temperature scaling of the transverse local dynamic structure factor in spectacular quantitative agreement with long-standing theoretical predictions. At the same time, already at rather low temperatures, we observe strong non-universal longitudinal fluctuations. To separate the two, we make use of an intrinsic leg-exchange symm…
Magnetic excitations in the strong-leg quantum spin ladder compound (C$_7$H$_{10}$N)$_2$CuBr$_4$ (known as DIMPY) in the field-induced Tomonaga-Luttinger spin liquid phase are studied by means of high-field electron spin resonance (ESR) spectroscopy. The presence of a gapped ESR mode with unusual non-linear frequency-field dependence is revealed experimentally. Using a combination of analytic and exact diagonalization methods, we compute the dynamical structure factor and identify this mode with longitudinal excitations in the antisymmetric channel. We argue that these excitations constitute a…
We present a 14N nuclear magnetic resonance study of a single crystal of CuBr4(C5H12N)2 (BPCB) consisting of weakly coupled spin-1/2 Heisenberg antiferromagnetic ladders. Treating ladders in the gapless phase as Luttinger liquids, we are able to fully account for (i) the magnetic field dependence of the nuclear spin-lattice relaxation rate 1/T_1 at 250 mK and for (ii) the phase transition to a 3D ordered phase occuring below 110 mK due to weak interladder exchange coupling. BPCB is thus an excellent model system where the possibility to control Luttinger liquid parameters in a continuous manne…
Evolution of the ESR absorption in a strong-leg spin ladder magnet (C$_7$H$_{10}$N$_2$)$_2$CuBr$_4$ (abbreviated as DIMPY) is studied from 300K to 400mK. Temperature dependence of the ESR relaxation follows a staircase of crossovers between different relaxation regimes. We ague that the main mechanism of ESR line broadening in DIMPY is uniform Dzyaloshinskii-Moria interaction ($|\vec{D}|=0.20$K) with an effective longitudinal component along an exchange bond of Cu ions within the legs resulting from the low crystal symmetry of DIMPY and nontrivial orbital ordering. The same Dzyaloshinskii-Mori…
Using micromechanical force magnetometry, we have measured the magnetization of the strong-leg spin-1/2 ladder compound (C$_7$H$_{10}$N)$_2$CuBr$_2$ at temperatures down to 45 mK. Low-temperature magnetic susceptibility as a function of field exhibits a maximum near the critical field H_c at which the magnon gap vanishes, as expected for a gapped one-dimensional antiferromagnet. Above H_c a clear minimum appears in the magnetization as a function of temperature as predicted by theory. In this field region, the susceptibility in conjunction with our specific heat data yields the Wilson ratio R_…
We report temperature-dependent neutron scattering measurements of the local dynamic structure factor in the quantum spin ladder (C$_{7}$H$_{10}$N)$_{2}$CuBr$_{4}$ in a magnetic field $H=9$~T, in its gapless quantum-critical phase. We show that the measured quantity has a scaling form consistent with expectations for a Tomonaga-Luttinger liquid with attraction. The measured Luttinger parameter $K\approx1.25$ and scaling function are in excellent agreement with density matrix renormalization group numerical calculations for the underlying spin Hamiltonian.
We consider an array of XX spin-1/2 chains coupled to acoustic phonons and placed in a magnetic field. Treating the phonons in the mean field approximation, we show that this system presents a first order transition as a function of the magnetic field between a partially magnetized distorted state and the fully polarized undistorted state at low temperature. This behavior results from the magnetostriction of the coupled chain system. A dip in the elastic constant of the material near the saturation field along with an anomaly in the magnetic susceptibility is predicted. We also predict the con…
The iron-selenides are important because of their superconducting properties. Here, an unexpected phenomenon is predicted to occur in an iron-selenide compound with a quasi-one-dimensional ladder geometry: BaFe$_2$Se$_3$ should be a magnetic ferrielectric system, driven by its magnetic block order via exchange striction. A robust performance (high $T_{\rm C}$ and large polarization) is expected. Different from most multiferroics, BaFe$_2$Se$_3$ is ferrielectric, with a polarization that mostly cancels between ladders. However, its strong magnetostriction still produces a net polarization that …
