arXiv subjects

C. P. Landee

Publications and source records attributed to C. P. Landee.

At least 19 recordsLinked to original sources

arXiv2022

Field-tunable Berezinskii-Kosterlitz-Thouless correlations in a Heisenberg magnet

We report the manifestation of field-induced Berezinskii-Kosterlitz-Thouless (BKT) correlations in the weakly coupled spin-1/2 Heisenberg layers of the molecular-based bulk material [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$. Due to the moderate intralayer exchange coupling of $J/k_\mathrm{B} = 6.8$ K, the application of laboratory magnetic fields induces a substantial $XY$ anisotropy of the spin correlations. Crucially, this provides a significant BKT regime, as the tiny interlayer exchange $J^\prime / k_\mathrm{B} \approx 1$ mK only induces 3D correlations upon close approach to the BKT transition with its exponential growth in the spin-correlation length. We employ nuclear magnetic resonance and $μ^{+}$SR measurements to probe the spin correlations that determine the critical temperatures of the BKT transition as well as that of the onset of long-range order. Further, we perform stochastic series expansion quantum Monte Carlo simulations based on the experimentally determined model parameters. Finite-size scaling of the in-plane spin stiffness yields excellent agreement of critical temperatures between theory and experiment, providing clear evidence that the nonmonotonic magnetic phase diagram of [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$ is determined by the field-tuned $XY$ anisotropy and the concomitant BKT physics.

cond-mat.str-el↗

arXiv2021

Freezing of molecular rotation in a paramagnetic crystal studied by $^{31}$P NMR

We present a detailed $^{31}$P nuclear magnetic resonance (NMR) study of the molecular rotation in the compound [Cu(pz)$_{2}$(2-HOpy)$_{2}$](PF$_{6}$)$_{2}$, where pz = C$_4$H$_4$N$_2$ and 2-HOpy = C$_5$H$_4$NHO. Here, a freezing of the PF$_6$ rotation modes is revealed by several steplike increases of the temperature-dependent second spectral moment, with accompanying broad peaks of the longitudinal and transverse nuclear spin-relaxation rates. An analysis based on the Bloembergen-Purcell-Pound (BPP) theory quantifies the related activation energies as $E_{a}/k_{B}$ = 250 and 1400 K. Further, the anisotropy of the second spectral moment of the $^{31}$P absorption line was calculated for the rigid lattice, as well as in the presence of several sets of PF$_6$ reorientation modes, and is in excellent agreement with the experimental data. Whereas the anisotropy of the frequency shift and enhancement of nuclear spin-relaxation rates is driven by the molecular rotation with respect to the dipole fields stemming from the Cu ions, the second spectral moment is determined by the intramolecular interaction of nuclear $^{19}$F and $^{31}$P moments in the presence of the distinct rotation modes.

cond-mat.str-el↗

arXiv2020

Extremely well isolated 2D spin-$1/2$ antiferromagnetic Heisenberg layers with small exchange coupling in the molecular-based magnet CuPOF

We report on a comprehensive characterization of the newly synthesized Cu$^{2+}$-based molecular magnet [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$ (CuPOF), where pz = C$_4$H$_4$N$_2$ and 2-HOpy = C$_5$H$_4$NHO. From a comparison of theoretical modeling to results of bulk magnetometry, specific heat, $μ^+$SR, ESR, and NMR spectroscopy, this material is determined as an excellent realization of the 2D square-lattice $S=1/2$ antiferromagnetic Heisenberg model with a moderate intraplane nearest-neighbor exchange coupling of $J/k_\mathrm{B} = 6.80(5)$ K, and an extremely small interlayer interaction of about 1 mK. At zero field, the bulk magnetometry reveals a temperature-driven crossover of spin correlations from isotropic to $XY$ type, caused by the presence of a weak intrinsic easy-plane anisotropy. A transition to long-range order, driven by the low-temperature $XY$ anisotropy under the influence of the interlayer coupling, occurs at $T_\mathrm{N} = 1.38(2)$ K, as revealed by $μ^+$SR. In applied magnetic fields, our $^1$H-NMR data reveal a strong increase of the magnetic anisotropy, manifested by a pronounced enhancement of the transition temperature to commensurate long-range order at $T_\mathrm{N} =2.8$ K and 7 T.

cond-mat.str-el↗

arXiv2019

Room-temperature structural phase transition in the quasi-2D spin-1/2 Heisenberg antiferromagnet Cu(pz)$_2$(ClO$_4$)$_2$

Cu(pz)$_2$(ClO$_4$)$_2$ (with pz denoting pyrazine C$_4$H$_4$N$_2$) is a two-dimensional spin-1/2 square-lattice antiferromagnet with $T_{\mathrm{N}}$ = 4.24 K. Due to a persisting focus on the low-temperature magnetic properties, its room-temperature structural and physical properties caught no attention up to now. Here we report a study of the structural features of Cu(pz)$_2$(ClO$_4$)$_2$ in the paramagnetic phase, up to 330 K. By employing magnetization, specific heat, $^{35}$Cl nuclear magnetic resonance, and neutron diffraction measurements, we provide evidence of a second-order phase transition at $T^{\star}$ = 294 K, not reported before. The absence of a magnetic ordering across $T^{\star}$ in the magnetization data, yet the presence of a sizable anomaly in the specific heat, suggest a structural order-to-disorder type transition. NMR and neutron-diffraction data corroborate our conjecture, by revealing subtle angular distortions of the pyrazine rings and of ClO$^-_4$ counteranion tetrahedra, shown to adopt a configuration of higher symmetry above the transition temperature.

cond-mat.mtrl-sci↗

arXiv2017

Quantum-critical spin dynamics in a Tomonaga-Luttinger liquid studied with muon-spin relaxation

We demonstrate that quantum-critical spin dynamics can be probed in high magnetic fields using muon-spin relaxation ($μ^{+}$SR). Our model system is the strong-leg spin ladder bis(2,3-dimethylpyridinium) tetrabromocuprate (DIMPY). In the gapless Tomonaga-Luttinger liquid phase we observe finite-temperature scaling of the $μ^{+}$SR $1/T_1$ relaxation rate which allows us to determine the Luttinger parameter $K$. We discuss the benefits and limitations of local probes compared with inelastic neutron scattering.

cond-mat.str-el↗

arXiv2016

Raman study of spin excitations in the tunable quantum spin ladder Cu(Qnx)(Cl$_{1-x}$Br$_x$)$_2$

Raman spectroscopy is used to study magnetic excitations in the quasi one dimensional $S=1/2$ quantum spin systems Cu(Qnx)(Cl$_{1-x}$Br$_x$)$_2$. The low energy spectrum is found to be dominated by a two-magnon continuum as expected from the numerical calculations for the Heisenberg spin ladder model. The continuum shifts to higher energies as more Br is introduced. The cutoff of the scattering increases faster than the onset indicating that the increase of exchange constant along the leg is the main effect on the magnetic properties. The upper and lower continuum thresholds are measured as a function of Br content across the entire range and compared to estimates based on previous bulk studies. We observe small systematic deviations that are discussed.

cond-mat.str-el↗

arXiv2016

Pressure and magnetic field effects on a quasi-2D spin-1/2 Heisenberg antiferromagnet

Cu(pz)2(ClO4)2 (with pz denoting pyrazine, C4H4N2) is among the best realizations of a two-dimensional spin-1/2 square-lattice antiferromagnet. Below T_N = 4.21 K, its weak interlayer couplings induce a 3D magnetic order, strongly influenced by external magnetic fields and/or hydrostatic pressure. Previous work, focusing on the [H, T] phase diagram, identified a spin-flop transition, resulting in a field-tunable bicritical point. However, the influence of external pressure has not been investigated yet. Here we explore the extended [p, H, T] phase diagram of Cu(pz)2(ClO4)2 under pressures up to 12 kbar and magnetic fields up to 7.1 T, via magnetometry and 35Cl nuclear magnetic resonance (NMR) measurements. The application of magnetic fields enhances T_XY , the crossover temperature from the Heisenberg to the XY model, thus pointing to an enhancement of the effective anisotropy. The applied pressure has an opposite effect [dT_N/dp = 0.050(8) K/kbar], as it modifies marginally the interlayer couplings, but likely changes more significantly the orbital reorientation and the square-lattice deformation. This results in a remodeling of the effective Hamiltonian, whereby the field and pressure effects compensate each other. Finally, by comparing the experimental data with numerical simulations we estimate T_BKT, the temperature of the Berezinskii-Kosterlitz-Thouless topological transition and argue why it is inaccessible in our case.

cond-mat.str-el↗

arXiv2016

ESR modes in a Strong-Leg Ladder in the Tomonaga-Luttinger Liquid Phase

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 fingerprint of the spin dynamics in a strong-leg spin-1/2 Heisenberg antiferromagnetic ladder and owe its ESR observability to the uniform Dzyaloshinskii-Moriya interaction.

cond-mat.str-el↗

arXiv2014

The tunable quantum spin ladder Cu(Qnx)(Cl$_{(1-x)}$Br$_{x}$)$_{2}$

We report magnetic, specific heat and ESR measurements on a series of $S=1/2$ spin ladder compounds Cu(Qnx)(Cl$_{(1-x)}$Br$_{x}$)$_{2}$. Down to $T=2$ K all the observables can be described by the spin ladder model with about 1% of $S=1/2$ impurities in the background, which are present even in a nominally pure Cu(Qnx)Cl$_{2}$ and Cu(Qnx)Br$_{2}$, for the whole range of $0\leq x\leq1$. We extract ladder exchange constants $J_{l}(x)$ and $J_{r}(x)$ as well as the gap value $Δ(x)$ by comparing the experimental data to quantum Monte-Carlo simulations. As the ESR measurements show the $g$-factor of impurities to be precisely equal to $g$-factor of the ladder spins, we suppose the impurities to be the consequence of structural defects resulting in a broken ladder ends.

cond-mat.str-el↗

arXiv2013

Switching of anisotropy and phase diagram of a Heisenberg square lattice S=1/2 antiferromagnet Cu(pz)2(ClO4)2

Experiments in the antiferromagnetic phase of a quasi 2D $S=1/2$ quasi-square lattice antiferromagnet Cu(pz)2(ClO4)2 reveal a biaxial type of the anisotropy, instead of the easy-plane one, considered before. The weak in-plane anisotropy, found by means of electron spin resonance spectroscopy and magnetization measurements, is about an order of magnitude weaker, than the off-plane anisotropy. The weak in-plane anisotropy results in a spin-flop phase transition for the magnetic field aligned along easy axis, and, thereby, in a bicritical point on the phase diagram. A remarkable feature of the weak in-plane anisotropy is the abrupt change of its sign at the spin-flop point. This anisotropy switching disappears at the tilting of magnetic field to the easy axis by the angle of 10$^\circ$ within the plane. The nature of the abrupt anisotropy reversal remains unclear. The phase diagram is characterized by the increase of the ordering temperature in the magnetic field used, except for a dip near the bicritical point.

cond-mat.str-el↗

arXiv2012

ESR of coupled spin-1/2 chains: unveiling zig-zag-type interchain correlations

By means of electron spin resonance investigations we revealed the crucial role of the interchain coupling in the spin dynamics of the spin-1/2 Heisenberg antiferromagnetic (AF) chain material copper-pyrazine-dinitrate, Cu(C$_4$H$_4$N$_2$)(NO$_3$)$_2$. We found that the dominating interchain interaction is of a zig-zag type. This interaction gives rise to geometrical frustration effects and strongly influences the character of AF ordering. Combining our experimental findings with the results of a quasiclassical approach we argue that at low temperatures the system orders in an incommensurate spiral state.

cond-mat.str-el↗

arXiv2012

Wilson ratio of a Tomonaga-Luttinger liquid in a spin-1/2 Heisenberg ladder

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_W. The result supports the relation R_W=4K, where K is the Tomonaga-Luttinger-liquid parameter.

cond-mat.str-el↗

arXiv2010

Dynamics of the two-dimensional S=1/2 dimer system (C5H6N2F)2CuCl4

Inelastic neutron scattering was used to study a quantum S=1/2 antiferromagnetic Heisenberg system-Bis(2-amino-5-fluoropyridinium) Tetrachlorocuprate(II). The magnetic excitation spectrum was shown to be dominated by long-lived excitations with an energy gap as 1.07(3) meV. The measured dispersion relation is consistent with a simple two-dimensional square lattice of weakly-coupled spin dimers. Comparing the data to a random phase approximation treatment of this model gives the intra-dimer and inter-dimer exchange constants J=1.45(2) meV and J'=0.31(3) meV, respectively.

cond-mat.str-el↗

arXiv2010

Field-induced Tomonaga-Luttinger liquid phase of a two-leg spin-1/2 ladder with strong leg interactions

We study the magnetic-field-induced quantum phase transition from a gapped quantum phase that has no magnetic long-range order into a gapless phase in the spin-1/2 ladder compound bis(2,3-dimethylpyridinium) tetrabromocuprate (DIMPY). At temperatures below about 1 K, the specific heat in the gapless phase attains an asymptotic linear temperature dependence, characteristic of a Tomonaga-Luttinger liquid. Inelastic neutron scattering and the specific heat measurements in both phases are in good agreement with theoretical calculations, demonstrating that DIMPY is the first model material for an S=1/2 two-leg spin ladder in the strong-leg regime.

cond-mat.str-el↗

arXiv2010

Dynamics of a Heisenberg spin chain in the quantum critical regime: NMR experiment versus effective field theory

A comprehensive comparison between the magnetic field- and temperature-dependent low frequency spin dynamics in the antiferromagnetic spin-1/2 Heisenberg chain (AFHC) system copper pyrazine dinitrate, probed via the 13C-nuclear magnetic resonance (NMR) relaxation rate 1/T1, and the field theoretical approach in the Luttinger liquid (LL) regime has been performed. We have found a very good agreement between the experiment and theory in the investigated temperature and field range. Our results demonstrate how strongly the quantum critical point affects the spin dynamics of Heisenberg spin chain compounds.

cond-mat.str-el↗

arXiv2010

Spin Dynamics in $S=1/2$ Chains with Next-Nearest-Neighbor Exchange Interactions

Low-energy magnetic excitations in the spin-1/2 chain compound (C$_6$H$_9$N$_2$)CuCl$_3$ [known as (6MAP)CuCl$_3$] are probed by means of tunable-frequency electron spin resonance. Two modes with asymmetric (with respect to the $hν=gμ_B B$ line) frequency-field dependences are resolved, illuminating the striking incompatibility with a simple uniform $S=\frac{1}{2}$ Heisenberg chain model. The unusual ESR spectrum is explained in terms of the recently developed theory for spin-1/2 chains, suggesting the important role of next-nearest-neighbor interactions in this compound. Our conclusion is supported by model calculations for the magnetic susceptibility of (6MAP)CuCl$_3$, revealing a good qualitative agreement with experiment.

cond-mat.str-el↗

arXiv2010

The Two-Dimensional Square-Lattice S=1/2 Antiferromagnet Cu(pz)$_2$(ClO$_4$)$_2$

We present an experimental study of the two-dimensional S=1/2 square-lattice antiferromagnet Cu(pz)$_2$(ClO$_4$)$_2$ (pz denotes pyrazine - $C_4H_4N_2$) using specific heat measurements, neutron diffraction and cold-neutron spectroscopy. The magnetic field dependence of the magnetic ordering temperature was determined from specific heat measurements for fields perpendicular and parallel to the square-lattice planes, showing identical field-temperature phase diagrams. This suggest that spin anisotropies in Cu(pz)$_2$(ClO$_4$)$_2$ are small. The ordered antiferromagnetic structure is a collinear arrangement with the magnetic moments along either the crystallographic b- or c-axis. The estimated ordered magnetic moment at zero field is m_0=0.47(5)mu_B and thus much smaller than the available single-ion magnetic moment. This is evidence for strong quantum fluctuations in the ordered magnetic phase of Cu(pz)$_2$(ClO$_4$)$_2$. Magnetic fields applied perpendicular to the square-lattice planes lead to an increase of the antiferromagnetically ordered moment to m_0=0.93(5)mu_B at mu_0H=13.5T - evidence that magnetic fields quench quantum fluctuations. Neutron spectroscopy reveals the presence of a gapped spin excitations at the antiferromagnetic zone center, and it can be explained with a slightly anisotropic nearest neighbor exchange coupling described by J_1^{xy}=1.563(13)meV and J_1^z=0.9979(2)J_1^{xy}.

cond-mat.str-el↗

arXiv2010

Low frequency spin dynamics in the quantum magnet copper pyrazine dinitrate

The S=1/2 antiferromagnetic Heisenberg chain exhibits a magnetic field driven quantum critical point. We study the low frequency spin dynamics in copper pyrazine dinitrate (CuPzN), a realization of this model system of quantum magnetism, by means of $^{13}$C-NMR spectroscopy. Measurements of the nuclear spin-lattice relaxation rate $T_1^{-1}$ in the vicinity of the saturation field are compared with quantum Monte Carlo calculations of the dynamic structure factor. Both show a strong divergence of low energy excitations at temperatures in the quantum regime. The analysis of the anisotropic $T_1^{-1}$-rates and frequency shifts allows one to disentangle the contributions from transverse and longitudinal spin fluctuations for a selective study and to determine the transfer of delocalized spin moments from copper to the neighboring nitrogen atoms.

cond-mat.str-el↗