arXiv subjects

A. Paduan-Filho

Publications and source records attributed to A. Paduan-Filho.

At least 19 recordsLinked to original sources

arXiv2019

Microwave dynamics of pure and doped anisotropic S=1 chain antiferromagnet NiCl2-4SC(NH2)2

We studied electron spin resonance in a quantum magnet NiCl2-4SC(NH2)2, demonstrating a field-induced quantum phase transition from a quantum-disordered phase to an antiferromagnet. We observe two branches of the antiferromagnetic resonance of the ordered phase, one of them has a gap and the other is a Goldstone mode with zero frequency at a magnetic field along the four-fold axis. This zero frequency mode acquires a gap at a small tilting of the magnetic field with respect to this direction. The upper gap was found to be reduced in the doped compound Ni(Cl(1-x)Br(x))2-4SC(NH2)2 with $x=0.21$. This reduction is unexpected because of the previously reported rise of the main exchange constant in a doped compound. Further, a nonresonant diamagnetic susceptibility $χ^{\prime}$ was found for the ordered phase in a wide frequency range above the quasi-Goldstone mode. This dynamic diamagnetism is as large as the dynamic susceptibility of the paramagnetic resonance. We speculate that it originates from a two-magnon absorption band of low-frequency dispersive magnon branch.

cond-mat.str-el↗

arXiv2018

Detection of a Disorder-Induced Bose-Einstein Condensate in a Quantum Spin Material at High Magnetic Fields

The coupled spin-1 chains material NiCl$_2$-4SC(NH$_2$)$_2$ (DTN) doped with Br impurities is expected to be a perfect candidate for observing many-body localization at high magnetic field: the so-called "Bose glass", a zero-temperature bosonic fluid, compressible, gapless, incoherent, and short-range correlated. Using nuclear magnetic resonance (NMR), we critically address the stability of the Bose glass in doped DTN, and find that it hosts a novel disorder-induced ordered state of matter, where many-body physics leads to an unexpected resurgence of quantum coherence emerging from localized impurity states. An experimental phase diagram of this new "order-from-disorder" phase, established from NMR $T_1^{-1}$ relaxation rate data in the (13 $\pm$ 1)% Br-doped DTN, is found to be in excellent agreement with the theoretical prediction from large-scale quantum Monte Carlo simulations.

cond-mat.str-el↗

arXiv2017

Magnetic-field-induced ordered phase in the chloro-bridged copper(II) dimer system [Cu2(apyhist)2Cl2](ClO4)2

Specific heat and magnetization measurements of the compound [Cu2(apyhist)2Cl2](ClO4)2, where apyhist = (4-imidazolyl)ethylene-2-amino-1-ethylpyridine), were used to identify a magnetic-field-induced long-range antiferromagnetic ordered phase at low temperatures (T < 0.36 K) and magnetic fields (1.6 T < H < 5.3 T). This system consists of a Schiff base copper(II) complex, containing chloro-bridges between adjacent copper ions in a dinuclear arrangement, with an antiferromagnetic intradimer interaction |Jintra|/kB = 3.65 K linked by an antiferromagnetic coupling |Jinter|z/kB = 2.7 K. The magnetic-field-induced ordering behavior was analyzed using the mean field approximation and Monte Carlo simulation results. The obtained physical properties of the system are consistent with the description of the ordered phase as a Bose-Einstein Condensation (BEC) of magnetic excitations. We present the phase diagram of this compound, which shows one of the lowest critical magnetic field among all known members of the family of BEC quantum magnets.

cond-mat.str-el↗

arXiv2016

Crossover from one- to three-dimensional behavior in the S = 1/2 Heisenberg antiferromagnet Cu(N2H5)2(SO4)2

From experimental and theoretical analyses of magnetic and specific-heat properties, we present the complete magnetic phase diagram of the quasi-one-dimensional antiferromagnet Cu(N$_2$H$_5$)$_2$(SO$_4$)$_2$. On cooling and at zero magnetic field this compound enters a one-dimensional regime with short-range magnetic correlations, marked by a broad maximum in the specific heat and magnetic susceptibility at $T_\mathrm{max}\sim 2\,\mathrm{K}$, followed by an ordered antiferromagnetic phase below $T_\mathrm{N}\sim 1\,\mathrm{K}$ induced by small interchain couplings. The intermediate-temperate one-dimensional regime can be modeled using exact quantum-transfer-matrix calculations, which perfectly describe the nonmonotonic behavior of T_max as a function of the magnetic field, giving $J = 4.25\,\mathrm{K}$ for the intrachain exchange parameter. The analysis of magnetic specific-heat and susceptibility data at low temperature indicates that the interchain exchange couplings are an order of magnitude smaller than the coupling inside the chains.

cond-mat.str-el↗

arXiv2015

Dynamics of a bond-disordered $S=1$ quantum magnet near $z=1$ criticality

Neutron scattering is used to study NiCl$_{2-2x}$Br$_{2x}\cdot$4SC(NH$_2$)$_2$, $x=0.06$, a bond-disordered modification of the well-known gapped $S=1$ antiferromagnetic quantum spin system NiCl$_{2}\cdot$4SC(NH$_2$)$_2$. The magnetic excitation spectrum throughout Brillouin zone is mapped out at $T=60$ mK using high-resolution time-of-flight spectroscopy. It is found that the dispersion of spin excitation is renormalized, as compared to that in the parent compound. The lifetime of excitations near the bottom of the band is substantially decreased. No localized states are found below the gap energy $Δ\simeq0.2$ meV. At the same time, localized zero wave vector states are detected above the top of the band. The results are consistent with a more or less continuous random distribution of bond strengths, and a discrete, possibly bimodal, distribution of single-ion anisotropies in the disordered material.

cond-mat.str-el↗

arXiv2013

Criticality in a disordered quantum antiferromagnet by neutron diffraction

Field-induced magnetic ordering in the structurally disordered quantum magnets Ni(Cl$_{1-x}$Br$_x$)$_2$$\cdot$4SC(NH$_2$)$_2$, $x=8$% and 13%, is studied by means of neutron diffraction. The order parameter critical exponent is found to be very close to its value $β=0.5$ expected for magnetic Bose-Einstein condensation in the absence of disorder. This result applies to temperatures down to 40 mK, and a 1 T range in magnetic field. The crossover exponent is found to be $ϕ\sim 0.4$, for temperature ranges as small as 300 mK. Possible reasons for a discrepancy with recent numerical simulations and bulk measurements are discussed.

cond-mat.str-el↗

arXiv2012

Quantum-critical spin dynamics in quasi-one-dimensional antiferromagnets

By means of nuclear spin-lattice relaxation rate 1/T1, we follow the spin dynamics as a function of the applied magnetic field in two gapped one-dimensional quantum antiferromagnets: the anisotropic spin-chain system NiCl2-4SC(NH2)2 and the spin-ladder system (C5H12N)2CuBr4. In both systems, spin excitations are confirmed to evolve from magnons in the gapped state to spinons in the gapples Tomonaga-Luttinger-liquid state. In between, 1/T1 exhibits a pronounced, continuous variation, which is shown to scale in accordance with quantum criticality. We extract the critical exponent for 1/T1, compare it to the theory, and show that this behavior is identical in both studied systems, thus demonstrating the universality of quantum critical behavior.

cond-mat.str-el↗

arXiv2012

Magnetic excitations in the spin-1 anisotropic antiferromagnet $NiCl_2-4SC(NH_2)_2$

The spin-1 anisotropic antiferromagnet NiCl_2-4SC(NH2)_2 exhibits a field-induced quantum phase transition that is formally analogous to Bose-Einstein condensation. Here we present results of systematic high-field electron spin resonance (ESR) experimental and theoretical studies of this compound with a special emphasis on single-ion two-magnon bound states. In order to clarify some remaining discrepancies between theory and experiment, the frequency-field dependence of magnetic excitations in this material is reanalyzed. In particular, a more comprehensive interpretation of the experimental signature of single-ion two-magnon bound states is shown to be fully consistent with theoretical results. We also clarify the structure of the ESR spectrum in the so-called intermediate phase.

cond-mat.str-el↗

arXiv2010

Quantum fluctuations and strong mass renormalization in NiCl2-4SC(NH2)2

In a number of quantum paramagnets, magnetic field can induce a quantum phase transition to an antiferromagnetic state which exists for a range of fields Hc1 < H < Hc2. Generally, these compounds exhibit a significant asymmetry in their properties at low- and high-field transitions. Here we present detailed specific heat and thermal conductivity measurements in NiCl2-4SC(NH2)2 together with analytical and numerical results. We show that the asymmetry is caused by a strong renormalization of the effective mass of spin excitations due to quantum fluctuations for H<Hc1 that are absent for H<Hc2.

cond-mat.str-el↗

arXiv2010

Magnetoelectric effects in an organo-metallic quantum magnet

We observe a bilinear magnetic field-induced electric polarization of 50 $μC/m^2$ in single crystals of NiCl$_2$-4SC(NH$_2$)$_2$ (DTN). DTN forms a tetragonal structure that breaks inversion symmetry, with the highly polar thiourea molecules all tilted in the same direction along the c-axis. Application of a magnetic field between 2 and 12 T induces canted antiferromagnetism of the Ni spins and the resulting magnetization closely tracks the electric polarization. We speculate that the Ni magnetic forces acting on the soft organic lattice can create significant distortions and modify the angles of the thiourea molecules, thereby creating a magnetoelectric effect. This is an example of how magnetoelectric effects can be constructed in organo-metallic single crystals by combining magnetic ions with electrically polar organic elements.

cond-mat.mtrl-sci↗

arXiv2008

Character of magnetic excitations in a quasi-one-dimensional antiferromagnet near the quantum critical points: Impact on magneto-acoustic properties

We report results of magneto-acoustic studies in the quantum spin-chain magnet NiCl$_2$-4SC(NH$_2$)$_2$ (DTN) having a field-induced ordered antiferromagnetic (AF) phase. In the vicinity of the quantum critical points (QCPs) the acoustic $c_{33}$ mode manifests a pronounced softening accompanied by energy dissipation of the sound wave. The acoustic anomalies are traced up to $T > T_N$, where the thermodynamic properties are determined by fermionic magnetic excitations, the "hallmark" of one-dimensional (1D) spin chains. On the other hand, as established in earlier studies, the AF phase in DTN is governed by bosonic magnetic excitations. Our results suggest the presence of a crossover from a 1D fermionic to a 3D bosonic character of the magnetic excitations in DTN in the vicinity of the QCPs.

cond-mat.stat-mech↗

arXiv2008

A direct measurement of the Bose-Einstein Condensation universality class in NiCl$_2$-4SC(NH$_2$)$_2$ at ultra-low temperatures

In this work, we demonstrate field-induced Bose-Einstein condensation (BEC) in the organic compound NiCl$_2$-4SC(NH$_2$)$_2$ using AC susceptibility measurements down to 1 mK. The Ni $\textsl{S}$=1 spins exhibit 3D $\mathit{XY}$ antiferromagnetism between a lower critical field $H_{c1} \sim$ 2 T and a upper critical field $H_{c2} \sim$ 12 T. The results show a power-law temperature dependence of the phase transition line $H_{c1} (T) -H_{c1} (0) = aT^α$ with $α=$ 1.47$\pm$0.10 and $H_{c1} (0) = 2.053$ T, consistent with the 3D Bose-Einstein Condensation universality class. An abnormal change was found in the phase boundary near $H_{c2}$ at approximately 150 mK.

cond-mat.str-el↗

arXiv2008

Spin Dynamics of $Ni Cl_2-4SC(NH_2)_2$ in the Field-Induced Ordered Phase

$Ni Cl_2$-$4SC(NH_2)_2$ (known as DTN) is a spin-1 material with a strong single-ion anisotropy that is regarded as a new candidate for Bose-Einstein condensation (BEC) of spin degrees of freedom. We present a systematic study of the low-energy excitation spectrum of DTN in the field-induced magnetically ordered phase by means of high-field electron spin resonance measurements at temperatures down to 0.45 K. We argue that two gapped modes observed in the experiment can be consistently interpreted within a four-sublattice antiferromagnet model with a finite interaction between two tetragonal subsystems and unbroken axial symmetry. The latter is crucial for the interpretation of the field-induced ordering in DTN in terms of BEC.

cond-mat.str-el↗

arXiv2008

Bose-Einstein condensation in antiferromagnets close to the saturation field

At zero temperature and strong applied magnetic fields the ground sate of an anisotropic antiferromagnet is a saturated paramagnet with fully aligned spins. We study the quantum phase transition as the field is reduced below an upper critical $H_{c2}$ and the system enters a XY-antiferromagnetic phase. Using a bond operator representation we consider a model spin-1 Heisenberg antiferromagnetic with single-ion anisotropy in hyper-cubic lattices under strong magnetic fields. We show that the transition at $H_{c2}$ can be interpreted as a Bose-Einstein condensation (BEC) of magnons. The theoretical results are used to analyze our magnetization versus field data in the organic compound $NiCl_2$-$4SC(NH_2)_2$ (DTN) at very low temperatures. This is the ideal BEC system to study this transition since $H_{c2}$ is sufficiently low to be reached with static magnetic fields (as opposed to pulsed fields). The scaling of the magnetization as a function of field and temperature close to $H_{c2}$ shows excellent agreement with the theoretical predictions. It allows to obtain the quantum critical exponents and confirm the BEC nature of the transition at $H_{c2}$.

cond-mat.str-el↗

arXiv2007

Using magnetostriction to measure the spin-spin correlation function and magnetoelastic coupling in the quantum magnet NiCl$_2$-4SC(NH$_2$)$_2$

We report a method for determining the spatial dependence of the magnetic exchange coupling, $dJ/dr$, from magnetostriction measurements of a quantum magnet. The organic Ni $S = 1$ system NiCl$_2$-4SC(NH$_2$)$_2$ exhibits lattice distortions in response to field-induced canted antiferromagnetism between $H_{c1} = 2.1$ T and $H_{c2} = 12.6$ T. We are able to model the magnetostriction in terms of uniaxial stress on the sample created by magnetic interactions between neighboring Ni atoms along the c-axis. The uniaxial strain is equal to $(1/E)dJ_c/dx_c < S_{\bf r} \cdot S_{{\bf r}+ {\bf e}_c} >$, where $E$, $J_c$, $x_c$ and ${\bf e}_c$ are the Young's modulus, the nearest neighbor (NN) exchange coupling, the variable lattice parameter, and the relative vector between NN sites along the c-axis. We present magnetostriction data taken at 25 mK together with Quantum Monte Carlo calculations of the NN spin-spin correlation function that are in excellent agreement with each other. We have also measured Young's modulus using resonant ultrasound, and we can thus extract $dJ_c/dx_c = 2.5$ K/$Å$, yielding a total change in $J_c$ between $H_{c1}$ and $H_{c2}$ of 5.5 mK or 0.25% in response to an 0.022% change in length of the sample.

cond-mat.str-el↗

arXiv2007

Magnetic Excitations in the Spin-1 Anisotropic Heisenberg Antiferromagnetic Chain System NiCl$_2$-4SC(NH$_2$)$_2$

NiCl$_2$-4SC(NH$_2$)$_2$ (DTN) is a quantum S=1 chain system with strong easy-pane anisotropy and a new candidate for the Bose-Einstein condensation of the spin degrees of freedom. ESR studies of magnetic excitations in DTN in fields up to 25 T are presented. Based on analysis of the single-magnon excitation mode in the high-field spin-polarized phase and previous experimental results [Phys. Rev. Lett. 96, 077204 (2006)], a revised set of spin-Hamiltonian parameters is obtained. Our results yield $D=8.9$ K, $J_c=2.2$ K, and $J_{a,b}=0.18$ K for the anisotropy, intrachain, and interchain exchange interactions, respectively. These values are used to calculate the antiferromagnetic phase boundary, magnetization and the frequency-field dependence of two-magnon bound-state excitations predicted by theory and observed in DTN for the first time. Excellent quantitative agreement with experimental data is obtained.

cond-mat.str-el↗

arXiv2006

Magnetostriction in the Bose-Einstein Condensate quantum magnet NiCl2-4SC(NH2)2

The quantum magnet NiCl$_2$-4SC(NH$_2$)$_2$ is a candidate for observing Bose-Einstein Condensation of spin degrees of freedom in applied magnetic fields. An XY antiferromagnetic ordered state occurs in a dome-shaped region of the temperature-field phase diagram between H$_{c1}$ = 2.1 T and H$_{c2}$ = 12.6 T and below 1.2 K. BEC corresponds to the field-induced quantum phase transition into the ordered state. We investigate magnetostriction in single crystals of this compound at dilution refrigerator temperatures in magnetic fields up to 18 T, and as a function of magnetic field angle. We show that significant changes in the lattice parameters are induced by magnetic fields, and argue that these result from antiferromagnetic couplings between the Ni spins along the tetragonal c-axis. The magnetic phase diagram as a function of temperature, field, and field angle can be extracted from these data. We discuss the implications of these results to Bose-Einstein Condensation in this system.

cond-mat.str-el↗

arXiv2005

Bose-Einstein Condensation of S = 1 Ni spin degrees of freedom in NiCl2-4SC(NH2)2

It has recently been suggested that the organic compound NiCl$_2$-4SC(NH$_2$)$_2$ (DTN) exhibits Bose-Einstein Condensation (BEC) of the Ni spin degrees of freedom for fields applied along the tetragonal c-axis. The Ni spins exhibit 3D XY-type antiferromagnetic order above a field-induced quantum critical point at $H_{c1} \sim 2$ T. The Ni spin fluid can be characterized as a system of effective bosons with a hard-core repulsive interaction in which the antiferromagnetic state corresponds to a Bose-Einstein condensate (BEC) of the phase coherent $S = 1$ Ni spin system. We have investigated the the high-field phase diagram and the occurrence of BEC in DTN by means of specific heat and magnetocaloric effect measurements to dilution refrigerator temperatures. Our results indicate that a key prediction of BEC is satisfied; the magnetic field-temperature quantum phase transition line $H_c(T)-H_{c1} \propto T^α$ approaches a power-law at low temperatures, with an exponent $α= 1.47 \pm 0.06$ at the quantum critical point, consistent with the BEC theory prediction of $α= 1.5$.

cond-mat.str-el↗