Magnetocaloric Effect Measurements Research Articles

Quantum simulation of an extended Dicke model with a magnetic solid

The Dicke model describes the cooperative interaction of an ensemble of two-level atoms with a single-mode photonic field and exhibits a quantum phase transition as a function of light–matter coupling strength. Extending this model by incorporating short-range atom–atom interactions makes the problem intractable but is expected to produce new physical phenomena and phases. Here, we simulate such an extended Dicke model using a crystal of ErFeO3, where the role of atoms (photons) is played by Er3+ spins (Fe3+ magnons). Through terahertz spectroscopy and magnetocaloric effect measurements as a function of temperature and magnetic field, we demonstrated the existence of a novel atomically ordered phase in addition to the superradiant and normal phases that are expected from the standard Dicke model. Further, we elucidated the nature of the phase boundaries in the temperature–magnetic-field phase diagram, identifying both first-order and second-order phase transitions. These results lay the foundation for studying multiatomic quantum optics models using well-characterized many-body solid-state systems.

Sudden adiabaticity signals reentrant bulk superconductivity in UTe2.

There has been a recent surge of interest in UTe due to its unconventional magnetic field (H)-reinforced spin-triplet superconducting phases persisting at fields far above the simple Pauli limit for . Magnetic fields in excess of 35 T then induce a field-polarized magnetic state via a first-order-like phase transition. More controversially, for field orientations close to and above 40 T, electrical resistivity measurements suggest that a further superconducting state may exist. However, no Meissner effect or thermodynamic evidence exists to date for this phase making it difficult to exclude alternative scenarios. In this paper, we describe a study using thermal, electrical, and magnetic probes in magnetic fields of up to 55 T applied between the [010] (b) and [001] (c) directions. Our MHz conductivity data reveal the field-induced state of low or vanishing electrical resistance; our simultaneous magnetocaloric effect measurements (i.e. changes in sample temperature due to changing magnetic field) show the first definitive evidence for adiabaticity and thermal behavior characteristic of bulk field-induced superconductivity.

Magnetic field induced reentrant multipolar ordering in the distorted kagome-lattice antiferromagnet Dy3Ru4Al12

We report on ultrasonic and magnetocaloric-effect measurements of the hexagonal antiferromagnet ${\mathrm{Dy}}_{3}{\mathrm{Ru}}_{4}{\mathrm{Al}}_{12}$ having a distorted kagome lattice. We observed a pronounced softening of the transverse modulus, ${C}_{44}$, above 30 T applied along [100], indicating an as-yet-unidentified magnetic field induced phase transition. We determined the field-temperature phase diagrams using pulsed magnetic fields up to 55.2 T, applied along [100] and [001]. Optimizing crystal-electric-field parameters within the mean-field approximation, we conclude that the enhancement of the field induced phase-transition temperature is due to electric quadrupolar and magnetic octupolar mediated interactions. We propose that the order parameter of the magnetic field induced phase transitions is the electric quadrupole ${O}_{zx}$, facilitated by octupole-mediated interactions.

Magnetic phase diagrams and large magnetocaloric effects of the two-dimensional antiferromagnetic triangular lattice of Gd3+ ions in KBaGd(BO3)2

We report a detailed study of the magnetic properties of KBaGd(BO$_3$)$_2$, in which magnetic Gd$^{3+}$ ($S=7/2$) ions form into two-dimensional triangular layers. Magnetization, specific heat and magnetocaloric effect (MCE) measurements have been performed on KBaGd(BO$_3$)$_2$ single crystals. The results show that a long-range antiferromagnetic state is established below $T_{\rm N}=0.24$ K. In zero fields, only about half of the full entropy is released at $T_{\rm N}$, indicating that not all the magnetic moments are frozen below the ordering temperature, as expected from the geometrical frustration of the triangular spin lattice. Further studies under external fields were performed down to 50 mK, and the magnetic phase diagrams are established with magnetic fields applied both within and perpendicular to the triangular plane. KBaGd(BO$_3$)$_2$ serves as an example of a two-dimensional triangular lattice with large spin values ($S=7/2$) and can be directly compared with the iso-structure KBaR(BO$_3$)$_2$ (R = Dy-Yb) family of doublet ground states, which exhibit effective spins of $S=1/2$.

Complex magnetic phase diagram with a small phase pocket in a three-dimensional frustrated magnet CuInCr4S8

Frustrated magnets with a strong spin-lattice coupling can show rich magnetic phases and the associated fascinating phenomena. A promising platform is the breathing pyrochlore magnet ${\mathrm{CuInCr}}_{4}{\mathrm{S}}_{8}$ with localized $S=3/2\phantom{\rule{4pt}{0ex}}{\mathrm{Cr}}^{3+}$ ions, which is proposed to be effectively viewed as an $S=6$ Heisenberg antiferromagnet on the face-centered-cubic lattice. Here we unveil that ${\mathrm{CuInCr}}_{4}{\mathrm{S}}_{8}$ exhibits a complex magnetic phase diagram with a small phase pocket ($A$ phase) by means of magnetization, magnetostriction, magnetocapacitance, and magnetocaloric-effect measurements in pulsed high magnetic fields of up to 60 T. Remarkably, the appearance of $A$ phase is accompanied by anomalous magnetostrictive and magnetocapacitive responses, suggesting the emergence of helimagnetism in contrast to the neighboring commensurate magnetic phases. Besides, the high-entropy nature is confirmed in the high-temperature side of $A$ phase. These features are potentially related to a thermal fluctuation-driven multiple-$q$ state caused by the magnetic frustration, which has been theoretically predicted but yet experimentally undiscovered in insulating magnets.

Antiferromagnetism and Ising ground states in the rare-earth garnet Nd3Ga5O12

In this paper, we investigate the low temperature magnetic properties of the rare-earth garnet compound Nd$_3$Ga$_5$O$_{12}$ in detail by means of magnetization, specific heat and magnetocaloric effect measurements. The magnetic thermal properties along with the crystal field calculations reveal that the Nd$^{3+}$ ions form into a frustrated hyper-kagome lattice with connected triangles have an Ising-like ground state with the easy axis along the local [100], [010] and [001] directions. Instead of a quantum spin liquid ground state, an antiferromagnetically ordered state is found below $T_{\mathrm{N}}=0.52~\rm K$. With applying field in the [111] direction, the antiferromagnetic order is suppressed at the critical field of $B_{\mathrm{c}}=0.75~\rm T$, and enhancement of the critical fluctuations with linear crossover behaviors is observed near the critical point.

Field-induced anomalous magnetic state beyond the magnetically ordered state in the slightly distorted triangular S=12 rare-earth antiferromagnet CeZn3P3

Magnetic properties of ${\mathrm{CeZn}}_{3}{\mathrm{P}}_{3}$, which has been believed to have the same hexagonal ${\mathrm{ScAl}}_{3}{\mathrm{C}}_{3}$-type crystal structure as that of a spin dimer system of ${\mathrm{YbAl}}_{3}{\mathrm{C}}_{3}$ at room temperature, have been investigated by magnetization, magnetostriction, specific heat ($C$), and magnetocaloric effect measurements. In this research, we have found that ${\mathrm{CeZn}}_{3}{\mathrm{P}}_{3}$ certainly has a slightly deformed crystal structure from the hexagonal one even at room temperature, which is in contrast to the structural phase transition of ${\mathrm{YbAl}}_{3}{\mathrm{C}}_{3}$ occuring at around 80 K, although the very slight deformation along the $c$ plane, i.e., slightly deformed triangular lattice, and the formation of the multidomain structure are common to both compounds. ${\mathrm{CeZn}}_{3}{\mathrm{P}}_{3}$ is thought to maintain its deformed structure from a high-temperature region above room temperature to an extremely low-temperature region and shows a magnetic order below ${T}_{\mathrm{N}}=0.8$ K. The analysis of the temperature dependence of the magnetic susceptibility ($\ensuremath{\chi}$) and $C$ has revealed that a Kramers doublet ground state with an easy-plane type anisotropy on the $c$ plane is well isolated from the excited states by the crystal field splitting energy of more than 300 K. Above ${T}_{\mathrm{N}}, \ensuremath{\chi}$ makes a broad peak at around 2 K, which certainly originates from the dimer formation due to the slight deformation of the triangular lattice. On the other hand, below ${T}_{\mathrm{N}}$, a magnetic phase diagram reminiscent of a magnetic flower blooming on the $c$ plane was observed, which may have a close relation to a quantum effect of a quasi $S=\frac{1}{2}$ spin system and a contribution of the orbital component. With increasing magnetic field, we have found an anomalous magnetic state beyond the usual magnetically ordered state, where $C/T$ is anomalously enhanced. This anomalous magnetic state is similar to that observed in ${\mathrm{YbAl}}_{3}{\mathrm{C}}_{3}$ induced by the field, although the magnetic ground state in ${\mathrm{YbAl}}_{3}{\mathrm{C}}_{3}$ is a nonmagnetic dimer state different from the normal magnetically ordered state in ${\mathrm{CeZn}}_{3}{\mathrm{P}}_{3}$.

High-field phase diagram of Ni3V2O8 studied by specific heat and magnetocaloric effect measurements

The H–T phase diagram of Ni3V2O8 is very rich and remains puzzling in a high magnetic field range. Through the state-of-the-art specific heat measurement in pulsed high field to 35 T and magnetocaloric effect measurement up to 45 T, we successfully construct the high-field phase diagram of Ni3V2O8 for fields applied along the b axis. The phase boundaries are corrected for previous results by magnetization and magneto-optical measurements. The resulting phase diagram shows that the high temperature incommensurate (HTI) phase develops well to high fields and low temperatures. In addition to the early reported C′, C, low temperature incommensurate (LTI) and HTI phases, we explore a new magnetic ordered phase called HF1 in fields of 10–30 T. A multicritical point is also observed at 6 K and 8 T. Furthermore, the specific heat data reveal enhancements of the anomalies at ∼4 K, probably associated with a strong spin–lattice coupling in this frustrated multiferroic material.

Observation of inverse magnetocaloric effect in magnetic-field-induced austenite phase of Heusler alloys Ni50−xCoxMn31.5Ga18.5 (x=9 and 9.7)

Magnetocaloric effect (MCE), magnetization, specific heat, and magnetostriction measurements were performed in both pulsed and steady high magnetic fields to investigate the magnetocaloric properties of Heusler alloys Ni50-xCoxMn31.5Ga18.5 (x = 9 and 9.7). From direct MCE measurements for Ni41Co9Mn31.5Ga18.5 up to 56 T, a steep temperature drop was observed for magnetic-field-induced martensitic transformation (MFIMT), designated as inverse MCE. Remarkably, this inverse MCE is apparent not only with MFIMT, but also in the magnetic-field-induced austenite phase. Specific heat measurements under steady high magnetic fields revealed that the magnetic field variation of the electronic entropy plays a dominant role in the unconventional magnetocaloric properties of these materials. First-principles based calculations performed for Ni41Co9Mn31.5Ga18.5 and Ni45Co5Mn36.7In13.3 revealed that the magnetic-field-induced austenite phase of Ni41Co9Mn31.5Ga18.5 is more unstable than that of Ni45Co5Mn36.7In13.3 and that it is sensitive to slight tetragonal distortion. We conclude that the inverse MCE in the magnetic-field-induced austenite phase is realized by marked change in the electronic entropy through tetragonal distortion induced by the externally applied magnetic field.

Element-specific field-induced spin reorientation and tetracritical point in MnCr2S4

The ferrimagnetic spinel MnCr2S4 shows a variety of magnetic-field-induced phase transitions owing to bond frustration and strong spin-lattice coupling. However, the site-resolved magnetic properties at the respective field-induced phases in high magnetic fields remain elusive. Our soft x-ray magnetic circular dichroism studies up to 40 T directly evidence element-selective magnetic-moment reorientations in the field-induced phases. The complex magnetic structures are further supported by entropy changes extracted from magnetocaloric-effect measurements. Moreover, thermodynamic experiments reveal an unusual tetracritical point in the H-T phase diagram of MnCr2S4 due to strong spin-lattice coupling.

Capacitive detection of magnetostriction, dielectric constant, and magneto-caloric effects in pulsed magnetic fields.

We report on the development of a capacitance measuring system that allows measurements of capacitance in pulsed magnetic fields up to 61 T. By using this system, magnetic-field responses of various physical quantities, such as magnetostriction, magnetic-field-induced change in complex dielectric constant, and magneto-caloric effect, can be investigated in pulsed-magnetic-field conditions. Here, we examine the validity of our system for investigations of these magnetic-field-induced phenomena in pulse magnets. For the magnetostriction measurement, magnetostriction of a specimen can be measured through a change in the capacitance between two aligned electrodes glued on the specimen and a dilatometer. We demonstrate a precise detection of valley polarization in semimetallic bismuth through a magnetostriction signal with a resolution better than 10-6 of the relative length change. For the magnetic-field-induced change in complex dielectric constant, we successfully observed clear dielectric anomalies accompanied by magnetic/magnetoelectric phase transitions in multiferroic Pb(TiO)Cu4(PO4)4. For the measurement of magneto-caloric effect, a magnetic-field-induced change in sample temperature was verified for Gd3Ga5O12 with a capacitance thermometer made of a non-magnetic ferroelectric compound KTa1-xNbxO3 (x = 0.02) whose capacitance is nearly field-independent. These results show that our capacitance measuring system is a promising tool to study various magnetic-field-induced phenomena, which have been difficult to detect in pulsed magnetic fields.

Magnetic properties and near-room-temperature large magnetocaloric effect in (La1-xBix)0.67Ba0.33MnO3 (x = 0 - 0.3) ceramics

The magnetic and magnetocaloric properties of (La1-xBix)0.67Ba0.33MnO3 (for x = 0 - 0.3) ceramics are reported. Magnetization measurements reveal the onset of a ferromagnetic ordering (TC) in the range 336 K- 229 K which shifts towards low temperatures with increasing x. Magnetocaloric effect (MCE) measurements yield the maximum value of entropy change (-ΔSMmax) around TC that decreases from ∼6.19 J/ Kg/K for x = 0 to ∼4.79 J/ Kg/K for x = 0.3 for a field change of 9 T. Remarkable enhancement in the relative cooling power (RCP) is observed with the value increasing from ∼400.45 J/Kg for x = 0 to ∼472.81 J/Kg for x = 0.3. The substantial increase in the magnetocaloric properties of (La1-xBix)0.67Ba0.33MnO3 compounds compared to other compounds reported in the literature makes them potential candidates to be used for magnetic refrigeration purposes.

Low-Temperature Magnetism in a Triangular-Lattice Antiferromagnet, Cu3(OH)4(HCO2)2, Studied by Calorimetry

We report the results of specific-heat and magnetocaloric-effect measurements on a triangular-lattice antiferromagnet, Cu3(OH)4(HCO2)2. A magnetically-ordered phase is suppressed by applying magnet...

Simultaneous direct measurements of conventional and inverse magnetocaloric effects in Ni–Mn-based Heusler alloys using lock-in thermography technique

The second-order conventional and first-order inverse magnetocaloric effects (MCEs) in Ni–Mn-based quaternary Heusler alloys have been systematically investigated by means of the lock-in thermography technique, which enables the direct measurement of the MCE-induced temperature change in a periodic magnetic field. Through systematic measurements of the temperature dependence of the MCE signals, the tuning of the conventional and inverse MCEs with temperature for the same Heusler alloys has been demonstrated, where the phase transitions responsible for the MCEs are clearly distinguished. The lock-in thermography measurements show that some Ni–Mn-based Heusler alloys exhibit much smaller temperature changes due to the inverse MCEs in the periodic field as compared to the conventional MCEs, even though they exhibit a larger magnetic entropy change across the first-order transition responsible for the inverse MCEs. We discuss the origin of this behavior in terms of the field-induced entropy change and thermal hysteresis of the alloys. These findings will be useful not only in accelerating the optimization of inverse MCE materials but also in understanding the mechanism of the MCEs.

Emergent critical phenomenon in spin- 12 ferromagnetic-leg ladders: Quasi-one-dimensional Bose–Einstein condensate

We examine the magnetic-field-induced criticality of phase boundary near saturation field $H_{\mathrm{c}}$ in the spin-1/2 ferromagnetic (FM)-leg ladder 3-Cl-4-F-V [=3-(3-chloro-4-fluorophenyl)-1,5-diphenylverdazyl], the predominant interactions of which arise from FM chains (strong-leg type). Critical temperatures were precisely determined through dc magnetization, specific heat, and magnetocaloric effect measurements. The criticality of 3-Cl-4-F-V is characterized by a linear phase boundary with respect to $H_{\mathrm{c}}-H$ near $H\,=\,H_{\mathrm{c}}$. This behavior is similar to that of another strong-leg-type FM-leg ladder. The universal critical behavior in these strong-leg-type FM-leg ladders is expected to demonstrate the theoretically predicted quasi-one-dimensional Bose--Einstein condensation.

Thermodynamic Investigation of Metamagnetism in Pulsed High Magnetic Fields on Heavy Fermion Superconductor UTe2

We investigated the thermodynamic property of the heavy fermion superconductor UTe$_2$ in pulsed high magnetic fields. The superconducting transition in zero field was observed at $T_{\rm c}$=1.65 K as a sharp heat capacity jump. Magnetocaloric effect measurements in pulsed-magnetic fields obviously detected a thermodynamic anomaly accompanied by a first-order metamagnetic transition at $\mu$$_{0}$$H_{\rm m}$=36.0 T when the fields are applied nearly along the hard-magnetization $b$-axis. From the results of heat capacity measurements in magnetic fields, we found a drastic diverging electronic heat capacity coefficient of the normal state $\gamma$$_{\rm N}$ with approaching $H_{\rm m}$. Comparing with the previous works via the magnetic Clausius-Clapeyron relation, we unveil the thermodynamic details of the metamagnetic transition. The enhancement of the effective mass observed as the development of $\gamma_{\rm N}$ indicates that quantum fluctuation strongly evolves around $H_{\rm m}$; it assists the superconductivity emerging even in extremely high fields.

Enhanced magnetocaloric effect in manganite nanodisks

Manganites are an important class of materials that exhibit a large magnetocaloric effect (MCE). The large MCE is often accompanied by complex magnetic phase transitions associated with electronic phase separation (EPS) in manganites. In previous studies, the effect of EPS on MCE has been examined in chemically synthesized manganite nanoparticles, in which the EPS vanishes when the particle size is smaller than a few tens of nanometers. However, the surface area to volume ratio is high in these small nanoparticles and surface spin disordering can lead to controversial results for MCE measurements. In this study, we used $\mathrm{L}{\mathrm{a}}_{0.425}\mathrm{P}{\mathrm{r}}_{0.2}\mathrm{C}{\mathrm{a}}_{0.375}\mathrm{Mn}{\mathrm{O}}_{3}$ nanodisk arrays fabricated from epitaxially grown thin films as model systems to investigate how MCE changes during a clean transition from the EPS state in thin film and 2-\ensuremath{\mu}m-sized disk arrays to a single ferromagnetic state in 500-nm-sized disk arrays. The MCE of the 500-nm-sized disk array is almost twice that of its parent film. Our results present an approach to improve the MCE in manganite systems for future magnetic refrigeration applications.

Finite field regime for a quantum spin liquid in α−RuCl3

An external magnetic field can induce a transition in $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$ from an ordered zigzag state to a disordered state that is possibly related to the Kitaev quantum spin liquid. Here, we present field-dependent inelastic neutron scattering and magnetocaloric effect measurements implying the existence of an additional transition out of the quantum spin-liquid phase at an upper field limit ${B}_{u}$. The neutron scattering shows three distinct regimes of magnetic response. In the low-field ordered state the response shows magnon peaks; the intermediate-field regime shows only continuum scattering, and above ${B}_{u}$ the response shows sharp magnon peaks at the lower bound of a strong continuum. Measurable dispersion of magnon modes along the $(0,0,L)$ direction implies non-negligible interplane interactions. Combining the magnetocaloric effect measurements with other data, a $T\text{\ensuremath{-}}B$ phase diagram is constructed. The results constrain the range where one might expect to observe quantum spin-liquid behavior in $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$.

Giant reversible adiabatic temperature change and isothermal heat transfer of MnAs single crystals studied by direct method in high magnetic fields

The magnetocaloric effect (MCE) in single crystals of MnAs compound was studied both experimentally and theoretically. Direct measurement of MCE showed that the adiabatic temperature change (ΔTad) in a magnetic field of 10 T was 15 K. But direct measurement of the quasi-adiabatic heat transfer (ΔQ) of the sample yielded a value of 9500 J/kg in a magnetic field of 10 T. To date, it is the highest experimentally recorded value for ΔQ by direct measurement. Phenomenological considerations that take into account the interaction of magnetic and structural order parameters explain a number of anomalies in the magnetic and magnetocaloric properties of MnAs that were observed during the experiments.

Magnetocaloric effect in Gd5(Si,Ge)4 based alloys and composites

The research on magnetocaloric materials for applications concentrates, among other, on two parameters: the ordering temperature and the value of the magnetocaloric effect (MCE). The optimization consists in tuning the former without significant drop in the latter. These studies report on the magnetic susceptibility, magnetization curves, heat capacity and magnetocaloric effect measurements for compositionally and structurally modified Gd5Si4 compound. The modifications are based on the doping of the parent compound with an excess Gd atoms and substitution of Si with B as well as on the dimensional effect studied by mechanical milling. Moreover, composite samples of the type Gd:Gd5Si2Ge2 were investigated revealing the influence of the intergranular interactions on the magnetocaloric properties. It appears that these interventions enable a controllable steering of the ordering temperature shifting it towards the room temperature with, in some cases, minor reduction of the parameters characterizing MCE.