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Mark P. Zic

Publications and source records attributed to Mark P. Zic.

8 recordsLinked to original sources

Slow spin-lattice relaxation dynamics in YbVO4 revealed by extended thermal impedance spectroscopy from AC susceptibility and AC magnetocaloric measurements

Alternating (AC) magnetic fields can induce not only an alternating magnetization in materials, but also an alternating temperature via the magnetocaloric effect. The latter effect is typically neglected when performing AC susceptibility measurements, but consideration of both effects on an equal footing is necessary in order to reliably distinguish between internal and external causes of magnetic response and accurately extract quantitative information about relaxation processes. In order to address this, we have developed a method to measure the AC magnetocaloric effect that is compatible with AC susceptibility measurements, and also a framework to analyze these data in combination. We demonstrate the efficacy of this approach using YbVO4, a material for which strong single-ion anisotropy leads to slow spin-lattice relaxation at low temperatures via a phonon bottleneck effect. We report AC magnetic susceptibility and AC magnetocaloric effect measurements for this material as a function of field and frequency at a temperature of 3 K. We analyze the data using a discretized thermal model, and extract the field-dependence of the intrinsic spin-lattice relaxation rate. This demonstration experiment illustrates a general approach to quantitatively address multiple measured quantities in driven systems using a unified thermal circuit analysis. The thermal analysis methods presented in this report can be extended to study other magnetic, dielectric, and elastic materials exhibiting a complex response to an external driving field in the presence of internal and external relaxation, particularly when an energy dissipation process is within an accessible frequency regime.

cond-mat.mtrl-sci

Electro-nuclear quantum phase transition in TmVO$_4$

Hyperfine interactions couple nuclear and electronic degrees of freedom. The present work explores how hyperfine coupling within the Tm ions in TmVO$_4$ single crystals affects an electronic ferroquadrupole ordered ground state and its associated field-tuned quantum phase transition. For temperatures below the hyperfine energy scale, the nuclear moments reduce the critical field for the electronic order, resulting in a dramatic back-bending of the phase boundary delineating the ferroquadrupole order. This behavior is well described by a single-ion semiclassical mean-field model. Moreover, analysis of the effective Hamiltonian leads to a prediction of spontaneous nuclear magnetic order mediated by 4$f$ electrons, which in principle persists with the application of orthogonal antisymmetric strain, yielding a proposed electro-nuclear tetracritical point.

cond-mat.str-el

Realization of discretized response in rare-earth vanadates accessed by AC susceptibility and magnetocaloric methods

This report presents a new technique to probe the quantitative dynamical response of the magnetic field induced heating/cooling process in rare-earth vanadium materials. The approach combines AC susceptibility and AC caloric measurements to reveal the intrinsic timescale associated with the magnetic relaxation process of rare-earth ions at low temperatures. Utilizing the well-known crystal field effect in YbVO4, we prove and demonstrate a discretized thermal analysis through a common spin-lattice relaxation phenomenon. The demonstration experiment presented in this study provides a general approach to quantitatively address multiple measured quantities in one unified discretized thermal circuit analysis. It can be extended to study other magnetic, dielectric, and elastic materials exhibiting a complex response to an external driving field in the presence of intrinsic interactions and fluctuations, particularly when an energy dissipation process is within an accessible frequency regime.

cond-mat.mtrl-sci

Realization of giant elastocaloric cooling at cryogenic temperatures in TmVO$_4$ via a strain load/unload technique

The adiabatic elastocaloric effect relates changes in the strain that a material experiences to resulting changes in its temperature. While elastocaloric materials have been utilized for cooling in room temperature applications, the use of such materials for cryogenic cooling remains relatively unexplored. Here, we use a strain load/unload technique at low temperatures, similar to those employed at room-temperature, to demonstrate a large cooling effect in TmVO$_4$. For strain changes of $1.8 \cdot 10^{-3}$, the inferred cooling reaches approximately 50% of the material's starting temperature at 5 K, justifying the moniker "giant". Beyond establishing the suitability of this class of material for cryogenic elastocaloric cooling, these measurements also provide additional insight to the entropy landscape in the material as a function of strain and temperature, including the behavior proximate to the quadrupolar phase transition.

cond-mat.mtrl-sci

Role of magnetic ions in the thermal Hall effect of the paramagnetic insulator TmVO$_{4}$

In a growing number of materials, phonons have been found to generate a thermal Hall effect, but the underlying mechanism remains unclear. Inspired by previous studies that revealed the importance of Tb$^{3+}$ ions in generating the thermal Hall effect in a family of pyrochlores, we investigated the role of Tm$^{3+}$ ions in TmVO$_{4}$, a paramagnetic insulator with a different crystal structure. We observe a negative thermal Hall conductivity in TmVO$_{4}$ with a magnitude such that the Hall angle, $|κ_{xy}$/$κ_{xx}|$, is approximately 1 x 10$^{-3}$ at $H$ = 15 T and $T$ = 20 K, typical for a phonon-generated thermal Hall effect. In contrast to the negligible $κ_{xy}$ found in the nonmagnetic pyrochlore analog (where the Tb$^{3+}$ ions are replaced with Y$^{3+}$), we observe a negative $κ_{xy}$ in YVO$_{4}$ with a Hall angle of magnitude comparable to that of TmVO$_{4}$. This shows that the Tm$^{3+}$ ions are not essential for the thermal Hall effect in this family of materials. Interestingly, at an intermediate Y concentration of $x$ = 0.3 in Tm$_{1-x}$Y$_{x}$VO$_{4}$, $κ_{xy}$ was found to have a positive sign, pointing to the importance of impurities in the thermal Hall effect of phonons.

cond-mat.mtrl-sci

Disorder-induced local strain distribution in Y-substituted TmVO4

We report an investigation of the effect of substitution of Y for Tm in $Tm_{1-x}Y_xVO4$ via low-temperature heat capacity measurements, with the yttrium content $x$ varying from $0$ to $0.997$. Because the Tm ions support a local quadrupolar (nematic) moment, they act as reporters of the local strain state in the material, with the splitting of the ion's non-Kramers crystal field groundstate proportional to the quadrature sum of the in-plane tetragonal symmetry-breaking transverse and longitudinal strains experienced by each ion individually. Analysis of the heat capacity therefore provides detailed insights into the distribution of local strains that arise as a consequence of the chemical substitution. These local strains suppress long-range quadrupole order for $x>0.22$, and result in a broad Schottky-like feature for higher concentrations. Heat capacity data are compared to expectations for a distribution of uncorrelated (random) strains. For dilute Tm concentrations, the heat capacity cannot be accounted for by randomly distributed strains, demonstrating the presence of significant strain correlations between sites. For intermediate Tm concentrations, these correlations must still exist, but the data cannot be distinguished from that which would be obtained from a 2D Gaussian distribution. The cross-over between these limits is discussed in terms of the interplay of key length scales in the substituted material. The central result of this work, that local strains arising from chemical substitution are not uncorrelated, has implications for the range of validity of theoretical models based on random effective fields that are used to describe such chemically substituted materials, particularly when electronic nematic correlations are present.

cond-mat.str-el

Giant elastocaloric effect at low temperatures in TmVO$_4$ and implications for cryogenic cooling

Adiabatic decompression of para-quadrupolar materials has significant potential as a cryogenic cooling technology. We focus on TmVO$_4$, an archetypal material that undergoes a continuous phase transition to a ferroquadrupole-ordered state at 2.15 K. Above the phase transition, each Tm ion contributes an entropy of $k_B \ln{2}$ due to the degeneracy of the crystal electric field groundstate. Owing to the large magnetoelastic coupling, which is a prerequisite for a material to undergo a phase transition via the cooperative Jahn-Teller effect, this level splitting, and hence the entropy, can be readily tuned by externally-induced strain. Using a dynamic technique in which the strain is rapidly oscillated, we measure the adiabatic elastocaloric coefficient of single-crystal TmVO$_4$, and thus experimentally obtain the entropy landscape as a function of strain and temperature. The measurement confirms the suitability of this class of materials for cryogenic cooling applications, and provides insight to the dynamic quadrupole strain susceptibility.

cond-mat.str-el

Symmetry of magnetic correlations in spin-triplet superconductor UTe2

The temperature dependence of the low-energy magnetic excitations in the spin-triplet superconductor UTe$_2$ was measured via inelastic neutron scattering in the normal and superconducting states. The imaginary part of the dynamic susceptibility follows the behavior of interband correlations in a hybridized Kondo lattice with an appropriate characteristic energy. These excitations are a lower-dimensional analogue of phenomena observed in other Kondo lattice materials, such that their presence is not necessarily due to dominance of ferromagnetic or antiferromagnetic correlations. The onset of superconductivity alters the magnetic excitations noticeably on the same energy scales, suggesting that these changes originate from additional electronic structure modification.

cond-mat.str-el