Large out-of-equilibrium magnetocaloric effect in rare-earth zirconate pyrochlores

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Main Authors: Benton, O., Skourski, Y., Gorbunov, D., Miyata, A., Chattopadhyay, S., Wosnitza, J., Hatnean, M. Ciomaga, Balakrishnan, G., Zherlitsyn, S., Petrenko, O. A.
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Published: 2025
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author Benton, O.
Skourski, Y.
Gorbunov, D.
Miyata, A.
Chattopadhyay, S.
Wosnitza, J.
Hatnean, M. Ciomaga
Balakrishnan, G.
Zherlitsyn, S.
Petrenko, O. A.
author_facet Benton, O.
Skourski, Y.
Gorbunov, D.
Miyata, A.
Chattopadhyay, S.
Wosnitza, J.
Hatnean, M. Ciomaga
Balakrishnan, G.
Zherlitsyn, S.
Petrenko, O. A.
contents We explore the magnetic properties of Nd$_2$Zr$_2$O$_7$ and Pr$_2$Zr$_2$O$_7$ single crystals subjected to pulsed magnetic fields up to 60 T using magnetization and magnetocaloric-effect (MCE) measurements, with initial temperatures ranging from 2 to 31K. The MCE data exhibit pronounced and unconventional hysteresis loops, in which the sample temperature increases during both the up-sweep and down-sweep of the field. In Nd$_2$Zr$_2$O$_7$, the MCE further displays a striking plateau as a function of time, followed by a rapid temperature rise that begins at the maximum applied field, across pulses with differing peak-field strengths. Our magnetization measurements reveal an inferred temperature of the magnetic subsystem that differs significantly from the directly measured sample temperature and exhibits opposite hysteresis: the temperature is higher on the up-sweep than the down-sweep, unlike the direct measurements. These observations indicate a breakdown of thermal equilibrium between magnetic and lattice degrees of freedom on the timescale of the pulse ($\sim 10^{-1}$s). We interpret the results using a phenomenological model involving two thermally coupled subsystems - the magnetic ions and phonons, and a thermal reservoir, which accounts well for the behavior of Pr$_2$Zr$_2$O$_7$. However, it fails to reproduce the plateau seen in Nd$_2$Zr$_2$O$_7$. Agreement with Nd$_2$Zr$_2$O$_7$ data is improved substantially if we allow the thermal coupling between the magnetic and the lattice subsystems to depend on the product $\frac{HdH}{dt}$. Our results reveal anomalously slow heat transfer between magnetic and lattice subsystems and point toward a novel mechanism for dynamically controlling the heat flow in Nd$_2$Zr$_2$O$_7$ via the rate of magnetic field variation.
format Preprint
id arxiv_https___arxiv_org_abs_2511_22517
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Large out-of-equilibrium magnetocaloric effect in rare-earth zirconate pyrochlores
Benton, O.
Skourski, Y.
Gorbunov, D.
Miyata, A.
Chattopadhyay, S.
Wosnitza, J.
Hatnean, M. Ciomaga
Balakrishnan, G.
Zherlitsyn, S.
Petrenko, O. A.
Strongly Correlated Electrons
We explore the magnetic properties of Nd$_2$Zr$_2$O$_7$ and Pr$_2$Zr$_2$O$_7$ single crystals subjected to pulsed magnetic fields up to 60 T using magnetization and magnetocaloric-effect (MCE) measurements, with initial temperatures ranging from 2 to 31K. The MCE data exhibit pronounced and unconventional hysteresis loops, in which the sample temperature increases during both the up-sweep and down-sweep of the field. In Nd$_2$Zr$_2$O$_7$, the MCE further displays a striking plateau as a function of time, followed by a rapid temperature rise that begins at the maximum applied field, across pulses with differing peak-field strengths. Our magnetization measurements reveal an inferred temperature of the magnetic subsystem that differs significantly from the directly measured sample temperature and exhibits opposite hysteresis: the temperature is higher on the up-sweep than the down-sweep, unlike the direct measurements. These observations indicate a breakdown of thermal equilibrium between magnetic and lattice degrees of freedom on the timescale of the pulse ($\sim 10^{-1}$s). We interpret the results using a phenomenological model involving two thermally coupled subsystems - the magnetic ions and phonons, and a thermal reservoir, which accounts well for the behavior of Pr$_2$Zr$_2$O$_7$. However, it fails to reproduce the plateau seen in Nd$_2$Zr$_2$O$_7$. Agreement with Nd$_2$Zr$_2$O$_7$ data is improved substantially if we allow the thermal coupling between the magnetic and the lattice subsystems to depend on the product $\frac{HdH}{dt}$. Our results reveal anomalously slow heat transfer between magnetic and lattice subsystems and point toward a novel mechanism for dynamically controlling the heat flow in Nd$_2$Zr$_2$O$_7$ via the rate of magnetic field variation.
title Large out-of-equilibrium magnetocaloric effect in rare-earth zirconate pyrochlores
topic Strongly Correlated Electrons
url https://arxiv.org/abs/2511.22517