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The adiabatic elastocaloric effect measures the temperature change of a given system with strain and provides a thermodynamic probe of the entropic landscape in the temperature-strain space. Here, we demonstrate that the DC bias strain-dependence of AC elastocaloric effect allows decomposition of the latter into symmetric (rotation-symmetry-preserving) and antisymmetric (rotation-symmetry-breaking) strain channels, using a tetragonal [Formula: see text]-electron intermetallic DyB[Formula: see text]C[Formula: see text]-whose antiferroquadrupolar order breaks local fourfold rotational symmetries while globally remaining tetragonal-as a showcase example. We capture the strain evolution of its quadrupolar and magnetic phase transitions using both singularities in the elastocaloric coefficient and its jumps at the transitions, and the latter we show follows a modified Ehrenfest relation. We find that antisymmetric strain couples to the underlying order parameter in a biquadratic (linear-quadratic) manner in the antiferroquadrupolar (canted antiferromagnetic) phase, which are attributed to a preserved (broken) global tetragonal symmetry, respectively. The broken tetragonal symmetry in the magnetic phase is further evidenced by elastocaloric strain-hysteresis and optical birefringence. Additionally, within the staggered quadrupolar order, the observed elastocaloric response reflects a quadratic increase of entropy with antisymmetric strain, analogous to the role magnetic field plays for Ising antiferromagnetic orders by promoting pseudospin flips. Our results demonstrate AC elastocaloric effect as a compact and incisive thermodynamic probe into the coupling between electronic degrees of freedom and strain in free energy, which holds the potential for investigating and understanding the symmetry of a wide variety of ordered phases in broader classes of quantum materials.
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http://dx.doi.org/10.1073/pnas.2302800120 | DOI Listing |
Solid State Nucl Magn Reson
August 2025
Department of Chemistry & Biochemistry, Florida State University, Tallahassee, FL, 32306, USA; National High Magnetic Field Laboratory, Tallahassee, FL, 32310, USA. Electronic address:
Quadrupolar NMR crystallography guided crystal structure prediction (QNMRX-CSP) is a method for determining the crystal structures of organic solids. To date, our two previous QNMRX-CSP studies have relied upon on Cl solid-state NMR (SSNMR) spectroscopy, powder X-ray diffraction (PXRD), Monte-Carlo simulated annealing (MC-SA), and dispersion-corrected density functional theory (DFT-D2∗) calculations for the determination of crystal structures for organic HCl salts with known crystal structures, in order to benchmark the method and subject it to blind tests. Herein, we apply QNMRX-CSP for the de novo crystal structure determination of L-alaninamide HCl (L-Ala-NH), for which no crystal structure has been reported, using Cl SSNMR and PXRD data for structural prediction and refinement, along with C and N SSNMR data for subsequent structural validation.
View Article and Find Full Text PDFInorg Chem
August 2025
Department of Chemistry & Chemical Biology, McMaster University, 1280 Main St W, Hamilton, Ontario L8S 4L8, Canada.
NaSnGeO is a novel Na conductor that can be utilized in the next generation of all-solid-state Na batteries (ASSNIBs). Na ssNMR experiments were carried out on the NaSnGeO phase to investigate the Na dynamics for the three unique crystallographic Na sites under multiple field strengths (20, 11.7, and 7 T).
View Article and Find Full Text PDFJ Phys Chem Lett
August 2025
Department of Chemistry and Biomolecular Sciences, University of Ottawa, Ottawa, Ontario K1N 6N5, Canada.
Quadrupolar spin resonance (QSR) is radio frequency spectroscopy that provides a chemical fingerprint in the absence of a magnetic field. Materials may present QSR spectra featuring multiple overlapping isotopic resonances, leading to ambiguous spectral assignments. We show how the application of a weak magnetic field (≤50 mT) enables measurement of the nuclear gyromagnetic ratio associated with each resonance with sufficient precision for isotopic identification.
View Article and Find Full Text PDFPhys Rev Lett
June 2025
University of Toronto, Department of Physics, 60 Saint George Street, Toronto, Ontario M5S 1A7, Canada.
Motivated by advances in pump-probe experiments and light-driven phenomena, we theoretically study the impact of pumped and driven phonons in Mott insulators which host multipole moments, thus going beyond conventional dipolar magnetism. As a case study, we examine pseudospin-1/2 Mott insulators hosting quadrupolar and octupolar moments, and investigate the effect of resonantly exciting E_{g} phonon modes which couple linearly to the quadrupoles. We show that this leads to multipolar precession, with the backaction resulting in pseudochiral phonon dynamics in the octupolar ordered phase.
View Article and Find Full Text PDFJ Am Chem Soc
August 2025
Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States.
Magnesium-ion batteries hold the potential to outperform the energy density of lithium-ion batteries, given the divalent charge carried by each Mg cation, but remain in an early stage of development. Here, Mg solid-state nuclear magnetic resonance (ssNMR) is used to gain insight into the local structure and Mg-ion dynamics of candidate Mg-ion solid electrolytes, the antiperovskites MgSbN and MgAsN. Using the highest available magnetic field (35.
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