Giant elastocaloric effect at low temperatures in TmVO4 and implications for cryogenic cooling.

Adiabatic decompression of paraquadrupolar materials has significant potential as a cryogenic cooling technology. We focus on TmVO[Formula: see text], 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 [Formula: see text] 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 response of single-crystal TmVO[Formula: see text], 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 into the dynamic quadrupole strain susceptibility.

Elastocaloric signatures of symmetric and antisymmetric strain-tuning of quadrupolar and magnetic phases in DyB2C2.

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.

Elastocaloric determination of the phase diagram of Sr2RuO4.

One of the main developments in unconventional superconductivity in the past two decades has been the discovery that most unconventional superconductors form phase diagrams that also contain other strongly correlated states. Many systems of interest are therefore close to more than one instability, and tuning between the resultant ordered phases is the subject of intense research1. In recent years, uniaxial pressure applied using piezoelectric-based devices has been shown to be a particularly versatile new method of tuning2,3, leading to experiments that have advanced our understanding of the fascinating unconventional superconductor Sr2RuO4 (refs. 4-9). Here we map out its phase diagram using high-precision measurements of the elastocaloric effect in what we believe to be the first such study including both the normal and the superconducting states. We observe a strong entropy quench on entering the superconducting state, in excellent agreement with a model calculation for pairing at the Van Hove point, and obtain a quantitative estimate of the entropy change associated with entry to a magnetic state that is observed in proximity to the superconductivity. The phase diagram is intriguing both for its similarity to those seen in other families of unconventional superconductors and for extra features unique, so far, to Sr2RuO4.

Elastocaloric signature of nematic fluctuations.

The elastocaloric effect (ECE) relates changes in entropy to changes in strain experienced by a material. As such, ECE measurements can provide valuable information about the entropy landscape proximate to strain-tuned phase transitions. For ordered states that break only point symmetries, bilinear coupling of the order parameter with strain implies that the ECE can also provide a window on fluctuations above the critical temperature and hence, in principle, can also provide a thermodynamic measure of the associated susceptibility. To demonstrate this, we use the ECE to sensitively reveal the presence of nematic fluctuations in the archetypal Fe-based superconductor Ba([Formula: see text])2[Formula: see text] By performing these measurements simultaneously with elastoresistivity in a multimodal fashion, we are able to make a direct and unambiguous comparison of these closely related thermodynamic and transport properties, both of which are sensitive to nematic fluctuations. As a result, we have uncovered an unanticipated doping dependence of the nemato-elastic coupling and of the magnitude of the scattering of low-energy quasi-particles by nematic fluctuations-while the former weakens, the latter increases dramatically with increasing doping.

Nematic quantum criticality in an Fe-based superconductor revealed by strain-tuning.

Quantum criticality may be essential to understanding a wide range of exotic electronic behavior; however, conclusive evidence of quantum critical fluctuations has been elusive in many materials of current interest. An expected characteristic feature of quantum criticality is power-law behavior of thermodynamic quantities as a function of a nonthermal tuning parameter close to the quantum critical point (QCP). Here, we observed power-law behavior of the critical temperature of the coupled nematic/structural phase transition as a function of uniaxial stress in a representative family of iron-based superconductors, providing direct evidence of quantum critical nematic fluctuations in this material. These quantum critical fluctuations are not confined within a narrow regime around the QCP but rather extend over a wide range of temperatures and compositions.

Direct measurement of individual phonon lifetimes in the clathrate compound Ba7.81Ge40.67Au5.33.

Engineering lattice thermal conductivity requires to control the heat carried by atomic vibration waves, the phonons. The key parameter for quantifying it is the phonon lifetime, limiting the travelling distance, whose determination is however at the limits of instrumental capabilities. Here, we show the achievement of a direct quantitative measurement of phonon lifetimes in a single crystal of the clathrate Ba7.81Ge40.67Au5.33, renowned for its puzzling 'glass-like' thermal conductivity. Surprisingly, thermal transport is dominated by acoustic phonons with long lifetimes, travelling over distances of 10 to 100 nm as their wave-vector goes from 0.3 to 0.1 Å-1. Considering only low-energy acoustic phonons, and their observed lifetime, leads to a calculated thermal conductivity very close to the experimental one. Our results challenge the current picture of thermal transport in clathrates, underlining the inability of state-of-the-art simulations to reproduce the experimental data, thus representing a crucial experimental input for theoretical developments.Phonon lifetime is a fundamental parameter of thermal transport however its determination is challenging. Using inelastic neutron scattering and the neutron resonant spin-echo technique, Lory et al. determine the acoustic phonon lifetime in a single crystal of clathrate Ba7.81Ge40.67Au5.33.

Multiband Transport in CoSb3 Prepared by Rapid Solidification.

Nano-grained CoSb3 was prepared by melt-spinning and subsequent spark plasma sintering. The phonon thermal conductivity of skutterudites is known to be sensitive to the kind and the amount of guest atoms. Thus, unfilled CoSb3 can serve as model compound to study the impact of a nanostructure on the thermoelectric properties, especially the phonon thermal conductivity. Therefore, a series of materials was prepared differing only by the cooling speed during the quenching procedure. In contrast to clathrates, the microstructure of meltspun CoSb3 was found to be sensitive to the cooling speed. Although the phonon thermal conductivity, studied by means of Flash and 3ω measurements, was found to be correlated with the grain size, the bulk density of the sintered materials had an even stronger impact. Interestingly, the reduced bulk density did not result in an increased electrical resistivity. The influence of Sb and CoSb2 as foreign phase on the electronic properties of CoSb3 was revealed by a multi-band Hall effect analysis. While CoSb2 increases the charge carrier density, the influence of the highly mobile charge carriers introduced by elemental Sb on the thermoelectric properties of the composite offer an interesting perspective for the preparation of efficient thermoelectric composite materials.