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Joseph P. Heremans

Publications and source records attributed to Joseph P. Heremans.

At least 19 recordsLinked to original sources

Electrically tunable interfacial thermal conduction via electronic structure engineering in ${Au}$/$Bi_{1-x}$$Sb_{x}$ topological insulators

This work provides direct experimental evidence for the role of topological interface states in thermal conduction across a metal/topological insulator junction. It also shows that this conduction can be reversibly modulated by electrical current injection, offering a new approach toward active control of heat flow at solid-state interfaces. Specifically, the interfacial thermal conductance of ${Au}$/$Bi_{89}$$Sb_{11}$ and ${Au}$/$Bi_{87}$$Sb_{13}$ junctions demonstrates distinct temperature- and bias-dependent behavior. Both responses are attributed to carrier redistribution between topological interface and bulk band states, driven thermally by Fermi-Dirac broadening and electrically by quasi-Fermi-level shifts and WKB tunneling into nearby bulk bands. Control experiments using trivial semimetals and insulating interlayers further confirm the topological specificity of the effect. Such electrically tunable interfacial heat conduction positions interface electronic structure engineering as a promising route for active thermal management. In doing so, it lays the groundwork for a mechanically robust alternative to conventional structure-driven thermal control compatible with increasingly dense, high-power solid-state devices.

cond-mat.mes-hall↗

Design Principles for Topological Thermoelectrics

Conventional metals, insulators, and semimetals are constrained by fundamental limitations in terms of their thermoelectric performance. Topological materials offer certain features that allow them to circumvent these constraints, and potentially to form the basis for thermoelectric devices with unprecedented efficiency. In this article we review the thermoelectric performance of topological materials, focusing specifically on nodal semimetals, such as Weyl and nodal-line semimetals. We discuss how certain unique ``topological'' features of these materials -- namely their topologically protected band touching points, electron-hole degenerate lowest Landau level, and Berry curvature -- allow them to exhibit thermoelectric properties that go beyond what is possible in conventional materials, particularly in the presence of an applied magnetic field. We focus our discussion on the goal of achieving large figure of merit $zT$, and for each material class we summarize optimal \emph{design principles} for selecting materials that maximize thermoelectric efficiency. We then use these optimal design principles to design and implement a high-throughput database search for topological semimetals that are promising as thermoelectrics. In addition to highlighting a number of materials that are already known to have large magnetothermoelectric effects, our search uncovers twelve additional materials that are especially promising for near-future experiments.

cond-mat.mtrl-sci↗

Large Thermal Hall Effect in MnPS$_3$

Recent studies have demonstrated that the thermal Hall effect can originate from magnons (magnon Hall effect), phonons (phonon Hall effect), or their combination (magnon-polaron Hall effect). The magnon-polaron Hall effect, first observed in Fe2Mo3O8, is particularly intriguing as its thermal Hall signal can be remarkably large. In this study, we explore the thermal Hall effect in MnPS3, an insulating antiferromagnetic material exhibiting a spin-flop transition and significant magnetoelastic coupling, making it a strong candidate for studying the thermal Hall effect originating from spin-lattice coupling. We report an exceptionally large thermal Hall angle down to 4 K and show that it cannot be accounted for by standard calculations based on the intrinsic magnon-polaron Berry curvature. Our findings provide an in-depth analysis of the role of the spin-flop transition in the thermal properties of MnPS3 and call for further theory development on magnon-phonon coupling and scattering to reveal their influence on transverse heat transport.

cond-mat.mtrl-sci↗

Large phonon-drag thermopower polarity reversal in Ba-doped KTaO3

This study reports the observation of phonon-drag thermopower polarity reversal in Ba-doped KTaO3 thin films, mediated by electron-phonon Umklapp scattering. Epitaxial films with distinct carrier concentrations (3.7 x 10^20 cm^-3 and 4.9 x 10^19 cm^-3) were grown via molecular-beam epitaxy. In heavily doped samples, where the Fermi surface spans 80% of the Brillouin zone, the Umklapp condition is satisfied, reversing electron momentum. This manifests as a sign-reversal in the thermopower around 80 K upon cooling despite the sample having only n-type carriers. On the other hand, the lightly doped sample (4.9 x 10^19 cm^-3) exhibits only a negative thermopower down to 2 K. These results advance the understanding of Umklapp electron-phonon drag in oxides and highlight KTaO3's potential for engineering unconventional thermoelectric materials.

cond-mat.mtrl-sci↗

Ultrahigh Anomalous Nernst Thermopower and Thermal Hall Angle in YbMnBi2

Thermoelectrics (TEs) are solid-state devices that can realize heat-electricity conversion. Transverse TEs require materials with a large Nernst effect, which typically requires a strong applied magnetic field. However, topological materials with magnetic order offer an alternative pathway for achieving large Nernst via the anomalous Hall effect and the accompanying anomalous Nernst effect (ANE) that arise from band topology. Here, we show that YbMnBi2 with a low Hall density and a chemical potential near the Weyl points has, to the best of our knowledge, the highest ANE-dominated Nernst thermopower of any magnetic material, with $S_{yx}$ around 110 $μ$V/K ($T$ = 254 K, 5 T < $|μ_0 H|$ < 9 T applied along the spin canting direction), due to the synergism between classical contributions from filled electron bands, large Hall conductivity of topological origin, and large resistivity anisotropy. An appreciable thermal Hall angle of $0.02 < (\nabla_y T)/(\nabla_x T) < 0.06$ was observed (40 K < $T$ < 310 K, $μ_0 H$ = 9 T).

cond-mat.mtrl-sci↗

Electric field dependent thermal conductivity of relaxor ferroelectric PMN-33PT through changes in the phonon spectrum

In ferroelectric materials, an electric field has been shown to change the phonon dispersion sufficiently to alter the lattice thermal conductivity, opening the possibility that a heat gradient could drive a polarization flux, and technologically, also opening a pathway towards voltage-driven, all solid-state heat switching. In this report, we confirm the validity of the theory originally developed for Pb(Zr,Ti)O_3 (PZT) on the ferroelectric relaxor 0.67Pb[Mg_(1/3)Nb_(2/3)]O_3-0.33PbTiO_3 (PMN-33PT). In the theory, the change in sound velocity and thermal conductivity with electric field relates to the piezoelectric coefficients and the Gruneisen parameter. It predicts that in PMN-33PT the effect should be an order of magnitude larger, and of opposite sign as in PZT; this is confirmed here experimentally. The effects are measured on samples never poled before and on samples that underwent multiple field sweep cycles and passed through two phase transitions with change in temperature. The thermal conductivity changes are linked to variations in the piezoelectric coefficients and can be as large as 8-11% at room temperature and above. To date, this is the only means of heat conduction modulation that utilizes changes in the phonon spectrum. While this technology is in its infancy, it offers another path to future active thermal conduction control.

cond-mat.mtrl-sci↗

Revealing the EuCd_{2}As_{2} Semiconducting Band Gap via n-type La-Doping

EuCd_{2}As_{2} has attracted considerable interest as one of the few magnetic Weyl semimetal candidate materials, although recently there have been emerging reports that claim it to have a semiconducting electronic structure. To resolve this debate, we established the growth of n-type EuCd_{2}As_{2} crystals, to directly visualize the nature of the conduction band using angle resolve photoemission spectroscopy (ARPES). We show that La-doping leads to n-type transport signatures in both the thermopower and Hall effect measurements, in crystals with doping levels at 2 - 6 x 10^{17} e^{-} cm^{-3}. Both p-type and n-type doped samples exhibit antiferromagnetic ordering at 9 K. ARPES experiments at 6 K clearly show the presence of the conduction band minimum at 0.8 eV above the valence band maximum, which is further corroborated by the observation of a 0.71 - 0.72 eV band gap in room temperature diffuse reflectance absorbance measurements. Together these findings unambiguously show that EuCd_{2}As_{2} is indeed a semiconductor with a substantial band gap and not a topological semimetal.

cond-mat.mtrl-sci↗

Giant Magnetothermal Conductivity Switching in Semimetallic WSi$_{2}$ Single Crystals

Materials able to rapidly switch between thermally conductive states by external stimuli such as electric or magnetic fields can be used as all-solid-state thermal switches and open a myriad of applications in heat management, power generation and cooling. Here, we show that the large magnetoresistance that occurs in the highly conducting semimetal $α$-WSi$_{2}$ single crystals leads to dramatically large changes in thermal conductivity at temperatures <100 K. At temperatures <20 K, where electron-phonon scattering is minimized, the thermal conductivity switching ratio between zero field and a 9T applied field can be >7. We extract the electronic and lattice components of the from the thermal conductivity measurements and show that the Lorenz number for this material approximates the theoretical value of L$_{0}$. From the heat capacity and thermal diffusivity, the speed of thermal conductivity switching is estimated to range from 1 x 10$^{-4}$ seconds at 5 K to 0.2 seconds at 100 K for a 5-mm long sample. This work shows that WSi$_{2}$, a highly conducting multi-carrier semimetal, is a promising thermal switch component for low-temperature applications such cyclical adiabatic demagnetization cooling, a technique that would enable replacing $^{3}$He-based refrigerators.

cond-mat.mtrl-sci↗

Extraordinary Thermoelectric Properties of Topological Surface States in Quantum-Confined Cd3As2 Thin Films

Topological insulators and semimetals have been shown to possess intriguing thermoelectric properties promising for energy harvesting and cooling applications. However, thermoelectric transport associated with the Fermi arc topological surface states on topological Dirac semimetals remains less explored. In this work, we systematically examine thermoelectric transport in a series of topological Dirac semimetal Cd3As2 thin films grown by molecular beam epitaxy. Surprisingly, we find significantly enhanced Seebeck effect and anomalous Nernst effect at cryogenic temperatures when the Cd3As2 layer is thin. Combining angle-dependent quantum oscillation analysis, magnetothermoelectric measurement, transport modelling and first-principles simulation, we isolate the contributions from bulk and surface conducting channels and attribute the unusual thermoeletric properties to the topological surface states. Our analysis showcases the rich thermoelectric transport physics in quantum-confined topological Dirac semimetal thin films and suggests new routes to achieving high thermoelectric performance at cryogenic temperatures.

cond-mat.mtrl-sci↗

Magnon Diffusion Length and Longitudinal Spin Seebeck Effect in Vanadium Tetracyanoethylene (V[TCNE]$_x$, $x \sim 2$)

Spintronic, spin caloritronic, and magnonic phenomena arise from complex interactions between charge, spin, and structural degrees of freedom that are challenging to model and even more difficult to predict. This situation is compounded by the relative scarcity of magnetically-ordered materials with relevant functionality, leaving the field strongly constrained to work with a handful of well-studied systems that do not encompass the full phase space of phenomenology predicted by fundamental theory. Here we present an important advance in this coupled theory-experiment challenge, wherein we extend existing theories of the spin Seebeck effect (SSE) to explicitly include the temperature-dependence of magnon non-conserving processes. This expanded theory quantitatively describes the low-temperature behavior of SSE signals previously measured in the mainstay material yttrium iron garnet (YIG) and predicts a new regime for magnonic and spintronic materials that have low saturation magnetization, $M_S$, and ultra-low damping. Finally, we validate this prediction by directly observing the spin Seebeck resistance (SSR) in the molecule-based ferrimagnetic semiconductor vanadium tetracyanoethylene (V[TCNE]$_x$, $x \sim 2$). These results validate the expanded theory, yielding SSR signals comparable in magnitude to YIG and extracted magnon diffusion length ($λ_m>1$ $μ$ m) and magnon lifetime for V[TCNE]$_x$ ($τ_{th}\approx 1-10$ $μ$ s) exceeding YIG ($τ_{th}\sim 10$ ns). Surprisingly, these properties persist to room temperature despite relatively low spin wave stiffness (exchange). This identification of a new regime for highly efficient SSE-active materials opens the door to a new class of magnetic materials for spintronic and magnonic applications.

cond-mat.mtrl-sci↗

Magnetic field-controlled lattice thermal conductivity in MnBi2Te4

Phonon properties and the lattice thermal conductivity are not generally understood to be sensitive to magnetic fields. Using an applied field to change MnBi2Te4 between antiferromagnetic (AFM), canted (CAFM) and ferromagnetic (FM) phases we discovered a new way to control the lattice thermal conductivity, generating both a positive and a negative magnetic field dependence. We report the field dependence of the thermal conductivity, k, in the in-plane direction under an applied magnetic field along the cross-plane direction in MnBi2Te4 from 2K to 30K. k decreases with field in the AFM phase, saturates in the CAFM phase, and increases with field in the FM phase. We explain this in terms of the field-induced changes of the magnon gap which modifies which magnon-phonon scattering processes are allowed by energy conservation. We also report magneto-Seebeck coefficient, Nernst coefficient and thermal Hall data measured in the same configuration. This finding may open a way to design magnetically controlled heat switches.

cond-mat.mtrl-sci↗

Thermoelectrics: from Longitudinal to Transverse

In this article, we show fundamentals and recent advances on the transverse thermoelectric generation, in which a thermopower is generated in the direction perpendicular to an applied temperature gradient. Transverse thermoelectric generation is one of the central topics in condensed matter physics, and can be a breakthrough approach to solve long-standing technological problems with contact resistances in thermoelectric generators. We review here the six currently known driving mechanisms: the ordinary Nernst effect, the anomalous Nernst effect, goniopolar materials, the spin Seebeck effect, Seebeck-driven transverse thermoelectric generation, and ($p \times n$)-type multilayers. This article summarizes the principles and functionalities of these transverse thermoelectric effects and discusses their potential as "Future energy".

cond-mat.mtrl-sci↗

Magnon-induced Giant Anomalous Nernst Effect in Single Crystal MnBi

Thermoelectric modules are a promising approach to energy harvesting and efficient cooling. In addition to the longitudinal Seebeck effect, recently transverse devices utilizing the anomalous Nernst effect (ANE) have attracted interest. For high conversion efficiency, it is required that the material should have a large ANE thermoelectric power and low electrical resistance, the product of which is the ANE conductivity. ANE is usually explained in terms of intrinsic contributions from Berry curvature. Our observations suggest that extrinsic contributions also matter. Studying single-crystal MnBi, we find a very high ANE thermopower (~10 $μ$V/K) under 0.6 T at 80 K, and a transverse thermoelectric conductivity of over 40 A/Km. With insight from theoretical calculations, we attribute this large ANE predominantly to a new advective magnon contribution arising from magnon-electron spin-angular momentum transfer. We propose that introducing large spin-orbit coupling into ferromagnetic materials may enhance the ANE through the extrinsic contribution of magnons.

cond-mat.mtrl-sci↗

Giant anomalous Nernst signal in the antiferromagnet YbMnBi2

Searching for a high anomalous Nernst effect (ANE) is crucial for thermoelectric energy conversion applications because the associated unique transverse geometry facilitates module fabrication. Topological ferromagnets with large Berry curvatures show high ANEs; however, they face drawbacks such as strong magnetic disturbances and low mobility due to high magnetization. Herein, we demonstrate that YbMnBi2, a canted antiferromagnet, has a large ANE conductivity of ~10 Am-1K-1 that surpasses the common high values (i.e. 3-5 Am-1K-1) observed so far in ferromagnets. The canted spin structure of Mn guarantees a nonzero Berry curvature but generates only a weak magnetization three orders of magnitude lower than that of general ferromagnets. The heavy Bi with a large spin-orbit coupling enables a high ANE and low thermal conductivity, whereas its highly dispersive px/y orbitals ensure low resistivity. The high anomalous transverse thermoelectric performance and extremely small magnetization makes YbMnBi2 an excellent candidate for transverse thermoelectrics.

cond-mat.mtrl-sci↗

Identifying the Dirac point composition in Bi1-xSbx alloys using the temperature dependence of quantum oscillations

The thermal chiral anomaly is a new mechanism for thermal transport that occurs in Weyl semimetals (WSM). It is attributed to the generation and annihilation of energy at Weyl points of opposite chirality. The effect was observed in the Bi1-xSbx alloy system, at x=11% and 15%, which are topological insulators at zero field and driven into an ideal WSM phase by an external field. Given that the experimental uncertainty on x is of the order of 1%, any systematic study of the effect over a wider range of x requires precise knowledge of the transition composition xc at which the electronic bands at the L-point in these alloys have Dirac-like dispersions. At x>xc, the L-point bands are inverted and become topologically non-trivial. In the presence of a magnetic field along the trigonal direction, these alloys become WSMs. This paper describes how the temperature dependence of the frequency of the Shubnikov-de Haas oscillations F(x,T) at temperatures of the order of the cyclotron energy can be used to find xc and characterize the topology of the electronic Fermi surface. Alloys with topologically trivial bands have dF(x,T)/dT>0, those with Dirac/Weyl fermions display dF(x,T)/dT<0.

cond-mat.mtrl-sci↗

Thermal chiral anomaly in the magnetic-field induced ideal Weyl phase of Bi1-xSbx topological insulators

The chiral anomaly is the predicted break down of chiral symmetry in a Weyl semimetal with monopoles of opposite chirality when an electric field parallel to a magnetic field is applied. It occurs because of charge pumping from a positive chirality to a negative chirality monopole. Experimental observation of this fundamental effect has been plagued by concerns about the pathways of the current. Here, we unambiguously demonstrate the thermal analog of the chiral anomaly in topological insulator bismuth-antimony alloys driven into an ideal Weyl semimetal state by a Zeeman field, with the chemical potential pinned at the Weyl points, and in which the Fermi surface has no trivial pockets. The experimental signature is a large enhancement of the thermal conductivity in an applied magnetic field parallel to the thermal gradient that follows the Wiedemann-Franz law above 60 K. Absence of current flow avoids extrinsic effects that plague electrical measurements.

cond-mat.mtrl-sci↗

Thermal spin transport and spin in thermoelectrics

This article reviews the principles that govern the combined transport of spin, heat, and charge. The extensive thermodynamic quantity associated with spin transport is the magnetization; its Onsager-conjugate force is in general the derivative of the free energy with respect to the magnetization. Spins are carried in one of two ways: (1) by spin-polarized free electrons in magnetic metals and doped semiconductors, or (2) by spin waves (magnons) that reside on localized electrons on unfilled d- or f-shells of transition metal or rare-earth elements. The paper covers both cases in separate chapters. In both cases, it is possible to define a spin chemical potential whose gradient is the more practical conjugate force to spin transport. The paper further describes the anomalous Hall, spin Hall, and inverse spin Hall effects in magnetic and non-magnetic solids with strong spin-orbit coupling because these effects are used to generate and measure spin fluxes. Spin transport across interfaces is described next, and includes spin pumping and spin transfer torque. The final chapter then puts all these concepts together to describe the spin-Seebeck, spin-Peltier, and magnon-drag effects, which exist in ferromagnetic, antiferromagnetic, and even paramagnetic solids. Magnon-drag, in particular, is a high-temperature effect that boosts the thermopower of metals by an order of magnitude and that of semiconductors by a factor of 2 or 3 above the electronic diffusion thermopower. This is the only example where a spin-driven effect is larger than a charge-driven effect. Magnon drag leads a simple binary paramagnetic semiconductor, MnTe, to have zT > 1 without optimization. This shows how adding spin as an additional design parameter in thermoelectrics research is a new and promising approach toward the quest for high-zT materials.

cond-mat.mtrl-sci↗

Shallow impurity band in ZrNiSn

ZrNiSn and related half Heusler compounds are candidate materials for efficient thermoelectric energy conversion with a reported thermoelectric figure-of-merit of n-type ZrNiSn exceeding unity. Progress on p-type materials has been more limited, which has been attributed to the presence of an impurity band, possibly related to the presence of Ni interstitials in nominally vacant 4d position. The specific energetic position of this band, however, has not been resolved. Here, we report results of a concerted theory-experiment investigation for a nominally undoped ZrNiSn, based on measurements of electrical resistivity, Hall coefficient, Seebeck coefficient and Nernst coefficient, measured in a temperature range from 80 to 420 K. The results are analyzed with a semi-analytical model combining a density functional theory (DFT) description for ideal ZrNiSn, with a simple analytical correction for the impurity band. The model provides a good quantitative agreement with experiment, describing all salient features in the full temperature span for the Hall, conductivity, and Seebeck measurements, while also reproducing key trends in the Nernst results. This comparison pinpoints the impurity band edge to 40 meV below the conduction band edge, which agrees well with a separate DFT study of a supercell containing Ni interstitials. Moreover, we corroborate our result with a separate study of ZrNiSn0.9Pb0.1 sample showing similar agreement with an impurity band edge shifted to 32 meV below the conduction band.

cond-mat.mtrl-sci↗