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At least 235 records · Page 13

Ion diffusion coefficients in poly(3-alkylthiophenes) for energy conversion and biosensing: role of side-chain length and microstructure

Conductive polymers are promising materials as active elements for energy storage and conversion devices due to mixed ion–electron conduction. The ion diffusion coefficient is a relative measure of the efficacy of ion transport, allowing for comparison between materials and electrochemical conditions. In this work, diffusion coefficients of hexafluorophosphate (PF6–) counterions in poly(3-alkylthiophene) (P3AT) materials are measured as a function of both side-chain length and microstructure using electrochemical impedance spectroscopy (EIS). For semi-crystalline films, the diffusion coefficient is found to be anomalous and nearly independent of applied electrochemical potential. Here, the anomalous behavior of diffusion indicates that spin casting yields compact films with an enthalpic barrier to ion transport, attributed to ionic trapping. Diffusion coefficient values ~10 –11 cm 2 s –1 were measured for all films, indicating interchain spacing, in the absence of strong intermolecular interactions with the electrolyte, is not a viable design strategy to control ion transport. For the prototypical system of poly(3-hexylthiophene), we observe almost no potential dependence in ion transport for regioregular and regiorandom films of comparable molecular weight, with both exhibiting anomalous diffusion. Alternatively, changing the microstructure of poly(3-hexylthiophene) to a mostly amorphous, ion-imprinted structure yields ~500× increase in the diffusion coefficient to ~2 × 10 –8 cm 2 s –1 at 0.8 V vs. Ag/Ag + with behavior closer to ordinary diffusion. Collectively, these results indicate new insight into ion transport in conductive polymers, where ionic trapping effects can be mitigated through electrodeposition protocols over post-synthesis processing (i.e. spin coating).

14 SOLAR ENERGY↗

Anomalous magnetothermoelectric behavior in massive Dirac materials

Extensive studies of electron transport in Dirac materials have shown positive magnetoresistance (MR) and positive magnetothermopower (MTP) in a magnetic field perpendicular to the excitation current or thermal gradient. In contrast, measurements of electron transport often show a negative longitudinal MR and negative MTP for a magnetic field oriented along the excitation current or thermal gradient; this is attributed to the chiral anomaly in Dirac materials. In this paper, we report a very different magnetothermoelectric transport behavior in the massive Dirac material ZrTe5. Although thin flakes show a commonly observed positive MR in a perpendicular magnetic field, distinct from other Dirac materials, we observe a sharp negative MTP. In a parallel magnetic field, we still observe a negative longitudinal MR, however, a remarkable positive MTP is observed for the fields parallel to the thermal gradients. Our theoretical calculations suggest that this anomalous magnetothermoelectric behavior can be attributed to the screened Coulomb scattering. This work demonstrates the significance of impurity scattering in the electron transport of topological materials and provides deep insight into the magnetotransport phenomena in Dirac materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Emergence of asymmetric skew-scattering dominated anomalous Nernst effect in the spin gapless semiconductors Co 1+x Fe 1-x CrGa

Heusler alloy-based spin gapless semiconductors (SGSs) with very high Curie temperatures ( T C ) have recently gained enormous attention because of their unconventional electronic structures. They exhibit a nonzero band gap in one of the spin channels and a zero band gap in the other spin channel, making them an important class of materials for tunable spin transport. Here, we report the experimental observation of anomalous Nernst effect (ANE) in Co 1 + x Fe 1 - x CrGa ( x = 0 , 0.2, 0.4, and 0.5), which are the emerging quaternary Heusler alloy-based SGSs. While the electron-electron elastic scattering and the disorder-mediated weak localization effect play the major roles in electrical transport for all the samples at low temperatures, the magnon-drag effect was found to dominate the longitudinal thermoelectric transport. The ANE coefficient at room temperature increases from ≈ 0.018 μ V K - 1 for x = 0 to ≈ 0.063 μ V K - 1 for x = 0.5 , which is higher than that for Ni 81 Fe 19 and compressively strained SrRu O 3 films. Our analysis indicates that the observed ANE in these samples originates from asymmetric skew scattering of charge carriers.

36 MATERIALS SCIENCE↗

Large intrinsic anomalous Hall effect in SrIrO 3 induced by magnetic proximity effect

The anomalous Hall effect (AHE) is an intriguing transport phenomenon occurring typically in ferromagnets as a consequence of broken time reversal symmetry and spin-orbit interaction. It can be caused by two microscopically distinct mechanisms, namely, by skew or side-jump scattering due to chiral features of the disorder scattering, or by an intrinsic contribution directly linked to the topological properties of the Bloch states. Here we show that the AHE can be artificially engineered in materials in which it is originally absent by combining the effects of symmetry breaking, spin orbit interaction and proximity-induced magnetism. In particular, we find a strikingly large AHE that emerges at the interface between a ferromagnetic manganite (La 0.7 Sr 0.3 MnO 3 ) and a semimetallic iridate (SrIrO 3 ). It is intrinsic and originates in the proximity-induced magnetism present in the narrow bands of strong spin-orbit coupling material SrIrO 3 , which yields values of anomalous Hall conductivity and Hall angle as high as those observed in bulk transition-metal ferromagnets. These results demonstrate the interplay between correlated electron physics and topological phenomena at interfaces between 3d ferromagnets and strong spin-orbit coupling 5d oxides and trace an exciting path towards future topological spintronics at oxide interfaces.

36 MATERIALS SCIENCE↗

Origin of anomalous magnetotransport in kagome superconductors 𝐴⁢V 3 ⁢Sb 5 (𝐴 = K,Rb,Cs)

Multiple anomalous features in electronic spectra of metals with a kagome lattice structure—van Hove singularities, Dirac points, and flat bands—imply that materials containing this structural motif may lie at a nexus of topological and correlated electron physics. Due to the prospects of such exceptional electronic behavior, the recent discovery of superconductivity coexisting with charge-density wave (CDW) order in the layered kagome metals 𝐴⁢V 3 ⁢Sb 5 (𝐴 = K,Rb,Cs) has attracted considerable attention. Notably, these archetypal kagome metals express unconventional magnetotransport behavior, including an unexpected linear-in-𝐻 diagonal resistivity at low fields, and an even more peculiar, nonmonotonic sign-changing behavior of the Hall resistivity, which has been speculated to arise from a chiral CDW. We argue here that this unusual magnetotransport derives not from such unconventional phenomena, but rather from the unique fermiology of the 𝐴⁢V 3 ⁢Sb 5 materials. Specifically, it is caused by a large, concave hexagonal Fermi surface sheet formed in the close proximity to the van Hove singularities, which is backfolded into a small hexagonal sheet and two large triangular sheets in the CDW state. We introduce and analyze a model of the electronic structure of these Fermi surface sheets that allows for a full analytical treatment within Boltzmann kinetic theory and that enables semi-quantitative fits of our transport data. Specifically, we find that the anomalous magnetotransport behavior is caused by the confluence of strong reduction of the Fermi velocity near the van Hove singularities located near the vertices of the hexagonal sheet and sharp corners in Fermi surface generated by the CDW reconstruction. In conclusion, our analytical approach not only explains the anomalous magnetotransport in the kagome superconductors but also can be extended to a variety of metallic systems hosting singular features in their Fermi surfaces.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Anomalous thermal effect in Zr Te 5 observed via photothermal measurements

In this study, we explore the magneto-thermoelectric power (MTP) of $ZrTe$ 5 , a canonical Dirac semimetal, through a novel photothermal technique. Unlike conventional thermoelectric studies that rely on on-chip heaters and are limited by fabrication processes, especially for stress-sensitive materials, our approach utilizes photothermal effects to induce temperature gradients. Our experiments, applying a magnetic field approximately parallel and transverse to the photocurrent detection direction, reveal that the photothermal method efficiently and reliably extracts both diagonal and off-diagonal components of the thermoelectric coefficient of $ZrTe$ 5 . Here, we observe that the longitudinal MTP reproduces features previously reported in thermal transport studies, while the photoinduced transverse MTP confirms the anomalous Nernst effect. This photothermal measurement technique opens new avenues for investigating transport properties in a wide range of quantum materials, both in 3D and 2D systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Synthesis, Stability, and Magnetic Properties of Antiperovskite Co 3 PdN

Experimental synthesis and characterization of theoretically predicted compounds are important steps in the materials discovery pipeline. Here, we report on the synthesis of Co 3 PdN, which was recently predicted to be a stable magnetic antiperovskite. The Co 3 PdN thin films were grown by reactive sputtering and were confirmed to form in an antiperovskite crystal structure. The thermal stability of the compound is demonstrated up to 600 K by in situ X-ray diffraction, though the phase persists at slightly higher temperatures (700 K) in an air-free magnetometer. Both ab initio calculations and magnetization measurements find Co 3 PdN to be ferromagnetic with an experimentally determined Curie temperature of T C = 560 ± 5 K. The saturation magnetization of 1.2 μ B /Co found in the experiment is slightly lower than the 1.7 μ B /Co value expected by theory. A narrow magnetic hysteresis loop with a coercive field of 100 Oe at low temperature suggests that Co 3 PdN might be useful in electronic applications requiring fast switching of the magnetization vector. While prior prediction of Co 3 PdN showed a gapped electronic band structure for each spin channel, we show that this was due to incomplete sampling of Brillouin zone paths and that band crossings exist along R-X|M and X|M-R paths. The metallic nature of Co 3 PdN is further confirmed by temperature-dependent transport measurements, which also show a considerable anomalous Hall effect. Altogether, this work represents an appreciable step toward understanding the synthesis, structure, stability, and properties of a new magnetic material.

14 SOLAR ENERGY↗

Universal Kardar-Parisi-Zhang Dynamics in Integrable Quantum Systems

Although the Bethe ansatz solution of the spin-1/2 Heisenberg model dates back nearly a century, the anomalous nature of its high-temperature transport dynamics has only recently been uncovered. Indeed, numerical and experimental observations have demonstrated that spin transport in this paradigmatic model falls into the Kardar-Parisi-Zhang (KPZ) universality class. This has inspired the significantly stronger conjecture that KPZ dynamics, in fact, occur in all integrable spin chains with non-Abelian symmetry. Here, in this letter, we provide extensive numerical evidence affirming this conjecture. Moreover, we observe that KPZ transport is even more generic, arising in both supersymmetric and periodically driven models. Motivated by recent advances in the realization of SU(N)-symmetric spin models in alkaline-earth-based optical lattice experiments, we propose and analyze a protocol to directly investigate the KPZ scaling function in such systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Dynamics of magnetosphere-ionosphere coupling including turbulent transport

A two dimensional two-fluid MHD model including anomalous resistivity was used to investigate the dynamics of magnetosphere-ionosphere coupling. When a field-aligned current is generated on auroral field lines, the disturbance propagates towards the ionosphere in the form of a kinetic Alfven wave. When the current exceeds a critical value, microscopic turbulence is produced, which modifies the propagation of the Alfven wave. This process is modeled by a nonlinear collision frequency, which increases with the excess of the drift velocity over the critical value. Turbulence leads to absorption and reflection of the Alfven wave, partially decoupling the generator from the ionosphere. The approach to a steady-state is strongly dependent on the presence or absence of the turbulence. The current is self-limiting, since a current in excess of critical causes a diffusion of the magnetic field perturbation and a reduction of current.

Lysak, R. L.↗

Atmospheric Teleconnection over Eurasia Induced by Aerosol Radiative Forcing during Boreal Spring

The direct effects of aerosols on global and regional climate during boreal spring are investigated based on numerical simulations with the NASA Global Modeling and Assimilation Office finite-volume general circulation model (fvGCM) with Microphyics of Clouds with the Relaxed Arakawa Schubert Scheme (McRAS), using aerosol forcing functions derived from the Goddard Ozone Chemistry Aerosol Radiation and Transport model (GOCART). The authors find that anomalous atmospheric heat sources induced by absorbing aerosols (dust and black carbon) excite a planetary-scale teleconnection pattern in sea level pressure, temperature, and geopotential height spanning North Africa through Eurasia to the North Pacific. Surface cooling due to direct effects of aerosols is found in the vicinity and downstream of the aerosol source regions, that is, South Asia, East Asia, and northern and western Africa. Significant atmospheric heating is found in regions with large loading of dust (over northern Africa and the Middle East) and black carbon (over Southeast Asia). Paradoxically, the most pronounced feature in aerosol-induced surface temperature is an east west dipole anomaly with strong cooling over the Caspian Sea and warming over central and northeastern Asia, where aerosol concentrations are low. Analyses of circulation anomalies show that the dipole anomaly is a part of an atmospheric teleconnection pattern driven by atmospheric heating anomalies induced by absorbing aerosols in the source regions, but the influence was conveyed globally through barotropic energy dispersion and sustained by feedback processes associated with the regional circulations. The surface temperature signature associated with the aerosol-induced teleconnection bears striking resemblance to the spatial pattern of observed long-term trend in surface temperature over Eurasia. Additionally, the boreal spring wave train pattern is similar to that reported by Fukutomi et al. associated with the boreal summer precipitation seesaw between eastern and western Siberia. The results of this study raise the possibility that global aerosol forcing during boreal spring may play an important role in spawning atmospheric teleconnections that affect regional and global climates.

Kim, Maeng-Ki↗

Unexpected dependence of the anomalous Hall angle on the Hall conductivity in amorphous transition metal thin films

The anomalous Hall effect (AHE), and magnetic and electronic transport properties were investigated in a series of amorphous transition metal thin films— Fe x S i –x , Fe x Ge 1-x , Co x Ge 1–x , Co x Si 1–x , and Fe 1–y Co y Si. The experimental results are compared with density functional theory calculations of the density of Berry curvature and intrinsic anomalous Hall conductivity. In all samples, the longitudinal conductivity (σ xx ), magnetization (M), and Hall resistivity (ρ xy ) increase with increasing transition metal concentration; due to the structural disorder σ xx is lower in all samples than a typical crystalline metal. In the systems with Fe as the transition metal (including Fe 1–y Co y Si), the magnetization and AHE are large and in some cases greater than the crystalline analog. In all samples, the AHE is dominated by the intrinsic mechanism, arising from a nonzero, locally derived Berry curvature. The anomalous Hall angle (AHA) (= σ xy /σ xx ) is as large as 5% at low temperature. These results are compared with the AHAs reported in a broad range of crystalline and amorphous materials. Previous work has shown that in a typical crystalline ferromagnet the Hall conductivity (σ xy ) and σ xx are correlated and are usually either both large or both small, resulting in an AHA that decreases with increasing σ xy . By contrast, the AHA increases linearly with increasing σ xy in the amorphous systems. This trend is attributed to a generally low σ xx , while σ xy varies and can be large. In the amorphous systems, σ xx and σ xy are not coupled, and there may thus exist the potential to further increase the AHA by increasing σ xy .

36 MATERIALS SCIENCE↗

Anomalous Hall effects in chiral superconductors

We report theoretical results for the electronic contribution to thermal and electrical transport for chiral superconductors belonging to even or odd-parity E 1 and E 2 representations of the tetragonal and hexagonal point groups. Chiral superconductors exhibit novel properties that depend on the topology of the order parameter and Fermi surface, and—as we highlight—the structure of the impurity potential. An anomalous thermal Hall effect is predicted and shown to be sensitive to the winding number, ν, of the chiral order parameter via Andreev scattering that transfers angular momentum from the chiral condensate to excitations that scatter off the random potential. For heat transport in a chiral superconductor with isotropic impurity scattering, i.e., point-like impurities, a transverse heat current is obtained for ν = ± 1, but vanishes for | ν | > 1. This is not a universal result. For finite-size impurities with radii of order or greater than the Fermi wavelength, R ≥ ℏ / p f, the thermal Hall conductivity is finite for chiral order with | ν | ≥ 2, and determined by a specific Fermi-surface average of the differential cross-section for electron-impurity scattering. Our results also provide quantitative formulae for analyzing and interpreting thermal transport measurements for superconductors predicted to exhibit broken time-reversal and mirror symmetries.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Evidence of Ba-substitution induced spin-canting in the magnetic Weyl semimetal EuCd 2 As 2

Recently EuCd 2 As 2 was predicted to be a magnetic Weyl semimetal with a lone pair of Weyl nodes generated by A-type antiferromagnetism and protected by a rotational symmetry. However, it was soon discovered that the actual magnetic structure broke the rotational symmetry and internal pressure was later suggested as a route to stabilize the desired magnetic state. In this work we test this prediction by synthesizing a series of Eu 1-x BaxCd 2 As 2 single crystals and studying their structural, magnetic, and transport properties via both experimental techniques and first-principles calculations. We find that small concentrations of Ba (~3%–10%) lead to a small out-of-plane canting of the Eu moment. However, for higher concentrations this effect is suppressed and a nearly in-plane model is recovered. Studying the transport properties we find that all compositions show evidence of an anomalous Hall effect dominated by the intrinsic mechanism as well as large negative magnetoresistances in the longitudinal channel. A nonmonotonic evolution of the transport properties is seen across the series which correlates to the proposed canting suggesting canting may enhance the topological effects. Careful density functional theory calculations using an all-electron approach revise prior predictions finding a purely ferromagnetic ground state with in-plane moments for both the EuCd 2 As 2 and Eu 0.5 Ba 0.5 Cd 2 As 2 compounds, corroborating our experimental findings. This work suggests that Ba substitution can tune the magnetic properties in unexpected ways which correlate to changes in measures of topological properties, encouraging future work to locate the ideal Ba concentration for Eu moment canting.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Antiferromagnetic topological insulating state in $\mathrm{Tb_{0.02}Bi_{1.08}Sb_{0.9}Te_2S}$ single crystals

Topological insulators are emerging materials with insulating bulk and symmetry protected nontrivial surface states. One of the most fascinating transport behaviors in a topological insulator is the quantized anomalous Hall insulator, which has been observed in magnetic-topological-insulator-based devices. Here in this work, we report a successful doping of rare earth element Tb into Bi 1.08 Sb 0.9 Te 2 S topological insulator single crystals, in which the Tb moments are antiferromagnetically ordered below ~10 K. Benefiting from the in-bulk-gap Fermi level, transport behavior dominant by the topological surface states is observed below ~150 K. At low temperatures, strong Shubnikov–de Haas oscillations are observed, which exhibit 2D-like behavior. The topological insulator with long range magnetic ordering in rare earth doped Bi 1.08 Sb 0.9 Te 2 S single crystal provides an ideal platform for quantum transport studies and potential applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Biphasic Janus Particles Explain Self-Healing in Pt–Pd Diesel Oxidation Catalysts

The addition of Pd to Pt-based diesel oxidation catalysts is known to enhance performance and restrict the anomalous growth of Pt nanoparticles when subjected to aging at high temperatures in oxidative environments. To gain a mechanistic understanding, we studied the transport of the mobile Pt and Pd species to the vapor phase, since vapor phase transport is the primary route for sintering in these catalysts. The results are surprising: there is a 30-fold drop in the effective vapor pressure of Pt in the Pt-Pd catalysts compared to monometallic Pt. At the same time, there is a significant enhancement in the vapor pressure of Pd, compared to PdO, which otherwise has a negligible vapor pressure at the aging temperature. Such behavior cannot be explained simply by alloying Pt and Pd in the metallic phase, or a core-shell morphology where a PdO shell covers a Pt core. Transmission electron microscopic examination of catalysts aged up to 50 h in air at 800 °C shows that the particles exhibit a biphasic “Janus”-like structure. The metal and oxide phases are conjoined, exposing a metal and an oxide face to the gas phase. The high mobility of the Pt and Pd allows them to be partitioned into the metal and oxide phases, in apparent thermodynamic equilibrium. The PdO helps to trap mobile PtO2 and as a result contains high concentrations of Pt oxide, consistent with its role in mitigating the transport of Pt to the vapor phase and preventing the growth of anomalously large particles. In turn, Pt allows Pd to remain metallic, allowing the catalyst to retain both metal and oxide functionality for catalysis. The regeneration of deactivated catalysts typically requires an external input, such as a change in the working environment from reducing to oxidizing or vice-versa. Here, we show that the mobile species, which are primary contributors to catalyst sintering are effectively returned to the active site, hence our use of the term “selfhealing”. The detailed insights into the inner workings of the Pt-Pd diesel oxidation catalysts can help provide clues to the design of robust and durable heterogeneous catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hydrodynamic thermoelectric transport in Corbino geometry

We study hydrodynamic electron transport in Corbino graphene devices. Due to the irrotational character of the flow, the forces exerted on the electron liquid are expelled from the bulk. We show that in the absence of Galilean invariance, force expulsion produces qualitatively new features in thermoelectric transport: (i) it results in drops of both voltage and temperature at the system boundaries and (ii) in conductance measurements in pristine systems, the electric field is not expelled from the bulk. We obtain thermoelectric coefficients of the system in the entire crossover region between charge neutrality and high electron density regime. The thermal conductance exhibits a sensitive Lorentzian dependence on the electron density. The width of the Lorentzian is determined by the fluid viscosity. Furthermore, this enables determination of the viscosity of electron liquid near charge neutrality from purely thermal transport measurements. In general, the thermoelectric response is anomalous: It violates the Matthiessen's rule, the Wiedemann-Franz law, and the Mott relation.

36 MATERIALS SCIENCE↗

Confinement-Induced Chiral Edge Channel Interaction in Quantum Anomalous Hall Insulators

In quantum anomalous Hall (QAH) insulators, the interior is insulating but electrons can travel with zero resistance along one-dimensional (1D) conducting paths known as chiral edge channels (CECs). These CECs have been predicted to be confined to the 1D edges and exponentially decay in the two-dimensional (2D) bulk. Here, in this Letter, we present the results of a systematic study of QAH devices fashioned in a Hall bar geometry of different widths under gate voltages. At the charge neutral point, the QAH effect persists in a Hall bar device with a width of only ~7⁢2 nm, implying the intrinsic decaying length of CECs is less than ~3⁢6 nm. In the electron-doped regime, we find that the Hall resistance deviates quickly from the quantized value when the sample width is less than 1 μ⁢m. Our theoretical calculations suggest that the wave function of CEC first decays exponentially and then shows a long tail due to disorder-induced bulk states. Therefore, the deviation from the quantized Hall resistance in narrow QAH samples originates from the interaction between two opposite CECs mediated by disorder-induced bulk states in QAH insulators, consistent with our experimental observations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Spin orbit torque in ferromagnet/topological-quantum-material heterostructures

The main objective of this proposal was to investigate the spin-orbital driven phenomena in topological insulator (TI)/ferromagnet (FM) or transition metal (TM) heterostructures. In particularly, we tried to utilize the spin-momentum locking properties on the surface of TIs to achieve ideal spin-orbit torques (SOTs). In practice, we found that the surface properties have been greatly modified, resulting in much more complicated magneto-transport behaviors than what is expected in SOT-driven magnetotransport. Through systematic and extended investigations, we start to unravel that the nonlinear magnetotransport properties, which was, in the past, mainly attributed to SOT-driven phenomena, can be used to infer the modification of the electronic band structures of TIs and spin textures in FMs which are closely related with charge-spin interconversion phenomena. Regarding the band structures In TIs, we find under electrostatic perturbations imposed by deposition of nonmagnetic TMs, the quantum well states formed on the surface of TIs develop substantial Rashba spin-splitting, which is detected as a bilinear magnetoresistance (BMR). Under magnetic perturbations, the nonlinear planar Hall effect (NPHE) in the topological surface states is greatly enhanced, possibly reflecting the modified surface band structure due to time-reversal symmetry breaking. In a double HM/FM heterostructure where the magnetic anisotropy can be robustly tuned, we observed second-harmonic Hall voltage responses corresponding to domain wall structures with fixed chirality, stabilized by interfacial Dzyaloshinskii–Moriya interaction (DMI). In addition, in the linear transport regime, we utilized inverse-SHE-induced anomalous Hall effect in Pt to probe the exchange bias on the surface of a doped magnetic insulator Tm 3 Fe 5 O 12 .

36 MATERIALS SCIENCE↗