Precise orientation of symmetry-mismatched epilayers on van der Waals (vdW) substrates via heteroepitaxy has commonly been achieved through surface treatment processes to accommodate weak interlayer registry and bonding strength, thereby limiting the range of material combinations for heterostructure design. In this study, we investigate the influence of lattice instabilities in a structurally modulated vdW TaCo2Te2 substrate on the growth and alignment of a symmetry-mismatched bulk CoxTey epilayer using in situ heating in a transmission electron microscope (TEM). We show that a Peierls-like lattice instability occurs in TaCo2Te2 at a transition temperature of ∼523 K, which was corroborated by phonon calculations. Postheat-treated samples reveal a thermally induced surface diffusion process and the dominant lateral growth of the CoxTey epilayer on the TaCo2Te2 vdW layers, as observed in cross-sectional TEM images. Temperature-dependent selected area electron diffraction (SAED) patterns reveal that the quasi-vdW CoxTey/TaCo2Te2 heterointerface acquires directional locking by aligning larger interlayer lattice mismatch along the lattice instability axis of TaCo2Te2, while preserving a strong lattice matching along the orthogonal direction. This heterostructure exhibits precise interlayer registry with one-dimensional lattice incommensuration along the lattice instability axis, resulting from structural distortion to accommodate lattice-mismatch strain. Moreover, the interfacial reconstruction of TaCo2Te2 back to the distorted phase stabilizes the lattice-locking of the quasi-vdW heterointerface at elevated temperatures. These findings encourage the expansion of material diversity for designing and predicting multidimensional heterostructures by leveraging lattice instabilities to guide epitaxy.
We demonstrated high-temperature based superconducting microwire detectors for mid-infrared applications, based on YBa2Cu3O7_delta (YBCO). We have used a hard oxide, Al2O3, as a mask material to achieve the microwires in meander geometry. We have achieved the photoresponse of microwire to radiation in the mid-infrared spectrum at wavelengths 3.25 and 4.25 mu m, at temperatures nearly ten times higher than those of existing low-temperature superconducting detectors. We showed a clear correlation between the photoresponse magnitude and the critical parameters of the superconductor, showcasing peak optical responses near the critical temperature and bias current density. Furthermore, our comprehensive electrical transport measurements conducted at various temperatures align closely with our optical response data. The demonstrated performance and versatility of these detectors underscore their potential for a wide array of applications spanning environmental monitoring, medical diagnostics, space exploration, and spectroscopic studies.
The recent discovery of an axial amplitude (Higgs) mode in the long-studied charge density wave (CDW) systems GdTe_3 and LaTe_3 suggests a heretofore unidentified hidden order. A theoretical study proposed that the axial Higgs results from a hidden ferroaxial component of the CDW, which could arise from non-trivial orbital texture. Here, we report extensive experimental studies on ErTe_3 and HoTe_3 that possess a high-temperature CDW similar to other RTe_3 (R = rare earth), along with an additional low-temperature CDW with an orthogonal ordering vector. Combining Raman spectroscopy with large-angle convergent beam electron diffraction (LACBED), rotational anisotropy second-harmonic generation (RA-SHG), and muon-spin relaxation (μSR), we provide unambiguous evidence that the high-temperature CDW breaks translation, rotation, and all vertical and diagonal mirror symmetries, but not time-reversal or inversion. In contrast, the low-temperature CDW only additionally breaks translation symmetry. Simultaneously, Raman scattering shows the high-temperature CDW produces an axial Higgs mode while the low-temperature mode is scalar. The weak monoclinic structural distortion and clear axial response in Raman and SHG are consistent with a ferroaxial phase in RTe_3 driven by coupled orbital and charge orders. Thus, our study provides a new standard for uncovering unconventional orders and confirms the power of Higgs modes to reveal them.
The investigation of all-solid-state sodium-sulfur batteries (ASSSBs) is still in its early stage, where the intermediates and mechanism of the complex 16-electron conversion reaction of the sulfur cathode remain unclear. Herein, this study presents a comprehensive investigation of the sulfur reaction mechanism in ASSSBs by combining electrochemical measurements, ex situ synchrotron X-ray absorption spectroscopy (XAS), in situ Raman spectroscopy, and first-principles calculations. This work, for the first time, proved that the sulfur cathode undergoes an intrinsic three-step solid-solid redox reaction following the thermodynamic principle under the extreme low rate (C-rates <= C/100) or at high temperature (>= 90 degrees C), where S8 is first reduced to long-chain polysulfides (Na2S5 and Na2S4), then to Na2S2, and finally to Na2S, resulting in a three-plateau voltage profile. However, under conventional battery test conditions, i.e., temperatures <= 60 degrees C and C-rates >= C/20, the Na2S2 phase is bypassed due to kinetic limitations, leading to a direct conversion from Na2S4 to Na2S, resulting in the commonly observed two-plateau voltage profile. First-principles calculations reveal that the formation energy of Na2S2 is only 4 meV per atom lower than the two-phase equilibrium of Na2S4 and Na2S, explaining its absence under kinetics-limited conditions. This work clarified the thermodynamic and kinetics-limited pathways of the 16-electron conversion reaction of the sulfur cathode in ASSSBs, providing valuable insights into the solid-state sodium-sulfur reaction mechanisms.
Anomalous transport of topological semimetals has generated significant interest for applications in optoelectronics, nanoscale devices, and interconnects. Understanding the origin of novel transport is crucial to engineering the desired material properties, yet their orders of magnitude higher transport than single-particle mobilities remain unexplained. This work demonstrates the dramatic mobility enhancements result from phonons primarily returning momentum to electrons due to phonon-electron dominating over phonon-phonon scattering. Proving this idea, proposed by Peierls in 1932, requires tuning electron and phonon dispersions without changing symmetry, topology, or disorder. This is achieved by combining de Haas - van Alphen (dHvA), electron transport, Raman scattering, and first-principles calculations in the topological semimetals MX_2 (M=Nb, Ta and X=Ge, Si). Replacing Ge with Si brings the transport mobilities from an order magnitude larger than single particle ones to nearly balanced. This occurs without changing the crystal structure or topology and with small differences in disorder or Fermi surface. Simultaneously, Raman scattering and first-principles calculations establish phonon-electron dominated scattering only in the MGe_2 compounds. Thus, this study proves that phonon-drag is crucial to the transport properties of topological semimetals and provides insight to further engineer these materials.
Flat bands that do not merely arise from weak interactions can produce exotic physical properties, such as superconductivity or correlated many-body effects. The quantum metric can differentiate whether flat bands will result in correlated physics or are merely dangling bonds. A potential avenue for achieving correlated flat bands involves leveraging geometrical constraints within specific lattice structures, such as the kagome lattice; however, materials are often more complex. In these cases, quantum geometry becomes a powerful indicator of the nature of bands with small dispersions. We present a simple, soft-chemical processing route to access a flat band with an extended quantum metric below the Fermi level. By oxidizing Ni-kagome material Cs 2 Ni 3 S 4 to CsNi 3 S 4 , we see a two orders of magnitude drop in the room temperature resistance. However, CsNi 3 S 4 is still insulating, with no evidence of a phase transition. Using experimental data, density functional theory calculations, and symmetry analysis, our results suggest the emergence of a correlated insulating state of unknown origin.
The investigation of all-solid-state sodium-sulfur batteries (ASSSBs) is in the early stage, where the intermediates and mechanism of the complex 16-electron conversion reaction of the sulfur cathode are still unclear. Herein, this study for the first time presents a comprehensive investigation of the sulfur reaction mechanism in ASSSBs by combining electrochemical measurements, ex-situ synchrotron X-ray absorption spectroscopy (XAS), in-situ Raman spectroscopy, and first-principles calculations. Based on the thermodynamic mechanism, the sulfur cathode undergoes a three-step solid-solid redox reaction, with S8 first reducing to Na2S5 and Na2S4, then to Na2S2, and finally to Na2S, resulting in a three-plateau voltage profile. However, under kinetic limitations, the Na2S2 phase is skipped, leading to a direct conversion from Na2S4 to Na2S and a two-plateau voltage profile. First-principles calculations reveal that the formation energy of Na2S2 is only 4 meV/atom lower than the two-phase equilibrium of Na2S4 and Na2S, explaining its absence under conventional cycling conditions. This work clarified the thermodynamic and kinetic limited pathways of the 16-electron conversion reaction of the sulfur cathode in ASSSBs, thereby facilitating the development of high-performance ASSSBs.
The quest to improve transparent conductors balances two key goals: increasing electrical conductivity and increasing optical transparency. To improve both simultaneously is hindered by the physical limitation that good metals with high electrical conductivity have large carrier densities that push the plasma edge into the ultra-violet range. Technological solutions reflect this trade-off, achieving the desired transparencies only by reducing the conductor thickness or carrier density at the expense of a lower conductance. Here we demonstrate that highly anisotropic crystalline conductors offer an alternative solution, avoiding this compromise by separating the directions of conduction and transmission. We demonstrate that slabs of the layered oxides Sr2RuO4 and Tl2Ba2CuO6+δ are optically transparent even at macroscopic thicknesses >2 μm for c-axis polarized light. Underlying this observation is the fabrication of out-of-plane slabs by focused ion beam milling. This work provides a glimpse into future technologies, such as highly polarized and addressable optical screens.
Topological semimetals have revealed a wide array of novel transport phenomena, including electron hydrodynamics, quantum field theoretic anomalies, and extreme magnetoresistances and mobilities. However, the scattering mechanisms central to the fundamental transport properties remain largely unexplored. Here, we reveal signatures of significant phonon-electron scattering in the type-II Weyl semimetal WP2 via temperature-dependent Raman spectroscopy. Over a large temperature range, we find that the decay rates of the lowest energy A(1) modes are dominated by phonon-electron rather than phonon-phonon scattering. In conjunction with first-principles calculations, a combined analysis of the momentum, energy, and symmetry-allowed decay paths indicates this results from finite momentum interband and intraband scattering of the electrons. The excellent agreement with theory further suggests that such results could be true for the acoustic modes. We thus provide evidence for the importance of phonons in the transport properties of topological semimetals and identify specific properties that may contribute to such behavior in other materials.
Whereas electron-phonon scattering relaxes the electron’s momentum in metals, a perpetual exchange of momentum between phonons and electrons may conserve total momentum and lead to a coupled electron-phonon liquid. Such a phase of matter could be a platform for observing electron hydrodynamics. Here we present evidence of an electron-phonon liquid in the transition metal ditetrelide, NbGe 2 , from three different experiments. First, quantum oscillations reveal an enhanced quasiparticle mass, which is unexpected in NbGe 2 with weak electron-electron correlations, hence pointing at electron-phonon interactions. Second, resistivity measurements exhibit a discrepancy between the experimental data and standard Fermi liquid calculations. Third, Raman scattering shows anomalous temperature dependences of the phonon linewidths that fit an empirical model based on phonon-electron coupling. We discuss structural factors, such as chiral symmetry, short metallic bonds, and a low-symmetry coordination environment as potential design principles for materials with coupled electron-phonon liquid.
The exploration of new materials, novel quantum phases, and devices requires ways to prepare cleaner samples with smaller feature sizes. Initially, this meant the use of a cleanroom that limits the amount and size of dust particles. However, many materials are highly sensitive to oxygen and water in the air. Furthermore, the ever-increasing demand for a quantum workforce, trained and able to use the equipment for creating and characterizing materials, calls for a dramatic reduction in the cost to create and operate such facilities. To this end, we present our cleanroom-in-a-glovebox, a system that allows for the fabrication and characterization of devices in an inert argon atmosphere. We demonstrate the ability to perform a wide range of characterization as well as fabrication steps, without the need for a dedicated room, all in an argon environment. Finally, we discuss the custom-built antechamber attached to the back of the glovebox. This antechamber allows the glovebox to interface with ultra-high vacuum equipment such as molecular-beam epitaxy and scanning tunneling microscopy.
Weyl semimetals are 3D phases of matter with topologically protected states that have remarkable macroscopic transport behaviors. As phonon dynamics and electron-phonon scattering play a critical role in the electrical and thermal transport, we pursue a fundamental understanding of the origin of these effects in type-I Weyl semimetals NbAs and TaAs. In the temperature-dependent Raman spectra of NbAs, we reveal a previously unreported Fano lineshape, a signature stemming from the electron-phonon interaction. Additionally, the temperature dependence of the $A_{1}$ phonon linewidths in both NbAs and TaAs strongly deviate from the standard model of anharmonic decay. To capture the mechanisms responsible for the observed Fano asymmetry and the atypical phonon linewidth, we present first principles calculations of the phonon self-energy correction due to the electron-phonon interaction. Finally, we investigate the relationship between Fano lineshape, electron-phonon coupling, and locations of the Weyl points in these materials. Through this study of the phonon dynamics and electron-phonon interaction in these Weyl semimetals, we consider specific microscopic pathways which contribute to the nature of their macroscopic transport.