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The coexistence of superconductivity and ferromagnetism is an intrinsically interesting research focus in condensed matter physics but the study is limited by low superconducting ($T_c$) and magnetic ($T_m$) transition temperatures in related materials. Here, we used a scanning superconducting quantum interference device to image the in-situ diamagnetic and ferromagnetic responses of RbEuFe$_4$As$_4$ with high $T_c$ and $T_m$. We observed significant suppression of superfluid density in vicinity of the magnetic phase transition, signifying fluctuation-enhanced magnetic scatterings between Eu spins and Fe 3$d$ conduction electrons. Intriguingly, we observed multiple ferromagnetic domains which should be absent in an ideal magnetic helical phase. The formation of these domains demonstrates a weak $c$-axis ferromagnetic component probably arising from Eu spin-canting effect, indicative of possible superconductivity-driven domain Meissner and domain vortex-antivortex phases as revealed in EuFe$_2$(As$_{0.79}$P$_{0.21}$)$_2$. Our observations highlight RbEuFe$_4$As$_4$ is a unique system which includes multiple interplay channels between superconductivity and ferromagnetism., Comment: 11 pages, 5 figures

Recent studies have focused on the relationship between charge density wave (CDW) collective electronic ground states and nontrivial topological states. Using angle-resolved photoemission and density functional theory, we establish that YTe$_3$ is a CDW-induced Kramers nodal line (KNL) metal, a newly proposed topological state of matter. YTe$_3$ is a non-magnetic quasi-2D chalcogenide with a CDW wave vector ($q_{\rm cdw}$) of 0.2907c$^*$. Scanning tunneling microscopy and low energy electron diffraction revealed two orthogonal CDW domains, each with a unidirectional CDW and similar YTe$_3$. The effective band structure (EBS) computations, using DFT-calculated folded bands, show excellent agreement with ARPES because a realistic x-ray crystal structure and twin domains are considered in the calculations. The Fermi surface and ARPES intensity plots show weak shadow bands displaced by $q_{\rm cdw}$ from the main bands. These are linked to CDW modulation, as the EBS calculation confirms. Bilayer split main and shadow bands suggest the existence of crossings, according to theory and experiment. DFT bands, including spin-orbit coupling, indicate a nodal line along the $\Sigma$ line from multiple band crossings perpendicular to the KNL. Additionally, doubly degenerate bands are only found along the KNL at all energies, with some bands dispersing through the Fermi level.

Polar and chiral crystal symmetries confer a variety of potentially useful functionalities upon solids by coupling otherwise noninteracting mechanical, electronic, optical, and magnetic degrees of freedom. We describe two unstudied phases of the 3D perovskite, CsSnBr$_3$, which emerge below 85 K due to the formation of Sn(II) lone pairs and their interaction with extant octahedral tilts. Phase II (77 K<$T$<85 K, space group $P2_1/m$) exhibits ferroaxial order driven by a noncollinear pattern of lone pair-driven distortions within the plane normal to the unique octahedral tilt axis, preserving the inversion symmetry observed at higher temperatures. Phase I ($T$<77 K, space group $P2_1$) additionally exhibits ferroelectric order due to distortions along the unique tilt axis, breaking both inversion and mirror symmetries. This polar and chiral phase exhibits second harmonic generation from the bulk and a large, intrinsic polarization$-$electrostriction coefficient along the polar axis ($Q_{22}\approx$1.1 m$^4$ C$^{-2}$), resulting in acute negative thermal expansion ($\alpha_V=-9\times10^{-5}$ K$^{-1}$) through the onset of spontaneous polarization. The unprecedented structures of phases I and II were predicted by recursively following harmonic phonon instabilities to generate a tree of candidate structures and subsequently corroborated by synchrotron X-ray powder diffraction and polarized Raman and $^{81}$Br nuclear quadrupole resonance spectroscopies. Relativistic electronic structure scenarios compatible with reported photoluminescence measurements are discussed. Together, the polar symmetry, small bandgap, large spin-orbit splitting of Sn 5$p$ orbitals, and predicted strain sensitivity of the symmetry-breaking distortions suggest bulk samples and epitaxial films of CsSnBr$_3$ or its neighboring solid solutions as strong candidates for bulk Rashba effects.

TaCo$_2$Te$_2$ is recently reported to be an air-stable, high mobility Van der Waals material with probable magnetic order. Here we investigate the scaling behavior of its magnetoresistance. We measured both the longitudinal ($\rho_{xx}$) and Hall ($\rho_{xy}$) magnetoresistivities of TaCo$_2$Te$_2$ crystals in magnetic fields parallel to the c-axis and found that the magnetoresistance violates the Kohler's rule $MR \sim f[H/\rho_0]$ while obeying the extended Kohler's rule $MR \sim f[H/(n_T\rho_0)]$, where $MR \sim [\rho_{xx}(H)-\rho_0]/\rho_0$, $H$ is the magnetic field, $n_T$ is a thermal factor, $\rho_{xx}(H)$ and $\rho_0$ are the resistivities at $H$ and zero field, respectively. While deviating from those of the densities of electrons ($n_e$) and holes ($n_h$) obtained from the two-band model analysis of the magnetoconductivities, the temperature dependence of $n_T$ is close to that of the Hall carrier densities $n_H$ calculated from the slopes of $\rho_{xy}(H)$ curves at low magnetic fields, providing a new way to obtain the thermal factor in the extended Kohler's rule.

We propose a first-principles model of minimum lattice thermal conductivity ($\kappa_{\rm L}^{\rm min}$) based on a unified theoretical treatment of thermal transport in crystals and glasses. We apply this model to thousands of inorganic compounds and discover a universal behavior of $\kappa_{\rm L}^{\rm min}$ in crystals in the high-temperature limit: the isotropically averaged $\kappa_{\rm L}^{\rm min}$ is independent of structural complexity and bounded within a range from $\sim$0.1 to $\sim$2.6 W/[m$\cdot$K], in striking contrast to the conventional phonon gas model which predicts no lower bound. We unveil the underlying physics by showing that for a given parent compound $\kappa_{\rm L}^{\rm min}$ is bounded from below by a value that is approximately insensitive to disorder, but the relative importance of different heat transport channels (phonon gas versus diffuson) depends strongly on the degree of disorder. Moreover, we propose that the diffuson-dominated $\kappa_{\rm L}^{\rm min}$ in complex and disordered compounds might be effectively approximated by the phonon gas model for an ordered compound by averaging out disorder and applying phonon unfolding. With these insights, we further bridge the knowledge gap between our model and the well-known Cahill-Watson-Pohl (CWP) model, rationalizing the successes and limitations of the CWP model in the absence of heat transfer mediated by diffusons. Finally, we construct graph network and random forest machine learning models to extend our predictions to all compounds within the Inorganic Crystal Structure Database (ICSD), which were validated against thermoelectric materials possessing experimentally measured ultralow $\kappa_{\rm L}$. Our work offers a unified understanding of $\kappa_{\rm L}^{\rm min}$, which can guide the rational engineering of materials to achieve $\kappa_{\rm L}^{\rm min}$.

We developed a generalized model that considers light as energy contributed through the thermalization of excited carriers to generate excitation-intensity- and temperature-dependent phase diagrams. We find that the model replicates the light-induced phase segregation behavior of the MAPb(I,Br)3 system. From there, we sought to study how best to design new, stable, mixed-halide alloys. The resultant first-principles predictions show that the pseudo halide anion BF4- suppresses phase segregation in FA0.83Cs0.17Pb(I0.6Br0.4)3, resulting in enhanced operating stability. The findings reveal that photostability is linked with the structure and electronic properties of materials and may be overcome using informed alloying strategies.

Recently, anomalies in the temperature dependences of the carrier density and/or mobility derived from analysis of the magnetoresistivities using the conventional two-band model have been used to unveil intriguing temperature-induced Lifshitz transitions in various materials. For instance, two temperature-driven Lifshitz transitions were inferred to exist in the Dirac nodal-line semimetal ZrSiSe, based on two-band model analysis of the Hall magnetoconductivities where the second band exhibits a change in the carrier type from holes to electrons when the temperature decreases below T = 106 K and a dip is observed in the mobility versus temperature curve at T = 80 K. Here, we revisit the experiments and two-band model analysis on ZrSiSe. We show that the anomalies in the second band may be spurious, because the first band dominates the Hall magnetoconductivities at T > 80 K, making the carrier type and mobility obtained for the second band from the two-band model analysis unreliable. That is, care must be taken in interpreting these anomalies as evidences for temperature-driven Lifshitz transitions. Our skepticism on the existence of such phase transitions in ZrSiSe is further supported by the validation of the Kohler's rule for magnetoresistances at temperatures below 180 K. This work showcases potential issues in interpreting anomalies in the temperature dependence of the carrier density and mobility derived from the analysis of magnetoconductivities or magnetoresistivities using the conventional two-band model.

Time-resolved multi-terahertz (THz) spectroscopy is used to observe an ultrafast, non-thermal electronic phase change in SnSe driven by interband photoexcitation with 1.55 eV pump photons. The transient THz photoconductivity spectrum is found to be Lorentzian-like, indicating charge localization and phase segregation. The rise of photoconductivity is bimodal in nature, with both a fast and slow component due to excitation into multiple bands and subsequent intervalley scattering. The THz conductivity magnitude, dynamics, and spectra show a drastic change in character at a critical excitation fluence of approximately 6 mJ/cm^2 due to a photo-induced phase segregation and a macroscopic collapse of the band gap., Comment: 5 pages, supplement appended

We report spin-polarized transient absorption for colloidal CdSe nanoplatelets as functions of thickness (2 to 6 monolayer thickness) and core/shell motif. Using electro-optical modulation of co- and cross-polarization pump-probe combinations, we sensitively observe spin-polarized transitions. Core-only nanoplatelets exhibit few-picosecond spin lifetimes that weakly increase with layer thickness. Spectral content of differenced spin-polarized signals indicate biexciton binding energies that decrease with increasing thickness and smaller values than previously reported. Shell growth of CdS with controlled thicknesses, which partially delocalize the electron from the hole, significantly increases the spin lifetime to ~49 picoseconds at room temperature. Implementation of ZnS shells, which do not alter delocalization but do alter surface termination, increased spin lifetimes up to ~100 ps, bolstering the interpretation that surface termination heavily influences spin coherence, likely due to passivation of dangling bonds. Spin precession in magnetic fields both confirms long coherence lifetime at room temperature and yields excitonic g-factor., Comment: Main text + supplementary, 18 pages total, 8 figures total

Two-dimensional (2D) halide perovskites have emerged as semiconductor platforms for realizing efficient and durable optoelectronic devices. However, the reproducible synthesis of 2D perovskite crystals with desired layer thickness (or n value) greater than 2, has been an enduring challenge due to the lack of kinetic control (temperature, time, stoichiometry) for each layer thickness. Here, we demonstrate a novel method term as the kinetically controlled space confinement (KCSC) for the deterministic growth of phase pure Ruddlesden-Popper (RP) and Dion-Jacobson (DJ) 2D perovskites. The phase-pure growth was achieved by progressively increasing the temperature (fixed time) or the crystallization time (fixed temperature), which allowed for an acute control of the crystallization kinetics. We also observe a systematic transformation from a lower n-value to n=3, 4, 5, 6 in 2D perovskites. In-situ photoluminescence spectroscopy and imaging suggest that the progressive transformation from lower to higher n-value occurs via intercalation of excess precursor ions. These experiments enabled the development of a machine learning assisted multi-parameter phase diagram, which predicts the growth of 2D phase with a specific n-value., Comment: 32 pages, 15 figures

AMn6Bi5 materials (A = Na, K, Rb and Cs) consisting of unique Mn-cluster chains emerge as a new family of superconductors with the suppression of their antiferromagnetic (AFM) order under high pressures. Here, we report transverse incommensurate spin density waves (SDWs) for the Mn atoms with a propagating direction along the chain axes as a ground state for KMn6Bi5 by single crystal neutron diffraction. The SDWs have a refined amplitude of ~2.46 Bohr magnetons for the Mn atoms in the pentagons and ~0.29 Bohr magnetons with a large standard deviation for Mn atoms in the center between the pentagons. AFM dominate both the nearest-neighbor Mn-Mn interactions within the pentagon and next-nearest-neighbor Mn-Mn interactions out of the pentagon (along the propagating wave). The SDWs exhibit both local and itinerant characteristics probably formed by a cooperative interaction between local magnetic exchange and conduction electrons. A significant magnetoelastic effect during the AFM transition, especially along the chain direction, has been demonstrated by temperature-dependent x-ray powder diffraction. Single crystal x-ray diffraction below the AFM transition revealed satellite peaks originating from charge density waves along the chain direction with a q-vector twice as large as the SDW one, pointing to a strong real space coupling between them. Our work not only manifests a fascinating interplay among spin, charge, lattice and one dimensionality to trigger intertwined orders in KMn6Bi5 but also provides important piece of information for the magnetic structure of the parent compound to understand the mechanism of superconductivity in this new family.

Direct visualization of ultrafast coupling between charge carriers and lattice degrees of freedom in photo-excited semiconductors has remained a long-standing challenge and is critical for understanding the light-induced physical behavior of materials under extreme non-equilibrium conditions. Here, by monitoring the evolution of the wave-vector resolved ultrafast electron diffraction intensity following above-bandgap photo-excitation, we obtain a direct visual of the structural dynamics in monocrystalline 2D perovskites. Analysis reveals a surprising, light-induced ultrafast lattice ordering resulting from a strong interaction between hot-carriers and the perovskite lattice, which induces an in-plane octahedra rotation, towards a more symmetric phase. Correlated ultrafast spectroscopy performed at the same carrier density as ultrafast electron diffraction reveals that the creation of a hot and dense electron-hole plasma triggers lattice ordering at short timescales by modulating the crystal cohesive energy. Finally, we show that the interaction between the carrier gas and the lattice can be altered by tailoring the rigidity of the 2D perovskite by choosing the appropriate organic spacer layer., Comment: 25 pages, 4 figures

Cubic energy materials such as thermoelectrics or hybrid perovskite materials are often understood to be highly disordered. In GeTe and related IV-VI compounds, this is thought to provide the low thermal conductivities needed for thermoelectric applications. Since conventional crystallography cannot distinguish between static disorder and atomic motions, we develop the energy-resolved variable-shutter pair distribution function technique. This collects structural snapshots with varying exposure times, on timescales relevant for atomic motions. In disagreement with previous interpretations, we find the time-averaged structure of GeTe to be crystalline at all temperatures, but with anisotropic anharmonic dynamics at higher temperatures that resemble static disorder at fast shutter speeds, with correlated ferroelectric fluctuations along the $<$100$>$c direction. We show that this anisotropy naturally emerges from a Ginzburg-Landau model that couples polarization fluctuations through long-range elastic interactions. By accessing time-dependent atomic correlations in energy materials, we resolve the long-standing disagreement between local and average structure probes, and show that spontaneous anisotropy is ubiquitous in cubic IV-VI materials., Comment: Published version, substantial changes, many references removed due to journal limits :-( Please see the supporting information online. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format (see conditions)

We report time- and angle-resolved photoemission spectroscopy on SnSe which currently attracts great interest due to its extremely high thermoelectric performance. Laser-assisted photoemission signals are observed within $\pm$20 fs of the pump pulse arrival. Around 30-50 fs after the photoexcitation, the conduction band minima are not populated by the photoexcited electrons while the valence bands are considerably broadened. In going from 90 fs to 550 fs after the photoexcitation, the photoexcited carriers are decayed into the multiple conduction band minima. The observed conduction bands are consistent with the band structure calculations. The multiple conduction minima suggest possibility of high and anisotropic thermoelectric performance of n-type SnSe single crystal if it is realized., Comment: 5 pages, 4 figures

Infrared laser systems are vital for applications in spectroscopy, communications, and biomedical devices, where infrared nonlinear optical (NLO) crystals are required for broadband frequency down-conversion. Such crystals need to have high non-resonant NLO coefficients, a large bandgap, low absorption coefficient, phase-matchability among other competing demands, e.g., a larger bandgap leads to smaller NLO coefficients. Here, we report the successful growth of single crystals of $\gamma$-NaAsSe$_2$ that exhibit a giant second harmonic generation (SHG) susceptibility of d$_{11}$=590 pm V$^{-1}$ at 2$\mu$m wavelength; this is ~ eighteen times larger than that of commercial AgGaSe$_2$ while retaining a similar bandgap of ~1.87eV, making it an outstanding candidate for quasi-phase-matched devices utilizing d$_{11}$. In addition, $\gamma$-NaAsSe$_2$ is both Type I and Type II phase-matchable, and has a transparency range up to 16$\mu$m wavelength. Thus $\gamma$-NaAsSe2 is a promising bulk NLO crystal for infrared laser applications., Comment: Main text: 21 pages, 4 figures

SnSe is a layered material that currently holds the record for bulk thermoelectric efficiency. The primary determinant of this high efficiency is thought to be the anomalously low thermal conductivity resulting from strong anharmonic coupling within the phonon system. Here we show that the nature of the carrier system in SnSe is also determined by strong coupling to phonons by directly visualizing polaron formation in the material. We employ ultrafast electron diffraction and diffuse scattering to track the response of phonons in both momentum and time to the photodoping of free carriers across the bandgap, observing the bimodal and anisotropic lattice distortions that drive carrier localization. Relatively large (\SI{18.7}{\angstrom}), quasi-1D polarons are formed on the \SI{300}{\femto\second} timescale with smaller (\SI{4.2}{\angstrom}) 3D polarons taking an order of magnitude longer (\SI{4}{\pico\second}) to form. This difference appears to be a consequence of the profoundly anisotropic electron-phonon coupling in SnSe, with strong Fr\"ohlich coupling only to zone center polar optical phonons. These results demonstrate that carriers in SnSe at optimal doping levels results in a high polaron density and that strong electron-phonon coupling is also critical to the thermoelectric performance of this benchmark material and potentially high-performance thermoelectrics more generally., Comment: 11 pages, 5 figures, includes supplemental information

A notable phenomenon in topological semimetals is the violation of Kohler$^,$s rule, which dictates that the magnetoresistance $MR$ obeys a scaling behavior of $MR = f(H/\rho_0$), where $MR = [\rho_H-\rho_0]/\rho_0$ and $H$ is the magnetic field, with $\rho_H$ and $\rho_0$ being the resistivity at $H$ and zero field, respectively. Here we report a violation originating from thermally-induced change in the carrier density. We find that the magnetoresistance of the Weyl semimetal, TaP, follows an extended Kohler$^,$s rule $MR = f[H/(n_T\rho_0)]$, with $n_T$ describing the temperature dependence of the carrier density. We show that $n_T$ is associated with the Fermi level and the dispersion relation of the semimetal, providing a new way to reveal information on the electronic bandstructure. We offer a fundamental understanding of the violation and validity of Kohler$^,$s rule in terms of different temperature-responses of $n_T$. We apply our extended Kohler$^,$s rule to BaFe$_2$(As$_{1-x}$P$_x$)$_2$ to settle a long-standing debate on the scaling behavior of the normal-state magnetoresistance of a superconductor, namely, $MR$ ~ $tan^2\theta_H$, where $\theta_H$ is the Hall angle. We further validate the extended Kohler$^,$s rule and demonstrate its generality in a semiconductor, InSb, where the temperature-dependent carrier density can be reliably determined both theoretically and experimentally.

Semiconductors with very low lattice thermal conductivities are highly desired for applications relevant to thermal energy conversion and management, such as thermoelectrics and thermal barrier coatings. Although the crystal structure and chemical bonding are known to play vital roles in shaping heat transfer behavior, material design approaches of lowering lattice thermal conductivity using chemical bonding principles are uncommon. In this work, we present an effective strategy of weakening interatomic interactions and therefore suppressing lattice thermal conductivity based on chemical bonding principles and develop a high-efficiency approach of discovering low $\kappa_{\rm L}$ materials by screening the local coordination environments of crystalline compounds. The followed first-principles calculations uncover 30 hitherto unexplored compounds with (ultra)low lattice thermal conductivities from thirteen prototype crystal structures contained in the inorganic crystal structure database. Furthermore, we demonstrate an approach of rationally designing high-performance thermoelectrics by additionally incorporating cations with stereochemically active lone-pair electrons. Our results not only provide fundamental insights into the physical origin of the low lattice thermal conductivity in a large family of copper-based compounds but also offer an efficient approach to discovery and design materials with targeted thermal transport properties., Comment: 14 pages, 9 figures

The development of efficient thermal energy management devices such as thermoelectrics, barrier coatings, and thermal data-storage disks often relies on compounds that possess very low lattice thermal conductivity ($\kappa_l$). Here, we present the computational prediction of a large family of 628 thermodynamically stable quaternary chalcogenides, AMM'Q$_3$ (A = alkali/alkaline earth/post-transition metals; M/M' = transition metals, lanthanides; Q = chalcogens) using high-throughput density functional theory (DFT) calculations. We validate the presence of low-$\kappa_l$ in this family of materials by calculating $\kappa_l$ of several predicted stable compounds using the Peierls-Boltzmann transport equation within a first-principles DFT framework. Our analysis reveals that the low-$\kappa_l$ in the AMM'Q$_3$ compounds originates from the presence of either a strong lattice anharmonicity that enhances the phonon scatterings or rattlers cations that lead to multiple scattering channels in their crystal structures. Our predictions suggest new experimental research opportunities in the synthesis and characterization of these stable, low-$\kappa_l$ compounds.

Layered heterostructure materials with two different functional building blocks can teach us about emergent physical properties and phenomena arising from interactions between the layers. We report the intergrowth compounds KLa$M$$_{1-x}$Te$_{4}$ ($M$ = Mn, Zn; $x\approx$ 0.35) featuring two chemically distinct alternating layers [LaTe$_3$] and [K$M$$_{1-x}$Te]. Their crystal structures are incommensurate, determined by single X-ray diffraction for the Mn compound and transmission electron microscope (TEM) study for the Zn compound. KLaMn$_{1-x}$Te$_{4}$ crystallizes in the orthorhombic superspace group $Pmnm$(01/2${\gamma}$)$s$00 with lattice parameters $a$ = 4.4815(3) {\AA}, $b$ = 21.6649(16) {\AA} and $c$ = 4.5220(3) {\AA}. It exhibits charge density wave (CDW) order at room temperature with a modulation wave vector $\mathbf{q}$ = 1/2$\mathbf{b}$* + 0.3478$\mathbf{c}$* originating from electronic instability of Te-square nets in [LaTe$_{3}$] layers. The Mn analog exhibits a cluster spin glass behavior with spin freezing temperature $T_{\mathrm{f}}$ $\approx$ 5 K attributed to disordered Mn vacancies and competing magnetic interactions in the [Mn$_{1-x}$Te] layers. The Zn analog also has charge density wave order at room temperature with a similar $\mathbf{q}$-vector having the $\mathbf{c}$* component ~ 0.346 confirmed by selected-area electron diffraction (SAED). Electron transfer from [K$M_{1-x}$Te] to [LaTe$_{3}$] layers exists in KLa$M_{1-x}$Te$_{4}$, leading to an enhanced electronic specific heat coefficient. The resistivities of KLa$M_{1-x}$Te$_{4}$ ($M$ = Mn, Zn) exhibit metallic behavior at high temperatures and an upturn at low temperatures, suggesting partial localization of carriers in the [LaTe$_{3}$] layers with some degree of disorder associated with the $M$ atom vacancies in the [$M_{1-x}$Te] layers., Comment: 1 table, 10 figures, 35 pages

New phases of matter emerge at the edge of magnetic instabilities. In local moment systems, such as heavy fermions, the magnetism can be destabilized by pressure, chemical doping, and, rarely, by magnetic field, towards a zero-temperature transition at a quantum critical point (QCP). Even more rare are instances of QCPs induced by pressure or doping in itinerant moment systems, with no known examples of analogous field-induced \textit{T} = 0 transitions. Here we report the discovery of a new itinerant antiferromagnet with no magnetic constituents, in single crystals of Ti$_3$Cu$_4$ with $T_N$ = 11.3 K. Band structure calculations point to an orbital-selective, spin density wave ground state, a consequence of the square net structural motif in Ti$_3$Cu$_4$. A small magnetic field, $H_C$ = 4.87 T, suppresses the long-range order via a continuous second-order transition, resulting in a field-induced QCP. The magnetic Gr\"uneisen ratio diverges as $H \rightarrow H_C$ and $T\rightarrow0$, with a sign change at $H_C$ and $T^{-1}$ scaling at $H~=~H_C$, providing evidence from thermodynamic measurements for quantum criticality for $H \parallel c$. Non-Fermi liquid (NFL) to Fermi liquid (FL) crossover is observed close to the QCP, as revealed by the power law behavior of the electrical resistivity.

Recently, halide perovskites have gained significant attention from the perspective of efficient spintronics owing to Rashba effect. This effect occurs as a consequence of strong spin-orbit coupling under noncentrosymmetric environment, which can be dynamic and/or static. However, there exist intense debates on the origin of broken inversion symmetry since the halide perovskites typically crystallize into a centrosymmetric structure. In order to clarify the issue, we examine both dynamic and static effects in the all-inorganic CsPbBr3 and organic-inorganic CH3NH3PbBr3 (MAPbBr3) perovskite single crystals by employing temperature- and polarization-dependent photoluminescence excitation spectroscopy. The perovskite single crystals manifest the dynamic effect by photon recycling in the indirect Rashba gap, causing dual peaks in the photoluminescence. But the effect vanishes in CsPbBr3 at low temperatures (< 50 K), accompanied by a striking color change of the crystal, arising presumably from lower degrees of freedom for inversion symmetry breaking associated with the thermal motion of the spherical Cs cation, compared with the polar MA cation in MAPbBr3. We also show that static Rashba effect occurs only in MAPbBr3 below 90 K due to surface reconstruction via MA-cation ordering, which likely extends across a few layers from the crystal surface to the interior. We further demonstrate that this static Rashba effect can be completely suppressed upon surface treatment with poly methyl methacrylate (PMMA) coating. We believe that our results provide a rationale for the Rashba effects in halide perovskites.

A method based on the Gibbs' adsorption isotherm is developed to calculate the decrease in interfacial free energy resulting from solute segregation at an internal interface, built on measured concentration profiles. Utilizing atom-probe tomography (APT), we first measure a concentration profile of the relative interfacial excess of solute atoms across an interface. To accomplish this we utilize a new method based on J. W. Cahn's formalism for the calculation of the Gibbs interfacial excess. We also introduce a method to calculate the decrease in interfacial free energy that is caused by the segregating solute atoms. This method yields a discrete profile of the decrease in interfacial free energies, which takes into account the measured concentration profile and calculated Gibbsian excess profile. We demonstrate that this method can be used for both homo- and hetero-phase interfaces and takes into account the actual distribution of solute atoms across an interface as determined by APT. It is applied to the case of the semiconducting system PbTe-PbS 12 mol.%-Na 1 mol.%, where Na segregation at the PbS/PbTe interface is anticipated to reduce the interfacial free energy of the {100} facets. We also consider the case of the nickel-based Alloy 600, where B and Si segregation are suspected to impede inter-granular stress corrosion cracking (IGSCC) at homo- (GB) and hetero-phase metal carbide (M7C3) interfaces. The concentration profiles associated with internal interfaces are measured by APT using an ultraviolet (wavelength = 355 nm) laser to dissect nanotips on an atom-by-atom and atomic plane-by-plane basis.

Magnetic topological semimetals, the latest member of topological quantum materials, are attracting extensive attention as they may lead to topologically-driven spintronics. Currently, magnetotransport investigations on these materials are focused on anomalous Hall effect. Here, we report on the magnetoresistance anisotropy of topological semimetal CeBi, which has tunable magnetic structures arising from localized Ce 4f electrons and exhibits both negative and positive magnetoresistances, depending on the temperature. We found that the angle dependence of the negative magnetoresistance, regardless of its large variation with the magnitude of the magnetic field and with temperature, is solely dictated by the field-induced magnetization that is orientated along a primary crystalline axis and flops under the influence of a rotating magnetic field. The results reveal the strong interaction between conduction electrons and magnetization in CeBi. They also indicate that magnetoresistance anisotropy can be used to uncover the magnetic behavior and the correlation between transport phenomena and magnetism in magnetic topological semimetals.

The charge and spin of the electrons in solids have been extensively exploited in electronic devices and in the development of spintronics. Another attribute of electrons - their orbital nature - is attracting growing interest for understanding exotic phenomena and in creating the next-generation of quantum devices such as orbital qubits. Here, we report on orbital-flop induced magnetoresistance anisotropy in CeSb. In the low temperature high magnetic-field driven ferromagnetic state, a series of additional minima appear in the angle-dependent magnetoresistance. These minima arise from the anisotropic magnetization originating from orbital-flops and from the enhanced electron scattering from magnetic multidomains formed around the first-order orbital-flop transition. The measured magnetization anisotropy can be accounted for with a phenomenological model involving orbital-flops and a spin-valve-like structure is used to demonstrate the viable utilization of orbital-flop phenomenon. Our results showcase a contribution of orbital behavior in the emergence of intriguing phenomena.

Nonequilibrium phase transition plays a pivotal role in a broad physical context from condensed matter to cosmology. Tracking the formation of non-equilibrium phases in condensed matter is challenging and requires a resolution of the long-range cooperativity on ultra-short timescales. Here, we study the spontaneous symmetry breaking transformation of a charge-density wave system from a stripe phase into a checkerboard state. Such a state is thermodynamically forbidden, but is introduced through a system quench using ultrashort, intense laser pulses. The dynamics is mediated by the soft modes that unfold spontaneously and order the field on a timescale ~1 ps. Using the coherent electron diffraction with ~100 fs resolution, we capture the entire course and demonstrate nonergodic behavior proximal to symmetry breaking that is crucial for stabilizing the hidden states. Remarkably, the thermalization due to carriers cooling arrests the remnants of the transient orders into the topological defects in the eventual state with distinct new properties that last for more than 1 ns. The fundamental dynamics observed here opens an intriguing perspective of controlling phase transitions in quantum materials far from equilibrium.

Hybrid organic-inorganic halide perovskite solar cells have emerged as leading candidates for third-generation photovoltaic technology. Despite the rapid improvement in power conversion efficiency (PCE) for perovskite solar cells in recent years, the low-frequency carrier kinetics that underlie practical roadblocks such as hysteresis and degradation remain relatively poorly understood. In an effort to bridge this knowledge gap, we perform here correlated low-frequency noise (LFN) and impedance spectroscopy (IS) characterization that elucidates carrier kinetics in operating perovskite solar cells. Specifically, we focus on planar cell geometries with a SnO2 electron transport layer and two different hole transport layers, namely, poly(triarylamine) (PTAA) and Spiro-OMeTAD. PTAA and Sprio-OMeTAD cells with moderate PCEs of 5 to 12 percent possess a Lorentzian feature at 200 Hz in LFN measurements that corresponds to a crossover from electrode to dielectric polarization. In comparison, Spiro-OMeTAD cells with high PCEs (15 percent) show four orders of magnitude lower LFN amplitude and are accompanied by a cyclostationary process. Through a systematic study of more than a dozen solar cells, we establish a correlation with noise amplitude, power conversion efficiency, and fill factor. Overall, this work establishes correlated LFN and IS as an effective methodology for quantifying low frequency carrier kinetics in perovskite solar cells, thereby providing new physical insights that can rationally guide ongoing efforts to improve device performance, reproducibility, and stability.

The pressure dependencies of the magnetic and superconducting transitions, as well as that of the superconducting upper critical field are reported for single crystalline EuRbFe$_4$As$_4$. Resistance measurements were performed under hydrostatic pressures up to 6.21 GPa and in magnetic fields up to 9 T. Zero-field-cool magnetization measurements were performed under hydrostatic pressures up to 1.24 GPa under 20 mT applied field. Superconducting transition temperature, $T_\text c$, up to 6.21 GPa and magnetic transition temperature, $T_\text M$, up to 1.24 GPa were obtained and a pressure-temperature phase diagram was constructed. Our results show that $T_\text c$ is monotonically suppressed upon increasing pressure. $T_\text M$ is linearly increased up to 1.24 GPa. For the studied pressure range, no signs of the crossing of $T_\text M$ and $T_\text c$ lines are observed. The normalized slope of the superconducting upper critical field is gradually suppressed with increasing pressure, which may be due to the continuous change of Fermi-velocity $v_F$ with pressure., Comment: 5 pages, 7 figures