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Mn 2+ doping imposes intriguing optoelectronic properties on lead-halide perovskites; however, its impact on their crystal structure remains unclear.
CaCo 2–y As 2 is a unique itinerant system having strong magnetic frustration. Here, we report the effect of electron doping on the physical properties resulting from Ni substitutions for Co. The single crystals of Ca(Co 1–x Ni x ) 2–y As 2 were characterized by single-crystal x-ray diffraction, energy-dispersive x-ray spectroscopy, magnetization M versus temperature T, magnetic field H, time t, and heat capacity C p (H, T) measurements. The A-type antiferromagnetic (AFM) transition temperature T N = 52 K for x = 0 decreases to 22 K with only 3% Ni substitution and is completely suppressed for x > 0.16. For 0.11 ≤ x ≤ 0.52 strong ferromagnetic (FM) fluctuations develop as revealed by magnetic susceptibility χ(T) = M(T) / H measurements. For x = 0.11 and 0.16 competing AFM and FM interactions result in a reentrant spin-glass behavior below T N , as evidenced by the observations of thermomagnetic hysteresis and magnetic relaxation. Enhanced FM fluctuations are also found for the x = 0.21 and 0.31 crystals, where χ c increases significantly at low T. A large χ anisotropy in these compositions where χ c is up to a factor of two larger than χ ab suggests that the FM spin fluctuations are quasi-1D in nature. Weak ferromagnetic contributions to the magnetization are found at T = 2 K for x = 0.11 –0.31. Heat-capacity Cp(T) measurements reveal the presence of FM quantum spin fluctuations for 0.11 ≤ x ≤ 0.52, where a logarithmic T dependence of Cp(T) / T is observed at low T. Here, the suppression of AFM order by the development of strong FM fluctuations in Ca(Co 1–x Ni x ) 2–y As 2 crystals suggests the presence of a FM quantum-critical point at x ≈ 0.20. Our density-functional theory (DFT) calculations confirm that FM fluctuations are enhanced by Ni substitutions for Co in CaCo 2–y As 2 . The Sommerfeld electronic heat-capacity coefficient is enhanced for x = 0, 0.21, and 0.42 by about a factor of two compared to DFT calculations of the density of states (DOS) at the Fermi energy, suggesting an enhancement of the DOS from electron-phonon and/or electron-electron interactions. The crystals with x > 0.52 do not exhibit FM spin fluctuations or magnetic order at T ≥ 1.8 K, which was found from the DFT calculations to arise from a Stoner transition. Superconductivity is not observed above 1.8 K for any of the compositions. Neutron-diffraction studies of crystals with x = 0.11 and 0.16 in the crossover regime (0.1 ≲ x ≲ 0.2) show no evidence of A-type ordering as observed in the parent compound with x = 0. Furthermore, no other common magnetic structures, such as ferromagnetic (FM), helical stacking of in-plane FM layers, or in-plane AFM structure, are found with an ordered moment greater than the uncertainty of 0.05 μ B per transition-metal atom.
The structure, magnetic, and magnetocaloric (MC) properties of orthorhombic nanocrystalline GdCrO 3 with six particle sizes: < d > = 87, 103, 145, 224, 318, and 352 nm are reported. The particle size was tailored by annealing under different temperatures and estimated by scanning electron microscopy. With increase in < d >, Goldschmidt tolerance factor t, orthorhombic strain s, and out-of-plane Cr–O 1 –Cr bond angle first decrease, reaching minimum values for < d > = 224 nm, and then increase for sample with < d > = 318 nm and 352 nm, thus showing a V-shaped variation. Temperature dependence of the magnetization (M) reveals an antiferromagnetic transition at ${T}_{\text{N}}^{\text{Cr}}\sim 168$ K for < d > ≥ 224 nm and ${T}_{\text{N}}^{\text{Cr}}\sim 167$ K for < d > < 224 nm and an essentially d-independent spin-reorientation at T SR = 9 K. M measured at 5 K and 7 T first increases with increase in < d >, reaching maximum value for sample with < d > = 224 nm, and then decreases for samples with < d > = 318 nm and 352 nm, showing an inverted-V variation with < d >. Similar < d >-dependence is observed for the magnetic entropy change (MEC) and relative cooling power (RCP) showing a close relationship between the structural and magnetic properties of GdCrO 3 nanoparticles investigated here. The 224 nm sample with the minimum values of t, s, and Cr–O 1 –Cr bond angle exhibits the maximum value of MEC (–ΔS) = 37.8 J kg –1 K –1 at 5 K under a field variation (ΔH) of 7 T and its large estimated RCP of 623.6 J Kg –1 is comparable with those of typical MC materials. Both (–ΔS) and RCP are shown to scale with the saturation magnetization MS, suggesting that MS is the crucial factor controlling their magnitudes. Assuming (–ΔS) ~ (ΔH) n , the temperature dependence of n for the six samples are determined, n varying between 1.3 at 5 K to n = 2.2 at 130 K in line with its expected magnitudes based on mean-field theory. Furthermore, these results on structure-property correlations and scaling in GdCrO 3 suggest that its MC properties are tunable for potential low-temperature magnetic refrigeration applications.
Extensive photochemical and spectroscopic properties of the V B - defect in hexagonal boron nitride are calculated, concluding that the observed photoemission associated with recently observed optically detected magnetic resonance is most likely of (1) 3 E'' → (1) 3 A' 2 origin. Rapid intersystem crossing from the defect's triplet to singlet manifolds explains the observed short excited-state lifetime and very low quantum yield. New experimental results reveal smaller intrinsic spectral bandwidths than previously recognized, interpreted in terms of spectral narrowing and zero-phonon-line shifting induced by the Jahn-Teller effect. Different types of computational methods are applied to map out the complex triplet and singlet defect manifolds, including the doubly ionized formulation of the equation-of-motion coupled-cluster theory that is designed to deal with the open-shell nature of defect states, and mixed quantum-mechanics/molecular-mechanics schemes enabling 5763-atom simulations. Finally, two other energetically feasible spectral assignments from among the singlet and triplet manifolds are considered, but ruled out based on inappropriate photochemical properties.
Growth parameters play a significant role in the crystal quality and physical properties of layered materials. Here we present a case study on a van der Waals magnetic NbFeTe 2 material. Two different types of polymorphic NbFeTe 2 phases, synthesized at different temperatures, display significantly different behaviors in crystal symmetry, electronic structure, electrical transport, and magnetism. While the phase synthesized at low temperature showing behavior consistent with previous reports, the new phase synthesized at high temperature, has completely different physical properties, such as metallic resistivity, long-range ferromagnetic order, anomalous Hall effect, negative magnetoresistance, and distinct electronic structures. Neutron diffraction reveals out-of-plane ferromagnetism below 70 K, consistent with the electrical transport and magnetic susceptibility studies. Finally, our work suggests that simply tuning synthetic parameters in a controlled manner could be an effective route to alter the physical properties of existing materials potentially unlocking new states of matter, or even discovering new materials.
Abstract Novel phases of matter with unique properties that emerge from quantum and topological protection present an important thrust of modern research. Of particular interest is to engineer these phases on demand using ultrafast external stimuli, such as photoexcitation, which offers prospects of their integration into future devices compatible with optical communication and information technology. Here, we use MeV Ultrafast Electron Diffraction (UED) to show how a transient three-dimensional (3D) Dirac semimetal state can be induced by a femtosecond laser pulse in a topological insulator ZrTe 5 . We observe marked changes in Bragg diffraction, which are characteristic of bond distortions in the photoinduced state. Using the atomic positions refined from the UED, we perform density functional theory (DFT) analysis of the electronic band structure. Our results reveal that the equilibrium state of ZrTe 5 is a topological insulator with a small band gap of ~ 25 meV, consistent with angle-resolved photoemission (ARPES) experiments. However, the gap is closed in the presence of strong spin-orbit coupling (SOC) in the photoinduced transient state, where massless Dirac fermions emerge in the chiral band structure. The time scale of the relaxation dynamics to the transient Dirac semimetal state is remarkably long, τ ~ 160 ps, which is two orders of magnitude longer than the conventional phonon-driven structural relaxation. The long relaxation is consistent with the vanishing density of states in Dirac spectrum and slow spin-repolarization of the SOC-controlled band structure accompanying the emergence of Dirac fermions.
Time-resolved diffuse scattering experiments have gained increasing attention due to their potential to reveal nonequilibrium dynamics of crystal lattice vibrations with full momentum resolution. Although progress has been made in interpreting experimental data on the basis of one-phonon scattering, understanding the role of individual phonons can be sometimes hindered by multiphonon excitations. In Ref. [M. Zacharias, H. Seiler, F. Caruso, D. Zahn, F. Giustino, P. C. Kelires, and R. Ernstorfer, Phys. Rev. Lett. 127, 207401 (2021)], we have introduced a rigorous approach for the calculation of the all-phonon inelastic scattering intensity of solids from first-principles. In the present work, we describe our implementation in detail and show that multiphonon interactions are captured efficiently by exploiting translational and time-reversal symmetries of the crystal. We demonstrate its predictive power by calculating the scattering patterns of monolayer molybdenum disulfide (MoS 2 ), bulk MoS 2 , and black phosphorus (bP), and we obtain excellent agreement with our measurements of thermal electron diffuse scattering. Remarkably, our results show that multiphonon excitations dominate in bP across multiple Brillouin zones, while in MoS 2 they play a less pronounced role. We expand our analysis for each system and examine the effect of individual atomic and interatomic vibrational motion on the diffuse scattering signals. We further demonstrate the high-throughput capability of our approach by reporting all-phonon scattering maps of two-dimensional MoSe 2 , WSe 2 , WS 2 , graphene, and CdI 2 , rationalizing in each case the effect of multiphonon processes. As a side point, we show that the special displacement method reproduces the thermally distorted configuration that generates precisely the all-phonon diffuse pattern. In conclusion, the present methodology opens the way for systematic calculations of the scattering intensity in crystals and the accurate interpretation of static and time-resolved inelastic scattering experiments.
Liquids, ubiquitous on earth, are prototypical disordered condensed matter. As the mediate phase between non-structured gases and ordered solids, liquids p ossess intriguing complexities that are absent on either extreme counter phase, especially when they are driven away from equilibrium. Despite decades of studies, the physics of liquids still keeps surprising us and challenges our understanding of condensed matter, emergent phenomena, and complex systems. Among the many interesting properties, the nature of collective dynamics in liquids remains elusive because of both the presence of strong interactions and the absence of translational invariance. This project studied the universal features of collective density fluctuations (or collective modes), which include both phonon-like excitations and collective relaxations, in the Q-dependent generalized hydrodynamic regime in liquids and liquid-like matter both at and away from equilibrium. We performed systematic studies of the fast collective dynamics (including both phonon-like excitations and collective relaxations) of four classes of liquids characterized by different fragilities and interactions using synergistically integrated coherent neutron scattering experiments (Inelastic Neutron Scattering (INS), Quasi-Elastic Neutron Scattering (QENS), and Neutron Spin Echo (NSE)), a ViscoElastic Hydrodynamics theory we have been developing, andMolecular Dynamics (MD) simulations and our analysis package LiquidLib. The transformative knowledge of the collective dynamics in liquids is important to understand and ultimately control the transport of mass, energy, and charge in liquids, both at and away from thermal equilibrium, which may will likely impact a wide range of disciplines.
Understanding the interplay between individual magnetic impurities and superconductivity is crucial for bottom-up construction of novel phases of matter. Sub-gap bound states that are used in this endeavor are typically considered as independent entities that each result from the exchange scattering between the respective impurity orbitals and electrons of the superconducting condensate. Here we present experimental evidence of individual multi-spin impurities where the sub-gap states are not independent. Specifically, we find that by tuning the energy of the state closest to zero through zero, all other sub-gap states change particle-hole asymmetry as well. We show that this can be understood by including Hund’s coupling, which favors high-spin configurations, into a multi-orbital Anderson model. Unlike for the case of independent spins, the transition we observe signals the simultaneous departure of more than one quasiparticle from the impurity, while the parity of the ground state may remain unchanged. Our results show that Hund’s coupling is not only crucial in generating high-spin impurities, but also to understand the transition between two distinct ground states, and should therefore be taken into account for e.g. impurity-based band-structure engineering.
Conventionally, the modulation of the intrinsic Weyl nodes in Weyl semimetals is challenging, due to topological protection. Here we report the structural dependence of the Weyl nodes in a Co2MnGa Heusler thin film via a temperature-dependent tetragonal distortion. The ability to manipulate these Weyl nodes allows for the control of the intrinsic electromagnetic properties. Temperature-dependent x-ray diffraction (XRD) measurements identify a compressive tetragonal distortion with decreasing temperature from 300 to 20 K. The calculated Weyl properties can be directly compared with experimental parameters through the temperature-dependent XRD measurements which show the intrinsic correlation between Weyl properties and important magnetic parameters. Further, the microscopic momentum space properties of Weyl nodes such as the distance (d W ), solid angle (Ω W ), tilt (φ W ), and nodal point energy (E W ) directly affect the macroscopic observable properties such as exchange stiffness (A), magnetization (M), and effective anisotropy field $H^{eff}_{K}$, as shown via structure-dependent density functional theory calculations. These predictions are experimentally observed as large variations in the bulk magnetization and effective anisotropy field as a function of temperature. These results highlight a unique degree of freedom in the control of macroscopic magnetic properties via the modulation of the intrinsic properties of Weyl nodes through structural distortions.
Highlights: • Four kinds of exact stripe soliton solutions in Bose–Einstein condensates with helicoidal spin–orbit coupling (SOC) are represented. • The influence of helicoidal SOC on the structure of stripe solitons are described in detail. • The corresponding spin polarization is expressed on the Bloch sphere. • The formation mechanism of stripe solitons and the interaction properties of moving stripe solitons are discussed. We present the exact analytical solution of stripe solitons on different backgrounds in Bose–Einstein condensates with helicoidal spin–orbit coupling (SOC). They are divided into two categories, one is stationary stripe soliton on zero background or period-wave background, the other is moving stripe soliton on zero background or plane-wave background. The period of stripe is determined by both strength and frequency of helicoidal SOC, and the oscillation amplitude of stripe is adjustable in the case of fixed total density. The corresponding spin polarization is expressed on Bloch sphere. For stationary soliton, the spin density vector take values in three directions, which is different from the Rashba–Dresslhaus coupling scheme. The spin density vectors display more complicated spatial distribution for moving stripe solitons. Meanwhile, the formation mechanism of stripe soliton and the interaction properties of moving stripe solitons are discussed. Our work enhances the understanding of stripe solitons, and is helpful for the observation of stripe phase.
Time-domain magneto-THz spectroscopy is utilized to study the frustrated magnet averievite Cu 5–x Zn x V 2 O 10 (CsCl). Pronounced THz resonances are observed in unsubstituted samples (x = 0) when cooling below the onset of short-range magnetic correlations. The influence of external magnetic effects confirms the magnetic origin of these resonances. Increasing Zn substitution suppresses the resonances, as frustration effects dominate, reflecting the nonmagnetic phases for x > 0.25 compounds. The temperature evolution of the THz spectra is complemented with electron spin resonance spectroscopy. This comparison allows a direct probe of the different contributions from magnetic order, frustration, and structural properties in the phase diagram of averievite. Furthermore, our results illustrate the effect of magnetic interactions in THz spectra of frustrated magnets.
The electronic structure of CeNiSn, which is a potential topological Kondo insulator and a Dirac nodal-loop semimetal, has been investigated by employing temperature (T) dependent angle-resolved photoemission spectroscopy (ARPES). The Fermi surfaces (FSs) and the band structures of CeNiSn for three orthogonal crystallographic planes are measured, in which both the very dispersive bands and the flat bands are observed, having mainly the Ni 3d character and the Ce 4f character, respectively. The measured FSs and ARPES bands agree reasonably well with the density functional theory (DFT) calculations. The Fermi-edge (E F ) photon energy (hν) map along k b (=k (010) ) shows that the metallic E F -crossing states on the (010) surface have the three-dimensional character, suggesting that the observed E F -crossing metallic states do not correspond to the topological surface states of the two-dimensional character. On the other hand, albeit weak, the features of the hourglass-type bulk band crossings are observed along SXS, with the energies and the slopes being similar to those predicted by the DFT calculations, supporting the Dirac semimetallic nature of CeNiSn. In T-dependent ARPES, the Ce 4f Kondo resonance states are clearly revealed at low T, which become much suppressed above ~80 K. This feature is consistent with the Kondo temperature of CeNiSn, estimated from its ρ(T) data. This work demonstrates the importance of the coherent Kondo states in determining the topological properties of CeNiSn.
Since the discovery of pressure-induced superconductivity in the two-leg ladder system BaFe 2 X 3 (X=S, Se), with the 3d iron electronic density n=6, quasi-one-dimensional iron-based ladders have attracted considerable attention. In this work, we use density-functional theory to predict that the novel n=6 iron ladder BaFe 2 Se 3 could be stable with a similar crystal structure as BaFe 2 Se 3 . Furthermore, our results also indicate that BaFe2Te3 will display a complex 2×2 block-type magnetic order. Due to the magnetic striction effects of this block order, BaFe2Te3 should be a magnetic noncollinear ferrielectric system with a net polarization 0.31μC/cm2. In summary, the similar electronic density and magnetic ground state of Te- and Se-based ladders indicates both should display similar properties. In particular, the physical and structural similarity with BaFe 2 Se 3 suggests that BaFe 2 Se 3 could become superconducting under high pressure.
We develop a low-energy continuum model for phonons in twisted moiré bilayers, based on a configuration-space approach. In this approach, interatomic force constants are obtained from density functional theory (DFT) calculations of untwisted bilayers with various in-plane shifts. This allows for efficient computation of phonon properties for any small twist angle, while maintaining DFT-level accuracy. Based on this framework, we show how the low-energy phonon modes, including interlayer shearing and layer-breathing modes, vary with the twist angle. As the twist angle decreases, the frequencies of the low-energy modes are reordered and the atomic displacement fields corresponding to phonon eigenmodes break translational symmetry, developing periodicity on the moiré length scale. Here, we demonstrate the capabilities of our model by calculating the phonon properties of three specific structures: bilayer graphene, bilayer molybdenum disulfide (MoS 2 ), and molybdenum diselenide-tungsten diselenide (MoSe 2 -WSe 2 ).
We have realized different honeycomb lattices for microwave photons in the 4 to 8 GHz band using superconducting spiral resonators. Each lattice comprises a few hundred sites. Two designs have been studied, one leading to two bands touching at the Dirac points and one where a gap opens at the Dirac points. Using a scanning laser technique to image the eigenmodes of this new type of photonic lattices, we are able to reconstruct their band structure. The measured bands are in excellent agreement with ab initio models that combine numerical simulations of the electromagnetic properties of the spiral resonator and analytical calculations.
Understanding the atomic-scale mechanisms that govern the structure of interfaces is critical across materials systems but particularly so for two-dimensional (2D) moiré materials. Here, we image, atom-by-atom, the thermally induced structural evolution of twisted bilayer transition metal dichalcogenides using in situ transmission electron microscopy. We observe low-temperature, local conversion of moiré superlattice into nanoscale aligned domains. Unexpectedly, this process occurs by nucleating a new grain within one monolayer, whose crystal orientation is templated by the other. The aligned domains grow through collective rotation of moiré supercells and hopping of 5|7 defect pairs at moiré boundaries. This provides mechanistic insight into the atomic-scale interactions controlling moiré structures and illustrates the potential to pattern interfacial structure and properties of 2D materials at the nanoscale.
Progress of the modern day condensed matter physics is to a large extent driven by the synthesis of new materials, advances in their experimental characterization and theoretical description. Recent discoveries of novel gapless Weyl semimetals, such as NaBi,CdAs, and BiTe-based films, in which magnetic dopants essentially suppress the gap, have added to the family of graphene and topological insulators actively investigated over the past decade. With the field of novel semimetals rapidly maturing, its focus necessarily shifts from demonstrations of the feasibility of such materials to their quantitative characterization. While the transport and optical properties of graphene and topological insulators are well captured within the picture of free non-interacting electrons, gapless 3D Weyl semimetals and narrow-gap 2D semiconductors with Dirac spectrum are known to be extremely susceptible to disorder and electron-electron interactions. This susceptibility obscures the manifestations of nontrivial band structure -- like quantum anomalous Hall effect -- of the new topological materials. Among particular projects to be addressed are: 1) optical conductivity of 3D gapless Dirac fermions in the presence of smooth disorder, 2) interplay of disorder and Coulomb interactions in the spectral properties of such fermions, 3) formation and structure of the impurity band with Coulomb supercritical clusters, 4) Coulomb interaction-driven renormalization of the electron spectrum and of the transport response in the presence of strong magnetic field, 5) instanton approach to the disorder-induced fluctuation states in zero-gap 3D materials, and 6) the role of disorder in quantum anomalous Hall effect. The proposal relies upon the investigators' previous broad expertise in interacting and disordered electron systems. The methods to be employed include perturbative diagrammatic technique, non-perturbative instanton and self-consistent approximations, hydrodynamics of electron liquid. Both analytical as well as numerical approaches are to be employed. The anticipated broader outcome of the proposal includes gaining an in-depth understanding of the interplay of the disorder and interactions under the conditions when this interplay has the most dramatic impact on observables. Traditionally, interaction effects are among the most challenging and interesting problems of condensed matter physics. Similarly, disordered systems typically present very difficult but extremely rich problems in the description of various materials. Importantly, understanding the spectral and transport properties of such materials not only presents the fundamental objective, but is also of particular interest for many applications, such as computation, memory, optics, plasmonics. In particular realization of the quantum anomalous Hall effect may lead to the development of low-power-consumption electronics. Indeed, a major constraint for practical use of the quantum Hall effect is limited by the requirement of the quantizing magnetic field. At the same time, the quantum anomalous Hall effect samples exhibit non-dissipative edge quantum transport in a zero magnetic field.