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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Nature of the ferromagnetic-antiferromagnetic transition in Y 1- x La x TiO 3

In this work, we explore the magnetically ordered ground state of the isovalently substituted Mott insulator Y 1- x La x TiO 3 for x≤ 0.3 via single-crystal growth, magnetometry, neutron diffraction, x-ray magnetic circular dichroism, muon spin rotation, and small-angle neutron scattering (SANS). We find that the decrease in the magnetic transition temperature on approaching the ferromagnetic-antiferromagnetic phase boundary at the La concentration xc ≈ 0.3 is accompanied by a strong suppression of both bulk and local ordered magnetic moments, along with a volume wise separation into magnetically ordered and paramagnetic regions. The thermal phase transition does not show conventional second-order behavior since neither a clear signature of dynamic critical behavior nor a power-law divergence of the magnetic correlation length is found for the studied substitution range; this finding becomes increasingly obvious with increasing La substitution. We find no evidence for a spin-glass phase. Finally, from SANS and magnetometry measurements, we discern a crossover from easy-axis to easy-plane magnetocrystalline anisotropy with increasing La substitution. These results indicate complex changes in magnetic structure upon approaching the phase boundary.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Gapless spinons and a field-induced soliton gap in the hyperhoneycomb Cu oxalate framework compound [(C 2 H 5 ) 3 NH] 2 Cu 2 (C 2 O 4 ) 3

Here, we report a detailed study of the specific heat and magnetic susceptibility of single crystals of a spin-liquid candidate: the hyperhoneycomb Cu oxalate framework compound [(C 2 H 5 ) 3 NH] 2 Cu 2 (C 2 O 4 ) 3 . The specific heat shows no anomaly associated with a magnetic transition at low temperatures down to T ~ 180 mK in zero magnetic field. We observe a large linear-in-T contribution to the specific heat γT, γ = 98 (1) mJ / mol K 2 , at low temperatures, indicative of the presence of fermionic excitations despite the Mott insulating state. The low-T specific heat is strongly suppressed by applied magnetic fields H, which induce an energy gap, Δ(H), in the spin-excitation spectrum. We use the four-component relativistic density-functional theory (DFT) to calculate the magnetic interactions, including the Dzyaloshinskii-Moriya antisymmetric exchange, which causes an effective staggered field acting on one copper sublattice. The magnitude and field dependence of the field-induced gap, Δ (H) ∝ H 2/3 , are accurately predicted by the soliton mass calculated from the sine-Gordon model of weakly coupled antiferromagnetic Heisenberg chains with all parameters determined by our DFT calculations. Thus our experiment and calculations are entirely consistent with a model of [(C 2 H 5 ) 3 NH] 2 Cu 2 (C 2 O 4 ) 3 in which anisotropic magnetic exchange interactions due to Jahn-Teller distortion cause one copper sublattice to dimerize, leaving a second sublattice of weakly coupled antiferromagnetic chains. We also show that this model quantitatively accounts for the measured temperature-dependent magnetic susceptibility. Thus [(C 2 H 5 ) 3 NH] 2 Cu 2 (C 2 O 4 ) 3 is a canonical example of a one-dimensional spin-1/2 Heisenberg antiferromagnet and not a resonating-valence-bond quantum spin liquid, as previously proposed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Phase coexistence at the first-order Mott transition revealed by pressure-dependent dielectric spectroscopy of κ - (BEDT-TTF) 2 - Cu 2 (CN) 3

The dimer Mott insulator kappa - (BEDT-TTF) 2 - Cu 2 (CN) 3 can be tuned into metallic and superconducting states on applying pressure of 1.5 kbar and more. We have performed dielectric measurements (7.5 kHz to 5 MHz) on kappa - (BEDT-TTF) 2 - Cu 2 (CN) 3 single crystals as a function of temperature (down to T = 8 K) and pressure (up to p = 4.3 kbar). In addition to the relaxor-like dielectric behavior seen below 50 K at p = 0, that moves toward lower temperatures with pressure, a second peak emerges in ε 1 (T) around T = 15 K. When approaching the insulator-metal boundary, this peak diverges rapidly reaching ε 1 ≈ 10 5 . Our dynamical mean-field theory calculations substantiate that the dielectric catastrophe at the Mott transition is not caused by closing the energy gap, but due to the spatial coexistence of correlated metallic and insulating regions. We discuss the percolative nature of the first-order Mott insulator-to-metal transition in all details.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Orbital-selective Mott phase and non-Fermi liquid in FePS 3

The layered metal phosphorous trisulfide FePS 3 is reported to be a Mott insulator at ambient conditions and to undergo structural and insulator-metal phase transitions under pressure. However, the character of the resulting metallic states has not been understood clearly so far. Here, we theoretically study the phase transitions of FePS 3 using first-principles methods based on density functional theory and embedded dynamical mean field theory. We find that the Mott transition in FePS 3 can be orbital selective, with t 2g states undergoing a correlation-induced insulator-to-metal transition while e g states remain gapped. We show that this orbital-selective Mott phase, which occurs only when nonhydrostatic pressure is used, is a bad metal (or non-Fermi liquid) with large fluctuating moments due to Hund's coupling. Further application of pressure increases the crystal-field splitting and converts the system to a conventional Fermi liquid with low-spin configurations dominant. Finally, our results show that FePS 3 is an example of a system that realizes an orbital-selective Mott phase, allowing tuning between correlated and uncorrelated metallic properties in an accessible pressure range (≤ 18 GPa).

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

An exciton crystal in a moiré excitonic insulator

Strong Coulomb interactions can drive electrons to crystallize into a Wigner lattice. Achieving the bosonic analogue—a crystal of excitons—has remained challenging owing to their short lifetimes and weaker interactions. Here we report the observation of a thermodynamically stable exciton crystal in an excitonic insulator coupled to a moiré potential. Using an electron–hole bilayer composed of a monolayer MoSe 2 and a WS 2 /WSe 2 moiré superlattice, we constructed a tunable extended Bose–Hubbard system with electrical control over exciton and charge doping in thermal equilibrium. Optical spectroscopy revealed spontaneous crystallization of long-lived excitons at one exciton filling per three moiré sites, manifested as strong Umklapp scattering peaks. Exciton transport measurements further showed a pronounced exciton resistance peak at the same filling. When doped away from net charge neutrality, this moiré electron–hole bilayer can host correlated insulating phases in which dipolar excitonic insulators form on top of the background of a hole Mott insulator or generalized Wigner crystals. In conclusion, these findings establish moiré electron–hole bilayers as a versatile platform for realizing correlated crystalline phases of bosons and fermions.

Qi, Ruishi [University of California, Berkeley, CA↗
DOE OSTI2020

Percolation and nanosecond fluctuators in V 2 O 3 films within the metal–insulator transition

Vanadium sesquioxide (V 2 O 3 ) exhibits a metal–insulator transition (MIT) at 160 K between a low temperature, monoclinic, antiferromagnetic Mott insulator and a high temperature, rhombohedral, paramagnetic, metallic phase. In thin films, a percolative transition takes place over a finite temperature range of phase coexistence. We study the fluctuating dynamics of this percolative MIT by measuring voltage noise spectra at both low frequencies (up to 100 kHz) and radio frequencies (between 10 MHz and 1 GHz). Noise intensity quadratic in bias is observed in the MIT region, as expected for resistive fluctuations probed nonperturbatively by the current. The low frequency noise resembles flicker-type 1/f β noise, often taking on the form of Lorentzian noise dominated by a small number of fluctuators as the volume fraction of the insulating phase dominates. Radio frequency noise intensity also quadratic in the bias current allows the identification of resistance fluctuations with lifetimes below 1 ns, approaching timescales seen in non-equilibrium pump–probe studies of the transition. We find quantitative consistency with a model for fluctuations in the percolative fraction. The thermodynamics of the MIT suggests that dominant fluctuations are ones that alter small volumes affecting the connectivity of domain boundaries. This noise serves as a sensitive and nonperturbative probe for the dynamics of switching phenomena in this system.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Metal-insulator transition in V 2 O 3 with intrinsic defects

Vanadium sesquioxide (V 2 O 3 ) is a Mott insulator exhibiting a temperature-dependent metal-insulator transition (MIT) at 165 K accompanied by both a magnetic and structural transition. Although it is expected to be a metal under conventional band theory, electron interactions at low temperature cause it to behave like an insulator, making it difficult to accurately model its electronic properties with standard ab initio methods. As such, accurate theoretical assessments of the MIT with point defects requires special attention to the type of functionals used. In this study, we conclude that the PBE + U functional provides the best compromise between accuracy and efficiency in calculating the properties related to the MIT between low-temperature and high-temperature V 2 O 3 . We use this functional to explore the various influences that intrinsic point defects will have on the MIT in V 2 O 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Band-mixing effects in one-dimensional charge transfer insulators

The low-energy properties of transition metal oxides (TMOs) are governed by the electrons occupying strongly correlated $d$-orbitals that are hybridized with surrounding ligand oxygen $p$ orbitals to varying degrees. Their physics is thus established by a complex interplay between the transition-metal (TM)-ligand hopping $t$, charge transfer energy $\Delta_\mathrm{CT}$, and on-site TM Hubbard repulsion $U$. Here, we study the spectral properties of a one-dimensional (1D) analog of such a $pd$ system, with alternating TM $d$ and ligand anion $p$ orbitals situated along a chain. Using the density matrix renormalization group method, we study the model's single-particle spectral function, x-ray absorption spectrum, and dynamical spin structure factor as a function of $\Delta_\mathrm{CT}$ and $U$. In particular, we present results spanning from the Mott insulating ($\Delta_\mathrm{CT} > U$) to negative charge transfer regime $\Delta_\mathrm{CT} < 0$ to gain a better understanding of the ground and momentum-resolved excited state properties of these different regimes. Our results can guide new studies on TMOs that seek to situate them within the Mott-Hubbard/charge transfer insulator classification scheme.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Achieving environmental stability in an atomically thin quantum spin Hall insulator via graphene intercalation

Atomic monolayers on semiconductor surfaces represent an emerging class of functional quantum materials in the two-dimensional limit — ranging from superconductors and Mott insulators to ferroelectrics and quantum spin Hall insulators. Indenene, a triangular monolayer of indium with a gap of ~ 120 meV is a quantum spin Hall insulator whose micron-scale epitaxial growth on SiC(0001) makes it technologically relevant. However, its suitability for room-temperature spintronics is challenged by the instability of its topological character in air. It is imperative to develop a strategy to protect the topological nature of indenene during ex situ processing and device fabrication. Here we show that intercalation of indenene into epitaxial graphene provides effective protection from the oxidising environment, while preserving an intact topological character. Our approach opens a rich realm of ex situ experimental opportunities, priming monolayer quantum spin Hall insulators for realistic device fabrication and access to topologically protected edge channels.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Twisting the Hubbard model into the momentum-mixing Hatsugai–Kohmoto model

The Hubbard model is a standard theoretical tool for studying materials with strong electron–electron interactions, such as cuprate superconductors. Unfortunately, interaction-driven phenomena, such as a transition into the strongly correlated Mott insulator phase, are difficult to treat with established theoretical techniques. However, the exactly solvable Hatsugai–Kohmoto model displays similar Mott physics. In this work we show how the Hatsugai–Kohmoto model can be deformed continuously into the Hubbard model. The trick is to systematically reintroduce all the momentum mixing that the original Hatsugai–Kohmoto model omits. This can be accomplished by grouping n momenta into a cell and hybridizing them, resulting in the momentum-mixing Hatsugai–Kohmoto model. We recover the Bethe ansatz ground-state energy of the one-dimensional Hubbard model to within 1% from only ten mixed momenta. Overall, the convergence scales as 1/n2 as opposed to the inverse linear behaviour of standard finite-cluster techniques. Our results for a square lattice reproduce all the known features from state-of-the-art simulations also with only a few mixed momenta. Consequently, we believe that the momentum-mixing Hatsugai–Kohmoto model offers an alternative tool for strongly correlated quantum matter.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Hund Physics Landscape of Two-Orbital Systems

Motivated by the recent discovery of superconductivity in infinite-layer nickelates RE 1–δ Sr δ NiO 2 (RE = Nd, Pr), we study the role of Hund coupling J in a quarter-filled two-orbital Hubbard model, which has been on the periphery of the attention. Here, a region of negative effective Coulomb interaction of this model is revealed to be differentiated from three- and five-orbital models in their typical Hund metal active fillings. We identify distinctive regimes including four different correlated metals, one of which stems from the proximity to a Mott insulator, while the other three, which we call “intermediate” metal, weak Hund metal, and valence-skipping metal, from the effect of J being away from Mottness. Defining criteria characterizing these metals is suggested, establishing the existence of Hund metallicity in two-orbital systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Mirror symmetry breaking in a model insulating cuprate

Among the most actively studied issues in the cuprates are the natures of the pseudogap and strange metal states and their relationship to superconductivity. There is general agreement that the low-energy physics of the Mott-insulating parent state is well captured by a two-dimensional spin S = 1/2 antiferromagnetic Heisenberg model. However, recent observations of a large thermal Hall conductivity in several parent cuprates appear to defy this simple model and suggest proximity to a magneto-chiral state that breaks all mirror planes that are perpendicular to the CuO 2 layers. Here we use optical second harmonic generation to directly resolve the point group symmetries of the model parent cuprate Sr 2 CuO 2 Cl 2 . We report evidence of an order parameter that breaks all perpendicular mirror planes and is consistent with a magneto-chiral state in zero magnetic field. Although this order is clearly coupled to the antiferromagnetism, we are unable to realize its time-reversed partner by thermal cycling through the antiferromagnetic transition temperature or by sampling different spatial locations. Finally, this suggests that the order onsets above the Neel temperature and may be relevant to the mechanism of pseudogap formation.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Nano-infrared imaging of metal insulator transition in few-layer 1T-TaS 2

Abstract Among the family of transition metal dichalcogenides, 1T-TaS 2 stands out for several peculiar physical properties including a rich charge density wave phase diagram, quantum spin liquid candidacy and low temperature Mott insulator phase. As 1T-TaS 2 is thinned down to the few-layer limit, interesting physics emerges in this quasi 2D material. Here, using scanning near-field optical microscopy, we perform a spatial- and temperature-dependent study on the phase transitions of a few-layer thick microcrystal of 1T-TaS 2 . We investigate encapsulated air-sensitive 1T-TaS 2 prepared under inert conditions down to cryogenic temperatures. We find an abrupt metal-to-insulator transition in this few-layer limit. Our results provide new insight in contrast to previous transport studies on thin 1T-TaS 2 where the resistivity jump became undetectable, and to spatially resolved studies on non-encapsulated samples which found a gradual, spatially inhomogeneous transition. A statistical analysis suggests bimodal high and low temperature phases, and that the characteristic phase transition hysteresis is preserved down to a few-layer limit.

42 ENGINEERING↗
DOE OSTI2021

Timescales of excited state relaxation in α–RuCl 3 observed by time-resolved two-photon photoemission spectroscopy

The nonequilibrium properties of strongly correlated materials present a target in the search for new phases of matter. It is important to observe the types of excitations that exist in these materials and their associated relaxation dynamics. We have studied the photoexcitations in a spin-orbit assisted Mott insulator α–RuCl 3 using time-resolved two-photon photoemission spectroscopy and transient reflection spectroscopy. We find that photoexcited carriers (doublons) in the upper Hubbard band rapidly relax to Mott-Hubbard excitons on a timescale of less than 200 fs. Subsequently, further relaxation of these lower-energy quasiparticles occurs with an energy-dependent time constant of that ranges from 370 to 600 fs due to exciton cooling. The population of Mott-Hubbard excitons persists for timescales up to several microseconds.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Theoretical study of the crystal and electronic properties of α - RuI 3

The material α-RuCl 3 , with a two-dimensional Ru honeycomb sublattice, has attracted considerable attention because it may be a realization of the Kitaev quantum spin liquid. Recently, a new honeycomb material, α-RuCl 3 , was prepared under moderately high pressure, and it is stable under ambient conditions. However, different from α-RuCl 3 , α-RuI 3 was reported to be a paramagnetic metal without long-range magnetic order down to 0.35 K. Here, the structural and electronic properties of the quasi-two-dimensional α-RuI 3 are theoretically studied. First, based on first-principles density functional theory calculations, the ABC stacking honeycomb-layer R$\bar{3}$ (No. 148) structure is found to be the most likely stacking order for α-RuI 3 along the c axis. Furthermore, both R$\bar{3}$ and P$\bar{3}$1c are dynamically stable because no imaginary frequency modes were obtained in the phononic dispersion spectrum without Hubbard U. Moreover, the different physical behavior of α-RuI 3 compared to α-RuCl 3 can be understood naturally. The strong hybridization between Ru 4d and I 5p orbitals decreases the “effective” atomic Hubbard repulsion, leading the electrons of RuI3 to be less localized than in RuCl 3 . As a consequence, the effective electronic correlation is reduced from Cl to I, leading to the metallic nature of α-RuI 3 . Based on the DFT+U (Ueff=2 eV) plus spin-orbital coupling, we obtained a spin-orbit Mott insulating behavior for α-RuCl 3 and, with the same procedure, a metallic behavior for α-RuI 3 , in good agreement with experimental results. Furthermore, when introducing large (unrealistic) U eff =6 eV, the spin-orbit Mott gap opens in α-RuI 3 as well, supporting the physical picture we are proposing. Our results provide guidance to experimentalists and theorists working on two-dimensional transition metal tri-iodide layered materials.

2-dimensional systems↗
DOE OSTI2020

Nanoscale Imaging and Control of Volatile and Non-Volatile Resistive Switching in VO 2

Control of the metal-insulator phase transition is vital for emerging neuromorphic and memristive technologies. The ability to alter the electrically driven transition between volatile and non-volatile states is particularly important for quantum-materials-based emulation of neurons and synapses. The major challenge of this implementation is to understand and control the nanoscale mechanisms behind these two fundamental switching modalities. In this study, in situ X-ray nanoimaging is used to follow the evolution of the nanostructure and disorder in the archetypal Mott insulator VO 2 during an electrically driven transition. Our findings demonstrate selective and reversible stabilization of either the insulating or metallic phases achieved by manipulating the defect concentration. This mechanism enables us to alter the local switching response between volatile and persistent regimes and demonstrates a new possibility for nanoscale control of the resistive switching in Mott materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Prediction of orbital-selective Mott phases and block magnetic states in the quasi-one-dimensional iron chain Ce 2 O 2 FeSe 2 under hole and electron doping

The recent detailed study of quasi-one-dimensional iron-based ladders, with the 3d iron electronic density n=6, has unveiled surprises, such as orbital-selective phases. However, similar studies for n=6 iron chains are still rare. Here a three-orbital electronic Hubbard model was constructed to study the magnetic and electronic properties of the quasi-one-dimensional n=6 iron chain Ce 2 O 2 FeSe 2 , with focus on the effect of doping. Specifically, introducing the Hubbard U and Hund J H couplings and studying the model via the density matrix renormalization group, we report the ground-state phase diagram varying the electronic density away from n=6. For the realistic Hund coupling J H /U=1/4, several electronic phases were obtained, including a metal, orbital-selective Mott, and Mott insulating phases. Doping away from the parent phase, the competition of many tendencies leads to a variety of magnetic states, such as ferromagnetism, as well as several antiferromagnetic and magnetic “block” phases. In the hole-doping region, two different interesting orbital-selective Mott phases were found: OSMP1 (with one localized orbital and two itinerant orbitals) and OSMP2 (with two localized orbitals and one itinerant orbital). Moreover, charge disproportionation phenomena were found in special doping regions. We argue that our predictions can be tested by simple modifications in the original chemical formula of Ce 2 O 2 FeSe 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗