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At least 1,351 records · Page 75
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Exciton valley depolarization in monolayer transition-metal dichalcogenides

The valley degree of freedom is a sought-after quantum number in monolayer transition-metal dichalcogenides. Similar to optical spin orientation in semiconductors, the helicity of absorbed photons can be relayed to the valley (pseudospin) quantum number of photoexcited electrons and holes. Also similar to the quantum-mechanical spin, the valley quantum number is not a conserved quantity. Valley depolarization of excitons in monolayer transition-metal dichalcogenides due to long-range electron-hole exchange typically takes a few ps at low temperatures. Exceptions to this behavior are monolayers MoSe 2 and MoTe 2 wherein the depolarization is much faster. Here, we elucidate the enigmatic anomaly of these materials, finding that it originates from Rashba-induced coupling of the dark and bright exciton branches next to their degeneracy point. When photoexcited excitons scatter during their energy relaxation between states next to the degeneracy region, they reach the light cone after losing the initial helicity. The valley depolarization is not as fast in monolayers WSe 2 , WS 2 , and MoS 2 , wherein the degeneracy is absent resulting in negligible Rashba-induced coupling between bright and dark excitons.

25 ENERGY STORAGE↗
DOE OSTI2025

Physics-Driven Construction of Compact Primitive Gaussian Density Fitting Basis Sets

We present a model-assisted density fitting (MADF) basis set generator, an algorithm for generating primitive atomic Gaussian density fitting (DF) basis sets (DFBSs) from a contracted Gaussian orbital basis set (OBS). The MADF algorithm produces DFBSs suitable for accurate robust DF approximation of 2-particle interactions in mean-field and correlated electronic structures. The algorithm is designed to (a) saturate the OBS product space by a large regularized set of primitive solid-harmonic Gaussian shells with nonuniform distribution of exponents, followed by (b) pruning of the shells according to their contributions to the 2- body energy of a correlated atomic ensemble. Building the DFBS generator model almost exclusively on mathematical and physical principles allows one to limit the number of parameters that control the density fitting error to three, with a single set of parameters sufficient for computations with all basis cardinal numbers, with and without correlation of core electrons, with and without scalar and spin-dependent relativistic effects, spanning almost all of the Periodic Table. Performance assessment included basis sets up to quadruple-ζ quality from several major basis set families, using molecules composed of main-group, d-block, and f-block elements. The resulting DF errors in Hartree−Fock and second-order MP2 energies (with relativistic all-electron treatments, when appropriate) were on the order of 20 and 10 μE h per electron, respectively.

Approximation↗
DOE OSTI2022

Orbital selective Kondo effect in heavy fermion superconductor UTe2

Abstract Heavy fermion systems emerge from the collective Kondo effect, and their superconductivity can serve as a promising platform for realizing next-generation quantum technologies. However, it has been a great challenge to explore many-body effects in heavy fermion systems with ab-initio approaches. We computed the electronic structure of UTe 2 without purposive judgements, such as intentional selection of on-site Coulomb interaction and disregarding spin-orbit coupling. We show that U-5 f electrons are highly localized in the paramagnetic normal state, giving rise to the Kondo effect. It is also found that the hybridization between U-5 f and U-6 d predominantly in the orthorhombic a b -plane is responsible for the high-temperature Kondo effect. In contrast, the hybridization between U-5 f and Te-5 p along the c -axis manifests the Kondo scattering at a much lower temperature, which could be responsible for the low-temperature upturn of the c -axis resistivity. Our results show that the electron correlation in UTe 2 is orbital selective, which naturally elucidates the recent experimental observations of anomalous temperature dependence of resistivity. Furthermore, we suggest that the Kondo effect is suppressed at high pressure owing to weak localization of magnetic moments, which results from enhanced U-5 f electron hopping. Our discovery provides significant insight toward understanding anisotropic quantum behavior including selective re-entrant superconductivity in heavy fermion UTe 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

On the origin of magnetic anisotropy in 4f-free ferromagnets based on the CaCu 5 structure *

Using first-principles calculations, we investigate the origin of magnetocrystalline anisotropy in a series of 4f-electron-free intermetallics with CaCu 5 -based structures: YCo 5 , YCo 4 B, and Y 3 Co 13 B 2 . The electronic structure of these compounds is characterized by a set of narrow 3d bands near the Fermi level. In YCo 5 the easy-axis anisotropy originates primarily in the spin–orbit coupling-induced mixing of the electronic states with Co d x 2 -y 2 and d xy character. The analysis of k-resolved anisotropy shows that positive contributions accumulate from the entire Brillouin zone but are particularly large near the k z = 0 plane. The analysis of the single-site and two-site terms reveals a large positive single-site contribution to the magnetocrystalline anisotropy from the Co atoms on the honeycomb sublattice, along with two-site contributions from both honeycomb and kagome sublattices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

The Electronic Structure of Zirconium and Hafnium Monochalcogenides

High-level ab initio CCSD(T) and spin–orbit icMRCI+Q calculations were used to predict potential energy curves (PECs) for the lowest-lying states of ZrO, ZrS, HfO, and HfS. The prediction of the ground state is basis set dependent at the icMRCI+Q level for ZrO and ZrS due to the small singlet–triplet splitting between the lowest 1 Σ + and 3 Δ states. CCSD(T) with a spin orbit correction predicted the 1 Σ + ground state in agreement with experiment. New all-electron basis sets were developed for Hf to improve the results over those predicted by use of effective core potentials (ECPs) that subsume the 4f electrons into the definition of the core. The use of the new DK-4f basis sets rather than ECPs became more important for HfO and HfS where there is a lack of a good core–valence separation. icMRCI+Q, CCSD(T), and DFT calculations for the spectroscopic parameters of ZrO, ZrS, HfO, and HfS were benchmarked with available experimental data. Bond dissociation energies (BDEs) of these four systems were calculated at the Feller–Peterson–Dixon (FPD) level to be 762.1 (ZrO), 543.5 (ZrS), 803.8 (HfO), and 575.1 kJ/mol (HfS), in excellent agreement with experiment. The HfS BDE was remeasured using the R3PI method, providing an updated experimental measurement of D 0 (HfS) = 5.978 ± 0.002 eV = 576.8 ± 0.2 kJ/mol. This experimental value, combined with experimental measurements of the ionization energies of Hf and HfS, gives the cationic BDE of D 0 (Hf + -S) = 5.124 ± 0.002 eV = 494.4 ± 0.2 kJ/mol.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Detection of a pair density wave state in UTe2

Abstract Spin-triplet topological superconductors should exhibit many unprecedented electronic properties, including fractionalized electronic states relevant to quantum information processing. Although UTe 2 may embody such bulk topological superconductivity 1–11 , its superconductive order parameter Δ( k ) remains unknown 12 . Many diverse forms for Δ( k ) are physically possible 12 in such heavy fermion materials 13 . Moreover, intertwined 14,15 density waves of spin (SDW), charge (CDW) and pair (PDW) may interpose, with the latter exhibiting spatially modulating 14,15 superconductive order parameter Δ( r ), electron-pair density 16–19 and pairing energy gap 17,20–23 . Hence, the newly discovered CDW state 24 in UTe 2 motivates the prospect that a PDW state may exist in this material 24,25 . To search for it, we visualize the pairing energy gap with μeV-scale energy resolution using superconductive scanning tunnelling microscopy (STM) tips 26–31 . We detect three PDWs, each with peak-to-peak gap modulations of around 10 μeV and at incommensurate wavevectors P i =1,2,3 that are indistinguishable from the wavevectors Q i =1,2,3 of the prevenient 24 CDW. Concurrent visualization of the UTe 2 superconductive PDWs and the non-superconductive CDWs shows that every P i : Q i pair exhibits a relative spatial phase δϕ ≈ π. From these observations, and given UTe 2 as a spin-triplet superconductor 12 , this PDW state should be a spin-triplet PDW 24,25 . Although such states do exist 32 in superfluid 3 He, for superconductors, they are unprecedented.

Science & Technology - Other Topics↗
DOE OSTI2024

Adsorption of Ag, Au, Cu, and Ni on MoS 2 : theory and experiment

Abstract Here, we present results of a computational and experimental study of adsorption of various metals on MoS2. In particular, we analyzed the binding mechanism of four metallic elements (Ag, Au, Cu, Ni) on MoS2. Among these elements, Ni exhibits the strongest binding and lowest mobility on the surface of MoS2. On the other hand, Au and Ag bond very weakly to the surface and have very high mobilities. Our calculations for Cu show that its bonding and surface mobility are between these two groups. Experimentally, Ni films exhibit a composition characterized by randomly oriented nanoscale clusters. This is consistent with the larger cohesive energy of Ni atoms as compared with their binding energy with MoS2, which is expected to result in 3D clusters. In contrast, Au and Ag tend to form atomically flat plateaued structures on MoS2, which is contrary to their larger cohesive energy as compared to their weak binding with MoS2. Cu displays a surface morphology somewhat similar to Ni, featuring larger nanoscale clusters. However, unlike Ni, in many cases Cu exhibits small plateaued surfaces on these clusters. This suggests that Cu likely has two competing mechanisms that cause it to span the behaviors seen in the Ni and Au/Ag film morphologies. These results indicate that calculations of the initial binding conditions could be useful for predicting film morphologies. In addition, out calculations show that the adsorption of adatoms with odd electron number like Ag, Au, and Cu results in 100% spin-polarization and integer magnetic moment of the system. Adsorption of Ni adatoms, with even electron number, does not induce a magnetic transition.

Harms, Haley↗
DOE OSTI2024

Particle-Hole Asymmetric Ferromagnetism and Spin Textures in the Triangular Hubbard-Hofstadter Model

In a lattice model subject to a perpendicular magnetic field, when the lattice constant is comparable to the magnetic length, one enters the “Hofstadter regime,” where continuum Landau levels become fractal magnetic Bloch bands. Strong mixing between bands alters the nature of the resulting quantum phases compared to the continuum limit; lattice potential, magnetic field, and Coulomb interaction must be treated on equal footing. Using determinant quantum Monte Carlo and density matrix renormalization group techniques, we study this regime numerically in the context of the Hubbard-Hofstadter model on a triangular lattice. In the field-filling phase diagram, we find a broad wedge-shaped region of ferromagnetic ground states for filling factor ν ≤ 1 , bounded below by filling factor ν = 1 and bounded above by half filling the lowest Hofstadter subband. We observe signatures of SU(2) quantum Hall ferromagnetism at filling factors ν = 1 and ν = 3 . The phases near ν = 1 are particle-hole asymmetric, and we observe a rapid decrease in ground-state spin polarization consistent with the formation of skyrmions only on the electron doped side. At large fields, above the ferromagnetic wedge, we observe a low-spin metallic region with spin correlations peaked at small momenta. We argue that the phenomenology of this region likely results from exchange interaction mixing fractal Hofstadter subbands. The phase diagram derived beyond the continuum limit points to a rich landscape to explore interaction effects in magnetic Bloch bands. Published by the American Physical Society 2024

Ding, Jixun K.↗
DOE OSTI2021

Infrared Light-Emitting Devices from Antenna-Coupled Luttinger Liquid Plasmons In Carbon Nanotubes

Electrically driven light-emitting devices provide highly energy-efficient lighting at visible wavelengths, and they have transformed photonic and electronic lighting applications. Efficient infrared light-emitting devices, however, have been challenging because band gap emission from semiconductors becomes inefficient in the mid-infrared to far-infrared spectral range. Here, in this paper, we investigate infrared light-emitting devices (IRLEDs) based on Luttinger liquid (LL) plasmons in one-dimensional (1D) metallic carbon nanotubes. Elementary excitations in LL are characterized by collective charge and spin excitations, i.e., plasmons and spinons. Consequently, electrons injected into the nanotubes transform efficiently into LL plasmons, a hybrid excitation of electromagnetic fields and electrons. We design nanoantennas coupled to the carbon nanotube to radiate LL plasmons into the far field. LL-based IRLEDs can be designed to selectively emit at wavelengths across the far- and mid-infrared spectra. An electrical-to-optical power conversion efficiency up to 3.2% may be achieved. Such efficient and narrowband LL-based IRLEDs can enable novel infrared nanophotonic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Entanglement Witness for Indistinguishable Electrons Using Solid-State Spectroscopy

Characterizing entanglement in quantum materials is crucial for advancing next-generation quantum technologies. Despite recent strides in witnessing entanglement in magnetic materials with distinguishable spin modes, quantifying entanglement in systems formed by indistinguishable electrons remains a formidable challenge. To solve this problem, we introduce a method to extract various four-fermion correlations by analyzing the nonlinearity in resonant inelastic x-ray scattering spectra. These correlations constitute the primary components of the cumulant two-particle reduced density matrix. We further derive bounds for its eigenvalues and demonstrate the linear scaling with fermionic entanglement depth, providing a reliable witness for entanglement. Using the material-relevant strongly correlated models as examples, we show how this entanglement witness can efficiently quantify multipartite entanglement across different phase regions, highlighting its advantage over quantum Fisher information. Published by the American Physical Society 2025

Liu, Tongtong (ORCID:0000000295324061)↗
DOE OSTI2023

Two-dimensional spin systems in PECVD-grown diamond with tunable density and long coherence for enhanced quantum sensing and simulation

Systems of spins engineered with tunable density and reduced dimensionality enable a number of advancements in quantum sensing and simulation. Defects in diamond, such as nitrogen-vacancy (NV) centers and substitutional nitrogen (P1 centers), are particularly promising solid-state platforms to explore. However, the ability to controllably create coherent, two-dimensional spin systems and characterize their properties, such as density, depth confinement, and coherence, is an outstanding materials challenge. We present a refined approach to engineer dense (≳1 ppm ∙ nm), 2D nitrogen, and NV layers in diamond using delta-doping during plasma-enhanced chemical vapor deposition epitaxial growth. We employ both traditional materials techniques, e.g., secondary ion mass spectrometry, alongside NV spin decoherence-based measurements to characterize the density and dimensionality of the P1 and NV layers. We find P1 densities of 5–10 ppm ∙ nm, NV densities between 1 and 3.5 ppm ∙ nm tuned via electron irradiation dosage, and depth confinement of the spin layer down to 1.6 nm. We also observe high (up to 0.74) ratios of NV to P1 centers and reproducibly long NV coherence times, dominated by dipolar interactions with the engineered P1 and NV spin baths.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Anomalous electrical transport behavior in the vicinity of the first-order magnetostructural transition in the giant magnetocaloric Gd 4 ScGe 4

Here, magnetic, specific heat, and electrical transport measurements of Gd 4 ScGe 4 single crystals reveal sharp, discontinuous, nearly anhysteretic first-order magnetostructural transformation at $T_C$ = 63 K. The electrical resistivity exhibits two distinct regions where it increases with decreasing temperature: between $T_C$ and 120 K, as well as below 3 K; electronic transport remains conventionally metallic at all other measured temperatures, up to 325 K. The dispersion of charge carriers due to electron-paramagnon scattering is the likely reason for the observed anomalous transport above $T_C$. Additionally, the existence of intermediate lattice states near the transition recognized by the spike in the interslab Ge-Ge distances is expected to reduce the mean free path of the electrons contributing to the unusual behavior of the electrical resistivity between $T_C$ and 120 K. Beyond conventional electronic and lattice terms, the third component of likely magnetic origin contributes to the low-temperature heat capacity; the presence of spin waves may be responsible for the increased electron-magnon scattering below 3 K. Minor magnetocrystalline anisotropy is observed with the b axis as the easy magnetization axis in Gd 4 ScGe 4 . A negative deviation from linearity in the temperature dependence of the inverse magnetic susceptibility is detected below 150 K.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Magnon damping and mode softening in quantum double-exchange ferromagnets

We present a comprehensive analysis of the magnetic excitations and electronic properties of fully quantum double-exchange ferromagnets, i.e. systems where ferromagnetic (FM) ordering emerges from the competition between spin, charge, and orbital degrees of freedom, but without the canonical approximation of using classical localized spins. Specifically, we investigate spin excitations within the Kondo lattice-like model, as well as a two-orbital Hubbard Hamiltonian in proximity to the orbital-selective Mott phase. Computational analysis of the magnon dispersion, damping, and spectral weight within these models reveals unexpected phenomena, such as magnon mode softening and the anomalous decoherence of magnetic excitations as observed in earlier experimental efforts, but explained here without the use of the phononic degrees of freedom. We show that these effects are intrinsically linked to incoherent spectral features near the Fermi level, which arise due to the quantum nature of the local (on-site) triplets. This incoherent spectrum leads to a Stoner-like continuum on which spin excitations scatter, governing magnon lifetime and strongly influencing the dynamical spin structure factor. Our study explores the transition from coherent to incoherent magnon spectra by varying the electron density. Furthermore, we demonstrate that the magnitude of the localized spin mitigates decoherence by suppressing the incoherent spectral contributions near the Fermi level. We also discuss the effective J 1 –J 2 spin Hamiltonian, which can accurately describe the large doping region characterized by the magnon-mode softening. Finally, we show that this behavior is also present in multiorbital models with partially filled orbitals, namely, in systems without localized spin moments, provided that the model is in a strong coupling regime. Our results potentially have far-reaching implications for understanding FM ordering in various multi-band systems. These findings establish a previously unknown direct connection between the electronic correlations of those materials and spin excitations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Spin-State and Reorganization Energy Considerations for Metal-Centered Photoredox Catalysis

Transition-metal complexes featuring metal-centered excited states have recently emerged as mechanistically distinct platforms for selective photochemistry, including photoredox catalysis. Among these, Co(III) complexes have demonstrated productive photoinduced electron transfer via the 3 T 1 metal-centered state. In contrast, photoreactivity from the 5 T 2 metal-centered state in Fe(II) polypyridyl complexes remains limited. Building on our prior report concerning reactivity associated with the 5 T 2 state in [Fe(tren(py) 3 )] 2+ (tren(py) 3 = tris(2-pyridylmethyliminoethyl)-amine), we introduced stronger-field ligands in an effort to increase excited-state energies of Fe(II) polypyridyl complexes and enhance reactivity. Despite achieving nanosecond-scale excited-state lifetimes and favorable thermodynamic driving forces, no photoreactivity was observed. Reinvestigation of the observations previously reported for [Fe(tren(py) 3 )] 2+ revealed interactions between the metal complex and the substrate in their respective ground states that mimicked dynamic quenching of the chromophore, prompting a reassessment of mechanistic considerations inherent in leveraging reductive chemistry from the 5 T 2 excited state of Fe(II). Our analysis indicates that electron transfer from the 5 T 2 excited state of a low-spin d6 metal is subject to significant barriers both in terms of reorganization energies and spin conservation that undermines its ability to act as an electron donor for photoredox catalysis. In contrast, ligand fields that are sufficient to stabilize the 3 T 1 excited state have available to them numerous spin-allowed and, in certain cases, near-barrierless pathways to engage in excited-state electron transfer (both oxidative and reductive depending on the identity of the metal). These results highlight the critical role of spin-state changes and their associated reorganization energy requirements in metal-centered photoredox catalysis.

charge transfer↗
DOE OSTI2023

Anomalous magnetoresistance by breaking ice rule in Bi2Ir2O7/Dy2Ti2O7 heterostructure

Abstract While geometrically frustrated quantum magnets host rich exotic spin states with potentials for revolutionary quantum technologies, most of them are necessarily good insulators which are difficult to be integrated with modern electrical circuit. The grand challenge is to electrically detect the emergent fluctuations and excitations by introducing charge carriers that interact with the localized spins without destroying their collective spin states. Here, we show that, by designing a Bi 2 Ir 2 O 7 /Dy 2 Ti 2 O 7 heterostructure, the breaking of the spin-ice rule in insulating Dy 2 Ti 2 O 7 leads to a charge response in the conducting Bi 2 Ir 2 O 7 measured as anomalous magnetoresistance during the field-induced Kagome ice-to-saturated ice transition. The magnetoresistive anomaly also captures the characteristic angular and temperature dependence of this ice-rule-breaking transition, which has been understood as magnetic monopole condensation. These results demonstrate a novel heteroepitaxial approach for electronically probing the transition between exotic insulating spin states, laying out a blueprint for the metallization of frustrated quantum magnets.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Novel phenomena in transition-metal oxide thin films and heterostructures with strong correlations and spin-orbit coupling

Transition-metal oxides have been a central subject of condensed matter physics for decades. In addition to novel electronic states driven by the influence of strong correlation, relativistic spin-orbit coupling effects have recently attracted much attention for their potential to explore topological phenomena. Here, in this article, we review various experimental and theoretical studies on transition-metal oxides with focus on thin films and heterostructures where their physics is much influenced by correlation effects and spin-orbit coupling. The combination of the heterostructure geometry together with correlation and topology leads to a variety of novel states here reviewed. We also discuss perspectives for future research in this broad promising area.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Unconventional Anomalous Hall Effect Driven by Self‐Intercalation in Covalent 2D Magnet Cr 2 Te 3

Covalent 2D magnets such as Cr 2 Te 3 , which feature self-intercalated magnetic cations located between monolayers of transition-metal dichalcogenide material, offer a unique platform for controlling magnetic order and spin texture, enabling new potential applications for spintronic devices. Here, it is demonstrated that the unconventional anomalous Hall effect (AHE) in Cr 2 Te 3 , characterized by additional humps and dips near the coercive field in AHE hysteresis, originates from an intrinsic mechanism dictated by the self-intercalation. This mechanism is distinctly different from previously proposed mechanisms such as topological Hall effect, or two-channel AHE arising from spatial inhomogeneities. Crucially, multiple Weyl-like nodes emerge in the electronic band structure due to strong spin-orbit coupling, whose positions relative to the Fermi level is sensitively modulated by the canting angles of the self-intercalated Cr cations. These nodes contribute strongly to the Berry curvature and AHE conductivity. This component competes with the contribution from bands that are less affected by the self-intercalation, resulting in a sign change in AHE with temperature and the emergence of additional humps and dips. The findings provide compelling evidence for the intrinsic origin of the unconventional AHE in Cr 2 Te 3 and further establish self-intercalation as a control knob for engineering AHE in complex magnets.

2D magnets↗