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At least 271 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Next-generation even-denominator fractional quantum Hall states of interacting composite fermions

The discovery of the fractional quantum Hall state (FQHS) in 1982 ushered a new era of research in many-body condensed matter physics. Among the numerous FQHSs, those observed at even-denominator Landau level filling factors are of particular interest as they may host quasiparticles obeying non-Abelian statistics and be of potential use in topological quantum computing. The even-denominator FQHSs, however, are scarce and have been observed predominantly in low-disorder two-dimensional (2D) systems when an excited electron Landau level is half filled. An example is the well-studied FQHS at filling factor ν = 5/2 which is believed to be a Bardeen-Cooper-Schrieffer-type, paired state of flux-particle composite fermions (CFs). Here, we report the observation of even-denominator FQHSs at ν = 3/10, 3/8, and 3/4 in the lowest Landau level of an ultrahigh-quality GaAs 2D hole system, evinced by deep minima in longitudinal resistance and developing quantized Hall plateaus. Quite remarkably, these states can be interpreted as even-denominator FQHSs of CFs, emerging from pairing of higher-order CFs when a CF Landau level, rather than an electron or a hole Landau level, is half-filled. Our results affirm enhanced interaction between CFs in a hole system with significant Landau level mixing and, more generally, the pairing of CFs as a valid mechanism for even-denominator FQHSs, and suggest the realization of FQHSs with non-Abelian anyons.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Pyrochlore-type lanthanide titanates and zirconates: Synthesis, structural peculiarities, and properties

This contribution provides a thorough examination of the structural characteristics of pyrochlore-type lanthanide titanates and zirconates Ln2Ti2O7 and Ln2Zr2O7, across various length scales. This paper also examines their processing, interesting physical properties (electrical, magnetic, and thermal characteristics), and responses to high pressure and ion irradiation. Brief sections on the elemental oxides' crystal chemistry, pertinent phase diagrams, and energetics of defect formation are also provided. Pyrochlore-type Ln2Ti2O7 and Ln2Zr2O7 stand out as truly multifunctional materials. Moreover, they have emerged as fascinating materials due to magnetic geometrical frustration, arising from the ordering of magnetic Ln3+ and non-magnetic Ti4+ (or Zr4+) cations into separate, interpenetrating lattices of corner-sharing tetrahedra. This results in a diverse array of exotic magnetic ground states, such as spin-ice (e.g., Dy2Ti2O7 or Ho2Ti2O7) or quantum spin ice (e.g., Tb2Ti2O7), observed at both low and room temperatures. They also exhibit varied electrical and electrochemical characteristics. Some members such as Gd2Zr2O7, function as fast ion conductors with a conductivity (σ) of ≈10−2 S·cm−1 at 800 °C and activation energy (Ea) ranging from 0.85 to 1.52 eV, depending on the degree of structural disorder. Others, such as Gd2TiMoO7, are mixed ionic-electronic conductors with σ ≈ 25 S·cm−1 at 1000 °C, making them promising candidate materials for applications in energy conversion and storage devices and oxygen separation membranes. Their exceptionally low thermal conductivity (e.g., κ ∼ 1.1–1.7 W·m−1·K−1 between 700 and 1200 °C for Ln2Zr2O7), close to the glass-like lower limit of highly disordered solids, positions them as valuable materials for thermal barrier coatings. They can also effectively accommodate actinides (e.g., Pu, Np, Cm, Am) in solid solutions and sustain prolonged exposure to radiation due to alpha-decay events, while preserving the integrity of the periodic atomic structure. Proposed as major components in actinide-bearing ceramics, they contribute to the long-term immobilization and disposal of long-lived waste radionuclides from nuclear programs. Some of these properties are displayed simultaneously, opening avenues for new applications. Despite the wealth of data available in the literature, this review highlights the need for a better understanding of order/disorder processes in pyrochlore-type materials and the influence of the structural length scale on their physical and chemical properties. Recent experimental evidence has revealed that pyrochlore short-range structure is far more complex than originally thought. Moreover, pyrochlore local structure is now believed to include short-range, lower symmetry, ordered domains, such as the orthorhombic weberite-type of structure. Notably, short- and long-range structures appear decoupled across different length scales and temperature regimes, and these differences persist even in well-ordered samples. We believe that the pyrochlore structure offers a unique opportunity for examining the interplay between chemical composition, defect chemistry, and properties. In Memoriam: Rodney C. Ewing, Fondly Remembered.

Physics↗
DOE OSTI2024

Anomalous interactions between mesons with nonzero spin and glueballs

Topologically nontrivial fluctuations control the anomalous interactions for the η and η ′ pseudoscalar mesons. We consider the anomalous interactions for mesons with higher spin, the heterochiral nonets with J P C = 1 + − and 2 − + . Under the approximation of a dilute gas of instantons, the mixing angle between nonstrange and strange mesons decreases strongly as J increases, and oscillates in sign. Anomalous interactions also open up new, rare decay channels. For glueballs, anomalous interactions indicate that the X ( 2600 ) state is primarily gluonic. Published by the American Physical Society 2024

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Higher-Form Anomalies on Lattices

We show that generic gapped quantum many-body states which respect an anomalous finite higher-form symmetry have an exponentially small overlap with any short-range entangled (SRE) state. Hence, anomalies of higher-form symmetries enforce $intrinsic$ long-range entanglement, which is in contrast with anomalies of ordinary (0-form) symmetries which are compatible with symmetric SRE states (specifically, symmetric cat states). As an application, we show that the anomalies of strong higher-form symmetries provide a diagnostic for mixed-state topological order in $d \geq 2$ spatial dimensions. We also identify a new (3+1)D intrinsic mixed-state topological order that does not obey remote-detectability by local decoherence of the (3+1)D Toric Code with fermionic loop excitations. This breakdown of remote detectability, as encoded in anomalies of strong higher-form symmetries, provides a partial characterization of intrinsically mixed-state topological order.

Feng, Yitao [Peking University, Beijing (China)] (↗
DOE OSTI2023

Information encoding in the spatial correlations of entangled twin beams

The ability to use the temporal and spatial degrees of freedom of quantum states of light to encode and transmit information is crucial for a robust and efficient quantum network. In particular, the potential offered by the large dimensionality of the spatial degree of freedom remains unfulfilled, as the necessary level of control required to encode information remains elusive. We encode information in the distribution of the spatial correlations of entangled twin beams by taking advantage of their dependence on the angular spectrum of the pump needed for four-wave mixing. We show that the encoded information can only be extracted through joint spatial measurements of the twin beams and not through individual beam measurements and that the temporal quantum correlations are not modified. The ability to engineer the spatial properties of twin beams will enable high-capacity quantum networks and quantum-enhanced spatially resolved sensing and imaging.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Discovery of correlated electron molecular orbital materials using graph representations

Correlated electron molecular orbital (CEMO) materials host emergent electronic states built from molecular orbitals localized over clusters of transition metal ions yet have historically been discovered sporadically and generally been treated as isolated case studies. Here we establish CEMO materials as a systematically discoverable class and introduce a graph-based framework to identify, classify, and organize transition-metal cluster motifs in inorganic solids. Starting from crystal structures in the Materials Project, we construct transition metal connectivity graphs, extract cluster motifs using a bond-cutting algorithm, and determine cluster point groups, effective cluster sublattice dimensionality, and translational symmetry. Applying this approach in a high-throughput screen of 34,548 compounds yields 5,306 cluster-containing materials, including 2,627 stable or metastable compounds with isolated clusters and 984 materials featuring mixed-metal clusters. The resulting dataset reveals symmetry and element dependent trends in cluster formation. By integrating cluster classification with flat band lattice topology and battery-relevant information, we provide further relevant information to multiple scientific communities. The accompanying open dataset, Cluster Finder software, and interactive web platform enable systematic exploration of cluster driven electronic phenomena and establish a general pathway for discovering correlated quantum materials and functional materials with cluster-based or extended metal-metal bonding in inorganic solids.

Akhond, Md. Rajbanul [Department of Chemistry, 800↗
DOE OSTI2022

Electronic structure of α - RuCl 3 by fixed-node and fixed-phase diffusion Monte Carlo methods

Layered material α-RuCl 3 has caught wide attention due to its possible realization of Kitaev's spin liquid and its electronic structure that involves the interplay of electron-electron correlations and spin-orbit effects. Several DFT+U studies have suggested that both electron-electron correlations and spin-orbit effects are crucial for accurately describing the band gap. This work studies the importance of these two effects using fixed-node and fixed-phase diffusion Monte Carlo calculations both in spin-averaged and explicit spin-orbit formalisms. In the latter, the Slater-Jastrow trial function is constructed from two-component spin orbitals using our recent quantum Monte Carlo (QMC) developments and thoroughly tested effective core potentials. Our results show that the gap in the ideal crystal is already accurately described by the spin-averaged case, with the dominant role being played by the magnetic ground state with significant exchange and electron correlation effects. We find qualitative agreement between hybrid DFT, DFT+U, and QMC. In addition, QMC results agree very well with available experiments, and we identify the values of exact Fock exchange mixing that provide comparable gaps. Explicit spin-orbit QMC calculations reveal that the effect of spin-orbit coupling on the gap is minor, of the order of 0.2 eV, which corresponds to the strength of the spin orbit of the Ru atom.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Tracing Long-Lived Atomic Coherences Generated via Molecular Conical Intersections

Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections, which generate coherences between electronic states in molecules. We show with accurate calculations performed on gas-phase methyl iodide that electronic coherences of spin-orbit-split states persist in atomic iodine after dissociation. Our simulation predicts a maximum magnitude of vibronic coherence in the molecular regime of 0.75% of the initially photoexcited state population. Upon dissociation, one-third of this coherence magnitude is transferred to a long-lived atomic coherence where vibrational decoherence can no longer occur. To trace these dynamics, we propose a tabletop experimental approach—heterodyned attosecond four-wave-mixing spectroscopy. This technique can temporally resolve small electronic coherence magnitudes and reconstruct the full complex coherence function via phase cycling. Hence, heterodyned attosecond four-wave-mixing spectroscopy leads the way to a complete understanding and optimal control of spin-orbit-coupled electronic states in photochemistry.

Chemical Physics↗
DOE OSTI2021

Phase diagram of YbZnGaO4 in applied magnetic field

Abstract Recently, Yb-based triangular-lattice antiferromagnets have garnered significant interest as possible quantum spin-liquid candidates. One example is YbMgGaO 4 , which showed many promising spin-liquid features, but also possesses a high degree of disorder owing to site-mixing between the non-magnetic cations. To further elucidate the role of chemical disorder and to explore the phase diagram of these materials in applied field, we present neutron scattering and sensitive magnetometry measurements of the closely related compound, YbZnGaO 4 . Our results suggest a difference in magnetic anisotropy between the two compounds, and we use key observations of the magnetic phase crossover to motivate an exploration of the field- and exchange parameter-dependent phase diagram, providing an expanded view of the available magnetic states in applied field. This enriched map of the phase space serves as a basis to restrict the values of parameters describing the magnetic Hamiltonian with broad application to recently discovered related materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Nonlinear quantum behavior of ultrashort-pulse optical parametric oscillators

The quantum features of ultrashort-pulse optical parametric oscillators (OPOs) are investigated theoretically in the nonlinear regime near and above threshold. Viewing the pulsed OPO as a multimode open quantum system, we rigorously derive a general input-output model that features nonlinear coupling among many cavity (i.e., system) signal modes and a broadband single-pass (i.e., reservoir) pump field. Under appropriate assumptions, our model produces a Lindblad master equation with multimode nonlinear Lindblad operators describing two-photon dissipation and a multimode four-wave-mixing Hamiltonian describing a broadband, dispersive optical cascade, which we show is required to preserve causality. To simplify the multimode complexity of the model, we employ a supermode decomposition to perform numerical simulations in the regime where the pulsed supermodes experience strong single-photon nonlinearity. We find that the quantum nonlinear dynamics induces pump depletion as well as corrections to the below-threshold squeezing spectrum predicted by linearized models. We also observe the formation of non-Gaussian states with Wigner-function negativity and show that the multimode interactions with the pump, both dissipative and dispersive, can act as effective decoherence channels. Finally, we briefly discuss some experimental considerations for potentially observing such quantum nonlinear phenomena with ultrashort-pulse OPOs on nonlinear nanophotonic platforms.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Charge order textures induced by non-linear couplings in a half-doped manganite

Abstract The self-organization of strongly interacting electrons into superlattice structures underlies the properties of many quantum materials. How these electrons arrange within the superlattice dictates what symmetries are broken and what ground states are stabilized. Here we show that cryogenic scanning transmission electron microscopy (cryo-STEM) enables direct mapping of local symmetries and order at the intra-unit-cell level in the model charge-ordered system Nd 1/2 Sr 1/2 MnO 3 . In addition to imaging the prototypical site-centered charge order, we discover the nanoscale coexistence of an exotic intermediate state which mixes site and bond order and breaks inversion symmetry. We further show that nonlinear coupling of distinct lattice modes controls the selection between competing ground states. The results demonstrate the importance of lattice coupling for understanding and manipulating the character of electronic self-organization and that cryo-STEM can reveal local order in strongly correlated systems at the atomic scale.

42 ENGINEERING↗
DOE OSTI2026

Multiple shape coexistence near {sup 118}Sn: First 0+ 3 lifetime measurement

The intruder bands in Sn isotopes, built on the 2p-2h excitation across the Z = 50 proton shell gap, are well-known examples of shape coexistence near the neutron mid-shell region. Spectroscopic signatures for shape coexistence include enhanced E0 transitions between the 0+ band heads. However, the underlying shape coexistence and mixing has been unclear because lifetime information for the excited 0+ states was incomplete in 118Sn. We thus present here the first measurement of the 0+ 3 lifetime in 118Sn using the fast-timing technique following thermal-neutron capture. The observed enhancement in ρ2(E0;0+ 3 → 0+ 2 ) of 150(30) milliunits provides compelling indications for multiple shape coexistence in 118Sn. Additionally, three distinct shapes in 116,118,120Sn naturally emerged in theoretical calculations based on the quantum-number-projected generator coordinate method employing a relativistic energy density functional.

Wu, F.↗
DOE OSTI2020

TurboRVB: A many-body toolkit for ab initio electronic simulations by quantum Monte Carlo

TurboRVB is a computational package for ab initio Quantum Monte Carlo (QMC) simulations of both molecular and bulk electronic systems. The code implements two types of well established QMC algorithms: Variational Monte Carlo (VMC) and diffusion Monte Carlo in its robust and efficient lattice regularized variant. A key feature of the code is the possibility of using strongly correlated many-body wave functions (WFs), capable of describing several materials with very high accuracy, even when standard mean-field approaches [e.g., density functional theory (DFT)] fail. The electronic WF is obtained by applying a Jastrow factor, which takes into account dynamical correlations, to the most general mean-field ground state, written either as an antisymmetrized geminal power with spin-singlet pairing or as a Pfaffian, including both singlet and triplet correlations. This WF can be viewed as an efficient implementation of the so-called resonating valence bond (RVB) Ansatz, first proposed by Pauling and Anderson in quantum chemistry [L. Pauling, The Nature of the Chemical Bond (Cornell University Press, 1960)] and condensed matter physics [P.W. Anderson, Mat. Res. Bull 8, 153 (1973)], respectively. The RVB Ansatz implemented in TurboRVB has a large variational freedom, including the Jastrow correlated Slater determinant as its simplest, but nontrivial case. Moreover, it has the remarkable advantage of remaining with an affordable computational cost, proportional to the one spent for the evaluation of a single Slater determinant. Therefore, its application to large systems is computationally feasible. The WF is expanded in a localized basis set. Several basis set functions are implemented, such as Gaussian, Slater, and mixed types, with no restriction on the choice of their contraction. The code implements the adjoint algorithmic differentiation that enables a very efficient evaluation of energy derivatives, comprising the ionic forces. Thus, one can perform structural optimizations and molecular dynamics in the canonical NVT ensemble at the VMC level. For the electronic part, a full WF optimization (Jastrow and antisymmetric parts together) is made possible, thanks to state-of-the-art stochastic algorithms for energy minimization. In the optimization procedure, the first guess can be obtained at the mean-field level by a built-in DFT driver. The code was efficiently parallelized by using a hybrid MPI-OpenMP protocol, which is also an ideal environment for exploiting the computational power of modern Graphics Processing Unit accelerators.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Hard–Soft Acid–Base Theory Explains Photoexcited Carrier Dynamics in Porphyrin/CNT Nanohybrids: Time-Domain Atomistic Analysis

We employ the fundamental chemical concepts of hard− soft acid−base to formulate general principles governing excited-state dynamics in zinc porphyrin (ZnP)/carbon nanotube (CNT) hybrids for energy photoconversion. Atomistic quantum dynamics simulations demonstrate that electron-withdrawing and donating substituents at the ZnP β-pyrrolic position strongly influence the dynamics. ZnP photoexcitation produces subpicosecond electron transfer (ET) from ZnP to CNT, in agreement with the experiment. Substitutions of CN by H and tBu accelerate the ET. The trend is directly related to the hard−soft acid−base concept because the soft−soft interaction between the t Bu- ZnP acid and the mild CNT base enhances the donor−acceptor coupling. Longer coherence and more active vibrational modes facilitate the ET in t Bu-ZnP/CNT. Electron−hole recombination in CN-ZnP/CNT occurs on a hundred picosecond time scale, nicely corroborated by the experiment. The exciton lifetime is extended beyond a nanosecond by the substitutions. The soft−soft interaction in t Bu-ZnP/ CNT increases the splitting between the highest occupied orbitals of the two subsystems, reduces their mixing, and decreases nonadiabatic coupling between the ground and excited states. Rapid decoherence and involvement of low-frequency vibrations favor longer lifetimes. Our investigation reveals that larger p K a of the β-pyrrolic acid gives rapid ET and slow recombination and provides detailed mechanistic information, essential for future optoelectronic applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Bi-chromatic intensity squeezing using four-wave mixing in 85 Rb vapor

We experimentally investigate four-wave mixing (FWM) in a diamond interaction scheme using 85 Rb vapor, and identify the optimal conditions for joint amplification and relative intensity squeezing of two optical fields: one near the 85 Rb D1 optical transition (λ = 794.6 nm) and the other in the telecom O-band (λ = 1324 nm). We achieved a reduction of relative intensity noise by up to 2.6 ± 0.4 dB compared with the shot noise level, signifying the non-classical quantum correlations. The observed level of intensity squeezing is primarily limited by the available pump laser power, which constrains the achievable FWM gain. Numerical simulations show good agreement with the experimental results.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Insights into the Growth Orientation and Phase Stability of Chemical-Vapor-Deposited Two-Dimensional Hybrid Halide Perovskite Films

Chemical vapor deposition (CVD) offers a large-area, scalable, and conformal growth of perovskite thin films without the use of solvents. Low-dimensional organic–inorganic halide perovskites, with alternating layers of organic spacer groups and inorganic perovskite layers, are promising for enhancing the stability of optoelectronic devices. Moreover, their multiple quantum-well structures provide a powerful platform for tuning excitonic physics. Here, in this work, we show that the CVD process is conducive to the growth of 2D hybrid halide perovskite films. Using butylammonium (BA) and phenylethylammonium (PEA) cations, the growth parameters of BA 2 PbI 4 and PEA 2 PbI 4 and mixed halide perovskite films were first optimized. These films are characterized by well-defined grain boundaries and display characteristic absorption and emission features of the 2D quantum wells. X-ray diffraction (XRD) and a noninteger dimensionality model of the absorption spectrum provide insights into the orientation of the crystalline planes. Unlike BA 2 PbI 4 , temperature-dependent photoluminescence measurements from PEA 2 PbI 4 show a single excitonic peak throughout the temperature range from 20 to 350 K, highlighting the lack of defect states. These results further corroborate the temperature-dependent synchrotron-based XRD results. Furthermore, the nonlinear optical properties of the CVD-grown perovskite films are investigated, and a high third harmonic generation efficiency is observed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Mechanistic Studies of an Iron-Catalyzed Intermolecular C–H Amination Reaction under Catalytic Conditions and Having a Large KIE

The conversion of C–H bonds into amines by nitrene insertion is an attractive transformation since it is both atom- and step-economical, and provides a direct route to functionalizing hydrocarbons. Using an iron catalyst [{( tBu pyrr) 2 pyr}Fe(OEt 2 )] (1-OEt 2 ) (( tBu pyrr) 2 pyr 2– = 3,5- t Bu 2 -bis(pyrrolyl)pyridine), we recently demonstrated the catalytic conversion of weak C–H bonds into secondary amines using aryl azides as the nitrene source [Zars, E.; Angew. Chem., Int. Ed. 2023, 62, e202311749]. Here, we describe detailed mechanistic studies of this intermolecular C–H amination reaction under catalytic conditions. We find by Variable Time Normalization Analysis (VTNA) that the conversion of xanthene (2-H 2 ) and 2,4,6-trimethyl-phenyl azide ( Me 3) catalyzed by 1-OEt 2 is an overall 3/2 order process, being 1 st order in 2-H 2 and half order in Me 3. A kinetic isotope effect study (KIE) using 2-d 2 results in a significant decrease in the rate (KIE = 61(15)), which clearly implicates the C–H insertion step as rate-determining. Furthermore, treatment of 1-OEt 2 with one equivalent of N 3 -2,6- i Pr 2 –C 6 H 3 yields the mixed-valence C–N coupled product [( tBu pyrr) 2 pyrFe-N═C(2,6 i Pr 2 –Ph)═N-(2,6 i Pr 2 –Ph))Fe tBu pyrrpyr(2-H-pyrr)] (5 iPr ). Quantum chemical calculations confirm the electronic structure of the mixed-valence dimer in 5 iPr and rationalize the Hammett correlation by a delicate balance in the dinuclearization of the catalytically active monomers. Calculations further indicate significant tunneling for the pivotal H atom abstraction by the iron-imidyl complex. Combining all these results allows us to propose a mechanism consisting of imido formation in equilibrium with a radical-coupled diiron system, followed by stepwise C–H insertion via a linear H atom abstraction transition state and subsequent radical rebound.

azides↗
DOE OSTI2020

High Performance Green LEDs for Solid State Lighting

The development of white LEDs for solid state lighting (SSL) has been driven in recent years by phosphor converted LEDs (pc-LEDs). However, losses (known as Stokes’ losses) between the blue pump LED and phosphor impose a fundamental efficiency limit of ~300 lm/W on pc-LEDs. White light can also be generated from color mixed LEDs (cm-LEDs), which employ red, green, blue, and amber LEDs and have a fundamental efficiency limit of ~400 lm/W. Efficient group III-nitride materials are used for the blue LED, while efficient group III-phosphide materials are used for the red LED component. Currently, the poor efficiency of green and amber LEDs (i.e. the “green gap”) is the primary limitation for cm-LEDs. Relative to nitride-based blue LEDs, green and amber nitride LEDs suffer from lower radiative recombination rates and higher nonradiative recombination rates, which ultimately lead to reduced internal quantum efficiency (IQE). The IQE represents the portion of all electron-hole recombination events that result in a photon. In addition, long-wavelength LEDs have lower electrical efficiency (EE) compared to their blue counterparts. Addressing the green gap, would ultimately enable cm-LEDs that rival or exceed the performance of pc-LEDs. Our project focused on III-nitride materials growth and characterization, device fabrication and testing, and semiconductor physics to understand efficiency limitations of green LEDs and develop solutions to these challenges. Insights gained during our research has led to novel long-wavelength LED designs which will enable efficient solid-state lighting.

30 DIRECT ENERGY CONVERSION↗