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At least 721 records · Page 40
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DOE OSTI2022

Control of electronic topology in a strongly correlated electron system

It is becoming increasingly clear that breakthrough in quantum applications necessitates materials innovation. In high demand are conductors with robust topological states that can be manipulated at will. This is what we demonstrate in the present work. We discover that the pronounced topological response of a strongly correlated “Weyl-Kondo” semimetal can be genuinely manipulated—and ultimately fully suppressed—by magnetic fields. We understand this behavior as a Zeeman-driven motion of Weyl nodes in momentum space, up to the point where the nodes meet and annihilate in a topological quantum phase transition. The topologically trivial but correlated background remains unaffected across this transition, as is shown by our investigations up to much larger fields. Our work lays the ground for systematic explorations of electronic topology, and boosts the prospect for topological quantum devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Triangular lattice quantum dimer model with variable dimer density

Abstract Quantum dimer models are known to host topological quantum spin liquid phases, and it has recently become possible to simulate such models with Rydberg atoms trapped in arrays of optical tweezers. Here, we present large-scale quantum Monte Carlo simulation results on an extension of the triangular lattice quantum dimer model with terms in the Hamiltonian annihilating and creating single dimers. We find distinct odd and even $${{\mathbb{Z}}}_{2}$$ Z 2 spin liquids, along with several phases with no topological order: a staggered crystal, a nematic phase, and a trivial symmetric phase with no obvious broken symmetry. We also present dynamic spectra of the phases, and note implications for experiments on Rydberg atoms.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Kagome qubit ice

Abstract Topological phases of spin liquids with constrained disorder can host a kinetics of fractionalized excitations. However, spin-liquid phases with distinct kinetic regimes have proven difficult to observe experimentally. Here we present a realization of kagome spin ice in the superconducting qubits of a quantum annealer, and use it to demonstrate a field-induced kinetic crossover between spin-liquid phases. Employing fine control over local magnetic fields, we show evidence of both the Ice-I phase and an unconventional field-induced Ice-II phase. In the latter, a charge-ordered yet spin-disordered topological phase, the kinetics proceeds via pair creation and annihilation of strongly correlated, charge conserving, fractionalized excitations. As these kinetic regimes have resisted characterization in other artificial spin ice realizations, our results demonstrate the utility of quantum-driven kinetics in advancing the study of topological phases of spin liquids.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Engineering the formation of spin-defects from first principles

The full realization of spin qubits for quantum technologies relies on the ability to control and design the formation processes of spin defects in semiconductors and insulators. We present a computational protocol to investigate the synthesis of point-defects at the atomistic level, and we apply it to the study of a promising spin-qubit in silicon carbide, the divacancy (VV). Our strategy combines electronic structure calculations based on density functional theory and enhanced sampling techniques coupled with first principles molecular dynamics. We predict the optimal annealing temperatures for the formation of VVs at high temperature and show how to engineer the Fermi level of the material to optimize the defect’s yield for several polytypes of silicon carbide. Our results are in excellent agreement with available experimental data and provide novel atomistic insights into point defect formation and annihilation processes as a function of temperature.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Mott insulators with boundary zeros

The topological classification of electronic band structures is based on symmetry properties of Bloch eigenstates of single-particle Hamiltonians. In parallel, topological field theory has opened the doors to the formulation and characterization of non-trivial phases of matter driven by strong electron-electron interaction. Even though important examples of topological Mott insulators have been constructed, the relevance of the underlying non-interacting band topology to the physics of the Mott phase has remained unexplored. Here, we show that the momentum structure of the Green’s function zeros defining the “Luttinger surface" provides a topological characterization of the Mott phase related, in the simplest description, to the one of the single-particle electronic dispersion. Considerations on the zeros lead to the prediction of new phenomena: a topological Mott insulator with an inverted gap for the bulk zeros must possess gapless zeros at the boundary, which behave as a form of “topological antimatter” annihilating conventional edge states. Placing band and Mott topological insulators in contact produces distinctive observable signatures at the interface, revealing the otherwise spectroscopically elusive Green’s function zeros.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Extracting the femtometer structure of strange baryons using the vacuum polarization effect

Abstract One of the fundamental goals of particle physics is to gain a microscopic understanding of the strong interaction. Electromagnetic form factors quantify the structure of hadrons in terms of charge and magnetization distributions. While the nucleon structure has been investigated extensively, data on hyperons are still scarce. It has recently been demonstrated that electron-positron annihilations into hyperon-antihyperon pairs provide a powerful tool to investigate their inner structure. We present a method useful for hyperon-antihyperon pairs of different types which exploits the cross section enhancement due to the effect of vacuum polarization at theJ/ψresonance. Using the 10 billionJ/ψevents collected with the BESIII detector, this allows a precise determination of the hyperon structure function. The result is essentially a precise snapshot of the$$\bar{\Lambda }{\Sigma }^{0}\,(\Lambda {\bar{\Sigma }}^{0})$$ Λ ¯ Σ 0 ( Λ Σ ¯ 0 ) transition process, encoded in the transition form factor ratio and phase. Their values are measured to beR = 0.860 ± 0.029(stat.) ± 0.015(syst.),$$\Delta {\Phi }_{\bar{\Lambda }{\Sigma }^{0}}=(1.011\pm 0.094({{\rm{stat.}}})\pm 0.010({{\rm{syst.}}}))\,{{\rm{r}}}ad$$ Δ Φ Λ ¯ Σ 0 = ( 1.011 ± 0.094 ( stat. ) ± 0.010 ( syst. ) ) r a d and$$\Delta {\Phi }_{\Lambda {\bar{\Sigma }}^{0}}=(2.128\pm 0.094({{\rm{stat.}}})\pm 0.010({{\rm{syst.}}}))\,{{\rm{r}}}ad$$ Δ Φ Λ Σ ¯ 0 = ( 2.128 ± 0.094 ( stat. ) ± 0.010 ( syst. ) ) r a d . Furthermore, charge-parity (CP) breaking is investigated in this reaction and found to be consistent with CP symmetry.

Science & Technology - Other Topics↗
DOE OSTI2025

Coherent phonon flatband generated in GaAs/AlAs superlattices via layer-selective optical pumping

Flatbands, characterized by their dispersionless energy levels in electronic, magnetic, and phononic systems, hold substantial potential for advancements in electronics and quantum information processing. Most flatbands exist in thermal equilibrium and cannot be easily created or annihilated externally, limiting their flexibility as switchable knobs for use in microelectronics and quantum applications. In our work, we demonstrate the generation of a coherent phonon flatband in a GaAs/AlAs superlattice using 800 nm femtosecond laser pulses. This coherent phonon flatband does not correspond to a phonon eigenmode at equilibrium and exhibits strong coupling with two branches of coherently excited longitudinal phonon modes. With molecular dynamics simulations, we show more generally that the coherent phonon flatband can be induced by coherently and spatially modulated optical excitations of superlattice structures. Our results highlight a pathway for coherent phonon flatband creation in the time domain that can be generalized to various superlattice systems, potentially inspiring the realization of coherent flatband generation of other quasiparticles.

Condensed-matter physics↗
DOE OSTI2026

Violation of detailed balance in non-equilibrium magnons observed by inelastic neutron scattering

Traditional inelastic neutron scattering (INS) characterizes excitations—such as phonons and magnons—in condensed matter systems at thermodynamic equilibrium. However, the most intriguing and puzzling many-body effects in open quantum systems often emerge from dissipative dynamics that are inherently out of equilibrium. Here, we use a combination of laser pumping and INS to experimentally observe long-lived nonequilibrium magnons in a two-dimensional (2D) square-lattice Heisenberg antiferromagnet. These nonequilibrium magnons manifest themselves as a violation of detailed balance in the dynamic structure factor and reach steady states under periodic driving, analogous to nonequilibrium steady states in driven dissipative systems. Furthermore, we show that the violation of detailed balance reflects the quantum-mechanical nature of the underlying dynamical system, where out-of-time-ordered correlations of creation and annihilation operators do not satisfy commutation relations. The in operando INS technique developed here provides a new approach to studying nonequilibrium magnons in prototypical 2D quantum magnets and can be extended to other systems, including one-dimensional spin chains and topological many-body spin systems, where nonequilibrium effects are widespread and rich in discovery potential.

Hua, Chengyun [Oak Ridge National Laboratory (ORNL↗
DOE OSTI2022

Tomographic detection of photon pairs produced from high-energy X-rays for the monitoring of radiotherapy dosing

Measuring the radiation dose reaching a patient’s body is difficult. Here we report a technique for the tomographic reconstruction of the location of photon pairs originating from the annihilation of positron–electron pairs produced by high-energy X-rays travelling through tissue. We used Monte Carlo simulations on pre-recorded data from tissue-mimicking phantoms and from a patient with a brain tumour to show the feasibility of this imaging modality, which we named ‘pair-production tomography’, for the monitoring of radiotherapy dosing. We simulated three image-reconstruction methods, one applicable to a pencil X-ray beam scanning through a region of interest, and two applicable to the excitation of tissue volumes via broad beams (with temporal resolution sufficient to identify coincident photon pairs via filtered back projection, or with higher temporal resolution sufficient for the estimation of a photon’s time-of-flight). In addition to the monitoring of radiotherapy dosing, we show that image contrast resulting from pair-production tomography is highly proportional to the material’s atomic number. The technique may thus also allow for element mapping and for soft-tissue differentiation.

62 RADIOLOGY AND NUCLEAR MEDICINE↗
DOE OSTI2020

Spatial separation of triplet excitons drives endothermic singlet fission

Molecules that undergo singlet fission, converting singlet excitons into pairs of triplet excitons, have potential as photovoltaic materials. The possible advantages of endothermic singlet fission (enhanced use of photon energy and larger triplet energies for coupling with common absorbers) motivated us to assess the role of exciton delocalization in the activation of this process. Here we report the synthesis of a series of linear perylene oligomers that undergo endothermic singlet fission and have endothermicities in the range 5-10 kBT at room temperature in solution. We study these compounds using transient spectroscopy and modelling to unravel the singlet and triplet dynamics. We show that the minimal number of coupled chromophores needed to undergo endothermic singlet fission is three, which provides sufficient statistical space for triplet excitons to separate and avoid annihilation - and a subsequent fast return to the singlet state. Our data additionally suggest that torsional motion of chromophores about the molecular axis following triplet-pair separation contributes to the increase in entropy, thus lengthening the triplet lifetime in longer oligomers.

14 SOLAR ENERGY↗
DOE OSTI2021

Subcycle contact-free nanoscopy of ultrafast interlayer transport in atomically thin heterostructures

Tunnelling is one of the most fundamental manifestations of quantum mechanics. The recent advent of lightwave-driven scanning tunnelling microscopy has revolutionized ultrafast nanoscience by directly resolving electron tunnelling in electrically conducting samples on the relevant ultrashort length- and timescales. In this work, we introduce a complementary approach based on terahertz near-field microscopy to perform ultrafast nano-videography of tunnelling processes even in insulators. The central idea is to probe the evolution of the local polarizability of electron–hole pairs with evanescent terahertz fields, which we detect with subcycle temporal resolution. In a proof of concept, we resolve femtosecond interlayer transport in van der Waals heterobilayers and reveal pronounced variations of the local formation and annihilation of interlayer excitons on deeply subwavelength, nanometre scales. Such contact-free nanoscopy of tunnelling-induced dynamics should be universally applicable to conducting and non-conducting samples and reveal how ultrafast transport processes shape functionalities in a wide range of condensed matter systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Three-dimensional neutron far-field tomography of a bulk skyrmion lattice

Abstract Magnetic skyrmions are localized non-collinear spin textures, characterized by an integer topological charge. Commonly observed in thin systems as two-dimensional sheets, in three dimensions skyrmions form tubes that are thought to nucleate and annihilate along their depth on points of vanishing magnetization. However, a lack of techniques that can probe the bulk of the material has made it difficult to perform experimental visualizations of skyrmion lattices and their stabilization through defects. Here we present three-dimensional visualizations of a bulk Co 8 Zn 8 Mn 4 skyrmion lattice through a tomographic algorithm applied to multiprojection small-angle neutron scattering measurements. Reconstructions of the sample show a disordered skyrmion lattice exhibiting three-dimensional topological transitions through emergent (anti)monopole branching and segmentation defect pathways. Our technique provides insights into skyrmion stabilization and topological transition pathways in a bulk skyrmion lattice, guiding the future development and manipulation of skyrmion materials for spintronic applications.

Physics↗
DOE OSTI2021

The asymmetry of antimatter in the proton

The fundamental building blocks of the proton—quarks and gluons—have been known for decades. However, we still have an incomplete theoretical and experimental understanding of how these particles and their dynamics give rise to the quantum bound state of the proton and its physical properties, such as its spin1. The two up quarks and the single down quark that comprise the proton in the simplest picture account only for a few per cent of the proton mass, the bulk of which is in the form of quark kinetic and potential energy and gluon energy from the strong force2. An essential feature of this force, as described by quantum chromodynamics, is its ability to create matter–antimatter quark pairs inside the proton that exist only for a very short time. Their fleeting existence makes the antimatter quarks within protons difficult to study, but their existence is discernible in reactions in which a matter–antimatter quark pair annihilates. In this picture of quark–antiquark creation by the strong force, the probability distributions as a function of momentum for the presence of up and down antimatter quarks should be nearly identical, given that their masses are very similar and small compared to the mass of the proton. Here we provide evidence from muon pair production measurements that these distributions are considerably different, with more abundant down antimatter quarks than up antimatter quarks over a wide range of momenta. These results are expected to revive interest in several proposed mechanisms for the origin of this antimatter asymmetry in the proton that had been disfavoured by previous results, and point to future measurements that can distinguish between these mechanisms.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Publisher Correction: The asymmetry of antimatter in the proton

The fundamental building blocks of the proton—quarks and gluons—have been known for decades. However, we still have an incomplete theoretical and experimental understanding of how these particles and their dynamics give rise to the quantum bound state of the proton and its physical properties, such as its spin1. The two up quarks and the single down quark that comprise the proton in the simplest picture account only for a few per cent of the proton mass, the bulk of which is in the form of quark kinetic and potential energy and gluon energy from the strong force2. An essential feature of this force, as described by quantum chromodynamics, is its ability to create matter–antimatter quark pairs inside the proton that exist only for a very short time. Their fleeting existence makes the antimatter quarks within protons difficult to study, but their existence is discernible in reactions in which a matter–antimatter quark pair annihilates. In this picture of quark–antiquark creation by the strong force, the probability distributions as a function of momentum for the presence of up and down antimatter quarks should be nearly identical, given that their masses are very similar and small compared to the mass of the proton3. Here we provide evidence from muon pair production measurements that these distributions are considerably different, with more abundant down antimatter quarks than up antimatter quarks over a wide range of momenta. These results are expected to revive interest in several proposed mechanisms for the origin of this antimatter asymmetry in the proton that had been disfavoured by previous results4, and point to future measurements that can distinguish between these mechanisms.

Dove, J.↗
DOE OSTI2024

X-ray linear dichroic tomography of crystallographic and topological defects

Abstract The functionality of materials is determined by their composition 1–4 and microstructure, that is, the distribution and orientation of crystalline grains, grain boundaries and the defects within them 5,6 . Until now, characterization techniques that map the distribution of grains, their orientation and the presence of defects have been limited to surface investigations, to spatial resolutions of a few hundred nanometres or to systems of thickness around 100 nm, thus requiring destructive sample preparation for measurements and preventing the study of system-representative volumes or the investigation of materials under operational conditions 7–15 . Here we present X-ray linear dichroic orientation tomography (XL-DOT), a quantitative, non-invasive technique that allows for an intragranular and intergranular characterization of extended polycrystalline and non-crystalline 16 materials in three dimensions. We present the detailed characterization of a polycrystalline sample of vanadium pentoxide (V 2 O 5 ), a key catalyst in the production of sulfuric acid 17 . We determine the nanoscale composition, microstructure and crystal orientation throughout the polycrystalline sample with 73 nm spatial resolution. We identify and characterize grains, as well as twist, tilt and twin grain boundaries. We further observe the creation and annihilation of topological defects promoted by the presence of volume crystallographic defects. The non-destructive and spectroscopic nature of our method opens the door to operando combined chemical and microstructural investigations 11,18 of functional materials, including energy, mechanical and quantum materials.

Science & Technology - Other Topics↗
DOE OSTI2020

Chemical manipulation of hydrogen induced high p-type and n-type conductivity in Ga 2 O 3

Advancement of optoelectronic and high-power devices is tied to the development of wide band gap materials with excellent transport properties. However, bipolar doping (n-type and p-type doping) and realizing high carrier density while maintaining good mobility have been big challenges in wide band gap materials. Here P-type and n-type conductivity was introduced in β-Ga 2 O 3 , an ultra-wide band gap oxide, by controlling hydrogen incorporation in the lattice without further doping. Hydrogen induced a 9-order of magnitude increase of n-type conductivity with donor ionization energy of 20 meV and resistivity of 10 -4 Ω.cm. The conductivity was switched to p-type with acceptor ionization energy of 42 meV by altering hydrogen incorporation in the lattice. Density functional theory calculations were used to examine hydrogen location in the Ga 2 O 3 lattice and identified a new donor type as the source of this remarkable n-type conductivity. Positron annihilation spectroscopy measurements confirm this finding and the interpretation of the experimental results. This work illustrates a new approach that allows a tunable and reversible way of modifying the conductivity of semiconductors and it is expected to have profound implications on semiconductor field. At the same time, it demonstrates for the first time p-type and remarkable n-type conductivity in Ga 2 O 3 which should usher in the development of Ga 2 O 3 devices and advance optoelectronics and high-power devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Direct evidence for low-energy electron emission following O LVV Auger transitions at oxide surfaces

Abstract Oxygen, the third most abundant element in the universe, plays a key role in the chemistry of condensed matter and biological systems. Here, we report evidence for a hitherto unexplored Auger transition in oxides, where a valence band electron fills a vacancy in the 2s state of oxygen, transferring sufficient energy to allow electron emission. We used a beam of positrons with kinetic energies of $$\sim 1$$ ∼ 1 eV to create O 2s holes via matter-antimatter annihilation. This made possible the elimination of the large secondary electron background that has precluded definitive measurements of the low-energy electrons emitted through this process. Our experiments indicate that low-energy electron emission following the Auger decay of O 2s holes from adsorbed oxygen and oxide surfaces are very efficient. Specifically, our results indicate that the low energy electron emission following the Auger decay of O 2s hole is nearly as efficient as electron emission following the relaxation of O 1s holes in $$\hbox {TiO}_2$$ TiO 2 . This has important implications for the understanding of Auger-stimulated ion desorption, Coulombic decay, photodynamic cancer therapies, and may yield important insights into the radiation-induced reactive sites for corrosion and catalysis.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Topologically distinct Weyl fermion pairs

Abstract A Weyl semimetal has Weyl nodes that always come in pairs with opposite chiralities. Notably, different ways of connection between nodes are possible and would lead to distinct topologies. Here we identify their differences in many respects from two proposed models with different vorticities. One prominent feature is the behaviour of zeroth Landau levels (LLs) under magnetic field. We demonstrate that the magnetic tunneling does not always expel LLs from zero energy because the number of zero-energy modes is protected by the vorticity of the Weyl nodes, instead of the chirality. Other respects in disorder effects for weak (anti-)localization, surface Fermi arcs, and Weyl-node annihilation, are interesting consequences that await more investigation in the future.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗