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At least 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Vacancies in graphene: an application of adiabatic quantum optimization

Quantum annealers have grown in complexity to the point that quantum computations involving a few thousand qubits are now possible. In this paper, with the intentions to show the feasibility of quantum annealing to tackle problems of physical relevance, we used a simple model, compatible with the capability of current quantum annealers, to study the relative stability of graphene vacancy defects. By mapping the crucial interactions that dominate carbon-vacancy interchange onto a quadratic unconstrained binary optimization problem, our approach exploits the ground state as well as the excited states found by the quantum annealer to extract all the possible arrangements of multiple defects on the graphene sheet together with their relative formation energies. Furthermore, this approach reproduces known results and provides a stepping stone towards applications of quantum annealing to problems of physical–chemical interest.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Accelerated kinetic Monte Carlo: A case study; vacancy and dumbbell interstitial diffusion traps in concentrated solid solution alloys

Vacancy and self-interstitial atomic diffusion coefficients in concentrated solid solution alloys can have a non-monotonic concentration dependence. Here, the kinetics of monovacancies and $\langle$100$\rangle$ dumbbell interstitials in Ni–Fe alloys are assessed using lattice kinetic Monte Carlo (kMC). The non-monotonicity is associated with superbasins, which impels using accelerated kMC methods. Detailed implementation prescriptions for first passage time analysis kMC (FPTA-kMC), mean rate method kMC (MRM-kMC), and accelerated superbasin kMC (AS-kMC) are given. The accelerated methods are benchmarked in the context of diffusion coefficient calculations. The benchmarks indicate that MRM-kMC underestimates diffusion coefficients, while AS-kMC overestimates them. In this application, MRM-kMC and AS-kMC are computationally more efficient than the more accurate FPTA-kMC. Our calculations indicate that composition dependence of migration energies is at the origin of the vacancy’s non-monotonic behavior. In contrast, the difference between formation energies of Ni–Ni, Ni–Fe, and Fe–Fe dumbbell interstitials is at the origin of their non-monotonic diffusion behavior. Additionally, the migration barrier crossover composition—based on the situation where Ni or Fe atom jumps have lower energy barrier than the other one—is introduced. KMC simulations indicate that the interplay between composition dependent crossover of migration energy and geometrical site percolation explains the non-monotonic concentration-dependence of atomic diffusion coefficients.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Discrete scale invariance of the quasi-bound states at atomic vacancies in a topological material

Recently, log-periodic quantum oscillations have been detected in the topological materials zirconium pentatelluride (ZrTe 5 ) and hafnium pentatelluride (HfTe 5 ), displaying an intriguing discrete scale invariance (DSI) characteristic. In condensed materials, the DSI is considered to be related to the quasi-bound states formed by massless Dirac fermions with strong Coulomb attraction, offering a feasible platform to study the long-pursued atomic-collapse phenomenon. Here, we demonstrate that a variety of atomic vacancies in the topological material HfTe 5 can host the geometric quasi-bound states with a DSI feature, resembling an artificial supercritical atom collapse. The density of states of these quasi-bound states is enhanced, and the quasi-bound states are spatially distributed in the “orbitals” surrounding the vacancy sites, which are detected and visualized by low-temperature scanning tunneling microscope/spectroscopy. By applying the perpendicular magnetic fields, the quasi-bound states at lower energies become wider and eventually invisible; meanwhile, the energies of quasi-bound states move gradually toward the Fermi energy (E F ). These features are consistent with the theoretical prediction of a magnetic field–induced transition from supercritical to subcritical states. The direct observation of geometric quasi-bound states sheds light on the deep understanding of the DSI in quantum materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Minimizing the diffusivity difference between vacancies and interstitials in multi-principal element alloys

Interstitial atoms usually diffuse much faster than vacancies, which is often the root cause for the ineffective recombination of point defects in metals under irradiation. Here, via ab initio modeling of single-defect diffusion behavior in the equiatomic NiCoCrFe(Pd) alloy, we demonstrate an alloy design strategy that can reduce the diffusivity difference between the two types of point defects. The two diffusivities become almost equal after substituting the NiCoCrFe base alloy with Pd. The underlying mechanism is that Pd, with a much larger atomic size (hence larger compressibility) than the rest of the constituents, not only heightens the activation energy barrier ( E a ) for interstitial motion by narrowing the diffusion channels but simultaneously also reduces E a for vacancies due to less energy penalty required for bond length change between the initial and the saddle states. Our findings have a broad implication that the dynamics of point defects can be manipulated by taking advantage of the atomic size disparity, to facilitate point-defect annihilation that suppresses void formation and swelling, thereby improving radiation tolerance.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Electron vacancy-level dependent hybrid photoionization of the F–@C60+molecule: A novel effect

Our previous studies [J. Phys. B 53, 125101 (2020); Euro. Phys. J. D 74, 191 (2020)] have predicted that the atom-fullerene hybrid photoionization properties for X = Cl, Br and I endohedrally confined in C60 are different before and after an electron transfers from C60 to the halogen. It was further found as a rule that the ionization dynamics is insensitive to the C60level the electron originates from to produce X–@C60+ . In the current study, we report an exception to this rule in F@C60. It is found that when the electron vacancy is situated in the C60level that participates in the hybridization in F–@C60+, the mixing becomes dramatically large leading to strong modifications in the photoionization of the hybrid levels. This novel effect is fundamentally based on a level-crossing phenomenon driven by the electron transfer in F@C60. But when the vacancy is at any other pure level of C60, the level-invariance is retained showing weak hybridization. Even though this case of F@C60 is an exception in the halogen@C60 series, the phenomenon can be more general and can occur with compounds of other atoms caged in a variety of fullerenes. Possible experimental studies are suggested to benchmark the present results.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Spin qubit properties of the boron-vacancy/carbon defect in the two-dimensional hexagonal boron nitride

Spin qubit defects in two-dimensional materials have a number of advantages over those in three-dimensional hosts including simpler technologies for defect creation and control, as well as qubit accessibility. In this work, we select the V B C B defect in the hexagonal boron nitride (hBN) as a possible optically controllable spin qubit and explain its triplet ground state and neutrality. In this defect a boron vacancy is combined with a carbon dopant substituting the closest boron atom to the vacancy. Our density-functional-theory calculations confirmed that the system has dynamically stable spin triplet and singlet ground states. As revealed from our linear response GW calculations, the spin-sensitive electronic states are localized around the three undercoordinated N atoms and make local peaks in the density of electronic states within the bandgap. Using the triplet and singlet ground state energies, as well as the energies of the optically excited states, obtained from solution to the Bethe–Salpeter equation, we construct the spin-polarization cycle, which is found to be favorable for the spin qubit initialization. The calculated zero-field splitting parameters ensure that the splitting energy between the spin projections in the triplet ground state is comparable to that of the known spin qubits. We thus propose the V B C B defect in hBN as a promising spin qubit.

2D BN↗
DOE OSTI2021

Impacts of vacancy-induced polarization and distortion on diffusion in Solid Electrolyte Li 3 OCl

We report that Lithium-rich oxychloride antiperovskites are promising solid electrolytes for enabling next-generation batteries. Here, we report a comprehensive study varying Li + concentrations in Li 3 OCl using ab initio molecular dynamics simulations. The simulations accurately capture the complex interactions between Li + vacancies (V$^'_{Li}$), the dominant mobile species in Li 3 OCl. The V$^'_{Li}$ polarize and distort the host lattice, inducing additional non-vacancy-mediated diffusion mechanisms and correlated diffusion events that reduce the activation energy barrier at concentrations as low as 1.5% V$^'_{Li}$. Our analyses of discretized diffusion events in both space and time illustrate the critical interplay between correlated dynamics, polarization and local distortion in promoting ionic conductivity in Li 3 OCl.

25 ENERGY STORAGE↗
DOE OSTI2025

Robustness of Vacancy-Bound Non-Abelian Anyons in the Kitaev Model in a Magnetic Field

Non-Abelian anyons in quantum spin liquids (QSLs) provide a promising route to fault-tolerant topological quantum computation. In the exactly solvable Kitaev honeycomb model, such anyons of the QSL state can be bound to nonmagnetic spin vacancies and endowed with non-Abelian statistics by an infinitesimal magnetic field. Here, we investigate how this approach for stabilizing non-Abelian anyons extends to a finite magnetic field represented by a proper Zeeman term. Through large-scale density-matrix renormalization group simulations, we compute the vacancy-anyon binding energy as a function of magnetic field for both the ferromagnetic and antiferromagnetic Kitaev models. Here, we find that anyon binding remains robust within the entire QSL phase for the ferromagnetic Kitaev model but breaks down already inside this phase for the antiferromagnetic Kitaev model. To compute a binding energy several orders of magnitude below the magnetic energy scale, we introduce both a refined definition and an extrapolation scheme based on carefully tailored perturbations.

Xiao, Bo [Oak Ridge National Laboratory (ORNL), Oa↗
DOE OSTI2020

Vibronic States and Their Effect on the Temperature and Strain Dependence of Silicon-Vacancy Qubits in 4$\textit{H}$-SiC

Silicon-vacancy qubits in silicon carbide ( Si C ) are emerging tools in quantum-technology applications due to their excellent optical and spin properties. In this paper, we explore the effect of temperature and strain on these properties by focusing on the two silicon-vacancy qubits, V1 and V2, in 4$\textit{H}$-SiC. We apply density-functional theory beyond the Born-Oppenheimer approximation to describe the temperature-dependent mixing of electronic excited states assisted by phonons. We obtain a polaronic gap of around 5 and 22 meV for the V1 and V2 centers, respectively, which results in a significant difference in the temperature-dependent dephasing and zero-field splitting of the excited states, which explains recent experimental findings. Finally, we also compute how crystal deformations affect the zero-phonon line of these emitters. Our predictions are important ingredients in any quantum applications of these qubits sensitive to these effects.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Split Ga vacancies and the unusually strong anisotropy of positron annihilation spectra in β–Ga 2 O 3

We report a systematic first-principles study on positron annihilation parameters in the β–Ga 2 O 3 lattice and Ga monovacancy defects complemented with orientation-dependent experiments of the Doppler broadening of the positron-electron annihilation. We find that both the β–Ga 2 O 3 lattice and the considered defects exhibit unusually strong anisotropy in their Doppler broadening signals. This anisotropy is associated with low symmetry of the β–Ga 2 O 3 crystal structure that leads to unusual kind of one-dimensional confinement of positrons even in the delocalized state in the lattice. In particular, the split Ga vacancies recently observed by scanning transmission electron microscopy produce unusually anisotropic positron annihilation signals. Furthermore, we show that in experiments, the positron annihilation signals in β–Ga 2 O 3 samples seem to be often dominated by split Ga vacancies.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Calculating the hyperfine tensors for group-IV impurity-vacancy centers in diamond using hybrid density functional theory

The hyperfine interaction is an important probe for understanding the structure and symmetry of defects in a semiconductor. Density functional theory has shown that it can provide useful first-principles predictions for both the hyperfine tensor and the hyperfine constants that arise from it. Recently there has been great interest in using group-IV impurity-vacancy color centers XV – (where X = Si, Ge, Sn, or Pb and V is a carbon vacancy) for important applications in quantum computing and quantum information science. In this paper we have calculated the hyperfine tensors for these XV – color centers using the HSE06 screened Hartree-Fock hybrid exchange-correlation functional with the inclusion of core electron spin polarization. We have compared our results to calculations which only use the PBE exchange-correlation functional without the inclusion of core electron spin polarization and we have found that our results are in very good agreement with available experimental results. Lastly, we have theoretically shown that these XV – color centers exhibit a Jahn-Teller distortion which explains the observed anisotropic distribution of the hyperfine constants among the neighboring 13 C nuclear spins.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Nuclear spin metrology with nitrogen vacancy center in diamond for axion dark matter detection

We present a method to directly detect the axion dark matter using nitrogen vacancy centers in diamonds. In particular, we use metrology leveraging the nuclear spin of nitrogen to detect axion-nucleus couplings. This is achieved through protocols designed for dark matter searches, which introduce a novel approach of quantum sensing techniques based on the nitrogen vacancy center. Although the coupling strength of the magnetic fields with nuclear spins is three orders of magnitude smaller than that with electron spins for conventional magnetometry, the axion interaction strength with nuclear spins is the same order of magnitude as that with electron spins. Furthermore, we can take advantage of the long coherence time by using the nuclear spins for the axion dark matter detection. Our method has the potential to be sensitive to a broad frequency range ≲ 100 Hz corresponding to the axion mass m a ≲ 4 × 10 − 13 eV . We present the detection limit of our method for both the axion-neutron and the axion-proton couplings and discuss its significance in comparison with other proposed ideas. We also show that the sensitivities of the NV center sensor to various spin species will open up new directions for constructing protocols that can mitigate magnetic noise effects. Published by the American Physical Society 2025

Chigusa, So (ORCID:0000000160054447)↗
DOE OSTI2022

Coalescence dynamics of prismatic dislocation loops due to vacancy supersaturation

Recovery processes in metals with a high defect concentration are at the heart of a structural alloy's usability in engineering applications. However, such processes take place via nonconservative mechanisms mediated by point defect diffusion and are governed by their interactions with the underlying microstructure. Indeed, one of the main challenges in studying recovery processes is their intrinsic multiscale complexity, which often negates the direct use of experimental techniques. Here, in this Research Letter, we study the mechanism of dislocation loop coalescence in metals by simulating the interaction dynamics between vacancies and prismatic loops using a stochastic framework that seamlessly bridges point defect kinetics with dislocation mechanics. Our simulations reveal two fundamental discoveries: first, that climb processes are governed by local fluctuations that are not captured by continuum elastodiffusion models, and, second, that prismatic loops create internal traps for vacancies, leading to the formation of rings around the perimeter of the loops that affect how coalescence takes place. Our results show an excellent agreement with in situ experimental observations of loop coalescence in Fe under irradiation.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Vacancy-tuned magnetism in LaMn x Sb 2

The layered AMP 2 (A = alkali-earth or rare-earth atom, M = transition metal, P = Sb, Bi) compounds are widely studied for their rich magnetism and electronic structure topology. We provide a detailed characterization of the magnetic and transport properties of LaMn x Sb 2 , an understudied member of the AMP 2 family. LaMn x Sb 2 forms with intrinsic Mn vacancies, and we demonstrate that by varying the starting ratio of La, Mn, and Sb, we can synthetically control the Mn occupancy and produce single crystals with x = 0.74 – 0.97. Magnetization and transport measurements indicate LaMn x Sb 2 has a rich temperature-composition (T–x) magnetic phase diagram with physical properties strongly influenced by the Mn occupancy. LaMn x Sb 2 orders antiferromagnetically at T 1 = 130–180 K, where T 1 increases with x. Below T 1 , the T–x phase diagram is complicated. At high x, there is a second transition T 2 that decreases in temperature as x is lowered, vanishing below x ≤ 0.85. A third, first-order, transition T 3 is detected at x ≈ 0.92, and the transition temperature increases as x is lowered, crossing above T 2 near x ≈ 0.9. On moving below x < 0.79, here we find the crystal structure changes from the P 4/nmm arrangement to an I$\bar{4}$2m structure with partially ordered Mn vacancies. The change in crystal structure results in the sudden appearance of two new low-temperature phases and a crossover between regimes of negative and positive magnetoresistance when x ≤ 0.78. Finally, we provide powder neutron diffraction for x = 0.93, and find that the high-x compositions first adopt a G-type antiferromagnetic structure with the Mn moments aligned within the ab plane, which is followed upon further cooling by a second transition to a different, noncollinear structure where the moments are rotated within the basal plane. Our results demonstrate that LaMn x Sb 2 is a highly tunable material with six unique magnetically ordered phases, depending on T and x.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Iodine Vacancies do not Cause Nonradiative Recombination in Halide Perovskites

The iodine vacancy (V I ) has frequently been discussed as a strong nonradiative recombination center in halide perovskites. This proposition was mainly based on the presence of charge-state transition levels in the band gap, as found in early first-principles calculations. In this work, we perform accurate hybrid-density-functional calculations for V I in CsPbI 3 , CsSnI 3 , and CsGeI 3 and find that V I does not have any transition levels in the band gap in CsPbI 3 , in contrast to the results from calculations based on semilocal functionals. The iodine vacancy V I does introduce levels in the band gap in CsSnI 3 and CsGeI 3 , but our explicitly computed nonradiative capture coefficients demonstrate that V I has a negligible impact on nonradiative recombination. Our study corrects a misunderstanding of the role of V I in the iodide-based perovskites, and shifts the focus toward identifying and mitigating actual recombination centers in order to further improve the optoelectronic performance.

14 SOLAR ENERGY↗
DOE OSTI2021

Depth-resolved cathodoluminescence and surface photovoltage spectroscopies of gallium vacancies in β-Ga 2 O 3 with neutron irradiation and forming gas anneals

The gallium vacancy is one of the dominant native point defects in β-Ga 2 O 3 , one that, together with its complexes, can have a major effect on free carrier densities and transport in this wide bandgap semiconductor. We used a combination of depth-resolved cathodoluminescence spectroscopy and surface photovoltage spectroscopy to identify the optical and energy-level properties of these defects as well as how their defect densities and spatial distributions vary with neutron irradiation and temperature-dependent-forming gas anneals. These studies reveal optical signatures that align closely with theoretical energy-level predictions. Likewise, our optical techniques reveal variations in these defect densities that are consistent with hydrogen passivation of gallium vacancies as a function of temperature and depth from the free Ga 2 O 3 surface. These techniques can help guide the understanding and control of dominant native point defects in Ga 2 O 3 .

42 ENGINEERING↗
DOE OSTI2023

Lithium-compatible and air-stable vacancy-rich Li 9 N 2 Cl 3 for high–areal capacity, long-cycling all–solid-state lithium metal batteries

Attaining substantial areal capacity (>3 mAh/cm 2 ) and extended cycle longevity in all–solid-state lithium metal batteries necessitates the implementation of solid-state electrolytes (SSEs) capable of withstanding elevated critical current densities and capacities. In this study, we report a high-performing vacancy-rich Li 9 N 2 Cl 3 SSE demonstrating excellent lithium compatibility and atmospheric stability and enabling high–areal capacity, long-lasting all–solid-state lithium metal batteries. The Li 9 N 2 Cl 3 facilitates efficient lithium-ion transport due to its disordered lattice structure and presence of vacancies. Notably, it resists dendrite formation at 10 mA/cm 2 and 10 mAh/cm 2 due to its intrinsic lithium metal stability. Furthermore, it exhibits robust dry-air stability. Incorporating this SSE in Ni-rich LiNi 0.83 Co 0.11 Mn 0.06 O 2 cathode-based all–solid-state batteries, we achieve substantial cycling stability (90.35% capacity retention over 1500 cycles at 0.5 C) and high areal capacity (4.8 mAh/cm 2 in pouch cells). These findings pave the way for lithium metal batteries to meet electric vehicle performance demands.

25 ENERGY STORAGE↗