Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “Atoms Molecules”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 415 records · Page 23

Nuclear cusps and singularities in the nonadditive kinetic potential bifunctional from analytical inversion

The non-additive kinetic potential $v^{\text{NAD}}$ is a key quantity in density-functional theory (DFT) embedding methods, such as frozen density embedding theory and partition DFT. $v^{\text{NAD}}$ is a bi-functional of electron densities $\rho_{\rm B}$ and $\rho_{\rm tot} = \rho_{\rm A} + \rho_{\rm B}$. It can be evaluated using approximate kinetic-energy functionals, but accurate approximations are challenging. The behavior of $v^{\text{NAD}}$ in the vicinity of the nuclei has long been questioned, and singularities were seen in some approximate calculations. In this article, the existence of singularities in $v^{\text{NAD}}$ is analyzed analytically for various choices of $\rho_{\rm B}$ and $\rho_{\rm tot}$, using the nuclear cusp conditions for the density and Kohn-Sham potential. It is shown that no singularities arise from smoothly partitioned ground-state Kohn-Sham densities. We confirm this result by numerical calculations on diatomic test systems HeHe, HeLi$^+$, and H$_2$, using analytical inversion to obtain a numerically exact $v^{\rm NAD}$ for the local density approximation. We examine features of $v^{\rm NAD}$ which can be used for development and testing of approximations to $v^{\rm NAD}[\rho_{\rm B},\rho_{\rm tot}]$ and kinetic-energy functionals.

74 ATOMIC AND MOLECULAR PHYSICS↗

Optical telecommunications-band clock based on neutral titanium atoms

Here, we propose an optical clock based on ultranarrow transitions in neutral titanium, which exhibit small blackbody radiation and quadratic Zeeman shifts and have wavelengths in the S-, C-, and L-telecommunications fiber bands, allowing for integration with robust laser technology. We calculate relevant properties using a high-precision relativistic hybrid method that combines configuration interaction and coupled-cluster approaches. To identify magic wavelengths, we have completed the largest-to-date direct dynamical polarizability calculations. Finally, we identify challenges that arise from magnetic dipole-dipole interactions and describe an approach to overcome them. A telecommunications-band atomic frequency standard will aid the deployment of optical clock networks and clock comparisons over long distances.

74 ATOMIC AND MOLECULAR PHYSICS↗

Quantum dynamics of non-Hermitian many-body Landau-Zener systems

Here, we develop a framework to solve a large class of linearly driven non-Hermitian quantum systems. Such a class of models in the Hermitian scenario is commonly known as multistate Landau-Zener models. The non-Hermiticity is due to the anti-Hermitian couplings between the diabatic levels. We find that there exists a conservation law, unique to this class of models, that describes the simultaneous growth of the unnormalized wave functions. These models have practical applications in Bose-Einstein condensates, and they can describe the dynamics of multispecies bosonic systems. The conservation law relates to a pair-production mechanism that explains the dissociation of diatomic molecules into atoms. We provide a general framework for both solvable and semiclassically solvable non-Hermitian Landau-Zener models. Our findings will open alternative avenues for a number of diverse emergent phenomena in explicitly time-dependent non-Hermitian quantum systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Optimization of algorithmic errors in analog quantum simulations

Due to rapidly improving quantum computing hardware, Hamiltonian simulations of relativistic lattice field theories have seen a resurgence of attention. Furthermore, this computational tool requires turning the formally infinite-dimensional Hilbert space of the full theory into a finite-dimensional one. For gauge theories, a widely used basis for the Hilbert space relies on the representations induced by the underlying gauge group, with a truncation that keeps only a set of the lowest dimensional representations. This works well at large bare gauge coupling, but becomes less efficient at small coupling, which is required for the continuum limit of the lattice theory. In this work, we develop a new basis suitable for the simulation of an SU(2) lattice gauge theory in the maximal tree gauge. In particular, we show how to perform a Hamiltonian truncation so that the eigenvalues of both the magnetic and electric gauge-fixed Hamiltonian are mostly preserved, which allows for this basis to be used at all values of the coupling. Little prior knowledge is assumed, so this may also be used as an introduction to the subject of Hamiltonian formulations of lattice gauge theories.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Photoluminescence, photophysics, and photochemistry of the V B - defect in hexagonal boron nitride

Extensive photochemical and spectroscopic properties of the V B - defect in hexagonal boron nitride are calculated, concluding that the observed photoemission associated with recently observed optically detected magnetic resonance is most likely of (1) 3 E'' → (1) 3 A' 2 origin. Rapid intersystem crossing from the defect's triplet to singlet manifolds explains the observed short excited-state lifetime and very low quantum yield. New experimental results reveal smaller intrinsic spectral bandwidths than previously recognized, interpreted in terms of spectral narrowing and zero-phonon-line shifting induced by the Jahn-Teller effect. Different types of computational methods are applied to map out the complex triplet and singlet defect manifolds, including the doubly ionized formulation of the equation-of-motion coupled-cluster theory that is designed to deal with the open-shell nature of defect states, and mixed quantum-mechanics/molecular-mechanics schemes enabling 5763-atom simulations. Finally, two other energetically feasible spectral assignments from among the singlet and triplet manifolds are considered, but ruled out based on inappropriate photochemical properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Microscopic force driving the photoinduced ultrafast phase transition: Time-dependent density functional theory simulations of IrTe 2

Photoinduced phase transitions can have complex and intriguing behaviors more than material ground-state dynamics. Understanding the underlying mechanism can help us to design new ways to manipulate the materials. A variety of mechanisms has been proposed to explain the photoinduced phase transitions of IrTe 2 , but a consensus has yet to be reached. Here, we study the photo-induced phase transitions of IrTe 2 by performing the real-time time-dependent density functional theory (rt-TDDFT) simulations in combination with the occupation constrained DFT method. We reveal that the microscopic driving force for the photo-induced phase transitions arises from the tendency to lower the energy levels occupied by the excited carriers, through the increase or decrease of the associated atomic pair distances, depending on whether the newly occupied states are antibonding or bonding states, respectively. The geometric constraints between different bonds represented by the Poisson ratio can bring together different tendencies from different atomic pairs, thus forming a complex intriguing dynamic picture depending on the intensity of the excitation. Furthermore, we also find that phonons don't play a primary role, but can assist the phase transition. These findings imply that one can control the structural phase transitions by selectively exciting photocarriers into designated atomic states using appropriate photon sources.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

GW band structure of monolayer MoS 2 using the SternheimerGW method and effect of dielectric environment

Monolayers of transition-metal dichalcogenides (TMD) hold great promise as future nanoelectronic and optoelectronic devices. An essential feature for achieving high device performance is the use of suitable supporting substrates, which can affect the electronic and optical properties of these two-dimensional (2D) materials. Here, we perform many-body GW calculations using the SternheimerGW method to investigate the quasiparticle band structure of monolayer MoS 2 subject to an effective dielectric screening model, which is meant to approximately describe substrate polarization in real device applications. We show that, within this model, the dielectric screening has a sizeable effect on the quasiparticle band gap, for example the gap renormalization is as large as 250 meV for MoS 2 with model screening corresponding to SiO 2 . Within the G 0 W 0 approximation, we also find that the inclusion of the effective screening induces a direct band gap, in contrast to the unscreened monolayer. We also find that the dielectric screening induces an enhancement of the carrier effective masses by as much as 27% for holes, shifts plasmon satellites, and redistributes quasiparticle weight. Our results highlight the importance of the dielectric environment in the design of 2D TMD-based devices.

36 MATERIALS SCIENCE↗

Harnessing the photonic local density of states in graphene moiré superlattices

In this work we investigate the electromagnetic local density of states (LDOS) near a twisted bilayer graphene (TBG) deposited over a general isotropic substrate. The band structure of the TBG is calculated within a tight-binding framework, and then used to determine the TBG's conductivity. The latter presents a nontrivial dependence upon the angle of twist, which shows up in the LDOS, allowing for a moiré pattern-dependent quantum emission. For some specific twist angles we show that it is possible to either enhance or decrease the LDOS by an order of magnitude at selected frequencies when compared to the monolayer. Furthermore, this impressive variation is explained in terms of the presence/absence of well defined surface plasmon polaritons (SPPs). Altogether our findings demonstrate that TBG is an alternative, versatile material platform for controlling spontaneous emission and enhancing light-matter interactions, and pave the way for further studies and applications of quantum emission in the emerging class of two-dimensional moiré materials.

36 MATERIALS SCIENCE↗

Harmonic generation predominantly from a single spin channel in a half metal

Harmonic generation in atoms and molecules has reshaped our understanding of ultrafast phenomena beyond the traditional nonlinear optics and has launched attosecond physics. Harmonics from solids represent a new frontier, where both majority and minority spin channels contribute to harmonics. This is true even in a ferromagnet whose electronic states are equally available to optical excitation. In this work, we demonstrate that harmonics can be generated {mostly} from a single spin channel in half metallic chromium dioxide. An energy gap in the minority channel greatly reduces the harmonic generation, so harmonics predominantly emit from the majority channel, with a small contribution from the minority channel. However, this is only possible when the incident photon energy is well below the energy gap in the minority channel, so all the transitions in the minority channel are virtual. The onset of the photon energy is determined by the transition energy between the dipole-allowed transition between the O-$2p$ and Cr-$3d$ states. Harmonics mainly from a single spin channel can be detected, regardless of laser field strength, as far as the photon energy is below the minority band energy gap. This prediction should be tested experimentally

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Microscopic characterization of Ising conformal field theory in Rydberg chains

Rydberg chains provide an appealing platform for probing conformal field theories (CFTs) that capture universal behavior in a myriad of physical settings. Focusing on a Rydberg chain at the Ising transition separating charge density wave and disordered phases, we establish a detailed link between microscopics and low-energy physics emerging at criticality. Here, we first construct lattice incarnations of primary fields in the underlying Ising CFT including chiral fermions, a nontrivial task given that the Rydberg chain Hamiltonian does not admit an exact fermionization. With this dictionary in hand, we compute correlations of microscopic Rydberg operators, paying special attention to finite, open chains of immediate experimental relevance. We further develop a method to quantify how second-neighbor Rydberg interactions tune the sign and strength of four-fermion couplings in the Ising CFT. Finally, we determine how the Ising fields evolve when four-fermion couplings drive an instability to Ising tricriticality. Our results pave the way to a thorough experimental characterization of Ising criticality in Rydberg arrays and can inform the design of novel higher-dimensional phases based on coupled critical chains.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Low-energy electronic structure of perovskite and Ruddlesden-Popper semiconductors in the Ba-Zr-S system probed by bond-selective polarized x-ray absorption spectroscopy, infrared reflectivity, and Raman scattering

Chalcogenides in perovskite and the related layered Ruddlesden-Popper crystal structures ( chalcogenide perovskites for brevity) are an exciting family of semiconductors but remain experimentally little studied. Chalcogenide perovskites share crystal structures and some physical properties with ionic compounds such as oxide and halide perovskites, but the metal-chalcogen bonds responsible for semiconducting behavior are substantially more covalent than in these more-studied perovskites. In this study, we use complementary experimental and theoretical methods to study how the mixed ionic-covalent Zr-S bonds support the electronic structure and physical properties of perovskite BaZrS 3 and Ruddlesden-Popper Ba 3 Zr 2 S 7 . We apply theoretical methods to assign features of experimentally measured x-ray absorption spectroscopy (XAS) to particular orbital transitions, enabling a clear physical interpretation of angle-dependent, polarized XAS data measured on single-crystal samples, and an atomistic view of the covalent bonding network that facilitates charge transport. Polarized Raman measurements identify signatures of crystalline anisotropy in Ba 3 Zr 2 S 7 and enable the first assignments of mode symmetry in this material. Infrared reflectivity reveals electronic transport properties that augur well for the use of chalcogenide perovskites in optoelectronic and energy-conversion technologies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Rainbow scars: From area to volume law

Quantum many-body scars (QMBS) constitute a new quantum dynamical regime in which rare “scarred” eigenstates mediate weak ergodicity breaking. One open question is to understand the most general setting in which these states arise. In this work, we develop a generic construction that embeds a new class of QMBS, rainbow scars, into the spectrum of an arbitrary Hamiltonian. Unlike other examples of QMBS, rainbow scars display extensive bipartite entanglement entropy while retaining a simple entanglement structure. Specifically, the entanglement scaling is volume-law for a random bipartition, while scaling for a fine-tuned bipartition is subextensive. When internal symmetries are present, the construction leads to multiple, and even towers, of rainbow scars revealed through distinctive non-thermal dynamics. Remarkably, certain symmetries can lead rainbow scars to arise in translation-invariant models. To this end, we provide an experimental road map for realizing rainbow scar states in a Rydberg-atom quantum simulator, leading to coherent oscillations distinct from the strictly sub-volume-law QMBS previously realized in the same system.

36 MATERIALS SCIENCE↗

Changes in polarization dictate necessary approximations for modeling electronic deexcitation intensity: Application to x-ray emission

Accurate simulation of electronic excitations and deexcitations are critical for complementing complex spectroscopic experiments and can provide validation to theoretical approaches. Here, using a generalized framework, we contrast the accuracy and validity of orbital-constrained and linear-response approaches that build upon Kohn-Sham density functional theory (DFT) to simulate emission spectra of electronic origin and propose an efficient approximation, named many-body x-ray emission spectroscopy or MBXES, for simulating such processes. We show analytically as well as with computed examples that for electronic (de)excitation leading to an appreciable change in polarization (i.e., density rearrangement), the adiabatic approximation in a response-based formalism will be inadequate for the calculation of oscillator strength. Thus, such a change (e.g., in the net electrostatic dipole moment of a finite system) can be used as a metric for evaluating the applicability of the adiabatic response-based approach and can be particularly valuable in x-ray emission spectroscopy. On the other hand, MBXES, the flexible method introduced in this paper, can compute oscillator strengths accurately at a much lower computational expense on the basis of two DFT-based self-consistent field calculations. Using illustrative examples of emission spectra, the efficacy of the MBXES method is demonstrated by comparison with its parent theory, orbital-optimized DFT, and with experiments.

74 ATOMIC AND MOLECULAR PHYSICS↗

Quantum spin liquids bootstrapped from Ising criticality in Rydberg arrays

Arrays of Rydberg atoms constitute a highly tunable, strongly interacting venue for the pursuit of exotic states of matter. We develop a strategy for accessing a family of fractionalized phases known as quantum spin liquids in two-dimensional Rydberg arrays. We specifically use effective field theory methods to study arrays assembled from Rydberg chains tuned to an Ising phase transition that famously hosts emergent fermions propagating within each chain. This highly entangled starting point allows us to naturally access spin liquids familiar from Kitaev's honeycomb model—albeit from an entirely different framework. In particular, we argue that finite-range repulsive Rydberg interactions, which frustrate nearby symmetry-breaking orders, can enable coherent propagation of emergent fermions between the chains in which they were born. Delocalization of emergent fermions across the full two-dimensional Rydberg array yields a gapless Z 2 spin liquid with a single massless Dirac cone. Here, the Rydberg occupation numbers exhibit universal power-law correlations that provide a straightforward experimental diagnostic of this phase. We further show that explicitly breaking symmetries perturbs the gapless spin liquid into gapped, topologically ordered descendants: Breaking lattice symmetries generates toric-code topological order, whereas introducing Floquet-mediated chirality generates non-Abelian Ising topological order. In the toric-code phase, we analytically construct microscopic incarnations of non-Abelian defects, which can be created and transported by dynamically controlling the atom positions in the array. Our work suggests that appropriately tuned Rydberg arrays provide a cold-atoms counterpart of solid-state “Kitaev materials” and, more generally, it spotlights a different angle for pursuing experimental platforms for Abelian and non-Abelian fractionalization.

36 MATERIALS SCIENCE↗

Efficient time-dependent orbital-free density functional theory: Semilocal adiabatic response

Orbital-free density functional theory and its time-dependent extension are efficient ab initio methods for calculating the electronic structure and dynamics of large systems. Through the calculation of the optical spectra of selected clusters, we reach three important conclusions: (1) The quality of the spectra is strongly affected by the quality of the corresponding ground-state electron density; (2) the adiabatic part of the electronic response to external perturbations can be safely evaluated at the semilocal level; and (3) the nonadiabatic, current-dependent part of the time-dependent Pauli potential is key to recover correct spectral envelopes.

36 MATERIALS SCIENCE↗

Enhancing two-photon spontaneous emission in rare earths using graphene and graphene nanoribbons

The enhancement of two-photon spontaneous emission (2PSE) from trivalent and divalent rare earth ions in proximity to graphene and graphene nanoribbons is calculated for achievable experimental conditions using a combination of finite difference time domain simulations and direct computation of transition rates between energy levels in rare earths. For Er 3+ , we find that the 2PSE rate is initially 8 orders lower than the single-photon spontaneous emission rate but that, with enhancement, 2PSE can reach 2.5% of the overall decay. When graphene nanoribbons are used, we also show that the emission of free-space photon pairs from Er 3+ at 3–3.2 μ⁢m via 2PSE can be increased by ~400. Our calculations show significantly less relative graphene-enhanced 2PSE than previous works, and we attribute this variation to differences in emitter size and assumed graphene mobility. Here, we also show that the internal energy structure of the ion can have an impact on the degree of 2PSE enhancement achievable and find that divalent rare earths are more favorable.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

In-plane Wilson loop for measurement of quantized non-Abelian Berry flux

Band topology of anomalous quantum Hall insulators can be precisely addressed by computing the Chern numbers of constituent nondegenerate bands, describing the presence of quantized, Abelian Berry flux through the two-dimensional Brillouin zone. Can Berry flux be captured for the SU (2) Berry connection of two -fold degenerate bands in spinful materials preserving space -inversion ($\mathscr{P}$) and time -reversal ($\mathscr{T}$) symmetries without detailed knowledge of underlying basis? We address this question by investigating the correspondence between a non -Abelian generalization of Stokes' theorem and the manifestly gauge -invariant eigenvalues of Wilson loops computed along in -plane contours which preserve the underlying crystalline symmetry. The importance of this correspondence is elucidated by performing natural number resolved classification of ab initio band structures of three-dimensional, Dirac materials. Further, our work underscores how identification of quantized Berry flux, both Abelian and non -Abelian, offers a unified framework for addressing first -order and higher -order topology of insulators and semimetals.

74 ATOMIC AND MOLECULAR PHYSICS↗

Adaptive time stepping for the two-time integro-differential Kadanoff-Baym equations

The nonequilibrium Green's function gives access to one-body observables for quantum systems. Of particular interest are quantities such as density, currents, and absorption spectra which are important for interpreting experimental results in quantum transport and spectroscopy. We present an integration scheme for the Green's function's equations of motion, the Kadanoff-Baym equations (KBE), which is both adaptive in the time integrator step size and method order as well as the history integration order. We analyze the importance of solving the KBE self-consistently and show that adapting the order of history integral evaluation is important for obtaining accurate results. To examine the efficiency of our method, we compare runtimes to a state-of-the-art fixed time step integrator for several test systems and show an order of magnitude speedup at similar levels of accuracy. Published by the American Physical Society 2024

97 MATHEMATICS AND COMPUTING↗