Brueckner-Goldstone many-body perturbation calculation of helium photoionization.
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Ishihara, T.↗
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Mixed Stochastic-Deterministic Approach for Many-Body Perturbation Theory Calculations
Here, we present an approach for GW calculations of quasiparticle energies with quasi-quadratic scaling by approximating high-energy contributions to the Green's function in its Lehmann representation with effective stochastic vectors. The method is easy to implement without altering the GW code, converges rapidly with stochastic parameters, and treats systems of various dimensionality and screening response. Our calculations on a 5.75° twisted MoS 2 bilayer show how large-scale GW methods include geometry relaxations and electronic correlations on an equal basis in structurally nontrivial materials.
36 MATERIALS SCIENCE↗
The approximate second order coupled-cluster method based on a size-consistent Brillouin–Wigner partitioning
We present a variant of the approximate second order coupled-cluster method (CC2) with a two-parameter size-consistent Brillouin–Wigner (BW-s) partitioning instead of a Møller–Plesset (MP) partitioning for the unperturbed Hamiltonian, which we refer to as BWs-CC2. The computational complexity of this model scales identically to CC2 with molecular size. Conventional CC2 and its regularized BWs-CC2 variants, as well as conventional MP2 and two of its regularized BW-s2 variants, were assessed on a 535 element database spanning thermochemistry, non-covalent interactions, barrier heights, and isomerization energies. To ensure a well-defined model chemistry, the assessment was performed using internally stable spin-polarized Hartree–Fock (HF) orbitals in the finite aug-cc-pVQZ basis without counterpoise corrections. As a result of using stable orbitals, contrary to conventional wisdom, we find that CC2 substantially outperforms MP2 on molecules with significantly spin contaminated reference orbitals without a significant increase in error on systems with a spin-pure reference, showing the value of its single substitutions. While no single choice of regularization parameters can be optimal for all datasets, we find that BWs-CC2 generally outperforms both CC2 and BW-s2 with a single judicious parameter choice. Additional tests on dipole moments and bond lengths of diatomics provide further support for the utility of this choice. Furthermore, the main outliers and poorest performing cases are associated with large amounts of spin-contamination in the HF reference, which is indicative of systems with either strong correlation or extensive artificial symmetry breaking. Overall, these findings argue that the perception of the quality of the CC2 ground state should be reevaluated and that it can be further improved upon by the soundly based BWs-CC2 variant with the recommended parameter choice.
Correlation energy↗
GPU Acceleration of Large-Scale Full-Frequency GW Calculations
Many-body perturbation theory is a powerful method to simulate electronic excitations in molecules and materials starting from the output of density functional theory calculations. By implementing the theory efficiently so as to run at scale on the latest leadership high-performance computing systems it is possible to extend the scope of GW calculations. Here, we present a GPU acceleration study of the full-frequency GW method as implemented in the WEST code. Excellent performance is achieved through the use of (i) optimized GPU libraries, e.g., cuFFT and cuBLAS, (ii) a hierarchical parallelization strategy that minimizes CPU-CPU, CPU-GPU, and GPU-GPU data transfer operations, (iii) nonblocking MPI communications that overlap with GPU computations, and (iv) mixed precision in selected portions of the code. A series of performance benchmarks has been carried out on leadership high-performance computing systems, showing a substantial speedup of the GPU-accelerated version of WEST with respect to its CPU version. Good strong and weak scaling is demonstrated using up to 25 920 GPUs. Finally, we showcase the capability of the GPU version of WEST for large-scale, full-frequency GW calculations of realistic systems, e.g., a nanostructure, an interface, and a defect, comprising up to 10 368 valence electrons.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Laser magnetic resonance in supersonic plasmas - The rotational spectrum of SH(+)
The rotational spectrum of v = 0 and v = 1X3Sigma(-)SH(+) was measured by laser magnetic resonance. Rotationally cold (Tr = 30 K), vibrationally excited (Tv = 3000 K) ions were generated in a corona excited supersonic expansion. The use of this source to identify ion signals is described. Improved molecular parameters were obtained; term values are presented from which astrophysically important transitions may be calculated. Accurate hyperfine parameters for both vibrational levels were determined and the vibrational dependence of the Fermi contact interaction was resolved. The hyperfine parameters agree well with recent many-body perturbation theory calculations.
Hovde, David C.↗
Delocalization of dark and bright excitons in flat-band materials and the optical properties of V2O5
Abstract The simplest picture of excitons in materials with atomic-like localization of electrons is that of Frenkel excitons, where electrons and holes stay close together, which is associated with a large binding energy. Here, using the example of the layered oxide V 2 O 5 , we show how localized charge-transfer excitations combine to form excitons that also have a huge binding energy but, at the same time, a large electron-hole distance, and we explain this seemingly contradictory finding. The anisotropy of the exciton delocalization is determined by the local anisotropy of the structure, whereas the exciton extends orthogonally to the chains formed by the crystal structure. Moreover, we show that the bright exciton goes together with a dark exciton of even larger binding energy and more pronounced anisotropy. These findings are obtained by combining first principles many-body perturbation theory calculations, ellipsometry experiments, and tight binding modelling, leading to very good agreement and a consistent picture. Our explanation is general and can be extended to other materials.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Magnetically confined surface and bulk excitons in a layered antiferromagnet
The discovery of two-dimensional van der Waals magnets has greatly expanded our ability to create and control nanoscale quantum phases. A unique capability emerges when a two-dimensional magnet is also a semiconductor that features tightly bound excitons with large oscillator strengths that fundamentally determine the optical response and are tunable with magnetic fields. Here, in this study, we report a previously unidentified type of optical excitation-a magnetic surface exciton-enabled by the antiferromagnetic spin correlations that confine excitons to the surface of CrSBr. Magnetic surface excitons exhibit stronger Coulomb attraction, leading to a higher binding energy than excitons confined in bulk layers, and profoundly alter the optical response of few-layer crystals. Distinct magnetic confinement of surface and bulk excitons is established by layer- and temperature-dependent exciton reflection spectroscopy and corroborated by ab initio many-body perturbation theory calculations. By quenching interlayer excitonic interactions, the antiferromagnetic order of CrSBr strictly confines the bound electron-hole pairs within the same layer, regardless of the total number of layers. Our work unveils unique confined excitons in a layered antiferromagnet, highlighting magnetic interactions as a vital approach for nanoscale quantum confinement, from few layers to the bulk limit.
36 MATERIALS SCIENCE↗
Renormalization of states and quasiparticles in many-body downfolding
We explore the principles of many-body Hamiltonian complexity reduction via downfolding on an effective low-dimensional representation. We show that the renormalization factor provides a unique measure of the quality of the compression as it directly represents the projection between the approximate stationary state of the many-body Hamiltonian and the full many-body wavefunction. Hence, the renormalization factor is a measure of fidelity between the effective (reduced-rank) description and the full many-body treatment for arbitrary (i.e., ground and excited) states. When the entire problem is mapped on a system of interacting quasiparticles [Romanova et al., npj Comput. Mater. 9, 126 (2023)], the effective Hamiltonians can faithfully reproduce the physics only when a clear energy scale separation exists between the subsystems and their environment. We also demonstrate that it is necessary to include quasiparticle renormalization at distinct energy scales, capturing the distinct interaction between subsystems and their surrounding environments. Numerical results from simple, exactly solvable models highlight the limitations and strengths of this approach, particularly for ground and low-lying excited states. This work lays the groundwork for applying dynamical downfolding techniques to problems concerned with (quantum) interfaces.
Green-functions technique↗
Dark-exciton energy splitting in monolayer W Se 2 : Insights from time-dependent density functional theory
Here, we present here a formalism based on time-dependent density functional theory to describe characteristics of both intra- and intervalley excitons in semiconductors, the latter of which had remained a challenge. Through the usage of an appropriate exchange-correlation kernel (nanoquanta), we trace the energy difference between the intra- and intervalley dark excitons in monolayer (1L) W Se 2 to the domination of the exchange part in the exchange-correlation energies of these states. Furthermore, our calculated transition contribution maps establish the momentum resolved weights of the electron-hole excitations in both bright and dark excitons thereby providing a comprehensive understanding of excitonic properties of 1L W Se 2 . We find that the states consist of hybridized excitations around the corresponding valleys which leads to brightening of the dark excitons, i.e., significantly decreasing their lifetime which is reflected in the PL spectrum. Using many-body perturbation theory, we calculate the phonon contribution to the energy band gap and the linewidths of the excited electrons, holes, and (bright) exciton to find that as the temperature increases the band gap significantly decreases, while the linewidths increase. Our work paves for describing the ultrafast charge dynamics of transition metal dichalcogenide within an ab initio framework.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Modeling Liquid Water by Climbing up Jacob’s Ladder in Density Functional Theory Facilitated by Using Deep Neural Network Potentials
Within the framework of Kohn–Sham density functional theory (DFT), the ability to provide good predictions of water properties by employing a strongly constrained and appropriately normed (SCAN) functional has been extensively demonstrated in recent years. Here, we further advance the modeling of water by building a more accurate model on the fourth rung of Jacob’s ladder with the hybrid functional, SCAN0. In particular, we carry out both classical and Feynman path-integral molecular dynamics calculations of water with the SCAN0 functional and the isobaric–isothermal ensemble. To generate the equilibrated structure of water, a deep neural network potential is trained from the atomic potential energy surface based on ab initio data obtained from SCAN0 DFT calculations. For the electronic properties of water, a separate deep neural network potential is trained by using the Deep Wannier method based on the maximally localized Wannier functions of the equilibrated trajectory at the SCAN0 level. The structural, dynamic, and electric properties of water were analyzed. The hydrogen-bond structures, density, infrared spectra, diffusion coefficients, and dielectric constants of water, in the electronic ground state, are computed by using a large simulation box and long simulation time. For the properties involving electronic excitations, we apply the GW approximation within many-body perturbation theory to calculate the quasiparticle density of states and bandgap of water. Compared to the SCAN functional, mixing exact exchange mitigates the self-interaction error in the meta-generalized-gradient approximation and further softens liquid water toward the experimental direction. For most of the water properties, the SCAN0 functional shows a systematic improvement over the SCAN functional. However, some important discrepancies remain. The H-bond network predicted by the SCAN0 functional is still slightly overstructured compared to the experimental results.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Finding predictive models for singlet fission by machine learning
Singlet fission (SF), the conversion of one singlet exciton into two triplet excitons, could significantly enhance solar cell efficiency. Molecular crystals that undergo SF are scarce. Computational exploration may accelerate the discovery of SF materials. However, many-body perturbation theory (MBPT) calculations of the excitonic properties of molecular crystals are impractical for large-scale materials screening. We use the sure-independence-screening-and-sparsifying-operator (SISSO) machine-learning algorithm to generate computationally efficient models that can predict the MBPT thermodynamic driving force for SF for a dataset of 101 polycyclic aromatic hydrocarbons (PAH101). SISSO generates models by iteratively combining physical primary features. The best models are selected by linear regression with cross-validation. The SISSO models successfully predict the SF driving force with errors below 0.2 eV. Based on the cost, accuracy, and classification performance of SISSO models, we propose a hierarchical materials screening workflow. Three potential SF candidates are found in the PAH101 set.
36 MATERIALS SCIENCE↗
Many-body perturbation theory with hybrid density functional theory starting points accelerated by adaptively compressed exchange
We report on the use of the adaptively compressed exchange (ACE) operator to accelerate many-body perturbation theory (MBPT) calculations, including G 0 W 0 and the Bethe–Salpeter equation (BSE), for hybrid density functional theory starting points. We show that by approximating the exact exchange operator with the low-rank ACE operator, substantial computational savings can be achieved with systematically controllable errors in the quasiparticle energies computed with full-frequency G 0 W 0 and the optical absorption spectra and vertical excitation energies computed by solving the BSE within density matrix perturbation theory. Our implementation makes use of the ACE-accelerated electronic Hamiltonian to carry out both G 0 W 0 and BSE without explicitly computing empty states. We show the robustness of the approach and present the computational gains obtained on both the central processing unit and graphics processing unit nodes. In conclusion, our work will facilitate the exploration and evaluation of fine-tuned hybrid starting points aimed at enhancing the accuracy of MBPT calculations without involving computationally demanding self-consistency in Hedin’s equations.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
First-Principles Understanding of Optical Excitations within Low-Dimensional Materials
The objective of this project is to utilize first-principles computational approaches to understand optical excitations within two-dimensional monolayers and heterostructures, with the ultimate goal of designing new materials by modifying the chemical and physical structure on the nanoscale. In 2D heterostructures, the nature and movement of the exciton is determined to a large extent by the electron-electron and electron-phonon strengths within individual monolayers, as well as the coupling between layers, all of which in turn depend on chemistry, solid-state screening properties, and quantum confinement. Controlling the nature and migration properties of excitons requires an understanding of the complex relationship between electrons, phonons, defects, disorder, and dynamics. The aim of this project is to determine, by analysis of highly accurate density functional theory (DFT) and many-body perturbation theory (MBPT) calculations, how these complexities can be decomposed into simple, tunable parameters. The specific goals of this project are to 1) understand electron conductivity, absorption and transparency of monolayer semiconductors and metals; 2) develop a theory of excitons near defects in low dimensions; and 3) understand the influence of inter-layer interactions in heterostructures.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Comprehensive Laboratory Measurements Resolving the LMM Dielectronic Recombination Satellite Lines in Ne-like Fe XVII Ions
We investigated experimentally and theoretically dielectronic recombination (DR) populating doubly excited configurations 3l3l¢ (LMM) in Fe XVII, the strongest channel for soft X-ray line formation in this ubiquitous species. We used two different electron beam ion traps and two complementary measurement schemes for preparing the Fe XVII samples and evaluating their purity, observing negligible contamination effects. This allowed us to diagnose the electron density in both EBITs. We compared our experimental resonant energies and strengths with those of previous independent work at a storage ring as well as those of configuration interaction, multiconfiguration Dirac–Fock calculations, and many-body perturbation theory. This last approach showed outstanding predictive power in the comparison with the combined independent experimental results. From these we also inferred DR rate coefficients, unveiling discrepancies from those compiled in the OPEN-ADAS and AtomDB databases.
Filipe Grilo↗
K-shell Emission from O vi Near 19 Å
Abstract Laboratory measurements of O vi K-shell emission lines are presented that are situated near the O viii Ly α line at 19 Å. The data provide additional rest-frame references for velocity determinations based on absorption features in the spectra of warm absorbers in active galactic nuclei and other astrophysical objects. They also provide benchmarks for testing atomic structure calculations of energy levels with electrons in a high principal quantum number ( n = 3, 4). Excellent agreement is found with our calculations using the many-body perturbation theory method, and we provide a complete listing of the O vi energy levels calculated with this approach.
Beiersdorfer, Peter (ORCID:000000030127599X)↗
Diagrammatic perturbation theory - N2 X1 Sigma/plus/g
The diagrammatic many-body perturbation theory is used to calculate the correlation energy of the nitrogen molecule in its electronic ground state. Using the algebraic approximation, the energy is evaluated through third order, including all many-body effects. (2/1) Pade approximants and variational upper bounds are constructed. For one of the perturbation expansions considered, the (2/1) Pade approximant leads to the recovery of 79.5 percent of the empirical correlation energy, while the variational upper bound recovers 72.0 percent. Three-body effects are examined in some detail. The relationships with previous work on N2 are discussed.
Wilson, S.↗
Bending effects and optical properties of WSe 2 nanoribbons of topological phase
A WSe 2 monolayer of 1T' phase is a large band gap quantum spin Hall insulator, supporting dissipationless charge and spin transports through the topologically protected edge states. Here, in this work, we explore the nanoribbon forms of 1T' phase WSe 2 by first-principles density functional calculations and the many-body perturbation GW and Bethe-Salpeter equation method. We found that the 1T' WSe 2 nanoribbon can show topological edge states with a ribbon width of ~4-6 nm. Those edge bands show crossing through the Fermi level an odd number of times, with one kind of spin-polarization connecting the valence band continuum and conduction band continuum. The topological features of the edge bands hold even under small and medium bending in the nanoribbon, while large bending induces large band splitting, resulting in a topological switch-off in the edge bands. The semiconducting 1T' WSe2 nanoribbon shows a large tunability with bending in optical absorption spectra and exciton states. The lowest-energy exciton is changed from optically dark in the flat nanoribbon to bright in the bent nanoribbons. These properties in the 1T' WSe 2 nanoribbons suggest potential applications in controllable quantum electronics and exciton-based quantum information processes.
36 MATERIALS SCIENCE↗