Wannier Function Approach to Realistic Coulomb Interactions in Layered Materials and Heterostructures

We introduce an approach to derive realistic Coulomb interaction terms in free standing layered materials and vertical heterostructures from ab-initio modelling of the corresponding bulk materials. To this end, we establish a combination of calculations within the framework of the constrained random phase approximation, Wannier function representation of Coulomb matrix elements within some low energy Hilbert space and continuum medium electrostatics, which we call Wannier function continuum electrostatics (WFCE). For monolayer and bilayer graphene we reproduce full ab-initio calculations of the Coulomb matrix elements within an accuracy of $0.2$eV or better. We show that realistic Coulomb interactions in bilayer graphene can be manipulated on the eV scale by different dielectric and metallic environments. A comparison to electronic phase diagrams derived in [M. M. Scherer et al., Phys. Rev. B 85, 235408 (2012)] suggests that the electronic ground state of bilayer graphene is a layered antiferromagnet and remains surprisingly unaffected by these strong changes in the Coulomb interaction.Comment: 12 pages, 8 figure

IL7RA haplotype-associated alterations in cellular immune function and gene expression patterns in multiple sclerosis

Interleukin-7 receptor alpha (IL7RA) is among the top listed candidate genes influencing the risk to develop multiple sclerosis (MS), an inflammatory demyelinating disease of the central nervous system. Soluble IL-7RA (sIL-7RA) protein and mRNA levels vary among the four common IL7RA haplotypes. Here we show and confirm that protective haplotype carriers have three times lower sIL-7RA serum levels than the other three haplotypes. High sIL-7RA concentrations significantly decrease IL-7-mediated STAT5 phosphorylation in CD4(+) T cells. Transcriptome analysis of unstimulated and stimulated CD4(+) T cells of MS patients carrying the different IL7RA haplotypes revealed complex and overlapping patterns in genes participating in cytokine signaling networks, apoptosis, cell cycle progression and cell differentiation. Our findings indicate that genetic variants of IL7RA result in haplotype-associated differential responsiveness to immunological stimuli that influence MS susceptibility not exclusively by varying levels of sIL-7RA

PROBING OPTICAL PROPERTIES OF CORRELATED CARBON DEFECTS IN HEXAGONAL-BN BY QUANTUM EMBEDDING APPROACH

In this work we study the optical properties of carbon dimer in bulk hexagonal boron nitride (BN). The utilization of density functional theory and many-body extended Hubbard models revealed the complex spectra, represented by bonding and anti-bonding states in-volved in optical transitions.The work was supported by the grant of the President of the Russian Federation, Project SP-2488.2021.1. The Flatiron Institute is a division of the Simons Foundation

Quantum embedding methods for correlated excited states of point defects: Case studies and challenges

A quantitative description of the excited electronic states of point defects and impurities is crucial for understanding materials properties, and possible applications of defects in quantum technologies. This is a considerable challenge for computational methods, since Kohn-Sham density functional theory (DFT) is inherently a ground-state theory, while higher-level methods are often too computationally expensive for defect systems. Recently, embedding approaches have been applied that treat defect states with many-body methods, while using DFT to describe the bulk host material. We implement such an embedding method, based on Wannierization of defect orbitals and the constrained random-phase approximation approach, and perform systematic characterization of the method for three distinct systems with current technological relevance: a carbon dimer replacing a B and N pair in bulk hexagonal BN (CBCN), the negatively charged nitrogen-vacancy center in diamond (NV-), and an Fe impurity on the Al site in wurtzite AlN (FeAl). In the context of these test-case defects, we demonstrate that crucial considerations of the methodology include convergence of the bulk screening of the active-space Coulomb interaction, the choice of exchange-correlation functional for the initial DFT calculation, and the treatment of the "double-counting"correction. For CBCN we show that the embedding approach gives many-body states in agreement with analytical results on the Hubbard dimer model, which allows us to elucidate the effects of the DFT functional and double-counting correction. For the NV- center, our method demonstrates good quantitative agreement with experiments for the zero-phonon line of the triplet-triplet transition. Finally, we illustrate challenges associated with this method for determining the energies and orderings of the complex spin multiplets in FeAl. © 2022 American Physical Society.National Science Foundation, NSF: DMR-1918455; Council on grants of the President of the Russian Federation: SP-2488.2021.1C.E.D. thanks A. Alkauskas, D. Wickramaratne, M. Zingl, A. Gali, M. Turiansky, T. Berkelbach, and A. Millis for fruitful conversations and comments on the manuscript. The Flatiron Institute is a division of the Simons Foundation. C.E.D. acknowledges support from the National Science Foundation under Grant No. DMR-1918455. The work of D.I.B. was supported by the grant of the President of the Russian Federation, Project No. SP-2488.2021.1

Downfolding from Ab Initio to Interacting Model Hamiltonians: Comprehensive Analysis and Benchmarking

Model Hamiltonians are regularly derived from first-principles data to describe correlated matter. However, the standard methods for this contain a number of largely unexplored approximations. For a strongly correlated impurity model system, here we carefully compare standard downfolding techniques with the best-possible ground-truth estimates for charge-neutral excited state energies and charge densities using state-of-the-art first-principles many-body wave function approaches. To this end, we use the vanadocene molecule and analyze all downfolding aspects, including the Hamiltonian form, target basis, double counting correction, and Coulomb interaction screening models. We find that the choice of target-space basis functions emerges as a key factor for the quality of the downfolded results, while orbital-dependent double counting correction diminishes the quality. Background screening to the Coulomb interaction matrix elements primarily affects crystal-field excitations. Our benchmark uncovers the relative importance of each downfolding step and offers insights into the potential accuracy of minimal downfolded model Hamiltonians.Comment: 15 pages (+8 pages Supplemental Material), 8 figure

The ground state of the carbon atom in strong magnetic fields

The ground and a few excited states of the carbon atom in external uniform magnetic fields are calculated by means of our 2D mesh Hartree-Fock method for field strengths ranging from zero up to 2.35 10^9 T. With increasing field strength the ground state undergoes six transitions involving seven different electronic configurations which belong to three groups with different spin projections S_z=-1,-2,-3. For weak fields the ground state configuration arises from the field-free 1s^2 2s^2 2p_0 2p_{-1}, S_z=-1 configuration. With increasing field strength the ground state involves the four S_z=-2 configurations 1s^22s2p_0 2p_{-1}2p_{+1}, 1s^22s2p_0 2p_{-1}3d_{-2}, 1s^22p_0 2p_{-1}3d_{-2}4f_{-3} and 1s^22p_{-1}3d_{-2}4f_{-3}5g_{-4}, followed by the two fully spin polarized S_z=-3 configurations 1s2p_02p_{-1}3d_{-2}4f_{-3}5g_{-4} and 1s2p_{-1}3d_{-2}4f_{-3}5g_{-4}6h_{-5}. The last configuration forms the ground state of the carbon atom in the high field regime \gamma>18.664. The above series of ground state configurations is extracted from the results of numerical calculations for more than twenty electronic configurations selected due to some general energetical arguments.Comment: 6 figures,acc. Phys.Rev.

High-resolution ptychographic imaging at a seeded free-electron laser source using OAM beams

Electromagnetic waves possessing orbital angular momentum (OAM) are powerful tools for applications in optical communications, new quantum technologies and optical tweezers. Recently, they have attracted growing interest since they can be harnessed to detect peculiar helical dichroic effects in chiral molecular media and in magnetic nanostructures. In this work, we perform single-shot per position ptychography on a nanostructured object at a seeded free-electron laser, using extreme ultraviolet OAM beams of different topological charge order $\ell$ generated with spiral zone plates. By controlling $\ell$, we demonstrate how the structural features of OAM beam profile determine an improvement of about 30% in image resolution with respect to conventional Gaussian beam illumination. This result extends the capabilities of coherent diffraction imaging techniques, and paves the way for achieving time-resolved high-resolution (below 100 nm) microscopy on large area samples.Comment: M. Pancaldi and F. Guzzi contributed equally to this wor