A5018513278- Advanced Chemical Physics Studies
- Machine Learning in Materials Science
- Spectroscopy and Quantum Chemical Studies
- Electron and X-Ray Spectroscopy Techniques
- Molecular Junctions and Nanostructures
- Graphene research and applications
- Quantum and electron transport phenomena
- Surface and Thin Film Phenomena
- Catalytic Processes in Materials Science
- Photochemistry and Electron Transfer Studies
- Luminescence and Fluorescent Materials
- Surface Chemistry and Catalysis
- Spectroscopy and Laser Applications
- 2D Materials and Applications
- Nonlinear Optical Materials Research
- Inorganic Fluorides and Related Compounds
- Magnetic confinement fusion research
- Covalent Organic Framework Applications
- Particle accelerators and beam dynamics
- Advanced Data Storage Technologies
- Metal-Organic Frameworks: Synthesis and Applications
- Crystallography and molecular interactions
- Thermal Expansion and Ionic Conductivity
- X-ray Spectroscopy and Fluorescence Analysis
- Solid-state spectroscopy and crystallography
TU Dresden
2022-2025
Aalto University
2017-2022
University of Zurich
2013-2017
Leipzig University
2012-2013
CP2K is an open source electronic structure and molecular dynamics software package to perform atomistic simulations of solid-state, liquid, molecular, biological systems. It especially aimed at massively parallel linear-scaling methods state-of-the-art ab initio simulations. Excellent performance for calculations achieved using novel algorithms implemented modern high-performance computing This review revisits the main capabilities efficient accurate The emphasis put on density functional...
The GW approximation of many-body perturbation theory is an accurate method for computing electron addition and removal energies molecules solids. In a canonical implementation, however, its computational cost O(N4) in the system size N, which prohibits application to many systems interest. We present full-frequency algorithm Gaussian-type basis, whose scales with N2 N3. implementation optimized massively parallel execution on state-of-the-art supercomputers suitable nanostructures gas,...
An extensive study of interaction energies in ion pairs pyrrolidinium and imidazolium ionic liquids is presented. The Cnmpyr Cnmim cations with varying alkyl chains from Methyl, Ethyl, n-Propyl to n-Butyl were combined a wide range routinely used IL anions such as chloride, bromide, mesylate (CH3SO3 or Mes), tosylate (CH3PhSO3 Tos), bis(trifluoromethanesulfonyl)amide (NTf2), dicyanamide (N(CN)2 dca), tetrafluoroborate (BF4) hexafluorophosphate (PF6). A number energetically favourable...
The GW method is routinely used to predict charged valence excitations in molecules and solids. However, the numerical techniques employed most efficient algorithms break down when computing core as measured by X-ray photoelectron spectroscopy (XPS). We present a full-frequency approach on real axis using localized basis enable treatment of levels GW. Our scheme based contour deformation technique allows for precise calculation self-energy, which has complicated pole structure states....
We present an accurate approach to compute X-ray photoelectron spectra based on the $GW$ Green's function method, that overcomes shortcomings of common density functional theory approaches. has become a popular tool valence excitations for wide range materials. However, core-level spectroscopy is thus far almost uncharted in $GW$. show single-shot perturbation calculations $G_0W_0$ approximation, which are routinely used states, cannot be applied core levels and suffer from extreme,...
Abstract Data science and machine learning in materials require large datasets of technologically relevant molecules or materials. Currently, publicly available molecular with realistic geometries spectral properties are rare. We here supply a diverse benchmark spectroscopy dataset 61,489 extracted from organic crystals the Cambridge Structural Database (CSD), denoted OE62. Molecular equilibrium reported at Perdew-Burke-Ernzerhof (PBE) level density functional theory (DFT) including van der...
The GW approximation has recently gained increasing attention as a viable method for the computation of deep core-level binding energies measured by X-ray photoelectron spectroscopy. We present comprehensive benchmark study different methodologies (starting point optimized, partial and full eigenvalue-self-consistent, Hedin shift, renormalized singles) molecular inner-shell excitations. demonstrate that all methods yield unique solution apply them to CORE65 set ethyl trifluoroacetate. Three...
We present a quantitatively accurate machine-learning (ML) model for the computational prediction of core-electron binding energies, from which X-ray photoelectron spectroscopy (XPS) spectra can be readily obtained. Our combines density functional theory (DFT) with
$GW$ is an accurate method for computing electron addition and removal energies of molecules solids. In a conventional implementation, however, its computational cost $O(N^4)$ in the system size $N$, which prohibits application to many systems interest. We present low-scaling algorithm with notably improved accuracy compared our previous [J. Phys. Chem. Lett. 2018, 9, 306-312]. This demonstrated frontier orbitals using $GW100$ benchmark set, yields mean absolute deviation only 6 meV respect...
We present an accurate computational approach to calculate absolute K-edge core electron excitation energies as measured by X-ray absorption spectroscopy. Our employs all-electron Bethe-Salpeter equation (BSE) formalism based on GW quasiparticle (BSE@GW) using numeric atom-centered orbitals (NAOs). The BSE@GW method has become increasingly popular for the computation of neutral valence molecules. However, it was so far not applied molecular energies. discuss influence different numerical...
In recent years, the GW method has emerged as a reliable tool for computing core-level binding energies. The contour deformation (CD) technique been established an efficient, scalable, and numerically stable approach to compute self-energy deep core excitations. However, calculations with CD face challenge of higher scaling respect system size N compared conventional quartic in valence-state algorithms. this work, we present CD-WAC [CD W analytic continuation (AC)], which reduces applied...
A novel method for including polarization effects within hybrid quantum mechanics/molecular mechanics (QM/MM) simulations of adsorbate-metal systems is presented. The interactions between adsorbate (QM) and metallic substrate (MM) are described at the MM level theory. Induction additionally accounted by applying image charge formulation. distribution induced modeled a set Gaussian charges (image charges) centered metal atoms. electrostatic response QM potential determined self-consistently...
With advanced synthetic techniques, a wide variety of well-defined graphene nanoribbons (GNRs) can be produced with atomic precision. Hence, finding the relation between their structures and properties becomes important for rational design GNRs. In this work, we explore complete chemical space gulf-edged zigzag (ZGNR-Gs), subclass GNRs in which edges miss carbon atoms regular sequence. We demonstrate that electronic ZGNR-Gs depend on four structural parameters: ribbon width, gulf edge size,...
Recently, the GW approach has emerged as a valuable tool for computing deep core-level binding energies measured in X-ray photoemission spectroscopy. However, fails to accurately predict shakeup satellite features, which arise from charge-neutral excitations accompanying ionization. In this work, we extend plus cumulant (GW + C) molecular 1s excitations, deriving conditions under C can be reliably applied processes. We present an efficient implementation with O(N4) scaling respect system...
Electrocatalytic reactions are influenced by various interfacial phenomena including nonspecific interaction forces. For many examples, their contributions to the catalytic cycle have yet be identified. Noncovalent interactions between electrode and electrolyte can described local electric field environment at interface experimentally accessible based on Vibrational Stark Effect. We herein present a carbon-based C2N-type electrocatalyst that is active for hydrogen evolution reaction contains...
The wetting of water on corrugated and flat hexagonal boron nitride (h-BN) monolayers Rh(111) is studied within a hybrid quantum mechanics/molecular mechanics (QM/MM) approach. Water treated by QM methods, whereas the interactions between liquid substrate are described at MM level. electrostatic properties reproduced assigning specifically generated partial charges to each atom. We propose method determine restrained potential (RESP) that can be applied periodic systems. Our approach based...
Four-center two-electron Coulomb integrals routinely appear in electronic structure algorithms. The resolution-of-the-identity (RI) is a popular technique to reduce the computational cost for numerical evaluation of these localized basis-sets codes. Recently, Duchemin and Blase proposed separable RI scheme [J. Chem. Phys. 150, 174120 (2019)], which preserves accuracy standard global method with metric permits formulation cubic-scaling random phase approximation (RPA) GW approaches. Here, we...
Electronic structure calculations based on many-body perturbation theory [e.g., GW or the random-phase approximation (RPA)] require function evaluations in complex time and frequency domain, for example, inhomogeneous Fourier transforms analytic continuation from imaginary axis to real axis. For transforms, time-frequency component of GreenX library provides grids that can be utilized low-scaling RPA implementations. In addition, adoption compact provided by our also reduces computational...
We present a relativistic correction scheme to improve the accuracy of 1s core-level binding energies calculated from Green's function theory in GW approximation, which does not add computational overhead. An element-specific corrective term is derived as difference between eigenvalues obtained self-consistent solutions non- or scalar-relativistic Kohn-Sham equations and four-component Dirac-Kohn-Sham for free neutral atom. examine dependence this on molecular environment amount exact...
Azizi et al., (2023). Time-frequency component of the GreenX library: minimax grids for efficient RPA and \textit{GW} calculations. Journal Open Source Software, 8(90), 5570, https://doi.org/10.21105/joss.05570
We present a new quantum embedding theory called dynamical configuration interaction (DCI) that combines wave function and Green's theories. DCI captures static correlation in correlated subspace with couples to high-energy, dynamic outside the many-body perturbation based on functions. In subspace, we use description avoid two-particle vertex, which greatly simplifies frequency structure of embedding. takes strengths both theories balance single, fully ab-initio concept. show treating...
Recent experimental duplexes of DNA stabilized by Ag cations, pairing homostrands guanine–guanine, cytosine–cytosine, adenine–thymine, and thymine–thymine, display much higher stability than the Watson–Crick paired duplexes; these broaden range applications for nanotechnology. Here we focus on silver-stabilized guanine in water. Using hybrid quantum mechanics/molecular mechanics simulations, propose an atomic structure Ag+-mediated duplex with two nucleobases per strand, G2–Ag2+–G2. We then...