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We perform ab initio simulations of the total and partial Auger decay widths of 1s^-1, 2s^-1, and 2p^-1 ionized hydrogen sulfide and 2s^-1 ionized argon with non-Hermitian quantum chemistry. We use coupled cluster theory with single and…

化学物理 · 物理学 2024-02-28 Jan Philipp Drennhaus , Anthuan Ferino-Pérez , Florian Matz , Thomas-C. Jagau

We report the first coupled-cluster study of Auger decay in heavy metals. The zinc atom is used as a case study due to its relevance to the Auger emission properties of the $^{67}$Ga radionuclide. Coupled-cluster theory combined with…

化学物理 · 物理学 2024-03-01 Anthuan Ferino-Pérez , Thomas-C. Jagau

The emission of an Auger electron is the predominant relaxation mechanism of core-vacant states in molecules composed of light nuclei. In this non-radiative decay process, one valence electron fills the core vacancy while a second valence…

化学物理 · 物理学 2023-01-24 Florian Matz , Thomas-C. Jagau

Vacancies in the L1 shell of atoms and molecules can decay non-radiatively via Coster-Kronig decay whereby the vacancy is filled by an electron from the L2,3 shell while a second electron is emitted into the ionization continuum. This…

化学物理 · 物理学 2024-07-26 Jan Philipp Drennhaus , Anthuan Ferino Pérez , Florian Matz , Thomas-C. Jagau

Efficiently and accurately computing molecular Auger electron spectra for larger systems is limited by the increasing complexity of the scaling in the number of doubly ionized final states with respect to the system size. In this work, we…

We report on theoretical Auger electron kinetic energy distribution originated from sequential two-step Auger decays of molecular double core-hole (DCH) state, using CH4, NH3 and H2CO molecules as representative examples. For CH4 and NH3…

化学物理 · 物理学 2015-05-30 Motomichi Tashiro , Kiyoshi Ueda , Masahiro Ehara

Results of the most sophisticated measurements in coincidence of the angular resolved K-shell photo- and Auger-electrons, and of two atomic ions produced by dissociation of N2 molecule, are analyzed. Detection of photoelectrons at certain…

Electronic resonances are metastable states with finite lifetimes, encountered in processes such as photodetachment, electron transmission, and Auger decay. Resonances appear in Hermitian quantum mechanics as increased density of states in…

化学物理 · 物理学 2025-11-10 Cansu Utku , Garrette Pauley Paran , Thomas-C. Jagau

We discuss a new strategy to compute partial Auger decay widths with equation-of-motion ionisation-potential coupled-cluster (EOMIP-CCSD) wave functions in the framework of non-Hermitian quantum mechanics, where the decaying character of…

化学物理 · 物理学 2025-02-04 Florian Matz , Angelos Gkogkos , Thomas-C. Jagau

Second-order Moller-Plesset perturbation theory (MP2) provides accurate correlation energies for periodic systems but suffers from finite-size errors (FSEs) that have inverse volume scaling due to the Coulomb kernel singularity in…

计算物理 · 物理学 2026-05-14 Stephen Jon Quiton , Juan D. F. Pottecher , Martin Head-Gordon , Lin Lin

We report on the application of the recently developed Fano-ADC(2,2) method to compute total and partial Auger decay widths of molecular core-hole states, including explicit evaluation of double Auger decay branching ratios. The method…

化学物理 · 物理学 2024-11-11 Přemysl Kolorenč

A new perturbative approach to canonical equation-of-motion coupled-cluster theory is presented using coupled-cluster perturbation theory. A second-order M{\o}ller-Plesset partitioning of the Hamiltonian is used to obtain the well known…

化学物理 · 物理学 2015-07-09 Jason N. Byrd , Varun Rishi , Ajith Perera , Rodney J. Bartlett

A mixed quantum mechanical and Monte Carlo method for calculating Auger spectra from nanoclusters is presented. The approach, based on a cluster method, consists of two steps. Ab initio quantum mechanical calculations are first performed to…

The calculation of the MP2 correlation energy for extended systems can be viewed as a multi-dimensional integral in the thermodynamic limit, and the standard method for evaluating the MP2 energy can be viewed as a trapezoidal quadrature…

计算物理 · 物理学 2023-04-10 Xin Xing , Xiaoxu Li , Lin Lin

We propose a computationally simple model of Auger and APECS line shapes from open-band solids. Part of the intensity comes from the decay of unscreened core-holes and is obtained by the two-body Green's function $G^{(2)}_{\omega}$, as in…

强关联电子 · 物理学 2009-10-31 A. Marini , M. Cini

Quantum chemical methods dealing with challenging systems while retaining low computational costs have attracted attention. In particular, many efforts have been devoted to developing new methods based on the second-order perturbation that…

化学物理 · 物理学 2023-10-30 Nhan Tri Tran , Hoang Thanh Nguyen , Lan Nguyen Tran

We present second-order molecular cluster perturbation theory (MCPT(2)), a linear scaling methodology to calculate arbitrarily large systems with explicit calculation of individual wavefunctions in a coupled-cluster framework. This new…

In this work we outline a general method for calculating Auger spectra in molecules, which accounts for the underlying symmetry of the system. This theory starts from Fano's formulation of the interaction between discrete and continuum…

材料科学 · 物理学 2021-02-23 Simone Taioli , Stefano Simonucci

We develop and test methods that include second and third-order perturbation theory (MP3) using orbitals obtained from regularized orbital-optimized second-order perturbation theory, $\kappa$-OOMP2, denoted as MP3:$\kappa$-OOMP2. Testing…

化学物理 · 物理学 2019-10-15 Luke W. Bertels , Joonho Lee , Martin Head-Gordon

Coupled-cluster theory with single and double excitations (CCSD) is a promising ab initio method for the electronic structure of three-dimensional metals, for which second-order perturbation theory (MP2) diverges in the thermodynamic limit.…

材料科学 · 物理学 2021-06-16 James M. Callahan , Malte F. Lange , Timothy C. Berkelbach
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