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Molecular absorption and photo-electron spectra can be efficiently predicted with real-time time-dependent density-functional theory (TDDFT). We show here how these techniques can be easily extended to study time-resolved pump-probe…

Atomic and Molecular Clusters · Physics 2013-01-10 Umberto De Giovannini , Gustavo Brunetto , Alberto Castro , Jessica Walkenhorst , Angel Rubio

Real-time simulations of laser-driven electron dynamics contain information about molecular optical properties through all orders in response theory. These properties can be extracted by assuming convergence of the power series expansion of…

We report successful implementation of the time-dependent second-order many-body perturbation theory using optimized orthonormal orbital functions called time-dependent optimized second-order many-body perturbation theory [TD-OMP2] to reach…

Chemical Physics · Physics 2020-08-26 Himadri Pathak , Takeshi Sato , Kenichi L. Ishikawa

We report the formulation of a new, cost-effective approximation method in the time-dependent optimized coupled-cluster (TD-OCC) framework [T. Sato et al., J. Chem. Phys. 148, 051101 (2018)] for first-principles simulations of multielectron…

Chemical Physics · Physics 2022-08-11 Himadri Pathak , Takeshi Sato , Kenichi L. Ishikawa

We present a combined imaginary-time/real-time time-dependent (TD) approach for evaluating linear absorption spectra of open-shell systems at the electron attachment (EA) and ionization potential (IP) equation-of-motion coupled-cluster…

Chemical Physics · Physics 2026-05-05 P. D. Varuna S. Pathirage , Stephen H. Yuwono , Xiaosong Li , A. Eugene DePrince

A stochastic approach to time-dependent density functional theory (TDDFT) is developed for computing the absorption cross section and the random phase approximation (RPA) correlation energy. The core idea of the approach involves…

Chemical Physics · Physics 2016-11-04 Yi Gao , Daniel Neuhauser , Roi Baer , Eran Rabani

Recently introduced time-dependent renormalized-natural orbital theory (TDRNOT) is extended towards a multi-component approach in order to describe H$_2^+$ beyond the Born-Oppenheimer approximation. Two kinds of natural orbitals, describing…

Chemical Physics · Physics 2017-11-21 A. Hanusch , J. Rapp , M. Brics , D. Bauer

As part of a general study of the time-dependent local density approximation (TDLDA), we here report calculations of optical activity of chiral molecules. The theory automatically satisfies sum rules and the Kramers-Kronig relation between…

Chemical Physics · Physics 2009-10-31 K. Yabana , G. F. Bertsch

Recent advances in laser technology allow us to follow electronic motion at its natural time-scale with ultra-fast time resolution, leading the way towards attosecond physics experiments of extreme precision. In this work, we assess the use…

Other Condensed Matter · Physics 2016-06-22 Jessica Walkenhorst , Umberto De Giovannini , Alberto Castro , Angel Rubio

We formulate a time-dependent density functional theory (TDDFT) in terms of the density matrix to study ultrafast phenomena in semiconductor structures. A system of equations for the density matrix components, which is equivalent to the…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 V. Turkowski , C. A. Ullrich

Based on the work done by an electromagnetic field on an atomic or molecular electronic system, a general gauge invariant formulation of transient absorption spectroscopy is presented within the semi-classical approximation. Avoiding…

We present an implementation of time-dependent density-functional theory (TDDFT) in the linear response formalism enabling the calculation of low energy optical absorption spectra for large molecules and nanostructures. The method avoids…

Time-dependent coupled-cluster method with time-varying orbital functions, called time-dependent optimized coupled- cluster (TD-OCC) method, is formulated for multielectron dynamics in an intense laser field. We have successfully derived…

Chemical Physics · Physics 2018-03-14 Takeshi Sato , Himadri Pathak , Yuki Orimo , Kenichi L. Ishikawa

We present a new formulation of the time-dependent self-interaction correction (TDSIC). It is derived variationally obeying explicitly the constraints on orthonormality of the occupied single-particle orbitals. The thus emerging rather…

Quantum Physics · Physics 2009-03-02 J. Messud , P. M. Dinh , P. -G. Reinhard , E. Suraud

We investigate optical absorption spectra obtained through time-dependent density functional theory (TD-DFT) based on nonempirical hybrid functionals that are designed to correctly reproduce the dielectric function. The comparison with…

Materials Science · Physics 2020-08-17 Alexey Tal , Peitao Liu , Georg Kresse , Alfredo Pasquarello

In the presence of a (time-dependent) macroscopic electric field the electron dynamics of dielectrics cannot be described by the time-dependent density only. We present a real-time formalism that has the density and the macroscopic…

Materials Science · Physics 2016-07-27 M. Grüning , D. Sangalli , C. Attaccalite

The exact exchange potential in time-dependent density-functional theory is defined as an orbital functional through the time-dependent optimized effective potential (TDOEP) method. We numerically solve the TDOEP integral equation for the…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 H. O. Wijewardane , C. A. Ullrich

Linear-response time-dependent (TD) density-functional theory (DFT) has been implemented in the pseudopotential wavelet-based electronic structure program BigDFT and results are compared against those obtained with the all-electron…

We present an implementation and analysis of a stochastic high performance algorithm to calculate the correlation energy of three dimensional periodic systems in second-order M{\o}ller-Plesset perturbation theory (MP2). In particular we…

Chemical Physics · Physics 2018-02-12 Tobias Schäfer , Benjamin Ramberger , Georg Kresse

While providing a highly accurate framework for simulating laser-induced many-electron dynamics in atom and molecules, including linear and nonlinear steady-state and transient absorption spectra, time-dependent coupled-cluster theory does…

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