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We compare the performance of an approach using real frequency dependent polarizability to compute optical absorption spectra to linear-response time-dependent density functional theory (TD-DFT) for small organic dyes, oligomers of…

Materials Science · Physics 2018-05-22 Ang Siong Tuan , Amrita Pal , Sergei Manzhos

We present a variational principle for the extraction of a time-dependent orthonormal basis from random realizations of transient systems. The optimality condition of the variational principle leads to a closed-form evolution equation for…

Numerical Analysis · Mathematics 2020-07-01 Hessam Babaee

Recently introduced time-dependent renormalized-natural-orbital theory (TDRNOT) is based on the equations of motion for the so-called natural orbitals, i.e., the eigenfunctions of the one-body reduced density matrix. Exact TDRNOT can be…

Atomic Physics · Physics 2016-01-13 M. Brics , J. Rapp , D. Bauer

We show that quantum optimal control theory (OCT) and time-dependent density-functional theory (TDDFT) can be combined to provide realistic femtosecond laser pulses for an enhanced ionization yield in many-electron systems. Using the…

Atomic Physics · Physics 2015-06-17 M. Hellgren , E. Rasanen , E. K. U. Gross

An $\it{ab \,\, initio}$ based fully microscopic approach is applied to study the nonlinear optical response of bulk Tellurium. The structural and electronic properties are calculated from first principles using the shLDA-1/2 method within…

Optics · Physics 2021-08-20 S. C. Liebscher , M. K. Hagen , J. Hader , J. V. Moloney , S. W. Koch

Recent theoretical studies on the nonlinear response of spin and orbital degrees of freedom have discovered spin and orbital analogs of the photocurrent, with potential for characterizing topological materials and for applications. In this…

Mesoscale and Nanoscale Physics · Physics 2026-04-01 Kakeru Tanaka , Hiroaki Ishizuka

The primary computational challenge when simulating nonadiabatic ab initio molecular dynamics is the unfavorable compute costs of electronic structure calculations with molecular size. Simple electronic structure theories, like…

Chemical Physics · Physics 2023-06-28 Justin J. Talbot , Martin Head-Gordon , Stephen J. Cotton

Time-dependent orbital-free density functional theory (TD-OFDFT) is an efficient ab-initio method for calculating the electronic dynamics of large systems. In comparison to standard TD-DFT, it computes only a single electronic state…

Chemical Physics · Physics 2021-12-15 Kaili Jiang , Xuecheng Shao , Michele Pavanello

A combined approach of first-principles density-functional calculations and the systematic cluster-expansion scheme is presented. The dipole, quadrupole, and Coulomb matrix elements obtained from ab initio calculations are used as an input…

Materials Science · Physics 2016-06-29 O. Vänskä , M. Ljungberg , P. Springer , D. Sánchez-Portal , M. Kira , S. W. Koch

We formulate gaussian and circular random-matrix models representing a coupled system consisting of an absorbing and an amplifying resonator, which are mutually related by a generalized time-reversal symmetry. Motivated by optical…

Quantum Physics · Physics 2012-12-21 Christopher Birchall , Henning Schomerus

Time-dependent structural reliability analysis of nonlinear dynamical systems is non-trivial; subsequently, scope of most of the structural reliability analysis methods is limited to time-independent reliability analysis only. In this work,…

Machine Learning · Statistics 2024-09-21 Navaneeth N. , Souvik Chakraborty

We derive equations of motion for bivariational wave functions with orthogonal adaptive basis sets and specialize the formalism to the coupled cluster ansatz. The equations are related to the biorthogonal case in a transparent way, and…

Chemical Physics · Physics 2023-11-06 Mads Greisen Højlund , Alberto Zoccante , Ove Christiansen

A robust and efficient frequency dependent and non-local exchange-correlation $f_{xc}(r,r';\omega)$ is derived by imposing time-dependent density-functional theory (TDDFT) to reproduce the many-body diagrammatic expansion of the…

Materials Science · Physics 2009-11-10 A. Marini , R. Del Sole , A. Rubio

We present accurate optical spectra of semiconductors and insulators within a pure Kohn-Sham time-dependent density-functional approach. In particular, we show that the onset of the absorption is well reproduced when comparing to…

Materials Science · Physics 2020-03-18 Sarah Cavo , J. A. Berger , Pina Romaniello

We investigate the numerical stability of time-dependent coupled-cluster theory for many-electron dynamics in intense laser pulses, comparing two coupled-cluster formulations with full configuration interaction theory. Our numerical…

Time-dependent electronic structure methods provide an efficient, accurate, and robust alternative to traditional time dependent methods for computing both linear and non-linear optical properties. With this in mind, we have developed the…

Chemical Physics · Physics 2026-01-26 Thomas Knoll , Benjamin G. Levine

Time-dependent quantities are calculated in the linear response limit for a correlated one dimensional model atom driven by an external quadrupolar time-dependent field. Besides the analysis of the time-evolving energy change in the…

Quantum Physics · Physics 2015-01-29 I. Nagy , I. Aldazabal , M. L. Glasser

We present a comprehensive theoretical framework for calculating the linear and nonlinear optical responses of time-periodic quantum systems. Using density matrix evolution in the Floquet basis and adopting the length gauge, our approach…

Materials Science · Physics 2025-03-10 S. Sajad Dabiri , Reza Asgari

In the present work, a new time-dependent exchange theory is presented wherein the symmetry constraints, on a multi-electron wavefunction, are properly accounted for. In so doing, the equations of motion, incorporating the required…

Computational Physics · Physics 2007-05-23 Charles A. Weatherford

Using a super-operator formulation of linearized time-dependent density-functional theory, the dynamical polarizability of a system of interacting electrons is given a matrix continued-fraction representation whose coefficients can be…

Materials Science · Physics 2009-11-11 B. Walker , A. M. Saitta , R. Gebauer , S. Baroni