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Long-range charge transfer excited states are notoriously badly underestimated in time-dependent density functional theory (TDDFT). We resolve how {\it exact} TDDFT captures charge transfer between open-shell species: in particular the role…

Chemical Physics · Physics 2009-11-11 Neepa T. Maitra

The adiabatic approximation in time-dependent density functional theory (TDDFT) yields reliable excitation spectra with great efficiency in many cases, but fundamentally fails for states of double excitation character. We discuss how…

Chemical Physics · Physics 2015-05-27 Peter Elliott , Sharma Goldson , Chris Canahui , Neepa T. Maitra

In the past decade, classical dynamical density functional theory (DDFT) has been developed and widely applied to the Brownian dynamics of interacting colloidal particles. One of the possible derivation routes of DDFT from the microscopic…

Soft Condensed Matter · Physics 2014-01-28 Raphael Wittkowski , Hartmut Löwen , Helmut R. Brand

We explore a new formalism to study the nonlinear electronic density response based on Kohn-Sham density functional theory (KS-DFT) at partially and strongly quantum degenerate regimes. It is demonstrated that the KS-DFT calculations are…

Plasma Physics · Physics 2022-05-10 Zhandos Moldabekov , Jan Vorberger , Tobias Dornheim

Charge transfer complexes are materials with a wide range of interesting optical and electronic properties. They have seen a great deal of research over the past decade, both in device development as well as research to elucidate the…

Materials Science · Physics 2024-06-04 Satwik Ramanjanappa , Edward R Van Keuren

Inspired by the formulation of quantum-electrodynamical time-dependent density functional theory (QED-TDDFT) by Rubio and coworkers, we propose an implementation that uses dimensionless amplitudes for describing the photonic contributions…

Materials Science · Physics 2021-08-20 Junjie Yang , Qi Ou , Zheng Pei , Hua Wang , Binbin Weng , Kieran Mullen , Yihan Shao

Photo-active systems are characterized by their capacity of absorbing light energy and transforming it. Usually, more than one chromophore is involved in the light absorption and excitation transport processes in complex systems.…

Materials Science · Physics 2019-05-21 Joaquim Jornet-Somoza , Irina Lebedeva

We show that the analytic structure of the dynamical xc kernels of semiconductors and insulators can be sensed in terms of its poles which mark physically relevant frequencies of the system where the counter-phase motion of discrete…

Materials Science · Physics 2023-04-19 D. R. Gulevich , Ya. V. Zhumagulov , V. Kozin , I. V. Tokatly

We derive an exact representation of the exchange-correlation energy within density functional theory (DFT) which spawns a class of approximations leading to correct long-range asymptotic behavior. In what amounts to be the simplest…

Materials Science · Physics 2009-11-10 Roi Baer , Daniel Neuhauser

Linear-response time-dependent density functional theory (LR-TDDFT) simulations of disordered extended systems require averaging over different snapshots of ion configurations to minimize finite size effects due to the snapshot--dependence…

Computational Physics · Physics 2023-07-19 Zhandos A. Moldabekov , Jan Vorberger , Mani Lokamani , Tobias Dornheim

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

We describe the inclusion of electrodynamic fields in Time-Dependent Density Functional Theory (TDDFT) by incorporating both the induced scalar and vector potentials within the time-dependent Kohn-Sham equation. The Hamiltonian is described…

Chemical Physics · Physics 2020-07-01 Dor Gabay , Ali Yilmaz , Vitaliy Lomakin , Amir Boag , Amir Natan

The influence of inner electrons on the ionization dynamics in strong laser fields is investigated in a wavelength regime where the inner electron dynamics is usually assumed to be negligible. The role of inner electrons is of particular…

Atomic Physics · Physics 2014-03-11 J. Rapp , D. Bauer

An atomic-orbital basis set framework is presented for carrying out velocity- gauge real-time time-dependent density functional theory (TDDFT) simulations in periodic systems employing range-separated hybrid functionals. Linear optical…

Materials Science · Physics 2018-10-02 C. D. Pemmaraju

We calculate the energy deposition by very short laser pulses in SiO_2 (alpha-quartz) with a view to establishing systematics for predicting damage and nanoparticle production. The theoretical framework is time-dependent density functional…

Materials Science · Physics 2015-11-18 S. A. Sato , K. Yabana , Y. Shinohara , T. Otobe , K. M. Lee , G. F. Bertsch

Delivering the full benefits of first principles calculations to battery materials demands the development of accurate and computationally-efficient electronic structure methods that incorporate the effects of the electrolyte environment…

Simulations and diagnostics of high-energy-density plasmas and warm dense matter rely on models of material response properties, both static and dynamic (frequency-dependent). Here, we systematically investigate variations in dynamic…

Using dynamical density functional theory (DDFT) methods we investigate the laning instability of a sheared colloidal suspension. The nonequilibrium ordering at the laning transition is driven by non-affine particle motion arising from…

Soft Condensed Matter · Physics 2018-01-03 Alberto Scacchi , Andrew J. Archer , Joseph M. Brader

In principle, we should not need the time-dependent extension of density-functional theory (TDDFT) for excitations, and in particular not for Molecular Dynamics (MD) studies: the theorem by Hohenberg and Kohn teaches us that for any…

Strongly Correlated Electrons · Physics 2015-05-27 J. L. Alonso , Alberto Castro , Pablo Echenique , Angel Rubio

First-order nonadiabatic coupling matrix elements (fo-NACMEs) are the basic quantities in theoretical descriptions of electronically nonadiabatic processes that are ubiquitous in molecular physics and chemistry. Given the large size of…

Chemical Physics · Physics 2021-05-25 Zikuan Wang , Chenyu Wu , Wenjian Liu