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The development of analytic-gradient methodology for excited states within conventional time-dependent density-functional theory (TDDFT) would seem to offer a relatively inexpensive alternative to better established quantum-chemical…

Other Condensed Matter · Physics 2010-08-11 Felipe Cordova , L. Joubert Doriol , Andrei Ipatov , Mark E. Casida , Claudia Filippi , Alberto Vela

For closed-shell systems, the local density approximation (LDA) and the LYP, BLYP, and B3LYP functionals are shown to be compatible with reference-state one-particle density-matrix theory, where this recently introduced formalism is based…

Chemical Physics · Physics 2009-11-10 James P. Finley

We theoretically investigate the three-dimensional (3D) electron dynamics of graphene in real space under strong laser fields using time-dependent density functional theory (TDDFT). We successfully reproduce the reversal of current…

Mesoscale and Nanoscale Physics · Physics 2026-02-11 S. Li , M. Tani , A. Hashmi , K. L. Ishikawa

The general expectation that, in principle, time-dependent density functional theory (TDDFT) be an exact formulation of the time-evolution of an interacting N-electron system is critically reexamined. It is demonstrated that the previous…

Other Condensed Matter · Physics 2007-08-13 J. Schirmer , A. Dreuw

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

Thermally activated delayed fluorescence has been reported in a number of OLED emitter materials engineered to have low singlet-triplet energy gaps. Here we derive closed solutions for steady state and transient behaviors, and apply these…

Chemical Physics · Physics 2016-04-11 Mitchell C. Nelson

The formation of H$^{3+}$ from ethane, propane, and butane dications was investigated with time-dependent density-functional theory (TDDFT) simulations. This approach offers the benefit of simultaneously addressing nuclear and electronic…

Chemical Physics · Physics 2025-08-14 C. Jiang , Samuel S. Taylor , Kedong Wang , Cody L. Covington , Kalman Varga

Time-dependent density-functional theory (TDDFT) is a computationally efficient first-principles approach for calculating optical spectra in insulators and semiconductors, including excitonic effects. We show how exciton wave functions can…

Materials Science · Physics 2020-12-29 Jared R. Williams , Nicolas Tancogne-Dejean , Carsten A. Ullrich

In this study, we propose a theoretical framework to investigate the interactions between flexible polymer chains, specifically polyelectrolytes (PEs). By calculating the system's free energy while considering position-dependent mutual…

Soft Condensed Matter · Physics 2024-05-13 Souradeep Ghosh

Triplet excitons have been the focus of considerable attention with regards to the functioning of polymer solar cells, because these species are long-lived and quench subsequently generated singlet excitons in their vicinity. The role of…

Chemical Physics · Physics 2018-02-14 Florian Steiner , John M. Lupton , Jan Vogelsang

The reliable prediction of optical and fundamental gaps of finite size systems using density functional theory requires to account for the potential self-interaction error, which is notorious for degrading the description of charge transfer…

Chemical Physics · Physics 2016-10-26 O. S. Bokareva , M. F. Shibl , M. J. Al-Marri , T. Pullerits , O. Kühn

We discuss two problems which are particularly challenging for approximations in time-dependent density functional theory (TDDFT) to capture: momentum-distributions in ionization processes, and memory-dependence in real-time dynamics. We…

Materials Science · Physics 2010-03-22 Arun K. Rajam , Paul Hessler , Christian Gaun , Neepa T. Maitra

This paper develops a quantitatively accurate first-principles description for the frequency and the linewidth of collective electronic excitations in inhomogeneous weakly disordered systems. A finite linewidth in general has intrinsic and…

Mesoscale and Nanoscale Physics · Physics 2009-11-07 C. A. Ullrich , G. Vignale

The engineering of the optical response of materials is a paradigm that demands microscopic-level accuracy and reliable predictive theoretical tools. Here we compare and contrast the dispersive permittivity tensor, using both a low-energy…

Materials Science · Physics 2021-09-29 Mohammad Alidoust , Erlend E. Isachsen , Klaus Halterman , Jaakko Akola

An approximate solution to the time-dependent density functional theory (TDDFT) response equations for finite systems is developed, yielding corrections to the single-pole approximation. These explain why allowed Kohn-Sham transition…

Materials Science · Physics 2009-11-07 H. Appel , E. K. U. Gross , K. Burke

The low-lying singlet and triplet spectrum in conjugated polymers clearly show that the mechanism proposed by Lin et al. to explain their electric field dependence of singlet to triplet yield ratios is wrong. This comment, from theoretical…

Strongly Correlated Electrons · Physics 2007-05-23 S. Mazumdar , Mousumi Das , S. Ramasesha

The localization length of a low energy tightly bound electron-hole pair (excitons) is calculated by exact diagonalization for small interacting disordered systems. The exciton localization length (which corresponds to the thermal…

Mesoscale and Nanoscale Physics · Physics 2009-10-31 Richard Berkovits

The time-dependent density functional based tight-binding (TD-DFTB) approach is generalized to account for fractional occupations. In addition, an on-site correction leads to marked qualitative and quantitative improvements over the…

Materials Science · Physics 2013-02-15 A. Domínguez , B. Aradi , T. Frauenheim , V. Lutsker , T. A. Niehaus

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

Most applications of time-dependent density-functional theory (TDDFT) use the adiabatic local-density approximation (ALDA) for the dynamical exchange-correlation potential Vxc(r,t). An exact (i.e., nonadiabatic) extension of the…

Mesoscale and Nanoscale Physics · Physics 2015-06-25 C. A. Ullrich