Adapting approximate-memory potentials for time-dependent density functional theory

Kurzweil, Yair; Baer, Roi

doi:10.1103/physrevb.77.085121

Cited by 15 publications

(12 citation statements)

References 25 publications

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“…For example, representing driven few-state dynamics, in particular Rabi oscillations, by adiabatic functionals has been found to be difficult [39,40]. However, implementation of functionals that include effects non-local in time [41] into realistic three-dimensional simulations have remained a challenge. Currently, the applicability of adiabatic functionals to ultrafast phenomena can only be assessed by comparison with experiment.…”

Section: Methodsmentioning

confidence: 99%

Controlling ultrafast currents by the nonlinear photogalvanic effect

et al. 2015

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We investigate the effect of broken inversion symmetry on the generation and control of ultrafast currents in a transparent dielectric (SiO 2 ) by strong femtosecond optical laser pulses. Ab initio simulations based on time-dependent density functional theory predict ultrafast direct currents that can be viewed as a nonlinear photogalvanic effect. Most surprisingly, the direction of the current undergoes a sudden reversal above a critical threshold value of laser intensity of about I 3 10 c 13Ẃ cm −2 . We trace this switching to the transition from nonlinear polarisation currents to the tunnelling excitation regime. The latter is found to be sensitive to the relative orientation between laser polarisation and chemical bonds. We demonstrate control of the ultrafast currents by the time delay between two laser pulses. While two temporally separated laser pulses lead to currents along one direction their temporal overlap can reverse the current. We find the ultrafast current control by the nonlinear photogalvanic effect to be remarkably robust and insensitive to the laser-pulse shape and the carrier-envelope phase.

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Section: Methodsmentioning

confidence: 99%

Controlling ultrafast currents by the nonlinear photogalvanic effect

et al. 2015

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“…The inclusion of memory is next to impossible with local TDXC approximations to TDDFT because Galilean invariance and the 0-force conditions cannot be imposed (107)(108)(109) as there is no stationary principle for nonadiabatic functionals in TDDFT (110). These problems prompted KS-like developments within time-dependent current-density functionals (109,111,112), metric or deformation tensor functionals (106,(113)(114)(115)(116), and potential-adaptation methods (117,118). Another problem with adiabatic semilocal functionals within TDKS theory is that they predict too low excitation energies for long-range charge-transfer excitations (CTEs) (38,45,52,119,120).…”

Section: Generalized Kohn-sham Approach To Time-dependent Density Funmentioning

confidence: 99%

Tuned Range-Separated Hybrids in Density Functional Theory

Baer

Livshits

Salzner

2010

Annu. Rev. Phys. Chem.

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747

846

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We review density functional theory (DFT) within the Kohn-Sham (KS) and the generalized KS (GKS) frameworks from a theoretical perspective for both time-independent and time-dependent problems. We focus on the use of range-separated hybrids within a GKS approach as a practical remedy for dealing with the deleterious long-range self-repulsion plaguing many approximate implementations of DFT. This technique enables DFT to be widely relevant in new realms such as charge transfer, radical cation dimers, and Rydberg excitations. Emphasis is put on a new concept of system-specific range-parameter tuning, which introduces predictive power in applications considered until recently too difficult for DFT.

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“…As of today, very few applications of TDDFT have been carried out with nonadiabatic, explicitly memorydependent xc functionals [68][69][70][71]. Due to its simplicity, the overwhelming majority of time-dependent Kohn-Sham calculations use the adiabatic LDA (ALDA),…”

Section: A the Time-dependent XC Potentialmentioning

confidence: 99%

A Brief Compendium of Time-Dependent Density Functional Theory

2013

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Time-dependent density-functional theory (TDDFT) is a formally exact approach to the timedependent electronic many-body problem which is widely used for calculating excitation energies. We present a survey of the fundamental framework, practical aspects, and applications of TDDFT. This paper is mainly intended for non-experts (students or researchers in other areas) who would like to learn about the present state of TDDFT without going too deeply into formal details. I. PREFACEThis paper presents an introduction to and a survey of time-dependent density-functional theory (TDDFT). The purpose of the paper is to explain in a nutshell what TDDFT is and what it can do. We will discuss the basics of the formal framework of TDDFT as well as the current state of the art, skipping over details of the proofs, and highlight some of the most important applications. Readers who would like a more detailed treatment and more literature references are encouraged to consult recent books [1, 2] and review articles [3][4][5].TDDFT is a theoretical approach to the dynamical quantum many-body problem; it can be used to describe quantum systems that are not stationary. As a consequence, TDDFT provides formally exact and practically convenient methods to calculate electronic excitation energies. By contrast, density-functional theory (DFT) is a ground-state theory: in other words, it is used to find the ground state of a quantum system and calculate related quantities of interest, such as the ground-state energy. In many, if not most, situations of practical interest, we have to determine the ground state of the system before we can study its dynamics or calculate its excitations.The beginnings of ground-state DFT date back to the years 1964/65 when the famous papers by Hohenberg and Kohn [6] and Kohn and Sham [7] were published. Since then, DFT has developed into a dominating method for electronic structure calculations in physics, chemistry, materials science, and many other areas (see Ref.[8] for a recent up-to-date account of DFT). Although TDDFT is of much more recent origin [9], it now has reached a similar status for calculating electronic excitations.TDDFT uses many familiar concepts from DFT, most prominently, the Kohn-Sham idea of replacing the real interacting many-body system by a noninteracting system that reproduces the same density. But there are also many concepts that are unique to the time-dependent case, such as memory and initial-state dependence. To gain a thorough understanding of TDDFT it is hence advisable to begin with a study of the basic concepts of DFT. We refer the reader to the very nice introductions to DFT by Capelle [10] and by Burke and Wagner [11]. There exist a number of books on DFT, some of which are very accessible to newcomers in the field [12,13], others are more advanced [14].

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Adapting approximate-memory potentials for time-dependent density functional theory

Cited by 15 publications

References 25 publications

Controlling ultrafast currents by the nonlinear photogalvanic effect

Controlling ultrafast currents by the nonlinear photogalvanic effect

Tuned Range-Separated Hybrids in Density Functional Theory

A Brief Compendium of Time-Dependent Density Functional Theory

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