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The construction of density-functional approximations is explored by modeling the adiabatic connection em locally, using energy densities defined in terms of the electrostatic potential of the exchange-correlation hole. These local models…

Chemical Physics · Physics 2016-05-04 Stefan Vuckovic , Tom Irons , Andreas Savin , Andrew M. Teale , Paola Gori-Giorgi

The exact exchange-correlation (XC) potential in time-dependent density-functional theory (TDDFT) is known to develop steps and discontinuities upon change of the particle number in spatially confined regions or isolated subsystems. We…

Mesoscale and Nanoscale Physics · Physics 2019-03-27 Daniel Vieira , K. Capelle , C. A. Ullrich

Time-dependent (TD) density functional theory (TDDFT) promises a numerically tractable account of many-body electron dynamics provided good simple approximations are developed for the exchange-correlation (XC) potential functional (XCPF).…

Other Condensed Matter · Physics 2008-08-29 Roi Baer

We study the exact Time-Dependent Potential Energy Surface (TDPES) in the presence of strong non-adiabatic coupling between the electronic and nuclear motion. The concept of the TDPES emerges from the exact factorization of the full…

Chemical Physics · Physics 2013-02-07 Ali Abedi , Federica Agostini , Yasumitsu Suzuki , E. K. U. Gross

Most present applications of time-dependent density functional theory use adiabatic functionals, i.e. the effective potential at time t is determined solely by the density at the same time. This paper discusses a method that aims to go…

Strongly Correlated Electrons · Physics 2009-11-10 Yair Kurzweil , Roi Baer

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

We show that as an electron transfers between closed-shell molecular fragments at large separation, the exact correlation potential of time-dependent density functional theory gradually develops a step and peak structure in the bonding…

Chemical Physics · Physics 2014-02-11 Johanna I. Fuks , Peter Elliott , Angel Rubio , Neepa T. Maitra

The exact nuclear time-dependent potential energy surface arises from the exact decomposition of electronic and nuclear motion, recently presented in [A. Abedi, N. T. Maitra, and E. K. U. Gross, Phys. Rev. Lett. 105, 123002 (2010)]. Such…

Chemical Physics · Physics 2015-06-16 Federica Agostini , Ali Abedi , Yasumitsu Suzuki , E. K. U. Gross

We use Lanczos exact diagonalization to compute the exact exchange-correlation (xc) potential of a Hubbard chain with large binding energy ("the bulk") followed by a chain with zero binding energy ("the vacuum"). Several results of density…

Strongly Correlated Electrons · Physics 2015-06-11 Valentina Brosco , Zujian Ying , José Lorenzana

We introduce a new class of exchange-correlation potentials for a static and time-dependent Density Functional Theory of strongly correlated systems in 3D. The potentials are obtained via Dynamical Mean Field Theory and, for strong enough…

Strongly Correlated Electrons · Physics 2015-05-18 Daniel Karlsson , Antonio Privitera , Claudio Verdozzi

Nonadiabatic quantum interferences emerge whenever nuclear wavefunctions in different electronic states meet and interact in a nonadiabatic region. In this work, we analyze how nonadiabatic quantum interferences translate in the context of…

Chemical Physics · Physics 2016-08-03 Basile F. E. Curchod , Federica Agostini , E. K. U. Gross

We obtain an exact solution of the time-dependent Schroedinger equation for a two-electron system confined to a plane by an isotropic parabolic potential whose curvature is periodically modulated in time. From this solution we compute the…

Condensed Matter · Physics 2009-10-31 Irene D'Amico , Giovanni Vignale

Accurately describing excited states within Kohn-Sham (KS) density functional theory (DFT), particularly those which induce ionization and charge transfer, remains a great challenge. Common exchange-correlation (xc) approximations are…

Materials Science · Physics 2021-02-09 Eli Kraisler , M. J. P. Hodgson , E. K. U. Gross

The appearance of so-called exceptional points in the complex spectra of non-Hermitian systems is often associated with phenomena that contradict our physical intuition. One example of particular interest is the state-exchange process…

Adiabatic time-dependent density functional theory fails for excitations of a heteroatomic molecule composed of two open-shell fragments at large separation. Strong frequency-dependence of the exchange-correlation kernel is necessary for…

Other Condensed Matter · Physics 2009-11-11 Neepa T. Maitra , David G. Tempel

We point out an error in the argument [PRL 105, 013002 (2010)] that the time independence of the occupation numbers in the adiabatic approximation follows from the invariance of the ground-state interaction energy functional with respect to…

Chemical Physics · Physics 2010-11-08 Ryan Requist , Oleg Pankratov

We put forward new approach for the development of a non-local density functional by a direct modeling of the shape of exchange-correlation (xc) hole in inhomogeneous systems. The functional is aimed at giving an accurate xc-energy and an…

Other Condensed Matter · Physics 2013-08-05 Klaas J. H. Giesbertz , Robert van Leeuwen , Ulf von Barth

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

A review of the approximations in any time-dependent density functional calculation of excitation energies is given. The single-pole approximation for the susceptibility is used to understand errors in popular approximations for the…

Materials Science · Physics 2007-05-23 Kieron Burke , Martin Petersilka , E. K. U. Gross

In time-dependent density-functional theory, exchange and correlation (xc) beyond the adiabatic local density approximation can be described in terms of viscoelastic stresses in the electron liquid. In the time domain, this leads to a…

Mesoscale and Nanoscale Physics · Physics 2009-11-10 H. O. Wijewardane , C. A. Ullrich