# Time-dependent density functional theory beyond Kohn-Sham Slater determinants.

@article{Fuks2016TimedependentDF, title={Time-dependent density functional theory beyond Kohn-Sham Slater determinants.}, author={Johanna I Fuks and S{\o}ren E B Nielsen and Michael Ruggenthaler and Neepa T. Maitra}, journal={Physical chemistry chemical physics : PCCP}, year={2016}, volume={18 31}, pages={ 20976-85 } }

When running time-dependent density functional theory (TDDFT) calculations for real-time simulations of non-equilibrium dynamics, the user has a choice of initial Kohn-Sham state, and typically a Slater determinant is used. We explore the impact of this choice on the exchange-correlation potential when the physical system begins in a 50 : 50 superposition of the ground and first-excited state of the system. We investigate the possibility of judiciously choosing a Kohn-Sham initial state that…

## 18 Citations

### Electron scattering in time-dependent density functional theory

- PhysicsThe European Physical Journal B
- 2018

Abstract
It was recently shown [Suzuki et al., Phys. Rev. Lett. 119, 263401 (2017)] that peak and valley structures in the exact exchange-correlation potential of time-dependent density functional…

### Time-dependent density functional theory for charge-transfer dynamics: review of the causes of failure and success*

- Physics
- 2016

Abstract
The present study is an effort to unveil and characterize the failure and success of real-time Time-dependent density functional theory simulated charge transfer dynamics. To this aim, we…

### Developing new and understanding old approximations in TDDFT.

- PhysicsFaraday discussions
- 2020

An expression for the exact time-dependent exchange-correlation potential suggests that the accuracy of an adiabatic approximation is intimately related to the deviation between the natural orbital occupation numbers of the physical system and those of the Kohn-Sham system.

### Machine learning exchange-correlation potential in time-dependent density-functional theory

- Physics
- 2020

We propose a machine-learning-based approach to develop the exchange-correlation potential of time-dependent density-functional theory (TDDFT). The neural network projection from the time-varying…

### Exploring non-adiabatic approximations to the exchange-correlation functional of TDDFT.

- PhysicsPhysical chemistry chemical physics : PCCP
- 2018

Several preliminary approximations are explored, their fulfillment of known exact conditions are evaluated, and their performance on simple model systems for which available exact solutions indicate the significance of going beyond the adiabatic approximation are tested.

### Dual-Functional Tamm-Dancoff Approximation: A Convenient Density Functional Method that Correctly Describes S1/S0 Conical Intersections.

- PhysicsThe journal of physical chemistry letters
- 2017

A new, conceptually simple, easy- to-implement, and easy-to-use way to employ time-dependent Kohn-Sham density functional theory that has global accuracy comparable with the conventional single-functional version and that recovers the double cone topology of the potential energy surfaces at S1/S0 conical intersection seams is presented.

### Inverse Kohn-Sham Density Functional Theory: Progress and Challenges.

- Computer ScienceThe journal of physical chemistry letters
- 2021

New ideas to make iKS problems more tractable, provide an overall strategy for performing numerical density-to-potential inversions, and discuss challenges and future directions are introduced.

### Numerical construction of the density-potential mapping

- PhysicsThe European Physical Journal B
- 2018

Abstract
We demonstrate how a recently developed method Nielsen et al. [Nielsen et al., EPL 101, 33001 (2013)] allows for a comprehensive investigation of time-dependent density functionals in…

### Charge transfer in time-dependent density functional theory

- PhysicsJournal of physics. Condensed matter : an Institute of Physics journal
- 2017

Dynamical step and peak features in the exact functional evolving over time, that are missing in the functionals currently used in TDDFT, are described.

### Force balance approach for advanced approximations in density functional theories.

- PhysicsThe Journal of chemical physics
- 2019

This work proposes a systematic and constructive way to determine the exchange-correlation potentials of density-functional theories including vector potentials based on equations of motion of current quantities and is feasible both in the ground-state and the time-dependent settings.

## References

SHOWING 1-10 OF 74 REFERENCES

### Analytic density-functionals with initial-state dependence and memory

- Physics
- 2013

We analytically construct the wave function that, for a given initial state, produces a prescribed density for a quantum ring with two non-interacting particles in a singlet state. In this case the…

### Many-body quantum dynamics from the density

- Physics
- 2013

We present a local control scheme to construct the external potential v that, for a given initial state, produces a prescribed time-dependent density in an interacting quantum many-body system. This…

### Kinetic and interaction components of the exact time-dependent correlation potential.

- PhysicsThe Journal of chemical physics
- 2014

This work analyzes the xc potential by decomposing it into kinetic and interaction components and comparing each with their exact-adiabatic counterparts, for a range of dynamical situations in model one-dimensional two-electron systems.

### Challenging adiabatic time-dependent density functional theory with a Hubbard dimer: the case of time-resolved long-range charge transfer.

- PhysicsPhysical chemistry chemical physics : PCCP
- 2014

This work explores an asymmetric two-fermion Hubbard dimer to test the accuracy of the adiabatic approximation of time-dependent density functional theory in modelling time-resolved charge transfer, and shows that the model shares essential features of a ground state long-range molecule in real-space and reproduces essential traits of the CT dynamics.

### Existence, uniqueness, and construction of the density-potential mapping in time-dependent density-functional theory

- MathematicsJournal of physics. Condensed matter : an Institute of Physics journal
- 2015

This work reviews the mapping from densities to potentials in quantum mechanics, which is the basic building block of time-dependent density-functional theory and the Kohn-Sham construction and presents an extension of the density-potential mapping to include vector-potentials and photons.

### Time-Dependent Density-Functional Theory: Concepts and Applications

- Chemistry
- 2012

1. Introduction 2. Review of ground-state density-functional theory 3. Fundamental existence theorems 4. Time-dependent Kohn-Sham scheme 5. Time-dependent observables 6. Properties of the…

### Absence of dynamical steps in the exact correlation potential in the linear response regime

- Physics
- 2013

Recent work [Phys. Rev. Lett. 109, 266404 (2012)] showed that the exact exchange-correlation potential of time-dependent density-functional theory generically displays dynamical step structures.…

### Time-dependent density-functional theory meets dynamical mean-field theory: real-time dynamics for the 3D Hubbard model.

- PhysicsPhysical review letters
- 2011

A new class of exchange-correlation potentials for a static and time-dependent density-functional theory of strongly correlated systems in 3D, obtained via dynamical mean-field theory and exhibit a discontinuity at half-filling density, a signature of the Mott transition.

### Exact density-functional potentials for time-dependent quasiparticles.

- PhysicsPhysical review letters
- 2012

We calculate the exact Kohn-Sham potential that describes, within time-dependent density-functional theory, the propagation of an electron quasiparticle wave packet of nonzero crystal momentum added…