Related papers: Is it possible to construct excited-state energy f…
Following a recent work [Gal, Phys. Rev. A 64, 062503 (2001)], a simple derivation of the density-functional correction of the Hartree-Fock equations, the Hartree-Fock-Kohn-Sham equations, is presented, completing an integrated view of…
We develop tangent space methods for projected entangled-pair states (PEPS) that provide direct access to the low-energy sector of strongly-correlated two-dimensional quantum systems. More specifically, we construct a variational ansatz for…
The essence of atomic structure theory, quantum chemistry, and computational materials science is solving the multi-electron stationary Schr\"odinger equation. The Quantum Monte Carlo-based neural network wave function method has surpassed…
It has recently been observed [Phys. Rev. Lett. 113, 113002 (2014)] that the ground-state energy may be obtained directly as a simple sum of augmented Kohn-Sham orbital energies, where it was ascertained that the corresponding one-body…
Variational calculations of excited electronic states are carried out by finding saddle points on the surface that describes how the energy of the system varies as a function of the electronic degrees of freedom. This approach has several…
We present and discuss some ideas concerning an ``average-pair-density functional theory'', in which the ground-state energy of a many-electron system is rewritten as a functional of the spherically and system-averaged pair density. These…
The computation of excited electronic states is an important application for quantum computers. In this work, we simulate the excited state spectra of four aromatic heterocycles on IBM superconducting quantum computers, focusing on active…
This Perspective describes current computational efforts in the field of simulating photodynamics of transition metal complexes. We present the typical workflows and feature the strengths and limitations of the different contemporary…
Computation of electronic spectra is one of the most important applications of methods capturing static electron correlation, including complete-active-space self-consistent field (CASSCF) and post-CASSCF theories. Performance of these…
Electronic structure calculations are routinely carried out within the framework of density-functional theory, often with great success. For electrons in reduced dimensions, however, there is still a need for better approximations to the…
We prove the general chemical potential theorem: the noninteracting one-electron orbital energies in DFT ground states and $\Delta$SCF excited states are corresponding chemical potentials of electron addition or removal, from an…
The accurate quantum chemical calculation of excited states is a challenging task, often requiring computationally demanding methods. When entire ground and excited potential energy surfaces (PESs) are desired, e.g., to predict the…
We introduce the multistate iterative qubit coupled cluster (MS-iQCC) method, a quantum-inspired algorithm that runs efficiently on classical hardware and is designed to predict both ground and excited electronic states of molecules.…
A very specific ensemble of ground and excited states is shown to yield an exact formula for any excitation energy as a simple correction to the energy difference between orbitals of the Kohn-Sham ground state. This alternative scheme…
A new dimensional scaling method for the calculation of excited states of multielectron atoms is introduced. By including the principle and orbital quantum numbers in the dimension parameter, we obtain an energy expression for excited…
Quantum technologies exploiting bipartite entanglement could be made more efficient by using states having the minimum amount of energy for a given entanglement degree. Here, we study how to generate these states in the case of a bipartite…
We demonstrate that, rather than resorting to high-cost dynamic correlation methods, qualitative failures in excited-state potential energy surface predictions can often be remedied at no additional cost by ensuring that optimal molecular…
We employ quantum Monte Carlo to obtain chemically accurate vertical and adiabatic excitation energies, and equilibrium excited-state structures for the small, yet challenging, formaldehyde and thioformaldehyde molecules. A key ingredient…
Quantum Monte Carlo (QMC) methods have proven to be highly accurate for computing excited states, but the choice of optimization strategies for multiple states remains an active topic of investigation. In this work, we revisit the…
Excited state normal modes analysis is systematically applied to investigate and compare relaxation and internal conversion dynamics of a free-base porphyrin with a novel functional porphyrin derivative. We discuss strenghts and limitation…