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We propose a state-averaged orbital optimization scheme for improving the accuracy of excited states of the electronic structure Hamiltonian for use on near-term quantum computers. Instead of parameterizing the orbital rotation operator in…

Chemical Physics · Physics 2024-04-09 Joel Bierman , Yingzhou Li , Jianfeng Lu

The direct variational determination of the two-electron reduced-density matrix (2-RDM) is usually carried out under the assumption that the 2-RDM is a real-valued quantity. However, in systems that possess orbital angular momentum…

Chemical Physics · Physics 2019-09-18 Run R. Li , A. Eugene DePrince

We propose a state-specific orbital optimization scheme for improving the accuracy of excited states of the electronic structure Hamiltonian for the use on near-term quantum computers, which can be combined with any overlap-based…

Quantum Physics · Physics 2025-10-16 Guorui Zhu , Joel Bierman , Jianfeng Lu , Yingzhou Li

An energy functional for orbital based $O(N)$ calculations is proposed, which depends on a number of non orthogonal, localized orbitals larger than the number of occupied states in the system, and on a parameter, the electronic chemical…

mtrl-th · Physics 2016-09-07 Jeongnim Kim , Francesco Mauri , Giulia Galli

We demonstrate how to determine numerically nearly exact orthonormal orbitals that are optimal for evaluation of the energy of arbitrary (correlated) states of atoms and molecules by minimization of the energy Lagrangian. Orbitals are…

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…

Chemical Physics · Physics 2020-06-18 Lan Nguyen Tran , Eric Neuscamman

The goal of the present paper is to make a numerical analysis of parametric optimization of low thrust orbital maneuver. An orbital maneuver occurs when it is necessary to modify the orbit a space vehicle to change its function or to…

Earth and Planetary Astrophysics · Physics 2023-07-14 Antonio Fernando Bertachini de Almeida Prado

Selective configuration interaction methods approximate correlated molecular ground- and excited states by considering only the most relevant Slater determinants in the expansion. While a recently proposed neural-network-assisted approach…

We study several approaches to orbital optimization in selected configuration interaction plus perturbation theory (SCI+PT) methods, and test them on the ground and excited states of three molecules using the semistochastic heatbath…

Chemical Physics · Physics 2021-07-14 Yuan Yao , C. J. Umrigar

Variational optimization of orbitals in time-independent density functional calculations of excited electronic states presents a significant challenge, as excited states typically correspond to saddle points on the electronic energy…

Chemical Physics · Physics 2026-04-02 Yorick L. A. Schmerwitz , Elli Selenius , Gianluca Levi

The ground state of atoms from H to Ar was calculated using a self-interaction correction to local and gradient dependent density functionals. The correction can significantly improve the total energy and makes the orbital energies…

Atomic and Molecular Clusters · Physics 2013-08-29 Simon Klüpfel , Peter Klüpfel , Hannes Jonsson

In this work, trions in two-dimensional (2D) space are studied by variational method with trial wavefunctions being constructed by linear combinations of 2D slater-type orbitals (STOs). Via this method, trion energy levels and wavefunctions…

Mesoscale and Nanoscale Physics · Physics 2021-07-28 Yao-Wen Chang , Yia-Chung Chang

Spatially localized one-electron orbitals, orthogonal and nonorthogonal, are widely used in electronic structure theory to describe chemical bonding and speed up calculations. In order to avoid linear dependencies of localized orbitals, the…

Chemical Physics · Physics 2020-03-04 Ziling Luo , Rustam Z. Khaliullin

Existing algorithms for the optimal control of quantum observables are based on locally optimal steps in the space of control fields, or as in the case of genetic algorithms, operate on the basis of heuristics that do not explicitly take…

Quantum Physics · Physics 2007-08-27 Raj Chakrabarti , Rebing Wu , Herschel Rabitz

A technique of designing antenna excitation realizing orthogonal states is presented. It is shown that a symmetric antenna geometry is required in order to achieve orthogonality with respect to all physical quantities. A maximal number of…

Signal Processing · Electrical Eng. & Systems 2021-06-23 Michal Masek , Lukas Jelinek , Miloslav Capek

We investigate the suitability of natural orbitals as a basis for describing many-body excitations. We analyze to which extend the natural orbitals describe both bound as well as ionized excited states and show that depending on the…

Other Condensed Matter · Physics 2011-01-14 N. Helbig , I. V. Tokatly , A. Rubio

The quantum phase estimation algorithm stands as the primary method for determining the ground state energy of a molecular electronic Hamiltonian on a quantum computer. In this context, the ability to initialize a classically tractable…

The difficulty of an optimization task in quantum information science depends on the proper mathematical expression of the physical target. Here we demonstrate the power of optimization functionals targeting an arbitrary perfect two-qubit…

In this paper we study the problem of designing periodic orbits for a special class of hybrid systems, namely mechanical systems with underactuated continuous dynamics and impulse events. We approach the problem by means of optimal control.…

Optimization and Control · Mathematics 2017-02-16 Sara Spedicato , Giuseppe Notarstefano

The dominantly orbital state method allows a semiclassical description of quantum systems. At the origin, it was developed for two-body relativistic systems. Here, the method is extended to treat two-body Hamiltonians and systems with three…

Quantum Physics · Physics 2013-06-07 Claude Semay , Fabien Buisseret
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