相关论文: Improving excited state potential energy surfaces …
Utilizing quantum computer to investigate quantum chemistry is an important research field nowadays. In addition to the ground-state problems that have been widely studied, the determination of excited-states plays a crucial role in the…
Highly excited vibrational states of an isolated molecule encode the vibrational energy flow pathways in the molecule. Recent studies have had spectacular success in understanding the nature of the excited states mainly due to the extensive…
In this work, we revisited the idea of using the coupled-cluster ground state formalism to target excited states. Our main focus was targeting doubly excited states and double core hole states. Typical equation-of-motion (EOM) approaches…
We present a novel energy-based localization procedure able to localize molecular orbitals into specific spatial regions. The method is applied to several cases including both conjugated and non-conjugated systems. The obtained localized…
The mean-field solutions of electronic excited states are much less accessible than ground state (e.g.\ Hartree-Fock) solutions. Energy-based optimization methods for excited states, like $\Delta$-scf, tend to fall into the lowest solution…
In the construction of diabatic vibronic Hamiltonians for quantum dynamics in the excited-state manifold of molecules, the coupling constants are often extracted solely from information on the excited-state energies. Here, a new protocol is…
A systematic method for determining correlated wavefunctions of extended systems in the ground and excited states is presented. It allows to fully exploit the power of quantum-chemical programs designed for correlation calculations of…
We propose a new ansatz for the ground-state wave function of quantum many-body systems on a lattice. The key idea is to cover the lattice with plaquettes and obtain a state whose configurational weights can be optimized by means of a…
Accurate yet efficient modeling of chemical systems with pronounced static correlation in their excited states remains a significant challenge in quantum chemistry, as most electronic structure methods that can adequately capture static…
The computation of small concise and comprehensible excited state wave functions is needed because many electronic processes occur in excited states. But since the excited energies are saddle points in the Hilbert space of wave functions,…
Conical intersections serve as critical gateways in photochemical reactions, enabling rapid nonradiative transitions between potential energy surfaces that underpin fundamental processes such as photosynthesis or vision. Their calculation…
A quantum Monte Carlo method is introduced to optimize excited state trial wavefunctions. The method is applied in a correlation function Monte Carlo calculation to compute ground and excited state energies of bosonic van der Waals clusters…
In a tight binding framework, we analyze the characteristics of electronic states in strongly disordered materials (hopping sites are placed randomly with no local order) with tunneling matrix elements decaying exponentially in the atomic…
We report excited-state spectroscopy on a quantum dot side-coupled to a quantum wire with accurate energy estimation. Our method utilizes periodic voltage pulses on the dot, and the energy calibration is performed with reference to the bias…
Within the present noisy intermediate-scale quantum-computing era, hybrid quantum-classical-processor algorithms have emerged as promising avenues for tackling electronic-structure eigenproblems. Among them, the so-called…
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…
Molecular crystals are a prototypical class of van der Waals (vdW) bound organic materials with excited state properties relevant for optoelectronics applications. Predicting the structure and excited state properties of molecular crystals…
We propose a new block localized excitation (BLE) method to directly construct diabatic excited states without the need to first compute the adiabatic states. The new method is capable to keep any electrons, spins, and excitations localized…
A recently developed self-healing diffusion Monte Carlo algorithm [PRB 79, 195117] is extended to the calculation of excited states. The formalism is based on an excited-state fixed-node approximation and the mixed estimator of the…
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…