Related papers: Fully self-consistent optimization of the Jastrow-…
The Coupled Cluster (CC) method is used to compute the electronic correlation energy in atoms and molecules and often leads to highly accurate results. However, due to its single-reference nature, standard CC in its projected form fails to…
The time-dependent restricted-active-space self-consistent-field singles (TD-RASSCF-S) method is presented for investigating TD many-electron dynamics in atoms and molecules. Adopting the SCF notion from the muticonfigurational TD…
Treating electron correlation more accurately and efficiently is at the heart of the development of electronic structure methods. In the present work, we explore the use of stochastic approaches to evaluate high-order electron correlation…
Quantum Monte Carlo methods are accurate and promising many body techniques for electronic structure calculations which, in the last years, are encountering a growing interest thanks to their favorable scaling with the system size and their…
Although the linear method is one of the most robust algorithms for optimizing non-linearly parametrized wavefunctions in variational Monte Carlo, it suffers from a memory bottleneck due to the fact at each optimization step a generalized…
Computationally efficient and accurate quantum mechanical approximations to solve the many-electron Schr\"odinger equation are at the heart of computational materials science. In that respect the coupled cluster hierarchy of methods plays a…
Accurate determination of electronic properties of correlated oxides remains a significant challenge for computational theory. Traditional Hubbard-corrected density functional theory (DFT+U) frequently encounters limitations in precisely…
The multi-configurational self-consistent field theory is considered the standard starting point for almost all multireference approaches required for strongly-correlated molecular problems. The limitation of the approach is generally given…
Growth in computational resources has lead to the application of real space diffusion quantum Monte Carlo (DMC) to increasingly heavy elements. Although generally assumed to be small, we find that when using standard techniques the…
We describe a method for imposing the correct electron-nucleus (e-n) cusp in molecular orbitals expanded as a linear combination of (cuspless) Gaussian basis functions. Enforcing the e-n cusp in trial wave functions is an important asset in…
The complete active space self-consistent field (CASSCF) method is the principal approach employed for studying strongly correlated systems. However, exact CASSCF can only be performed on small active spaces of ~20 electrons in ~20 orbitals…
We benchmark ionisation and excitation energies of transition-metal atoms Sc-Zn with a transcorrelated Hamiltonian combined with pseudopotentials. The similarity transformed Hamiltonian provides compact TC wave functions in affordable…
A framework for developing new approximate electronic structure methods is presented, in which the correlation energy of a many-electron system in the ground state is computed as in the single-reference second-order many-body perturbation…
Quantum Monte Carlo (QMC) is an advanced simulation methodology for studies of manybody quantum systems. In this review, we focus on the electronic structure QMC, i.e., methods relevant for systems described by the electron-ion…
We analyze the accuracy and sample complexity of variational Monte Carlo approaches to simulate the dynamics of many-body quantum systems classically. By systematically studying the relevant stochastic estimators, we are able to: (i) prove…
When combined with highly expressive ansatz functions such as neural quantum states, variational Monte Carlo (VMC) constitutes a versatile numerical approach to tackle the quantum many-body problem in and out of equilibrium. However, its…
Transcorrelated methods provide an efficient way of partially transferring the description of electronic correlations from the ground state wavefunction directly into the underlying Hamiltonian. In particular, Dobrautz et al. [Phys. Rev. B,…
The quantum Monte Carlo (QMC) is one of the most promising many-body electronic structure approaches. It employs stochastic techniques for solving the stationary Schr\" odinger equation and for evaluation of expectation values. The key…
We report successful implementation of the time-dependent second-order many-body perturbation theory using optimized orthonormal orbital functions called time-dependent optimized second-order many-body perturbation theory [TD-OMP2] to reach…
We present a combination of the bi-orthogonal orbital optimisation framework with the recently introduced xTC version of transcorrelation. This allows us to implement non-iterative perturbation based methods on top of the transcorrelated…