Related papers: Quantitative Molecular Orbital Energies within a $…
A new cumulant-based $GW$ approximation for the retarded one-particle Green's function is proposed, motivated by an exact relation between the improper Dyson self-energy and the cumulant generating function. Qualitative aspects of this…
We report unphysical irregularities and discontinuities in some key experimentally-measurable quantities computed within the GW approximation of many-body perturbation theory applied to molecular systems. In particular, we show that the…
The calculation time for the energy of atoms and molecules scales exponentially with system size on a classical computer but polynomially using quantum algorithms. We demonstrate that such algorithms can be applied to problems of chemical…
We present first-principles calculations of the impact ionization rate (IIR) in the $GW$ approximation ($GW$A) for semiconductors. The IIR is calculated from the quasiparticle (QP) width in the $GW$A, since it can be identified as the decay…
Quantum simulations of molecular systems on quantum computers often employ minimal basis sets of Gaussian orbitals. In comparison with more realistic basis sets, quantum simulations employing minimal basis sets require fewer qubits and…
The ab initio calculation of quasiparticle (QP) energies is a technically and computationally challenging problem. In condensed matter physics the most widely used approach to determine QP energies is the GW approximation. Although the GW…
We describe an all-electron $G_0W_0$ implementation for periodic systems with $k$-point sampling implemented in a crystalline Gaussian basis. Our full-frequency $G_0W_0$ method relies on efficient Gaussian density fitting integrals and…
In the pursuit of numerically identifying the ground state of quantum many-body systems, approximate quantum wavefunction ansatzes are commonly employed. This study focuses on the spectral decomposition of these approximate quantum…
We describe the relationship between the GW approximation and various equation-of-motion (EOM) coupled-cluster (CC) theories. We demonstrate the exact equivalence of the G$_0$W$_0$ approximation and the propagator theory for an…
Using multiwavelets, we have obtained total energies and corresponding atomization energies for the GGA-PBE and hybrid-PBE0 density functionals for a test set of 211 molecules with an unprecedented and guaranteed $\mu$Hartree accuracy.…
We investigate the convergence of quasi-particle energies for periodic systems to the thermodynamic limit using increasingly large simulation cells corresponding to increasingly dense integration meshes in reciprocal space. The…
We present a novel hybrid quantum/classical (QM/MM) approach to the calculation of charged excitations in molecular solids based on the many-body Green's function $GW$ formalism. Molecules described at the $GW$ level are embedded into the…
We introduce a systematic hierarchy of one-body Green's function methods derived from the $GW$ approximation, constructed by progressively reducing the dynamical content of the self-energy. Starting from the fully dynamical Dyson…
Molecular excitations in the liquid-phase environment are renormalized by the surrounding solvent molecules. Herein, we employ the GW approximation to investigate the solvation effects on the ionization energy of phenol in various solvent…
The ionization potential (IP) is an important parameter providing essential insights into the reactivity of chemical systems. IPs are also crucial for designing, optimizing, and understanding the functionality of modern technological…
The many-body perturbation theory within the $GW$ approximation is a widely used method for describing the electronic band structures in real materials. Its application to large-scale systems is, however, impeded by its high computational…
We present a molecular extension of our recently proposed Green's function embedding method, interacting-bath dynamical embedding theory (ibDET), for computing charged excitation energies at the $GW$ and EOM-CCSD levels. Starting from…
Many-body perturbation theory within the G$_0$W$_0$ approximation is used to determine molecular orbital level alignment at a liquid water/Pt(111) interface generated through $ab~ initio$ molecular dynamics. Molecular orbital energy levels…
A simple and computationally efficient scheme to calculate approximate imaginary-frequency dependent polarizability, hence asymptotic van der Waals coefficient, within density functional theory is proposed. The dynamical dipolar…
In this thesis, attention is paid to small experimental testbed applications with respect to the quantum phase estimation algorithm, the core approach for finding energy eigenvalues. An iterative scheme for quantum phase estimation (IPEA)…