Related papers: Environment effects on X-ray absorption spectra wi…
Quantum embedding approaches involve the self-consistent optimization of a local fragment of a strongly correlated system, entangled with the wider environment. The `energy-weighted' density matrix embedding theory (EwDMET) was established…
X-ray absorption spectroscopy yields direct access to the electronic and geometric structure of hybrid inorganic-organic interfaces formed upon adsorption of complex molecules at metal surfaces. The unambiguous interpretation of…
Time-dependent density functional theory is widely used to describe excitations of many-fermion systems. In its many applications, 3D coordinate-space representation is used, and infinite-domain calculations are limited to a finite volume…
Carbon capture is vital for decarbonizing heavy industries such as steel and chemicals. Metal-organic frameworks (MOFs), with their high surface area and structural tunability, are promising materials for CO2 capture. This study focuses on…
Density matrix embedding theory (DMET) describes finite fragments in the presence of a surrounding environment. In contrast to most embedding methods, DMET explicitly allows for quantum entanglement between both. In this chapter, we discuss…
An approximate method based on adiabatic time dependent density functional theory (TDDFT) is presented, that allows for the description of the electron dynamics in nanoscale junctions under arbitrary time dependent external potentials. In…
The atomistic resolution recently achieved by ultrafast spectroscopies demands corresponding theoretical advances. Real-time time-dependent density-functional theory (RT-TDDFT) with Ehrenfest dynamics offers an optimal trade-off between…
We integrate the all-electron electronic structure code FHI-aims into the general ChemShell package for solid-state embedding (QM/MM) calculations. A major undertaking in this integration is the implementation of pseudopotential…
A first-principles study of the adsorption of a single water molecule on a layer of graphitic carbon nitride employing an embedding approach is presented. The embedding approach involves an algorithm to obtain localized Wannier orbitals of…
Widely employed Near-Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy probes a system by excitation of core electrons to unoccupied states. A variety of different methodologies are available to simulate corresponding spectra from…
Including the effect of the molecular environment in the numerical modeling of time-resolved electronic spectroscopy remains an important challenge in computational spectroscopy. In this contribution, we present a general approach for the…
Quantum computing has shown great potential in various quantum chemical applications such as drug discovery, material design, and catalyst optimization. Although significant progress has been made in quantum simulation of simple molecules,…
The real-time electronic dynamics on material surfaces is critically important to a variety of applications. However, their simulations have remained challenging for conventional methods such as the time-dependent density-functional theory…
Development of the electronic kinetic-energy density functional is a subject of major interest in theoretical physics and chemistry. In this work, the nonlocal kinetic-energy functional is developed in terms of the response function for the…
Ultra-fast electronic phenomena originating from finite temperature, such as nonlinear optical excitation, can be simulated with high fidelity via real-time time dependent density functional theory (rt-TDDFT) calculations with hybrid…
An embedding method for solving the time-dependent Schr\"odinger equation is developed using the Dirac-Frenkel variational principle. Embedding allows the time-evolution of the wavefunction to be calculated explicitly in a limited region of…
Deep-learning models have enabled performance leaps in analysis of high-dimensional functional MRI (fMRI) data. Yet, many previous methods are suboptimally sensitive for contextual representations across diverse time scales. Here, we…
We develop a quantum embedding method that enables accurate and efficient treatment of interactions between molecules and an environment, while explicitly including many-body correlations. The molecule is composed of classical nuclei and…
First principle theoretical modeling of out-of-equilibrium processes observed in attosecond pump-probe transient absorption spectroscopy (TAS) triggering pure electron dynamics remains a challenging task, specially for heavy elements and/or…
In this work, we extend the x-ray constrained wavefunction fitting approach, a key method in quantum crystallography for charge density reconstruction, to incorporate experimental observables beyond x-ray diffraction. Unlike traditional…