Related papers: Using molecular similarity to construct accurate s…
Transport in molecular electronic devices is different from that in semiconductor mesoscopic devices in two important aspects: (1) the effect of the electronic structure and (2) the effect of the interface to the external contact. A…
A new scheme of first-principles computation for strongly correlated electron systems is proposed. This scheme starts from the local-density approximation (LDA) at high-energy band structure, while the low-energy effective Hamiltonian is…
Linear-scaling electronic structure methods based on the calculation of moments of the underlying electronic Hamiltonian offer a computationally efficient and numerically robust scheme to drive large-scale atomistic simulations, in which…
Molecular dynamics simulation and recent theory are used to examine density correlations in semidilute solutions of highly charged, intrinsically flexible and hydrophilic polyelectrolytes in low salt. Quantitative comparison with no…
The theory of correlated electron systems is formulated in a form which allows to use as a reference point an ab initio band structure theory (AIBST). The theory is constructed in two steps. As a first step the total Hamiltonian is…
We incorporate explicit, non-perturbative treatment of spin-orbit coupling into ab initio auxiliary-field quantum Monte Carlo (AFQMC) calculations. The approach allows a general computational framework for molecular and bulk systems in…
Modeling the electronic and optical properties of organic semiconductors remains a challenge for theory, despite the remarkable progress achieved in the last three decades. The complexity of these systems, including structural (dis)order…
The exact interaction energy of a many-electron system is determined by the electron pair density, which is not well-approximated in standard Kohn-Sham density functional models. Here we study the (complicated but well-defined) exact…
We proposed the molecular hyper-message passing network (MolHMPN) that predicts the properties of a molecule with prior knowledge-guided subgraph. Modeling higher-order connectivities in molecules is necessary as changes in both the…
We propose a computationally lean, two-stage approach that reliably predicts self-assembly behavior of complex charged molecules on a metallic surfaces under electrochemical conditions. Stage one uses ab initio simulations to provide…
Koopmans-compliant functionals emerge naturally from extending the constraint of piecewise linearity of the total energy as a function of the number of electrons to each fractional orbital occupation. When applied to approximate…
We implement and benchmark the frozen core approximation, a technique commonly adopted in electronic structure theory to reduce the computational cost by means of mathematically fixing the chemically inactive core electron states. The…
The similarity of local atomic environments is an important concept in many machine-learning techniques which find applications in computational chemistry and material science. Here, we present and discuss a connection between the…
A widely used approximation to the exchange-correlation functional in density functional theory is the local density approximation (LDA), typically derived from the properties of the homogeneous electron gas (HEG). We previously introduced…
The symmetry-projected Hartree--Fock ansatz for the electronic structure problem can efficiently account for static correlation in molecules, yet it is often unable to describe dynamic correlation in a balanced manner. Here, we consider a…
By fitting to a database of ab-initio forces and energies, we can extract pair potentials for alloys, with a simple six-parameter analytic form including Friedel oscillations, which give a remarkably faithful account of many complex…
Intramolecular electron transfer capability of all metal aromatic and anti-aromatic aluminum cluster compounds is studied in terms of density functional theory based global and local reactivity descriptors. This study will provide important…
Many quantum chemical similarity measures have been derived and substantiated by applying concepts and quantities from information theory to the electron density. To justify the use of information theory, the electron density is usually…
We use ab initio density functional theory to study the equilibrium geometry and electronic structure of few-layer grey arsenic. In contrast to the bulk structure that is semimetallic, few-layer grey As displays a significant band gap that…
Theoretical concepts in condensed matter physics are typically verified and also developed by exploiting computer simulations mostly in simple models. Predictions based on these usually isotropic models are often at odds with measurement…