相关论文: Nonlocal Subsystem Density Functional Theory

Scalable quantum-classical embedding is essential for chemically meaningful simulations on near-term NISQ hardware. Using QDFT, we show systematic recovery of correlation energy relative to the DFT baseline, benchmarked against CCSD in a…

We propose a method that incorporates explicit derivative discontinuity of the total energy with respect to the number of electrons and treats both delocalization and static correlation effects in density functional calculations. Our…

We study model one-dimensional chemical systems (representative of their three-dimensional counterparts) using the strictly-correlated electrons (SCE) functional, which, by construction, becomes asymptotically exact in the limit of infinite…

Time-dependent density functional theory (TDDFT) is rapidly emerging as a premier method for solving dynamical many-body problems in physics and chemistry. The mathematical foundations of TDDFT are established through the formal existence…

We propose a new molecular simulation framework that combines the transferability, robustness and chemical flexibility of an ab initio method with the accuracy and efficiency of a machine learned force field. The key to achieve this mix is…

Perdew et al. [Phys. Rev. Lett 49, 1691 (1982)] discovered and proved two different properties of exact Kohn-Sham density functional theory (DFT): (i) The exact total energy versus particle number is a series of linear segments between…

We propose an approach that links density functional theory (DFT) and molecular dynamics (MD) simulation to study fluid behavior in nanopores in contact with bulk (macropores). It consists of two principal steps. First, the theoretical…

Quantum--Mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those…

Dynamical Mean-Field Theory (DMFT) has opened new perspectives for the investigation of strongly correlated electron systems and greatly improved our understanding of correlation effects in models and materials. In contrast to…

Typical density functional theory (DFT) and approximations thereto solve the many-electron ground state problem by working from a numerically efficient non-interacting Kohn-Sham reference system; and benefit from useful minimization…

The density functional theory (DFT) is a remarkably successful theory of electronic structure of matter. At the foundation of this theory lies the Kohn-Sham (KS) equation. In this paper, we describe the long-time behaviour of the…

Density functional theory (DFT), one of the most widely utilized methods available to computational chemistry, fails to describe systems with statically correlated electrons. To address this shortcoming, in previous work we transformed DFT…

The inverse problem of Kohn-Sham density functional theory (DFT) is often solved in an effort to benchmark and design approximate exchange-correlation potentials. The forward and inverse problems of DFT rely on the same equations but the…

Molecular dynamics (MD) simulation, which is considered an important tool for studying physical and chemical processes at the atomic scale, requires accurate calculations of energies and forces. Although reliable energies and forces can be…

Understanding the nanoscale effects controlling the dynamics of a contact line -- defined as the line formed at the junction of two fluid phases and a solid -- has been a longstanding problem in fluid mechanics pushing experimental and…

The treatment of degenerate states within Kohn-Sham density functional theory (KS-DFT) is a problem of longstanding interest. We propose a solution to this mapping from the interacting degenerate system to that of the noninteracting fermion…

Modern density functional theory (DFT) calculations employ the Kohn-Sham (KS) system of non-interacting electrons as a reference, with all complications buried in the exchange-correlation energy (Exc). The adiabatic connection formula gives…

The systematic underestimation of band gaps is one of the most fundamental challenges in semilocal density functional theory (DFT). In addition to hindering the application of DFT to predicting electronic properties, the band gap problem is…

Green technologies rely on green solvents and fluids. Among them, supercritical CO2 already finds many important applications. The molecular level understanding of the dynamics and structure of this supercritical fluid is a prerequisite to…

We propose a novel scheme to bring reduced density matrix functional theory (RDMFT) into the realm of density functional theory (DFT) that preserves the accurate density functional description at equilibrium, while incorporating accurately…