化学物理
Recently, thermally-assisted-occupation density functional theory (TAO-DFT) [J.-D. Chai, J. Chem. Phys. 136, 154104 (2012)] has been demonstrated to be an efficient and accurate electronic structure method for studying the ground-state…
A unitary coupled-cluster (UCC)-based self-consistent electron propagator theory (EPT) is proposed for the description of electron-detached and electron-attached states. Two practical schemes, termed IP/EA-UCC3 and IP/EA-qUCCSD, are…
We propose mixed quantum-classical equations of motion that unify electronic coherence and phase evolution simultaneously within the exact factorization framework. Our derivation shows that incorporating the second-order electron-nuclear…
Glyphosate, the most widely used herbicide worldwide, crystallizes through complex intermolecular interactions that are strongly influenced by synthesis-derived impurities. Understanding this process at the molecular scale is critical for…
In many cases, the predictions of machine learning interatomic potentials (MLIPs) can be interpreted as a sum of body-ordered contributions, which is explicit when the model is directly built on neighbor density correlation descriptors, and…
Accurately capturing the complex interaction between CO2 and water in porous media at the pore scale is essential for various geoscience applications, including carbon capture and storage (CCS). We introduce a comprehensive dataset…
The dissociation micro-states (DMS) of an $N$-protic acid are described using set theory notation. This facilitates the mathematical description of the dissociation micro-equilibrium (DME). In particular, the DME constants are easily…
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…
X-ray absorption spectroscopy (XAS) is an indispensable tool to characterize the atomic-scale three-dimensional local structure of the system, in which XANES is the most important energy region to reflect the three-dimensional structure.…
The development of a novel exact two-component (X2C) scheme with the inclusion of the picture-change correction for the fluctuation potential, the X2Ccorr scheme, is reported, hereby establishing a hierarchy of X2C schemes with systematic…
This Review is devoted to the presentation of the exact factorization as a framework employed to study a variety of quantum-mechanical many-body problems. Since its original formulation in the 70s, the main applications of the exact…
We have studied the effect of zwitterionic form of the amino acid on the electron attachment to DNA using thymine glycine as a model system. The electron attachment to thymine in the presence of glycine takes place through a "doorway…
Personal care formulations often contain synthetic and non-biodegradable ingredients, such as silicone and mineral oils, which can offer a unique performance. However, due to regulations like the EU ban of Octamethylcyclotetrasiloxane (D4),…
Strong coupling between molecular excitations and quantized electromagnetic fields in optical cavities provides a powerful means to control the physical and chemical properties of molecular systems. Here, we study electron transfer (ET)…
We present a microscopic, parameter-free approach for computing the photoluminescence spectra of a single semiconductor nanocrystal. The method derives exciton-phonon coupling directly from the semi-empirical pseudopotential framework and…
Wavefunction-based quantum methods are some of the most accurate tools for predicting and analyzing the electronic structure of molecules, in particular for accounting for dynamical electron correlation. However, most methods of including…
A peculiar electron correlation effect, leading to orbital rotation upon ionization, theoretically predicted long ago, was never experimentally characterized. The effect is expected to appear prominently in the photoionization of chiral…
Machine-learned (ML) coarse-grained (CG) models are a promising tool for significantly enhancing the efficiency of molecular simulations by systematically removing degrees of freedom while retaining fidelity to the underlying fine-grained…
Atomistic simulations of electrochemical interfaces remain challenging due to the long time scales required to adequately sample the structure of the electric double layer. The emergence of efficient, short-range machine learning…
Interpretable reaction coordinates are essential for understanding rare conformational transitions in molecular dynamics. The Atomistic Mechanism Of Rare Events in Molecular Dynamics (AMORE-MD) framework enhances interpretability of…