化学物理
Electro-sorption (ES) is a research frontier in electrochemical separation, with proven potential applications in desalination, wastewater treatment, and selective resource extraction. However, due to the limited adsorption capacity of film…
We investigate the endofullerene system $^3$He@C$_{60}$ with a four-dimensional Potential Energy Surface (PES) to include the three He translational degrees of freedom and C$_{60}$ cage radius. We compare MP2, SCS-MP2, SOS-MP2, RPA@PBE and…
Machine learning has emerged as a promising paradigm to study the quantum dissipative dynamics of open quantum systems. To facilitate the use of our recently published ML-based approaches for quantum dissipative dynamics, here we present an…
Simulations of the dynamics of dissipative quantum systems utilize many methods such as physics-based quantum, semiclassical, and quantum-classical as well as machine learning-based approximations, development and testing of which requires…
A general-order open-shell coupled-cluster method based on spatial orbitals is formulated. The method is an extension of the partial-spin adaptation (PSA) scheme from Janssen and Schaefer (Theor. Chim. Acta, 79, 1-42, 1991). By increasing…
We modify the reweighting factor of the projector used in diffusion Monte Carlo to reduce the time-step error of the total energy. Further, we present a reweighting scheme that has the desirable feature that it is exactly size-consistent,…
The search for new phases is an important direction in materials science. The phase transition of sulfides results in significant changes in catalytic performance, such as MoS2 and WS2. Cubic pentlandite [cPn, (Fe, Ni)9S8] can be a…
The reactive uptake of $\mathrm{N_2O_5}$ on sea-spray aerosol plays a key role in regulating NO$_\mathrm{x}$ concentration in the troposphere. Despite numerous field and laboratory studies, a microscopic understanding of its heterogeneous…
Metal-organic frameworks (MOFs) are promising materials for gas sensing but are often limited to single-use detection. We demonstrate a hybridization strategy synergistically deploying conductive MOFs (cMOFs) and conductive polymers (cPs)…
Finding collective variables to describe some important coarse-grained information on physical systems, in particular metastable states, remains a key issue in molecular dynamics. Recently, machine learning techniques have been intensively…
Water shows anomalous properties that are enhanced upon supercooling. The unusual behavior is observed in both H$_2$O and D$_2$O, however with different temperature dependences for the two isotopes. It is often noted that comparing the…
We present two alternative methods for optimizing minimum energy conical intersection (MECI) molecular geometries without knowledge of the derivative coupling (DC). These methods are based on the utilization of Lagrange multipliers: i) one…
DFT calculations yield useful ground-state energies and densities, while Green's function techniques (such as $GW$) are mostly used to produce spectral functions. From the Galitskii-Migdal formula, we extract the exchange-correlation of DFT…
We present an efficient particle-particle random phase approximation (ppRPA) approach that predicts accurate excitation energies of point defects, including the nitrogen-vacancy (NV$^-$) and the silicon-vacancy (SiV$^0$) centers in diamond…
The light-harvesting excitonic properties of poly(phenylene ethynylene) (PPE) extended dendrimers (tree-like {\pi}-conjugated macromolecules) involve a directional cascade of local excitation-energy transfer (EET) processes occurring from…
Machine learning (ML) provides access to fast and accurate quantum chemistry (QC) calculations for various properties of interest such as excitation energies. It is often the case that high accuracy in prediction using an ML model, demands…
Molecular conformation optimization is crucial to computer-aided drug discovery and materials design. Traditional energy minimization techniques rely on iterative optimization methods that use molecular forces calculated by a physical…
The task of computing wavefunctions that are accurate, yet simple enough mathematical objects to use for reasoning has long been a challenge in quantum chemistry. The difficulty in drawing physical conclusions from a wavefunction is often…
In this work, the vibrational dynamics and spectroscopy of deuterated water molecules (D$_{2}$O) mimicking dense water layers at room temperature on the surfaces of two different C/N based materials with different N content and pore size,…
The latest experimental [Noll et al. Atmos. Chem. Phys. 20(2020)5269] and theoretical [Brooke et al. J. Quant. Spectr. Rad. Transfer 168(2016)142] data on the OH emission intensities are analyzed with use of the NIDL. It is found that the…