化学物理
We introduce a GPU-accelerated multigrid Gaussian-Plane-Wave density fitting (FFTDF) approach for efficient Fock builds and nuclear gradient evaluations within Kohn-Sham density functional theory, as implemented in the GPU4PySCF module of…
Previous research based on electronic structure calculations and molecular dynamics (MD) simulations have demonstrated that graphdiyne (GDY) is a very suitable two-dimensional membrane for the separation of small molecules in a gas mixture…
Machine-learned interatomic potentials (MLIPs), particularly graph neural network (GNN)-based models, offer a promising route to achieving near-density functional theory (DFT) accuracy at significantly reduced computational cost. However,…
By reducing resolution, coarse-grained models greatly accelerate molecular simulations, unlocking access to long-timescale phenomena, though at the expense of microscopic information. Recovering this fine-grained detail is essential for…
We present a theoretical investigation on the electronic structure and properties of radium monochalcogenides, with chalcogens O, S, and Se, as well as the ionic species RaO +/-. Our approach combines fully relativistic and partially…
We solve the orientation recovery of a tumbling protein in the gas phase from single-event measurements of the spatial positions of its ions after an X-ray laser induced explosion. We simulate diffracted X-ray signal and ion dynamics under…
Nonlinear spectroscopy provides a unique perspective to understand time-resolved molecular dynamics under vibrational strong coupling (VSC). Herein, equilibrium-nonequilibrium cavity molecular dynamics simulations are performed to compute…
Why kinetically stable oil droplets in water spontaneously acquire a negative charge remains one of the most vigorously debated questions in interfacial science. Here, we combine neural-network based deep potential molecular dynamics with a…
We present an improved version of the sum-of-Gaussians tensor neural network (SOG-TNN) architecture for solving many-electron Schr\"{o}dinger equation for one-dimensional soft-Coulomb systems. Model reduction techniques are introduced to…
The renewable energy sector critically needs low-cost and environmentally neutral energy storage solutions throughout the entire device life cycle. However, the limited performance of standard water-based electrochemical systems prevents…
Density functional theory (DFT) offers an exceptional balance between accuracy and efficiency, but practical density functional approximations face an unavoidable trade-off among simplicity, accuracy, and transferability. A systematic…
Exciton transport in molecular aggregates is a fundamental process governing the performance of organic optoelectronics and light-harvesting systems. While most theoretical studies have emphasized long-time transport behavior, recent…
Molecular orientation techniques are becoming available in the study of elementary chemical processes, in order to highlight those structural and dynamical properties that would be concealed by random rotational motions. Recently successful…
In multi-dimensional time-resolved spectroscopic experiments, multiple (more than two) short laser pulses with variable pulse delay times are employed for the time-resolved exploration of the photoinduced dynamics of molecular chromophores.…
In this work, we assess two widely used scissors-correction schemes for first-principles calculations of second-harmonic generation in representative borate and phosphate ultraviolet nonlinear-optical (UV-NLO) crystals, namely scheme-L…
We propose the integral-equation formalism of population dynamics (IEPDYN) to describe the population dynamics of distinct configurational states. According to classical reaction dynamics theory, the probability density associated with a…
Solid state nuclear magnetic resonance (ss-NMR) is one of the most sensitive and popular techniques for structure elucidation in geometrically complex crystalline materials, such as zeolites. Synergistic support from computational modelling…
Microscopic understanding of liquid properties is essential for advancing a wide range of applications from energy applications such as nuclear reactors and batteries to biomedical applications including drug delivery and microfluidics.…
Here we present a density matrix based KS inversion method formulated entirely within a Gaussian basis representation to optimize a KS potential matrix that reproduces a target electron density. Inverse Kohn-Sham (KS) density functional…
Machine-learned interatomic potentials hold the promise to enable the modeling of highly concentrated liquids over meaningful timescales, far from reach for current ab initio electronic structure methods. Here we evaluate the performances…