化学物理
In this work, we study the quantum dynamics of a photoisomerization reaction employing a two-electronic-state three-vibrational-mode model of the 2-cis-penta-2,4-dieniminium cation (cis-PSB3). In particular, we address two main issues: the…
Machine learning potentials have achieved great success in accelerating atomistic simulations. Many of them relying on atom-centered local descriptors are natural for parallelization. More recent message passing neural network (MPNN) models…
An ab initio approach formulated under an entropy-inspired repartitioning of the electronic Hamiltonian is presented. This ansatz produces orbital eigenvalues each shifted by entropic contributions expressed as subsets of scaled pair…
Accelerating quantum dynamical simulations with quantum computing has received considerable attention but remains a significant challenge. In variational quantum algorithms for quantum dynamics, designing an expressive and shallow-depth…
Applying quantum chemistry algorithms to large-scale systems requires substantial computational resources scaled with the system size and the desired accuracy. To address this, ByteQC, a fully-functional and efficient package for…
Trivalent lanthanide ion-doped nanoparticles are widely employed as nanoscale thermometers, driving rapid advancements in real-world applications. When the Luminescence Intensity Ratio (LIR) technique is used, these thermometric systems…
Ab initio molecular dynamics (AIMD) based on density functional theory (DFT) has become a workhorse for studying the structure, dynamics, and reactions in condensed matter systems. Currently, AIMD simulations are primarily carried out at…
The dynamics for the NO($X^2 \Pi$) + N($^4$S) $\leftrightarrow$ N$_{2}(X^{1}\Sigma_{g}^{+}$) + O($^{3}$P) reaction was followed in the $^3$A' electronic state using state-to-state (STS) and Arrhenius-based rates from two different…
The high-temperature atom exchange and dissociation reaction dynamics of the O($^3$P) + O$_2(^3\Sigma_g^{-} )$ system are investigated based on a new reproducing kernel-based representation of high-level multi-reference configuration…
Extracting molecular properties from a wave function can be done through the linear response (LR) formalism or, equivalently, the equation of motion (EOM) formalism. For a simple model system, He in a 6-31G basis, it is here shown that…
Coarse-graining complex molecular systems to lower-dimensional reaction coordinates is a powerful approach for capturing their effective dynamics. The generalized Langevin equation (GLE) provides an exact framework for modeling…
This chapter overviews sulfur chemical speciation and behavior in different types of hydrothermal fluids across the lithosphere, spanning from active geothermal systems to basinal brines, to metamorphic and magmatic-hydrothermal fluids. The…
We present path integral Monte Carlo simulation results for the equation of state of solid parahydrogen between $ 0.024 \, {\r{A}}^{-3} $ and $ 0.1 \, {\r{A}}^{-3} $ at $ T = 4.2 \, $ K. The simulations are performed using non-additive…
We present an isotropic ab initio (para-H$_2$)$_4$ four-body interaction potential energy surface (PES). The electronic structure calculations are performed at the correlated coupled-cluster theory level, with single, double, and…
Room temperature single photon sources (SPS) are crucial for developing the next generation quantum technologies. Quantum dots (QDs), recently, have been reported as promising materials as SPS at room temperature. By optimizing the single…
We present a first principles strategy for developing state-specific density functional approximations for excited states. We first clarify why approaches based on conventional ground state approximations miss density-driven correlations,…
Previously obtained expressions describing the intensity of stationary fluorescence emitted by a multicomponent solution were significantly improved by using matrix calculus. Then, using a similar technique, new expressions describing the…
The balance between localised and delocalised electron distribution in the N,N'-dimethylpiperazine (DMP) molecule in the 3s Rydberg excited state and in the fully ionised DMP$^+$ provides a valuable test of density functionals, in…
Highly flexible Jastrow factors have found significant use in stochastic electronic structure methods such as variational Monte Carlo (VMC) and diffusion Monte Carlo, as well as in quantum chemical transcorrelated (TC) approaches, which…
Quantum many-body methods provide a systematic route to computing electronic properties of molecules and materials, but high computational costs restrict their use in large-scale applications. Due to the complexity in many-electron…