Chemical Physics
Phase-space electronic structure theory offers up a new and powerful approach for tackling problems with coupled nuclear-electronic dynamics in a fashion that goes beyond Born-Oppenheimer (BO) theory. Whereas BO theory stipulates that we…
The oxidation state (OS) is an essential chemical concept that embodies chemical intuition but cannot be computed with well-defined physical laws. We establish a data-driven paradigm, with its implementation as Tsinghua Oxidation States in…
Identifying organic molecules with desirable properties from the extensive chemical space can be challenging, particularly when property evaluation methods are time-consuming and resource intensive. In this study, we illustrate this…
Drawing inspiration from the domain of image super-resolution, we view the electron density as a 3D grayscale image and use a convolutional residual network to transform a crude and trivially generated guess of the molecular density into an…
Understanding how molecules arrange on surfaces is fundamental to surface chemistry and essential for the rational design of catalytic and functional materials. In particular, the energetically most stable configuration provides valuable…
Electron-phonon coupling (EPC) is fundamental for understanding the behavior of molecules and crystals, influencing phenomena such as charge transport, energy transfer, phase transitions, and polaron formation. Accurate computational…
Light-driven molecular nanomotors hold promise for applications in material science and biomedicine. Significant efforts have focused on improving their efficiency, often targeting single candidate molecules. Here, we present a systematic…
Ultrafast multistage electron transfer (ET) in molecular systems with multiple redox centers is fundamental to photochemical energy conversion, including processes in natural photosynthesis, molecular optoelectronics, and organic…
We have implemented relativistic formulations of DIP-EOMCCSD and DIP-EOMCCSDT within the 1eX2C and DC-, DCG-, and DCB-X2C frameworks. Direct comparisons against full 4c-DIP-EOMCCSD calculations show excellent agreement with…
Coupling molecular transition dipole moments to surface-plasmon polaritons (SPPs) results in the formation of new optical quasiparticles, i.e., plexcitons. Mixing the specific properties of matter excitations and light modes has proven to…
We develop a non-linear and non-empirical (nlane) double hybrid density functional derived from an accurate interpolation of the adiabatic connection in density functional theory, incorporating the correct asymptotic expansions. By bridging…
High-quality potential energy surfaces (PES) are a prerequisite for quantitative atomistic simulations, with both quantum and classical dynamics approaches. The ultimate test for the validity of a PES are comparisons with judiciously chosen…
Neural network quantum states (NQS) have emerged as a powerful and flexible framework for addressing quantum many-body problems. While successful for model Hamiltonians, their application to molecular systems remains challenging for several…
In Coupled-Cluster (CC) theory, unphysical complex energies may arise in the presence of strong magnetic fields, near conical intersections, or in systems exhibiting complex Abelian point group symmetries. This issue originates from the…
Liquid electrolytes adsorbed at the surface of metallic electrodes display a multitude of structures that can largely differ from the parent bulk system, both in terms of composition and local organization. In particular, the existence of…
The end-to-end dynamics of the smallest energized Criegee intermediate, H$_2$COO, was characterized for vibrational excitation close to and a few kcal/mol above the barrier for hydrogen transfer. From an aggregate of at least 5 $\mu$s of…
Conical intersections play a pivotal role in excited-state quantum dynamics. Capturing transient molecular structures near conical intersections remains challenging due to the rapid timescales and subtle structural changes involved. We…
Modeling charge transfer well can require treating post-excitation orbital relaxations and handling medium to large molecules in realistic environments. By combining a state-specific correlation treatment with such orbital relaxations,…
Machine learning has emerged as a powerful tool in atomistic simulations, enabling the identification of complex patterns in molecular systems limiting human intervention and bias. However, the practical implementation of these methods…
This work presents a strategy to efficiently and safely account for decoherence in the fewest switches surface hopping method. Standard decoherence corrections often lead to too strong coherence suppression. A simple and general solution to…