化学物理
Ultrafast multidimensional spectroscopies are powerful tools that can access charge and energy flow in complex materials, shifting chemical kinetics, and even many-body interactions in correlated matter. However, current implementations…
The liquid-vapor critical behavior of water is strongly influenced by both ionic solutes and confinement. Molecular dynamics simulations of aqueous NaCl solutions using the TIP4P/2005 water model and the Madrid-2019 ion parameters reveal a…
Hydrogen cyanide (HCN) is a well-known product in combustion, astrophysical, and plasma environments, but its isomer, hydrogen isocyanide (HNC), remains unexplored in molecular plasmas. Here, we report on the detection and quantification of…
Rydberg excited states of molecules pose a challenge for electronic structure calculations because of their highly diffuse electron distribution. Even large and elaborate atomic basis sets tend to underrepresent the long-range tail, overly…
Spectroscopic techniques that are sensitive to molecular chirality are important analytical tools to quantitatively determine enantiomeric excess and purity of chiral molecular samples. Many chiroptical processes however produce weak…
Variational optimization of orbitals in time-independent density functional calculations of excited electronic states presents a significant challenge, as excited states typically correspond to saddle points on the electronic energy…
In this work, we propose a simple method to resolve the eigenstates located at the band gap edges of an electronic eigenspectrum using only the quasi-purified one-particle density matrix as input. The theoretical framework relies on the…
We assess the dielectrically consistent reference interaction site model (DRISM) as an implicit electrolyte framework for modeling the electrochemical double layer, and compare it with the Poisson-Boltzmann model and explicit molecular…
We study a system consisting of an infinite one-dimensional molecular chain and a locally coupled probe. Starting from the Hamiltonian of the chain-probe composite and the corresponding spectral densities, we evaluate the heat current…
We introduce a GPU-accelerated implementation of time-dependent density functional theory with the minimal auxiliary basis approach (TDDFT-risp) in GPU4PySCF, together with large system demonstrations carried out using the Tamm--Dancoff…
Chemical reaction sampling critically depends on collective variables (CVs) that capture the slow degrees of freedom governing reactive transformations. However, existing reaction CVs are often defined in geometric space or learned in a…
The wave-particle duality of massive macromolecules -- such as the fullerene C$_{60}$ -- is a well-established quantum phenomenon. However, whether the quantum behavior of large organic molecules actively dictates the macroscopic structure…
Optically addressable molecular triplet spins provide a chemically tunable platform for quantum application, but their coherence is often limited by interactions with surrounding spin baths. Here we demonstrate controlled suppression of…
While configuration interaction singles (CIS) provides a computationally efficient description of excited states, it systematically overestimates excitation energies and performs poorly for strongly correlated systems, partly due to the…
Recurrent fluorescence (RF) is an important relaxation mechanism in polycyclic aromatic hydrocarbons (PAHs), which could stabilize them and contribute to the production of aromatic infrared bands that are observed in the infrared spectra of…
In light of major developments over the past decades in both quantum computing and simulations on classical hardware, it is a serious challenge to identify a real-world problem where quantum advantage is expected to appear. In quantum…
This book provides an introduction to path integral methods and their application to modeling atomistic processes. The book covers both the foundational theory and recently developed simulation techniques. The text provides a self-contained…
We present a computationally efficient relativistic formulation of the equation-of-motion coupled-cluster method for the double electron attachment problem. In this work, the exact two-component Hamiltonian within the atomic mean-field…
After melting, at ambient pressure, the density of water continues to increase with temperature until it reaches a maximum around 4 {\deg}C. For nearly a century, this phenomenon has been qualitatively attributed to a mixture of ordered and…
The discovery of polymers with targeted properties is challenged by the vast chemical design space and the limited availability of consistent, high-quality data across multiple properties. In this work, an integrated polymer informatics…