化学物理
The adaptive derivative-assembled problem-tailored variational quantum eigensolver (ADAPT-VQE) is one of the most widely used algorithms for electronic structure calculations in quantum computers. It adaptively selects operators based on…
Water's unique hydrogen-bonding network and anomalous properties pose significant challenges for accurately modeling its structural, thermodynamic, and transport behavior across varied conditions. Although machine-learned potentials have…
Modeling inorganic glasses requires an accurate representation of interatomic interactions, large system sizes to allow for intermediate-range structural order, and slow quenching rates to eliminate kinetically trapped structural motifs.…
CHEMSMART (Chemistry Simulation and Modeling Automation Toolkit) is an open-source, Python-based framework designed to streamline quantum chemistry workflows for homogeneous catalysis and molecular modeling. By integrating job preparation,…
Two-dimensional electronic spectroscopy (2DES) provides rich information about how the electronic states of molecules, proteins, and solid-state materials interact with each other and their surrounding environment. Atomistic molecular…
With the widespread use of self-consistent field methods, including Hartree-Fock and Density Functional Theory, the implications of accelerating these methods are immense. To this end, we develop a tensor hypercontraction construction with…
Model Hamiltonians offer a cost-effective way to capture the key physics of large $\pi$-conjugated systems. In this work, we combine the Pariser--Parr--Pople (PPP) model Hamiltonian with pair Coupled Cluster Doubles (pCCD)-based methods to…
From soap-covered dishes to freshly cleaned floors, surfactants can make surfaces slippery; yet, the underlying mechanism remains poorly understood. Here, we identify the molecular origin behind this ubiquitous phenomenon using macroscopic…
Ab initio path integral Monte Carlo (PIMC) simulations constitute the gold standard for the estimation of a broad range of equilibrium properties of a host of interacting quantum many-body systems spanning conditions from ultracold atoms to…
In situ polymerization of conductive polymers (CPs) represents a transformative approach in bioelectronics, by enabling the controlled growth of electrically active materials right at the tissue or device surface to create seamless…
In this study, we provide a novel wave packet propagation method that generalizes the Hagedorn approach by introducing alternative primitive basis sets that are better suited to describe different physical processes. More precisely, in our…
We present a combined experimental and theoretical study of the vibrationally resolved valence photoelectron spectra of the complete series of thiouracils (2-thiouracil, 4-thiouracil and 2,4-dithiouracil) for binding energies between 8 and…
Understanding the solvation structure of electrolytes is crucial for optimizing the performance and stability of lithium-ion batteries. Novel electrolytes are essential for enhancing electrolyte structure and ensuring better integration…
Second order stochastic optimization methods, such as the linear method, couple the updates of different parameters and, in so doing, allow statistical uncertainty in one parameter to affect the update of other parameters. In simple tests,…
The development of new electronic structure methods is a very time consuming and error prone process when done by hand. SpinAdaptedSecondQuantization is an open-source Julia package we have developed for working with automated electronic…
The appearance of angular momentum in the nuclear motion of molecular systems lacking inversion symmetry under imposed thermal gradients presents a novel mechanism with potential implications for spintronics, magnetic response, and energy…
Understanding how the electronic structure of electrodes influences electrocatalytic reactions has been a longstanding topic in the electrochemistry community, with predominant attention paid to metallic electrodes. In this work, we present…
The tris(2,4,6-trichlorophenyl)methyl radical (TTM) has inspired the synthesis of several luminescent diradicals and diradicaloids, providing an extraordinary opportunity to control the nature of the low-lying excited states by fine-tuning…
In the present work we report an implementation of the rank-reduced equation-of-motion coupled cluster method with approximate triple excitations (RR-EOM-CC3). The proposed variant relies on tensor decomposition techniques in order to…
Recent SO(3)-equivariant models embedded a molecule as a set of single atoms fixed in the three-dimensional space, which is analogous to a ball-and-stick view. This perspective provides a concise view of atom arrangements, however, the…