化学物理
Bottom-up coarse-grained (CG) modeling expands the spatial and temporal scales of molecular simulation by seeking a reduced, thermodynamically consistent representation of an atomistic model. Developments in CG theory have largely focused…
\texttt{MetaWave} is a C++ template-based architecture designed for unified implementation of nonrelativistic and relativistic wavefunction-based quantum chemical methods. It is highly modular, extendable, and efficient. This is achieved by…
We present an efficient orbital optimization procedure that combines the highly GPU accelerated, spin-adapted density matrix renormalization group (DMRG) method with the complete active space self-consistent field (CAS-SCF) approach for…
Indene (C$_9$H$_8$) is the only polycyclic pure hydrocarbon identified in the interstellar medium to date, with an observed abundance orders of magnitude higher than predicted by astrochemical models. The dissociation and radiative…
We develop SOS-RILT-MP2, an efficient Gaussian-based periodic scaled opposite-spin second-order M{\o}ller-Plesset perturbation theory (SOS-MP2) algorithm that utilizes the resolution-of-the-identity approximation (RI) combined with the…
Spincoated polystyrene films of different thickness from 78 nm to 1.3 {\mu}m on silicon wafers were treated by nitrogen ions with an energy of 20 keV. Ellipsometric measurements and FTIR spectra showed modification of the surface layer…
The coherence of light has been proposed as a quantum-mechanical control for enhancing light-harvesting efficiency. In particular, optical coherence can be manipulated by changing either the polarization state or spectral phase of the…
The accurate quantum chemical calculation of excited states is a challenging task, often requiring computationally demanding methods. When entire ground and excited potential energy surfaces (PESs) are desired, e.g., to predict the…
Active and reliable electrocatalysts are fundamental to renewable energy technologies. PdCoO2 has recently been recognized as a promising catalyst template for the hydrogen evolution reaction (HER) in acidic media thanks to the formation of…
Guided by perturbative analysis, we improve the accuracy of Aufbau suppressed coupled cluster theory in simple single excitations, multi-configurational single excitations, and charge transfer excitations while keeping the cost of its…
Reliable computational methodologies and basis sets for modeling x-ray spectra are essential for extracting and interpreting electronic and structural information from experimental x-ray spectra. In particular, the trade-off between…
Recent progress in machine learning (ML) has made high-accuracy quantum chemistry (QC) calculations more accessible. Of particular interest are multifidelity machine learning (MFML) methods where training data from differing accuracies or…
The development of machine learning (ML) methods has made quantum chemistry (QC) calculations more accessible by reducing the compute cost incurred in conventional QC methods. This has since been translated into the overhead cost of…
Least Squares Tensor Hypercontraction (LS-THC) has received some attention in recent years as an approach to reduce the significant computational costs of wavefunction based methods in quantum chemistry. However, previous work has…
Obtaining sub-chemical accuracy (1 kJ mol${}^{-1}$) for reaction energies of medium-sized gas-phase molecules is a longstanding challenge in the field of thermochemical modeling. The perturbative triples correction to CCSD, CCSD(T),…
Coupled cluster theory has had a momentous impact on the ab initio prediction of molecular properties, and remains a staple ingratiate in high-accuracy thermochemical model chemistries. However, these methods require inclusion of at least…
Understanding the process of molecular photoexcitation is crucial in various fields, including drug development, materials science, photovoltaics, and more. The electronic vertical excitation energy is a critical property, for example in…
One method of representing a high-rank tensor as a (hyper-)product of lower-rank tensors is the tensor hypercontraction (THC) method of Hohenstein et al. This strategy has been found to be useful for reducing the polynomial scaling of…
Similarity transformed equation-of-motion coupled cluster theory (STEOM-CC) is an alternative approach to equation-of-motion coupled cluster theory for excited states (EOMEE-CC) which uses a second similarity transformation of the…
The extension of least-squares tensor hypercontracted second- and third-order M{\o}ller-Plessett perturbation theory (LS-THC-MP2 and LS-THC-MP3) to open-shell systems is an important development due to the scaling reduction afforded by THC…