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We recently developed a scheme to use low-cost calculations to find a single twist angle where the coupled cluster doubles energy of a single calculation matches the twist-averaged coupled cluster doubles energy in a finite unit cell. We used initiator full configuration interaction quantum Monte Carlo as an example of an exact method beyond coupled cluster doubles theory to show that this selected twist angle approach had comparable accuracy in methods beyond coupled cluster. Furthermore, at least for small system sizes, we show that the same twist angle can also be found by comparing the energy directly (at the level of second-order Moller-Plesset theory), suggesting a route toward twist angle selection, which requires minimal modification to existing codes that can perform twist averaging.The auxiliary-field quantum Monte Carlo (AFQMC) method is a general numerical method for correlated many-electron systems, which is being increasingly applied in lattice models, atoms, molecules, and solids. Here, we introduce the theory and algorithm of the method specialized for real materials and present several recent developments. We give a systematic exposition of the key steps of AFQMC, closely tracking the framework of a modern software library we are developing. The building of a Monte Carlo Hamiltonian, projecting to the ground state, sampling two-body operators, phaseless approximation, and measuring ground state properties are discussed in detail. An advanced implementation for multi-determinant trial wave functions is described, which dramatically speeds up the algorithm and reduces the memory cost. We propose a self-consistent constraint for real materials, and discuss two flavors for its realization, either by coupling the AFQMC calculation to an effective independent-electron calculation or via the natural orbitals of the computed one-body density matrix.Gas dissolution or accumulation regulating in an aqueous environment is important but difficult in various fields. Here, we performed all-atom molecular dynamics simulations to study the dissolution/accumulation of gas molecules in aqueous solutions. It was found that the distribution of gas molecules at the solid-water interface is regulated by the direction of the external electric field. Gas molecules attach and accumulate to the interface with an electric field parallel to the interface, while the gas molecules depart and dissolve into the aqueous solutions with a vertical electric field. The above phenomena can be attributed to the redistribution of water molecules as a result of the change of hydrogen bonds of water molecules at the interface as affected by the electric field. RGDyK This finding reveals a new mechanism of regulating gas accumulation and dissolution in aqueous solutions and can have tremendous applications in the synthesis of drugs, the design of microfluidic device, and the extraction of natural gas.Despite the remarkable progress of machine learning (ML) techniques in chemistry, modeling the optoelectronic properties of long conjugated oligomers and polymers with ML remains challenging due to the difficulty in obtaining sufficient training data. Here, we use transfer learning to address the data scarcity issue by pre-training graph neural networks using data from short oligomers. With only a few hundred training data, we are able to achieve an average error of about 0.1 eV for the excited-state energy of oligothiophenes against time-dependent density functional theory (TDDFT) calculations. We show that the success of our transfer learning approach relies on the relative locality of low-lying electronic excitations in long conjugated oligomers. Finally, we demonstrate the transferability of our approach by modeling the lowest-lying excited-state energies of poly(3-hexylthiophene) in its single-crystal and solution phases using the transfer learning models trained with the data of gas-phase oligothiophenes. The transfer learning predicted excited-state energy distributions agree quantitatively with TDDFT calculations and capture some important qualitative features observed in experimental absorption spectra.Depositing a simple organic molecular glass-former 2-methyltetrahydrofuran (MTHF) onto an interdigitated electrode device via physical vapor deposition gives rise to an unexpected variety of states, as revealed by dielectric spectroscopy. Different preparation parameters, such as deposition temperature, deposition rate, and annealing conditions, lead, on the one hand, to an ultrastable glass and, on the other hand, to a continuum of newfound further states. Deposition below the glass transition temperature of MTHF leads to loss profiles with shape parameters and peak frequencies that differ from those of the known bulk MTHF. These loss spectra also reveal an additional process with Arrhenius-like temperature dependence, which can be more than four decades slower than the main structural relaxation peak. At a given temperature, the time constants of MTHF deposited between 120 K and 127 K span a range of more than three decades and their temperature dependencies change from strong to fragile behavior. This polyamorphism involves at least three distinct states, each persisting for a duration many orders of magnitude above the dielectric relaxation time. These results represent a significant expansion of a previous dielectric study on vapor deposited MTHF [B. Riechers et al., J. Chem. Phys. 150, 214502 (2019)]. Plastic crystal states and the effects of weak hydrogen bonding are discussed as structural features that could explain these unusual states.We extend Wertheim’s thermodynamic perturbation theory to derive the association free energy of a multicomponent mixture for which double bonds can form between any two pairs of the molecules’ arbitrary number of bonding sites. This generalization reduces in limiting cases to prior theories that restrict double bonding to at most one pair of sites per molecule. We apply the new theory to an associating mixture of colloidal particles (“colloids”) and flexible chain molecules (“linkers”). The linkers have two functional end groups, each of which may bond to one of several sites on the colloids. Due to their flexibility, a significant fraction of linkers can “loop” with both ends bonding to sites on the same colloid instead of bridging sites on different colloids. We use the theory to show that the fraction of linkers in loops depends sensitively on the linker end-to-end distance relative to the colloid bonding-site distance, which suggests strategies for mitigating the loop formation that may otherwise hinder linker-mediated colloidal assembly.