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Alloys are active in CO2 electroreduction due to their unique electronic and geometric structures. Nevertheless, CO2 reduction selectivity is still low due to the low concentration of CO2 near the catalyst surface and the high energy barrier for CO2 activation. This paper describes an AuCu nanochain aerogel (NC-AuCu) with abundant grain boundaries (GBs) that promote the accumulation and activation of CO2 for further electrochemical reduction, employing in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy and density functional theory calculations. GBs can induce a strong local electric field to concentrate the electrolyte cations and thus accumulate CO2 near the catalyst surface. NC-AuCu exhibits a superior Faradaic efficiency of close to 100% for CO2 electroreduction to CO at an extremely low overpotential of 110 mV with a high CO partial current density of 28.6 mA cm-2 in a flow cell. Coupling with a Si solar cell to convert solar energy to CO, a very high conversion efficiency of ∼13.0% is achieved. It potentially provides broad interest for further academic research and industry applications.The hierarchical equations of motion (HEOM) theory is one of the standard methods to rigorously describe open quantum dynamics coupled to harmonic environments. Such a model is used to capture non-Markovian and non-perturbative effects of environments appearing in ultrafast phenomena. In the regular framework of the HEOM theory, the environment correlation functions are restricted to linear combinations of exponential functions. In this article, we present a new formulation of the HEOM theory including treatment of non-exponential correlation functions, which enables us to describe general environmental effects more efficiently and stably than the original theory and other generalizations. The library and its Python binding we developed to perform simulations based on our approach, named LibHEOM and PyHEOM, respectively, are provided as the supplementary material.Electron ratchets are non-equilibrium electronic devices that break inversion symmetry to produce currents from non-directional and random perturbations, without an applied net bias. They are characterized by strong parameter dependence, where small changes in operating conditions lead to large changes in the magnitude and even direction of the resulting current. This high sensitivity makes electron ratchets attractive research subjects, but leads to formidable challenges in their deeper study, and particularly to their useful application. This perspective reviews the progress that was made in the field starting from the first experimental electron ratchets in the late 1990s, and how the field spawned multiple designs with very different properties. We discuss the possible uses of electron ratchets in sensing and energy harvesting, and the specific issues encountered when idealized behavior meets complex reality. We promote an application-driven approach where complexity is not necessarily detrimental and argue that a system level perspective would be beneficial over reductionism. We highlight several promising research directions, which revolve around the intentional study of complex effects, and the modeling of realistic devices.We propose and validate several variants of the optimally tuned range-separated hybrid functionals (OT-RSHs) including different density functional approximations for predicting the fluorescence lifetimes of different categories of fluorophores within the time-dependent density functional theory (TD-DFT) framework using both the polarizable continuum and state-specific solvation models. Our main idea originates from performing the optimal tuning in the presence of a contribution of the exact-like exchange at the short-range part, which, in turn, leads to the small values of the range-separation parameter, and computing the fluorescence lifetimes using the models including no or small portions of the short-range exact-like exchange. Particular attention is also paid to the influence of the geometries of emitters on fluorescence lifetime computations. It is shown that our developed OT-RSHs along with the polarizable continuum model can be considered as the promising candidates within the TD-DFT framework for the prediction of fluorescence lifetimes for various fluorophores. We find that the proposed models not only outperform their standard counterparts but also provide reliable data better than or comparable to the conventional hybrid functionals with both the fixed and interelectronic distance-dependent exact-like exchanges. Furthermore, it is also revealed that when the excited state geometries come into play, more accurate descriptions of the fluorescence lifetimes can be achieved. Hopefully, our findings can give impetus for future developments of OT-RSHs for computational modeling of other characteristics in fluorescence spectroscopy as well as for verification of the related experimental observations.We introduce the Nuclear-Electronic All-Particle Density Matrix Renormalization Group (NEAP-DMRG) method for solving the time-independent Schrödinger equation simultaneously for electrons and other quantum species. In contrast to the already existing multicomponent approaches, in this work, we construct from the outset a multi-reference trial wave function with stochastically optimized non-orthogonal Gaussian orbitals. By iterative refining of the Gaussians' positions and widths, we obtain a compact multi-reference expansion for the multicomponent wave function. We extend the DMRG algorithm to multicomponent wave functions to take into account inter- and intra-species correlation effects. The efficient parameterization of the total wave function as a matrix product state allows NEAP-DMRG to accurately approximate the full configuration interaction energies of molecular systems with more than three nuclei and 12 particles in total, which is currently a major challenge for other multicomponent approaches. We present the NEAP-DMRG results for two few-body systems, i.e., H2 and H3 +, and one larger system, namely, BH3.The most common bulk acoustic wave device used in biosensing applications is the quartz crystal microbalance (QCM), in which a resonant pure shear acoustic wave is excited via electrodes on both major faces of a thin AT-cut quartz plate. For biosensing, the QCM is used to detect the capture of a target by a target-capture film. The sensitivity of the QCM is typically based solely on the detection of mechanical property changes, as electrical property change detection is limited by the electrode on its sensing surface. A modification of the QCM called the lateral field excited (LFE) QCM (LFE-QCM) has been developed with a bare sensing surface as both electrodes are now on a single face of the quartz plate. Compared to the QCM, the LFE-QCM exhibits significantly higher sensitivity to both electrical and mechanical property changes. This paper presents theoretical and experimental aspects of LFE-QCMs. selleck products In particular, the presence and strength of the usual and newfound LFE-QCM modes depend on the electrical properties of the film and/or sensing environment.