Electrocatalysis by atomic catalysts is a major focus of chemical and energy conversion effort. Although transition-metal-based bulk electrocatalysts for electrochemical application on energy conversion processes have been reported frequently, anchoring the stable transition-metal atoms (e.g. nickel and iron) still remains a practical challenge. Here we report a strategy for fabrication of ACs comprising only isolated nickel/iron atoms anchored on graphdiyne. Our findings identify the very narrow size distributions of both nickel (1.23 Å) and iron (1.02 Å), typical sizes of single-atom nickel and iron. The precision of this method motivates us to develop a general approach in the field of single-atom transition-metal catalysis. Such atomic catalysts have high catalytic activity and stability for hydrogen evolution reactions.

The exciton-dissociation and charge-recombination processes in organic solar cells based on pentacene/C(60) heterojunctions are investigated by means of quantum-mechanical calculations. The electronic couplings and the rates of exciton dissociation and charge recombination have been evaluated for several geometrical configurations of the pentacene/C(60) complex, which are relevant to bilayer and bulk heterojunctions. The results suggest that, irrespective of the actual pentacene-fullerene orientation, both pentacene-based and C(60)-based excitons are able to dissociate efficiently. Also, in the case of parallel configurations of the molecules at the pentacene/C(60) interface, the decay of the lowest charge-transfer state to the ground state is calculated to be very fast; as a result, it can compete with the dissociation process into mobile charge carriers. Since parallel configurations are expected to be found more frequently in bulk heterojunctions than in bilayer heterojunctions, the performance of pentacene/C(60) bulk-heterojunction solar cells is likely to be more affected by charge recombination than that of bilayer devices.

It is a highly desirable but difficult task to predict the molecular fluorescence quantum efficiency from first principles. The molecule in the excited state can undergo spontaneous radiation, conversion of electronic energy to nuclear motion, or chemical reaction. For relatively large molecules, it is impossible to obtain the full potential energy surfaces for the ground state and the excited states to study the excited-state dynamics. We show that, under harmonic approximation by considering the Duschinsky rotation effect, the molecular fluorescence properties can be quantitatively calculated from first principles coupled with our correlation function formalism for the internal conversion. In particular, we have explained the peculiar fluorescence behaviors of two isomeric compounds, cis,cis-1,2,3,4-tetraphenyl-1,3-butadiene and 1,1,4,4-tetraphenyl-butadiene, the former being nonemissive in solution and strongly emissive in aggregation or at low temperature, and the latter being strongly emissive in solution. The roles of low-frequency phenyl ring twist motions and their Duschinsky mode mixings are found to be crucial, especially to reveal the temperature dependence. As an independent check, we take a look at the well-established photophysics of 1,4-diphenylbutadiene for its three different conformers. Both the calculated radiative and nonradiative rates are in excellent agreement with the available experimental measurements.