Comments on “Global and Regional Entropy Production by Radiation Estimated from Satellite Observations”

A recent paper by Kato and Rose reports a negative correlation between the annual mean entropy production rate of the climate and the absorption of solar radiation in the CERES SYN1deg dataset, using the simplifying assumption that the system is steady in time. It is shown here, however, that when the nonsteady interannual storage of entropy is accounted for, the dataset instead implies a positive correlation; that is, global entropy production rates increase with solar absorption. Furthermore, this increase is consistent with the response demonstrated by an energy balance model and a radiative–convective model. To motivate this updated analysis, a detailed discussion of the conceptual relationship between entropy production, entropy storage, and entropy flows is provided. The storage-corrected estimate for the mean global rate of entropy production in the CERES dataset from all irreversible transfer processes is 81.9 mW m−2 K−1 and from only nonradiative processes is 55.2 mW m−2 K−1 (observations from March 2000 to February 2018).

Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals

Nonradiative processes limit optoelectronic functionality of nanocrystals and curb their device performance. Nevertheless, the dynamic structural origins of nonradiative relaxations in such materials are not understood. Here, femtosecond electron diffraction measurements corroborated by atomistic simulations uncover transient lattice deformations accompanying radiationless electronic processes in colloidal semiconductor nanocrystals. Investigation of the excitation energy dependence in a core/shell system shows that hot carriers created by a photon energy considerably larger than the bandgap induce structural distortions at nanocrystal surfaces on few picosecond timescales associated with the localization of trapped holes. On the other hand, carriers created by a photon energy close to the bandgap of the core in the same system result in transient lattice heating that occurs on a much longer 200 picosecond timescale, dominated by an Auger heating mechanism. Elucidation of the structural deformations associated with the surface trapping of hot holes provides atomic-scale insights into the mechanisms deteriorating optoelectronic performance and a pathway towards minimizing these losses in nanocrystal devices.

Температурная зависимость интенсивности селективного излучения линии R-=SUB=-1-=/SUB=- при лазерно-термическом нагреве рубина

Temperature dependence of intensity of R1 line selective emission at laser thermal heating of ruby was experimentally investigated and explained by competition of radiative and nonradiative processes.

Conical Intersections at the Nanoscale: Molecular Ideas for Materials

The ability to predict and describe nonradiative processes in molecules via the identification and characterization of conical intersections is one of the greatest recent successes of theoretical chemistry. Only recently, however, has this concept been extended to materials science, where nonradiative recombination limits the efficiencies of materials for various optoelectronic applications. In this review, we present recent advances in the theoretical study of conical intersections in semiconductor nanomaterials. After briefly introducing conical intersections, we argue that specific defects in materials can induce conical intersections between the ground and first excited electronic states, thus introducing pathways for nonradiative recombination. We present recent developments in theoretical methods, computational tools, and chemical intuition for the prediction of such defect-induced conical intersections. Through examples in various nanomaterials, we illustrate the significance of conical intersections for nanoscience. We also discuss challenges facing research in this area and opportunities for progress.

Влияние фотоиндуцированных процессов на поверхности квантовых точек на эффективность переноса электрона в структурах "Наночастицы TiO-=SUB=-2-=/SUB=-/Квантовые Точки"

The effect of photoinduced processes on the CdSe/ZnS quantum dots surface on the functionality of TiO2 nanoparticles/quantum dots hybrid structures has been studied. We demonstrate that pre-irradiation of QDs layers allows for a threefold increase in the photoinduced electron transfer efficiency in the structures. It was shown that photoinduced processes affect both the efficiency of nonradiative processes in QDs and electron transfer conditions in hybrid structures.