Several protocols are proposed to build continuous energy surfaces of many-body quantum systems, regarding both energy and states. The standard variational principle is augmented with constraints on state overlap, ensuring arbitrary precision on continuity. As an illustration, the lowest energy and excited state paths relevant for the ^{240}Pu asymmetric fission are studied.
View Article and Find Full Text PDFLight-dependent reduction of carbon dioxide (CO) into value-added products can be catalyzed by a variety of molecular complexes. Here we report a rare example of a structurally characterized artificial enzyme, resulting from the combination of a heme binding protein, heme oxygenase, with cobalt-protoporphyrin IX, with good activity for the photoreduction of CO to carbon monoxide (CO). Using a copper-based photosensitizer, thus making the photosystem free of noble metals, a large turnover frequency value of ∼616 h, a turnover value of ∼589, after 3 h reaction, and a CO vs H selectivity of 72% were obtained, establishing a record among previously reported artificial CO reductases.
View Article and Find Full Text PDFMetal-dependent formate dehydrogenases are very promising targets for enzyme optimization and design of bio-inspired catalysts for CO reduction, towards innovative strategies for climate change mitigation. For effective application of these enzymes, the catalytic mechanism must be better understood, and the molecular determinants clarified. Despite numerous studies, several doubts persist, namely regarding the role played by the possible dissociation of the SeCys ligand from the Mo/W active site.
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