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Photoreactions Create Superconducting Materials
Abstract
One of the potentially transformative areas of scientific development is to achieve superconductivity at room temperature. Recently, the photochemical synthesis was carried out to prepare carbonaceous sulfur hydride (CSH) systems with room-temperature superconductivity at high pressure. In this work, we present a first-principles study aiming to unravel the photoreaction of sulfur with molecular hydrogen using the time-dependent excited-state molecular dynamics (TDESMD) methodology. Individual TDESMD trajectory provides details about reactions that lead to a number of allotropes of sulfur and their hydrogenated forms. Simulated mass spectra based on an ensemble of TDESMD trajectories provide the distribution of sulfanes along reaction pathways. It is found that the photoreaction starts with ring opening of cyclic S8, which may then react with two H radicals to form S8H2 as a result of the homolytic dissociation of H2. The sulfur cluster will undergo the elimination of small fragments, which can later recombine into a variety of sulfanes. The most abundant fragments generated along trajectories are H2S, S4H2, and S8H2. The final sulfur-bearing products are a mixture of sulfanes with various chains and rings. The mechanistic and conformational information obtained from this work allows us to better understand the photoreaction, and potentially, give insights into the preparation of high Tc materials using similar reactants.
Supporting agencies: D.S.K. thanks the DOE BES NERSC facility for computational resources, allocation award No. 91202, “Computational Modeling of Photo-catalysis and Photo-induced Charge Transfer Dynamics on Surfaces”, supported by the Office of Science of the DOE under Contract DE-AC02-05CH11231. D.S.K. acknowledges the support of the National Science Foundation under Grant CHE-1944921. Authors thank David Micha, Oleg Prezhdo, Sergei Tretiak, Svetlana Kilina, Andrei Kryjevski, Bakhtiyor Rasulev, Aaron Forde, Amiradi Alesadi, Meade Eriksen for discussions and editorial suggestions.
About the Authors
Y. Han
North Dakota State University, Department of Chemistry and Biochemistry
United States
United States
Yulun Han.
Fargo
D. Kilin
North Dakota State University, Department of Chemistry and Biochemistry
United States
United States
Dmitri Kilin.
Fargo
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Review
For citations:
Han Y., Kilin D. Photoreactions Create Superconducting Materials. Zhurnal Prikladnoii Spektroskopii. 2023;90(3):520-1-520-8.
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