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      Unveiling the role of upper excited electronic states in the photochemistry and laser performance of anti-B18H22

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          Abstract

          Using the first laser borane, anti-B 18H 22, as a case study, our combined experimental and theoretical approach unravels the photophyscial and photochemical molecular dynamics of a highly efficient luminophore in an excited electronic state.

          Abstract

          In the search for innovative new light sources, the discovery that solutions of the boron hydride anti-B 18H 22 generate photostable blue laser emission stands out in its significance as the first laser borane. Surprisingly, though, the laser performance of anti-B 18H 22 (∼10% efficiency) does not match the expectations based on its exceptional photophysical properties ( Φ f = 0.97 and high photostability). To understand this contradiction, we herein present an investigation into the upper excited states of the anti-B 18H 22 photophysical system, which we suggest to be the most relevant factor to its laser performance. The use of computational quantum chemistry, laser and UV-vis spectroscopy, NMR spectroscopy, and mass spectrometry unveil the role of the upper excited states on the laser performance of anti-B 18H 22, showing that efficient excited state absorption (ESA) leads to the population of these states, and results not only in the loss of laser efficiency, but also in the activation of chemically reactive relaxation pathways and the formation of photochemically produced novel molecular species. The likely composition of these photoproducts, formed upon prolonged high intensity laser irradiation, is inferred from their molecular masses, NMR properties, and calculated natural orbitals. Together, these results are of key importance to the complete understanding of the anti-B 18H 22 photophysical system and provide valuable information to chemists and laser physicists working to mitigate deficiencies and enhance the performance of the next generation of borane lasers and borane-based photoactive materials.

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          Most cited references7

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          Lasers

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            Solid-State Laser Engineering

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              Boron Science, New Technologies and Applications

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                Author and article information

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                Journal
                JMCCCX
                Journal of Materials Chemistry C
                J. Mater. Chem. C
                Royal Society of Chemistry (RSC)
                2050-7526
                2050-7534
                October 1 2020
                2020
                : 8
                : 37
                : 12806-12818
                Affiliations
                [1 ]Institute of Physical Chemistry “Rocasolano”
                [2 ]Consejo Superior de Investigaciones Científicas (CSIC)
                [3 ]Madrid
                [4 ]Spain
                [5 ]Université de Lorraine and CNRS
                [6 ]LPCT
                [7 ]F-54000 Nancy
                [8 ]France
                [9 ]Departament de Química Física
                [10 ]Institut de Ciència Molecular
                [11 ]Universitat de València
                [12 ]46010 Valencia
                [13 ]Institute of Inorganic Chemistry of the Czech Academy of Sciences
                [14 ]250 68 Husinec-Řež
                [15 ]Czech Republic
                [16 ]Institute of Physics
                [17 ]Faculty of Science
                [18 ]University of South Bohemia
                [19 ]370 05 České Budějovice
                Article
                10.1039/D0TC02309D
                806e8764-fcfb-4bf2-a9aa-d8a6f3219b67
                © 2020

                http://rsc.li/journals-terms-of-use

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