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Soft X-ray Chlorine Photolysis on Chlorobenzene Ice: An Experimental and Theoretical Study.

Bruno Nunes Cabral TenorioFranciele KruczkiewiczFabio de A RibeiroDiana Paula Pinho AndradeHugo Milward Riani de LunaHeloisa Maria Boechat-RobertyMarco Antonio Chaer NascimentoAlexandre Braga RochaWania Wolff
Published in: The journal of physical chemistry. A (2019)
An experimental and theoretical study of the photoinduced homolysis of the carbon-chlorine bond in an ice matrix of chlorobenzene is presented. A condensed chlorobenzene film has been grown in situ and near edge X-ray fine structure (NEXAFS) spectra were collected after exposing the condensed film to a monochromatic photon beam centered at the 2822 eV resonant excitation of chlorine and at 2850 eV. The photoabsorption to the Cl 1s → σ* and Cl 1s → π* states has been measured and the hypothesis of free radical coupling reactions was investigated via time-dependent density functional theory (TD-DFT) and complete active space self-consistent field (CASSCF) calculations. Also, potential energy pathways to the C-Cl cleavage have been obtained at the CASSCF level to the Cl 1s → σ*, 1s → π*, and 1s → ∞ states. A strong dissociative character was only found for the Cl 1s → σ* resonance.
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