Journal article

Hydrogen-adduction to open-shell graphene fragments: spectroscopy, thermochemistry and astrochemistry

Gerard D O'Connor, Bun Chan, Julian A Sanelli, Katie M Cergol, Viktoras Dryza, Richard J Payne, Evan J Bieske, Leo Radom, Timothy W Schmidt

Chemical Science | Royal Society of Chemistry | Published : 2017

Abstract

We apply a combination of state-of-the-art experimental and quantum-chemical methods to elucidate the electronic and chemical energetics of hydrogen adduction to a model open-shell graphene fragment. The lowest-energy adduct, 1H-phenalene, is determined to have a bond dissociation energy of 258.1 kJ mol−1, while other isomers exhibit reduced or in some cases negative bond dissociation energies, the metastable species being bound by the emergence of a conical intersection along the high-symmetry dissociation coordinate. The gas-phase excitation spectrum of 1H-phenalene and its radical cation are recorded using laser spectroscopy coupled to mass-spectrometry. Several electronically excited sta..

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University of Melbourne Researchers

Grants

Awarded by Australian Research Council


Awarded by Australian Renewable Energy Agency Postdoctoral Fellowship


Funding Acknowledgements

This research was supported under Australian Research Councils Discovery Projects funding scheme (DP120102559, DP120100100 and DP1501425). T. W. S. and R. J. P. acknowledge the Australian Research Council for Future Fellowships (FT130100177 and FT130100150). G. D. O., K. M. C. and J. A. S. acknowledge the receipt of Australian Postgraduate Awards. V. D. acknowledges an Australian Renewable Energy Agency Postdoctoral Fellowship (6-F004) and support from the University of Melbourne's Early Career Researcher Grant Scheme. The National Computational Infrastructure National Facility (NCI NF) is thanked for generous allocations of supercomputer time.