Tracking ultrafast non-adiabatic dissociation dynamics of the deuterated water dication molecule

Iskandar, W.; Rescigno, T. N.; Orel, A. E.; Larsen, K. A.; Severt, T.; Streeter, Z. L.; Jochim, B.; Griffin, B.; Call, D.; Davis, V.; McCurdy, C. W.; Lucchese, R. R.; Williams, J. B.; Ben-Itzhak, I.; Slaughter, D. S.; Weber, T.

doi:10.1063/5.0219029

Tracking ultrafast non-adiabatic dissociation dynamics of the deuterated water dication molecule

Journal Article · Fri Jul 26 00:00:00 EDT 2024 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0219029· OSTI ID:2407321

^[1]; ^[1]; ^[2]; ^[3]; ^[4]; Streeter, Z. L. ^[5]; ^[4]; Griffin, B. ^[6]; ^[7]; ^[7]; ^[5]; ^[1]; Williams, J. B. ^[7]; ^[4]; ^[1]; ^[1]

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Univ. of California, Davis, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Kansas State Univ., Manhattan, KS (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Davis, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of Nevada, Reno, NV (United States)
Univ. of Nevada, Reno, NV (United States)

Here, we applied reaction microscopy to elucidate fast non-adiabatic dissociation dynamics of deuterated water molecules after direct photo-double ionization at 61 eV with synchrotron radiation. For the very rare D⁺ + O⁺ + D breakup channel, the particle momenta, angular, and energy distributions of electrons and ions, measured in coincidence, reveal distinct electronic dication states and their dissociation pathways via spin–orbit coupling and charge transfer at crossings and seams on the potential energy surfaces. Notably, we could distinguish between direct and fast sequential dissociation scenarios. For the latter case, our measurements reveal the geometry and orientation of the deuterated water molecule with respect to the polarization vector that leads to this rare 3-body molecular breakup channel. Aided by multi-reference configuration-interaction calculations, the dissociation dynamics could be traced on the relevant potential energy surfaces and particularly their crossings and seams. This approach also unraveled the ultrafast time scales governing these processes.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Sciences Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; FG02-86ER13491

OSTI ID:: 2407321

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 4 Vol. 161; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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