Direct mapping of curve-crossing dynamics in IBr by attosecond transient absorption spectroscopy

Kobayashi, Yuki; Chang, Kristina F.; Zeng, Tao; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1126/science.aax0076

Title: Direct mapping of curve-crossing dynamics in IBr by attosecond transient absorption spectroscopy

Journal Article · Fri Jul 05 00:00:00 EDT 2019 · Science

DOI:https://doi.org/10.1126/science.aax0076· OSTI ID:1580889

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Univ. of California, Berkeley, CA (United States)
Carleton Univ., Ottawa, ON (Canada)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

The electronic character of photoexcited molecules can abruptly change at avoided crossings and conical intersections. Here, we report direct mapping of the coupled interplay between electrons and nuclei in a prototype molecule, iodine monobromide (IBr), by using attosecond transient absorption spectroscopy. A few-femtosecond visible pulse resonantly excites the $B ({}^{3}Π_{0^{+}})$ , Y(0⁺), and Z(0⁺) states of IBr, and the photodissociation dynamics are tracked with an attosecond extreme-ultraviolet pulse that simultaneously probes the I-4dand Br-3dcore-level absorption edges. Direct comparison with quantum mechanical simulations unambiguously identifies the absorption features associated with adiabatic and diabatic channels at the B/Y avoided crossing and concurrent two-photon dissociation processes that involve the Y/Z avoided crossing. Finally, the results show clear evidence for rapid switching of valence-electronic character at the avoided crossing.

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); US Army Research Office (ARO); Natural Sciences and Engineering Research Council of Canada (NSERC); National Institutes of Health (NIH)

Grant/Contract Number:: AC02-05CH11231; CHE-1660417; W911-NF-14-1-0383; RGPIN-2016-06276; S10OF023532

OSTI ID:: 1580889

Journal Information:: Science, Vol. 365, Issue 6448; ISSN 0036-8075

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 66 works

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