Title: Photodissociation of aqueous ${\mathrm{I}}_3^{-}$ observed with liquid-phase ultrafast mega-electron-volt electron diffraction

Abstract

Developing femtosecond resolution methods for directly observing structural dynamics is critical to understanding complex photochemical reaction mechanisms in solution. We have used two recent developments, ultrafast mega-electron-volt electron sources and vacuum compatible sub-micron thick liquid sheet jets, to enable liquid-phase ultrafast electron diffraction (LUED). We have demonstrated the viability of LUED by investigating the photodissociation of tri-iodide initiated with a 400 nm laser pulse. This has enabled the average speed of the bond expansion to be measured during the first 750 fs of dissociation and the geminate recombination to be directly captured on the picosecond time scale.

Authors:

Ledbetter, Kathryn E.  ^[1];

• Search DOE PAGES for author "Ledbetter, Kathryn E."
• Search DOE PAGES for ORCID "0000-0002-3961-8524"

Biasin, E.  ^[2];

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• Search DOE PAGES for ORCID "0000-0002-7276-4224"

Nunes, J. P. F.  ^[3];

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• Search DOE PAGES for ORCID "0000-0003-0670-6023"

Centurion, M.  ^[4];

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• Search DOE PAGES for ORCID "0000-0002-5662-2293"

Gaffney, K. J.  ^[5];

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• Search DOE PAGES for ORCID "0000-0002-0525-6465"

Kozina, M.  ^[5];

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• Search DOE PAGES for ORCID "0000-0002-4747-345X"

Lin, M.-F.  ^[5];

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• Search DOE PAGES for ORCID "0000-0001-8086-2484"

Shen, X. ^[5]; Yang, J.  ^[2];

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• Search DOE PAGES for ORCID "0000-0002-5115-2413"

Wang, X. J.  ^[5];

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Wolf, T. J. A.  ^[2];

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• Search DOE PAGES for ORCID "0000-0002-0641-1279"

Cordones, A. A.  ^[2]

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• Search DOE PAGES for ORCID "0000-0001-9897-5380"

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+ Show Author Affiliations

1. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
3. Univ. of Nebraska, Lincoln, NE (United States
4. Univ. of Nebraska, Lincoln, NE (United States)
5. SLAC National Accelerator Lab., Menlo Park, CA (United States)

Publication Date:

Mon Dec 28 00:00:00 EST 2020

Research Org.:

SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

OSTI Identifier:

1728465

Alternate Identifier(s):

OSTI ID: 1749914; OSTI ID: 1749962

Grant/Contract Number:  

AC02-76SF00515; SC0014170; AC02-05CH11231

Resource Type:

Accepted Manuscript

Journal Name:

Structural Dynamics

Additional Journal Information:

Journal Volume: 7; Journal Issue: 6; Journal ID: ISSN 2329-7778

Publisher:

American Crystallographic Association/AIP

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Solution processes; Electron diffraction; Photochemical reactions; Liquids; Geminate recombination; Electron scattering; Photodissociation; Liquid phase ultrafast electron diffraction, Structural dynamics, Photochemistry