Coupling Pulse Radiolysis with Nanosecond Time-Resolved Step-Scan Fourier Transform Infrared Spectroscopy: Broadband Mid-Infrared Detection of Radiolytically Generated Transients

Grills, David C.; Layne, Bobby H.; Wishart, James F.

doi:10.1177/00037028221097429

Title: Coupling Pulse Radiolysis with Nanosecond Time-Resolved Step-Scan Fourier Transform Infrared Spectroscopy: Broadband Mid-Infrared Detection of Radiolytically Generated Transients

Journal Article · Wed May 25 00:00:00 EDT 2022 · Applied Spectroscopy

DOI:https://doi.org/10.1177/00037028221097429· OSTI ID:1869736

^[1]; Layne, Bobby H. ^[1]; Wishart, James F. ^[1]

Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA

We describe the first implementation of broadband, nanosecond time-resolved step-scan Fourier transform infrared (S ² -FT-IR) spectroscopy at a pulse radiolysis facility. This new technique allows the rapid acquisition of nano- to microsecond time-resolved infrared (TRIR) spectra of transient species generated by pulse radiolysis of liquid samples at a pulsed electron accelerator. Wide regions of the mid-infrared can be probed in a single experiment, which often takes < 20–30 min to complete. It is therefore a powerful method for rapidly locating the IR absorptions of short-lived, radiation-induced species in solution, and for directly monitoring their subsequent reactions. Time-resolved step-scan FT-IR detection for pulse radiolysis thus complements our existing narrowband quantum cascade laser-based pulse radiolysis-TRIR detection system, which is more suitable for acquiring single-shot kinetics and narrowband TRIR spectra on small-volume samples and in strongly absorbing solvents, such as water. We have demonstrated the application of time-resolved step-scan FT-IR spectroscopy to pulse radiolysis by probing the metal carbonyl and organic carbonyl vibrations of the one-electron-reduced forms of two Re-based CO ₂ reduction catalysts in acetonitrile solution. Transient IR absorption bands with amplitudes on the order of 1 × 10 ⁻³ are easily detected on the sub-microsecond timescale using electron pulses as short as 250 ns.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: SC0012704

OSTI ID:: 1869736

Alternate ID(s):: OSTI ID: 1863896

Report Number(s):: BNL-222954-2022-JAAM

Journal Information:: Applied Spectroscopy, Journal Name: Applied Spectroscopy Vol. 76 Journal Issue: 9; ISSN 0003-7028

Publisher:: SAGE PublicationsCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC
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PHYSICAL AND ANALYTICAL CHEMISTRY
Pulse radiolysis
Nanosecond time-resolved step-scan Fourier transform infrared spectroscopy
(S2-FT-IR)
Time-resolved infrared
TRIR

Title: Coupling Pulse Radiolysis with Nanosecond Time-Resolved Step-Scan Fourier Transform Infrared Spectroscopy: Broadband Mid-Infrared Detection of Radiolytically Generated Transients

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