Development of nanosecond time-resolved infrared detection at the LEAF pulse radiolysis facility

David Grills, Jaime A. Farrington, Bobby H. Layne, Jack M. Preses, Herbert J. Bernstein, James F. Wishart

Research output: Contribution to journalArticle

14 Citations (Scopus)

Abstract

When coupled with transient absorption spectroscopy, pulse radiolysis, which utilizes high-energy electron pulses from an accelerator, is a powerful tool for investigating the kinetics and thermodynamics of a wide range of radiation-induced redox and electron transfer processes. The majority of these investigations detect transient species in the UV, visible, or near-IR spectral regions. Unfortunately, the often-broad and featureless absorption bands in these regions can make the definitive identification of intermediates difficult. Time-resolved vibrational spectroscopy would offer much improved structural characterization, but has received only limited application in pulse radiolysis. In this paper, we describe in detail the development of a unique nanosecond time-resolved infrared (TRIR) detection capability for condensed-phase pulse radiolysis on a new beam line at the LEAF facility of Brookhaven National Laboratory. The system makes use of a suite of high-power, continuous wave external-cavity quantum cascade lasers as the IR probe source, with coverage from 2330 to 1051 cm-1. The response time of the TRIR detection setup is ∼40 ns, with a typical sensitivity of ∼100 μOD after 4-8 signal averages using a dual-beam probe/reference normalization detection scheme. This new detection method has enabled mechanistic investigations of a range of radiation-induced chemical processes, some of which are highlighted here.

Original languageEnglish
Article number044102
JournalReview of Scientific Instruments
Volume86
Issue number4
DOIs
Publication statusPublished - Apr 1 2015

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Radiolysis
radiolysis
Infrared radiation
pulses
Radiation
Vibrational spectroscopy
Quantum cascade lasers
Electrons
Absorption spectroscopy
Particle accelerators
probes
Absorption spectra
quantum cascade lasers
radiation
Thermodynamics
high energy electrons
continuous radiation
electron transfer
absorption spectroscopy
Kinetics

ASJC Scopus subject areas

  • Instrumentation

Cite this

Grills, D., Farrington, J. A., Layne, B. H., Preses, J. M., Bernstein, H. J., & Wishart, J. F. (2015). Development of nanosecond time-resolved infrared detection at the LEAF pulse radiolysis facility. Review of Scientific Instruments, 86(4), [044102]. https://doi.org/10.1063/1.4918728

Development of nanosecond time-resolved infrared detection at the LEAF pulse radiolysis facility. / Grills, David; Farrington, Jaime A.; Layne, Bobby H.; Preses, Jack M.; Bernstein, Herbert J.; Wishart, James F.

In: Review of Scientific Instruments, Vol. 86, No. 4, 044102, 01.04.2015.

Research output: Contribution to journalArticle

Grills, David ; Farrington, Jaime A. ; Layne, Bobby H. ; Preses, Jack M. ; Bernstein, Herbert J. ; Wishart, James F. / Development of nanosecond time-resolved infrared detection at the LEAF pulse radiolysis facility. In: Review of Scientific Instruments. 2015 ; Vol. 86, No. 4.
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