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 language | English |
|---|---|
| Article number | 044102 |
| Journal | Review of Scientific Instruments |
| Volume | 86 |
| Issue number | 4 |
| DOIs | |
| Publication status | Published - Apr 1 2015 |
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ASJC Scopus subject areas
- Instrumentation
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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 journal › Article
}
TY - JOUR
T1 - Development of nanosecond time-resolved infrared detection at the LEAF pulse radiolysis facility
AU - Grills, David
AU - Farrington, Jaime A.
AU - Layne, Bobby H.
AU - Preses, Jack M.
AU - Bernstein, Herbert J.
AU - Wishart, James F.
PY - 2015/4/1
Y1 - 2015/4/1
N2 - 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.
AB - 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.
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U2 - 10.1063/1.4918728
DO - 10.1063/1.4918728
M3 - Article
VL - 86
JO - Review of Scientific Instruments
JF - Review of Scientific Instruments
SN - 0034-6748
IS - 4
M1 - 044102
ER -