2D imaging of absolute methyl concentrations in nanosecond pulsed plasma by photo-fragmentation laser-induced fluorescence

van den Bekerom, Dirk; Richards, Caleb; Huang, Erxiong; Adamovich, Igor; Frank, Jonathan H.

doi:10.1088/1361-6595/ac8f6c

Title: 2D imaging of absolute methyl concentrations in nanosecond pulsed plasma by photo-fragmentation laser-induced fluorescence

Journal Article · Wed Nov 02 00:00:00 EDT 2022 · Plasma Sources Science and Technology

DOI: https://doi.org/10.1088/1361-6595/ac8f6c · OSTI ID:1923778

^[1];

^[2]; Huang, Erxiong ^[1];

^[2];

^[1]

Sandia National Lab. (SNL-CA), Livermore, CA (United States)
The Ohio State Univ., Columbus, OH (United States)

The methyl radical plays a central role in plasma-assisted hydrocarbon chemistry but is challenging to detect due to its high reactivity and strongly pre-dissociative electronically excited states. In this work, we report the development of a photo-fragmentation laser-induced fluorescence (PF-LIF) diagnostic for quantitative 2D imaging of methyl profiles in a plasma. This technique provides temporally and spatially resolved measurements of local methyl distributions, including in near-surface regions that are important for plasma-surface interactions such as plasma-assisted catalysis. The technique relies on photo-dissociation of methyl by the fifth harmonic of a Nd:YAG laser at 212.8 nm to produce CH fragments. These photofragments are then detected with LIF imaging by exciting a transition in the B-X(0, 0) band of CH with a second laser at 390 nm. Fluorescence from the overlapping A-X(0, 0), A-X(1, 1), and B-X(0, 1) bands of CH is detected near 430 nm with the A-state populated by collisional B-A electronic energy transfer. This non-resonant detection scheme enables interrogation close to a surface. The PF-LIF diagnostic is calibrated by producing a known amount of methyl through photo-dissociation of acetone vapor in a calibration gas mixture. We demonstrate PF-LIF imaging of methyl production in methane-containing nanosecond pulsed plasmas impinging on dielectric surfaces. Absolute calibration of the diagnostic is demonstrated in a diffuse, plane-to-plane discharge. Measured profiles show a relatively uniform distribution of up to 30 ppm of methyl. Relative methyl measurements in a filamentary plane-to-plane discharge and a plasma jet reveal highly localized intense production of methyl. The utility of the PF-LIF technique is further demonstrated by combining methyl measurements with formaldehyde LIF imaging to capture spatiotemporal correlations between methyl and formaldehyde, which is an important intermediate species in plasma-assisted oxidative coupling of methane.

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Research Organization:: Sandia National Laboratories (SNL-CA), Livermore, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Fusion Energy Sciences (FES)

Grant/Contract Number:: NA0003525

OSTI ID:: 1923778

Report Number(s):: SAND2022-10400J

Journal Information:: Plasma Sources Science and Technology, Journal Name: Plasma Sources Science and Technology Journal Issue: 9 Vol. 31; ISSN 0963-0252

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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