Dual-comb spectroscopy of ammonia formation in non-thermal plasmas

I Sadiek, AJ Fleisher, J Hayden, X Huang… - Communications …, 2024 - nature.com
I Sadiek, AJ Fleisher, J Hayden, X Huang, A Hugi, R Engeln, N Lang, JPH van Helden
Communications Chemistry, 2024nature.com
Plasma-activated chemical transformations promise the efficient synthesis of salient
chemical products. However, the reaction pathways that lead to desirable products are often
unknown, and key quantum-state-resolved information regarding the involved molecular
species is lacking. Here we use quantum cascade laser dual-comb spectroscopy (QCL-
DCS) to probe plasma-activated NH3 generation with rotational and vibrational state
resolution, quantifying state-specific number densities via broadband spectral analysis. The …
Abstract
Plasma-activated chemical transformations promise the efficient synthesis of salient chemical products. However, the reaction pathways that lead to desirable products are often unknown, and key quantum-state-resolved information regarding the involved molecular species is lacking. Here we use quantum cascade laser dual-comb spectroscopy (QCL-DCS) to probe plasma-activated NH3 generation with rotational and vibrational state resolution, quantifying state-specific number densities via broadband spectral analysis. The measurements reveal unique translational, rotational and vibrational temperatures for NH3 products, indicative of a highly reactive, non-thermal environment. Ultimately, we postulate on the energy transfer mechanisms that explain trends in temperatures and number densities observed for NH3 generated in low-pressure nitrogen-hydrogen (N2–H2) plasmas.
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