Experimental validation of a collision-radiation dataset for molecular hydrogen in plasmas

Keisuke Fujii, Keiji Sawada, Arseniy Kuzmin, Motoshi Goto, Masahiro Kobayashi, Liam H. Scarlett, Dmitry V. Fursa, Igor Bray, Mark C. Zammit, Theodore M. Biewer

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Abstract

Quantitative spectroscopy of molecular hydrogen has generated substantial demand, leading to the accumulation of diverse elementary process data encompassing radiative transitions, electron-impact transitions, predissociations, and quenching. However, their rates currently available are still sparse, and there are inconsistencies among those proposed by different authors. In this study, we demonstrate an experimental validation of such a molecular dataset by composing a collisional-radiative model (CRM) for molecular hydrogen and comparing experimentally obtained vibronic populations across multiple levels. From the population kinetics of molecular hydrogen, the importance of each elementary process in various parameter space is studied. In low-density plasmas (electron density n e ≲ 10 17 m − 3 ) the excitation rates from the ground states and radiative decay rates, both of which have been reported previously, determine the excited state population. The inconsistency in the excitation rates affects the population distribution the most significantly in this parameter space. However, in higher density plasmas ( n e ≳ 10 18 m − 3 ), the excitation rates from excited states become important, which have never been reported in the literature, and may need to be approximated in some way. In order to validate these molecular datasets and approximated rates, we carried out experimental observations for two different hydrogen plasmas; a low-density radio frequency heated plasma ( n e ≈ 10 16 m − 3 ) and the Large Helical Device (LHD) divertor plasma ( n e ≳ 10 18 m − 3 ). The visible emission lines from EF 1 Σ g + , H H ¯ 1 Σ g + , D 1 Π u ± , GK 1 Σ g + , I 1 Π g ± , J 1 Δ g ± , h 3 Σ g + , e 3 Σ u + , d 3 Π u ± , g 3 Σ g + , i 3 Π g ± , and j 3 Δ g ± states were observed simultaneously and their population distributions were obtained from their intensities. We compared the observed population distributions with the CRM prediction, in particular the CRM with the rates compiled by Janev et al., Miles et al., and those calculated with the molecular convergent close-coupling (MCCC) method. The MCCC prediction gives the best agreement with the experiment, particularly for the emission from the low-density plasma. However, the population distribution in the LHD divertor shows a worse agreement with the CRM than those from low-density plasma, indicating the necessity of the precise excitation rates from excited states. We also found that the rates for the electron attachment is inconsistent with experimental results. This requires further investigation.

Original languageEnglish
Article number092512
JournalPhysics of Plasmas
Volume31
Issue number9
DOIs
StatePublished - Sep 1 2024

Funding

This work was partly supported by the U.S. D.O.E Contract No. DE-AC05-00OR22725, the Australian Government through the Australian Research Council's Discovery Projects funding scheme (Project No. DP240101184), and by the United States Air Force Office of Scientific Research. K.F. would like to specifically acknowledge Oak Ridge National Laboratory's Laboratory Directed Research and Development program Project No. 11367. L.H.S is the recipient of an Australian Research Council Discovery Early Career Researcher Award (Project No. DE240100176) funded by the Australian Government. HPC resources were provided by the Pawsey Supercomputing Research Centre and the National Computational Infrastructure, with funding from the Australian Government and the Government of Western Australia, and the Texas Advanced Computing Center (TACC) at the University of Texas at Austin. M.C.Z would like to specifically acknowledge the support of the Los Alamos National Laboratory (LANL) ASC PEM Atomic Physics Project. LANL is operated by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under Contract No. 89233218NCA000001. M.C.Z. would like to acknowledge also Los Alamos National Laboratory's Laboratory Directed Research and Development program Project No. 20240391ER.

FundersFunder number
National Nuclear Security Administration
Australian Government
Air Force Office of Scientific Research
University of Texas at Austin
Los Alamos National Laboratory
Texas Advanced Computing Center
Government of Western Australia
Laboratory Directed Research and Development20240391ER
Oak Ridge National Laboratory's Laboratory Directed Research and DevelopmentDE240100176, 11367
U.S. Department of Energy89233218NCA000001
Australian Research CouncilDP240101184

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