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Infrared studies of ortho-para conversion at Cl-atom and H-atom impurity centers in cryogenic solid hydrogen

机译:低温固体氢中Cl原子和H原子杂质中心的邻位对位转换的红外研究

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摘要

We report infrared spectroscopic studies of H₂ ortho-para (o/p) conversion in solid hydrogen doped with Clatoms at 2 K while the Cl+H₂(v=1)→HCl+H infrared-induced chemical reaction is occurring. The Cl-atom doped hydrogen crystals are synthesized using 355 nm in situ photodissociation of Cl₂ precursor molecules. For hydrogen solids with high ortho-H₂ fractional concentrations (Xo=0.55), the o/p conversion kinetics is dominated by Cl-atom catalyzed conversion with a catalyzed conversion rate constant Kcc=1.16(11) min⁻¹ and the process is rate-limited by ortho-H₂ quantum diffusion. For hydrogen crystals with low ortho-H₂ concentrations (Xo=0.03), single-exponential decay of the ortho-H₂ concentration with time is observed which is attributed to H-atom catalyzed o/p conversion by the H-atoms produced during the infrared-induced Cl+H₂ reaction. The measured H-atom catalyzed o/p conversion kinetics indicates the H-atoms are mobile under these conditions in agreement with previous ESR measurements.
机译:我们报告了在2 K时Cl +掺杂的固体氢中H 2邻位对位(o / p)转化的红外光谱研究,同时发生了Cl + H 2(v = 1)→HCl + H红外诱导的化学反应。用355nm的Cl 2前体分子原位光解离合成了掺有Cl原子的氢晶体。对于具有高邻位H 2分数浓度(Xo = 0.55)的氢固体,o / p转化动力学主要由Cl原子催化的转化控制,催化的转化速率常数为Kcc = 1.16(11)min -1,该过程为速率受邻H 2量子扩散的限制。对于低邻位H 2浓度的氢晶体(Xo = 0.03),观察到邻位H 2浓度随时间呈单指数衰减,这归因于红外过程中产生的H原子对H原子催化的O / P转化。 -诱导的Cl + H 2反应。测得的H原子催化的O / P转换动力学表明H原子在这些条件下是可移动的,与先前的ESR测量一致。

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