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H$$_6$$$$^+$$ in irradiated solid $$para$$-hydrogen and its decay dynamics; Reinvestigation of quartet electron paramagnetic resonance lines assigned to H$$_2$$$$^-$$

放射線照射により固体パラ水素中に生成したH$$_6$$$$^+$$イオンの研究

熊田 高之; 田地川 浩人*; 高柳 敏幸*

Kumada, Takayuki; Tachikawa, Hiroto*; Takayanagi, Toshiyuki*

以前H$$_2$$$$^-$$と同定されていた放射線照射固体パラ水素中に観測された4本線の電子スピン共鳴(ESR)信号を再調査した。実験と理論計算値を照らし合わせた結果、4本線はH$$_2$$$$^-$$ではなくH$$_6$$$$^+$$のものであることが判明した。新しい同定のもとに、以前に測定されたオルト-パラ変換,同位体効果,量子拡散などのデータを全て解析し直した。本論文の最後には、気体水素の放射線分解ではH$$_3$$$$^+$$イオンが生じるのとは対照的に、固体水素に放射線を照射したときに生成するイオン種はH$$_6$$$$^+$$であるというモデル提案した。

The quartet ESR lines observed in X-ray irradiated solid parahydrogen, which have previously been assigned to H$$_2$$$$^-$$, are reinvestigated. We have reassigned the quartet lines to H$$_6$$$$^+$$ rather than H$$_2$$$$^-$$. Based on the new assignment, previous data have been reinterpreted as follows. The H$$_6$$$$^+$$ ion is composed of the collinearly aligned H$$_2$$$$^+$$ core at the center and two H$$_2$$ rotors at both ends. The ortho-para conversion of H$$_2$$$$^+$$ core of H$$_6$$$$^+$$ is completed within the time-scale of hours. H$$_6$$$$^+$$ diffuses quantum mechanically by the repetition of H$$_6$$$$^+$$ + H$$_2$$ $$rightarrow$$ H$$_2$$ + H$$_6$$$$^+$$ reaction, and the diffusion terminates by the reaction with a HD impurity as H$$_6$$$$^+$$ + HD $$rightarrow$$ H$$_5$$D$$^+$$ + H$$_2$$. Finally, we will propose a possible reason why H$$_6$$$$^+$$ is produced instead of H$$_3$$$$^+$$ in the irradiated solid H$$_2$$.

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パーセンタイル:61.67

分野:Chemistry, Physical

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