TY - JOUR
T1 - Diffusion of hydrogen fluoride in solid parahydrogen
AU - Ooe, Hiroki
AU - Miyamoto, Yuki
AU - Kuma, Susumu
AU - Kawaguchi, Kentarou
AU - Nakajima, Kyo
AU - Nakano, Itsuo
AU - Sasao, Noboru
AU - Tang, Jian
AU - Taniguchi, Takashi
AU - Yoshimura, Motohiko
PY - 2013/6/7
Y1 - 2013/6/7
N2 - We studied diffusion of hydrogen fluoride (HF) in solid parahydrogen (pH2) around 4 K. Diffusion rates were determined from time dependence of FT-IR spectra of HF monomers. The absorption of HF monomers shows temporal decay due to dimerization reaction via diffusion. It was found that the rates are affected by the sample temperature, the initial HF concentration, and annealing of samples. The observed non-Arrhenius-type temperature dependence suggests that the diffusion is dominated by a quantum tunneling process, that is, "quantum diffusion." Deceleration of the diffusion in condensed samples and acceleration in annealed samples were also observed. These results can be attributed to the fact that lower periodicity of samples due to impurities or defects suppresses the quantum tunneling. It seems to be difficult to explain the observed dependences by three possible diffusion mechanisms, exchange of chemical bonds, direct cyclic exchange, and exchange with mobile vacancy. Therefore, we propose a hypothetical mechanism by exchange of vacancies originating from quantum effect.
AB - We studied diffusion of hydrogen fluoride (HF) in solid parahydrogen (pH2) around 4 K. Diffusion rates were determined from time dependence of FT-IR spectra of HF monomers. The absorption of HF monomers shows temporal decay due to dimerization reaction via diffusion. It was found that the rates are affected by the sample temperature, the initial HF concentration, and annealing of samples. The observed non-Arrhenius-type temperature dependence suggests that the diffusion is dominated by a quantum tunneling process, that is, "quantum diffusion." Deceleration of the diffusion in condensed samples and acceleration in annealed samples were also observed. These results can be attributed to the fact that lower periodicity of samples due to impurities or defects suppresses the quantum tunneling. It seems to be difficult to explain the observed dependences by three possible diffusion mechanisms, exchange of chemical bonds, direct cyclic exchange, and exchange with mobile vacancy. Therefore, we propose a hypothetical mechanism by exchange of vacancies originating from quantum effect.
UR - http://www.scopus.com/inward/record.url?scp=84879134382&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84879134382&partnerID=8YFLogxK
U2 - 10.1063/1.4808035
DO - 10.1063/1.4808035
M3 - Article
C2 - 23758373
AN - SCOPUS:84879134382
SN - 0021-9606
VL - 138
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 21
M1 - 214309
ER -