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Title: Proton tunneling in low dimensional cesium silicate LDS-1

In low dimensional cesium silicate LDS-1 (monoclinic phase of CsHSi{sub 2}O{sub 5}), anomalous infrared absorption bands observed at 93, 155, 1210, and 1220 cm{sup −1} are assigned to the vibrational mode of protons, which contribute to the strong hydrogen bonding between terminal oxygen atoms of silicate chain (O–O distance = 2.45 Å). The integrated absorbance (oscillator strength) for those modes is drastically enhanced at low temperatures. The analysis of integrated absorbance employing two different anharmonic double-minimum potentials makes clear that proton tunneling through the potential barrier yields an energy splitting of the ground state. The absorption bands at 93 and 155 cm{sup −1}, which correspond to the different vibrational modes of protons, are attributed to the optical transition between the splitting levels (excitation from the ground state (n = 0) to the first excited state (n = 1)). Moreover, the absorption bands at 1210 and 1220 cm{sup −1} are identified as the optical transition from the ground state (n = 0) to the third excited state (n = 3). Weak Coulomb interactions in between the adjacent protons generate two types of vibrational modes: symmetric mode (93 and 1210 cm{sup −1}) and asymmetric mode (155 and 1220 cm{sup −1}). The broadmore » absorption at 100–600 cm{sup −1} reveals an emergence of collective mode due to the vibration of silicate chain coupled not only with the local oscillation of Cs{sup +} but also with the proton oscillation relevant to the second excited state (n = 2)« less
Authors:
;  [1] ;  [2] ; ;  [3] ;  [3] ;  [4]
  1. Department of Physics, Graduate School of Science, Tohoku University, Sendai 980-8578 (Japan)
  2. Interdisciplinary Cluster for Cutting Edge Research, Center for Energy and Environmental Science, Shinshu University, 3-15-1 Tokida, Ueda, Nagano 386-8567 (Japan)
  3. Department of Applied Chemistry, Faculty of Science and Engineering, Waseda University, Tokyo 169-8555 (Japan)
  4. (Japan)
Publication Date:
OSTI Identifier:
22490904
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 143; Journal Issue: 2; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ABSORPTION; ATOMS; CESIUM IONS; CESIUM SILICATES; EXCITATION; EXCITED STATES; GROUND STATES; HYDROGEN; INTERACTIONS; MONOCLINIC LATTICES; OSCILLATIONS; OSCILLATOR STRENGTHS; OXYGEN; PROTONS; TUNNEL EFFECT