Proton tunneling in low dimensional cesium silicate LDS-1

Hiroshi Matsui, Kei Iwamoto, Dai Mochizuki, Shimon Osada, Yusuke Asakura, Kazuyuki Kuroda

    Research output: Contribution to journalArticle

    3 Citations (Scopus)

    Abstract

    In low dimensional cesium silicate LDS-1 (monoclinic phase of CsHSi<inf>2</inf>O<inf>5</inf>), anomalous infrared absorption bands observed at 93, 155, 1210, and 1220 cm<sup>-1</sup> 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</sup>, 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</sup> 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</sup>) and asymmetric mode (155 and 1220 cm<sup>-1</sup>). The broad absorption at 100-600 cm<sup>-1</sup> reveals an emergence of collective mode due to the vibration of silicate chain coupled not only with the local oscillation of Cs<sup>+</sup> but also with the proton oscillation relevant to the second excited state (n = 2).

    Original languageEnglish
    Article number025102
    JournalJournal of Chemical Physics
    Volume143
    Issue number2
    DOIs
    Publication statusPublished - 2015 Jul 14

    Fingerprint

    Silicates
    Cesium
    cesium
    Protons
    silicates
    protons
    Excited states
    Ground state
    Absorption spectra
    vibration mode
    Optical transitions
    absorption spectra
    optical transition
    excitation
    ground state
    oscillations
    Infrared absorption
    Coulomb interactions
    oscillator strengths
    infrared absorption

    ASJC Scopus subject areas

    • Physics and Astronomy(all)
    • Physical and Theoretical Chemistry

    Cite this

    Matsui, H., Iwamoto, K., Mochizuki, D., Osada, S., Asakura, Y., & Kuroda, K. (2015). Proton tunneling in low dimensional cesium silicate LDS-1. Journal of Chemical Physics, 143(2), [025102]. https://doi.org/10.1063/1.4926445

    Proton tunneling in low dimensional cesium silicate LDS-1. / Matsui, Hiroshi; Iwamoto, Kei; Mochizuki, Dai; Osada, Shimon; Asakura, Yusuke; Kuroda, Kazuyuki.

    In: Journal of Chemical Physics, Vol. 143, No. 2, 025102, 14.07.2015.

    Research output: Contribution to journalArticle

    Matsui, H, Iwamoto, K, Mochizuki, D, Osada, S, Asakura, Y & Kuroda, K 2015, 'Proton tunneling in low dimensional cesium silicate LDS-1', Journal of Chemical Physics, vol. 143, no. 2, 025102. https://doi.org/10.1063/1.4926445
    Matsui H, Iwamoto K, Mochizuki D, Osada S, Asakura Y, Kuroda K. Proton tunneling in low dimensional cesium silicate LDS-1. Journal of Chemical Physics. 2015 Jul 14;143(2). 025102. https://doi.org/10.1063/1.4926445
    Matsui, Hiroshi ; Iwamoto, Kei ; Mochizuki, Dai ; Osada, Shimon ; Asakura, Yusuke ; Kuroda, Kazuyuki. / Proton tunneling in low dimensional cesium silicate LDS-1. In: Journal of Chemical Physics. 2015 ; Vol. 143, No. 2.
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