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Molecular amplified spontaneous emission in the far-infrared region

Research Project

Project/Area Number 16550022
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field Physical chemistry
Research InstitutionTokyo University of Science

Principal Investigator

TSUKIYAMA Koichi  Tokyo University of Science, Faculty of Science, Department of Chemistry, Professor, 理学部第一部, 教授 (20188519)

Project Period (FY) 2004 – 2005
Project Status Completed (Fiscal Year 2005)
Budget Amount *help
¥3,000,000 (Direct Cost: ¥3,000,000)
Fiscal Year 2005: ¥1,100,000 (Direct Cost: ¥1,100,000)
Fiscal Year 2004: ¥1,900,000 (Direct Cost: ¥1,900,000)
Keywordsamplified spontaneous emission / far-infrared / nitric oxide / Rydberg state
Research Abstract

The 8sσ state of NO is weakly predissociative and no fluorescence has been reported at any spectral regions so far, whereas two major ASE systems were observed around 27 μm and 14 μm. Judging from the low quantum efficiency of the detector above 25 μm, the emission intensities of the 27 μm band is evaluated to be at least two orders of magnitude stronger than the 14 μm band.
The 27 μm band
The band system around 27 μm is assigned to the 8sσ ^2Σ^+(ν=0)→7pσ ^2Σ^+(ν=0) transition. The observed rotational structure accords with the R branch. The corresponding P branch is located above 28 μm. The transition down to the lower pσ Rydberg members such as 8sσ→6pσ at 6.6 μm is not detectable. The absence of the sσ→pσ transitions with Δn=2 has been also pointed out for the 6sσ state. The 8sσ→7pπ ^2Π system around 23.5 μm is undetectable. This may be caused by s 〜 d mixing in the 8sσ state, leading to destructive interference of the 8sσ→7pπ and 7dσ→7pπ transition dipoles. A similar intensity reducti … More on of the nsσ→(n-1)pπ ASE systems was found for n=4,5 and 6. Cascade ASE from 7pσ (ν=0)→7sσ (ν=0) around 19 μm was not observed.
The 14 μm band
The band system around 14 μm is assigned to the 8sσ(ν=0)→6f(ν=0) transition. This is the first observation of the nsσ→n'finter-Rydberg ASE which violates the Δl=±1 selection rule. The transition moment is derived from the mixing of dσ character with 8sσ. Our analyses revealed that the peaks belong to the P branch where the quantum number ι (projection of the orbital angular momentum l onto the rotational axis) in the 6f state is +3. This assignment is in good accordance with our previous investigation in which the 4f(v=0)→sσ E^2Σ^+ (ν=0) ASE channel was open only for ι=+3. When the 6f(ν=0,L=+3) levels are directly populated from A^2Σ^+(ν=0), the ASE spectra were dominated by the band around 8 μm assigned to the 6f→5dσ transition.
The current observation implies that molecular ASE may be used as quasi-coherent pulsed light source in THz regions. As the higher (n【greater than or equal】9) Rydberg members are excited, the energy differences between the laser-prepared and the adjacent levels become smaller, potentially yielding longer ASE wavelengths. For instance, the energy difference between 10sσ ^2Σ^+(ν=0) and 9pσ ^2Σ^+(ν=0) states is〜165 cm^<-1>, corresponding to 60 μm (【approximately equal】 5.0 THz). Although continuous tuning is not feasible, robivational structures of molecules provide us with much wider choices of wavelength than atomic emissions. Less

Report

(3 results)
  • 2005 Annual Research Report   Final Research Report Summary
  • 2004 Annual Research Report
  • Research Products

    (12 results)

All 2006 2005 2004

All Journal Article (11 results) Book (1 results)

  • [Journal Article] Vibrational excitation of the v_2 mode of NH_3 by infrared free electron laser2006

    • Author(s)
      Y.Ogi, M.Kawashita, K.Tsukiyama
    • Journal Title

      Chem. Phys. Letters 421

      Pages: 96-100

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Vibrational excitation of the ν_2 mode of NH_3 by infrared free electron laser2006

    • Author(s)
      Yoshihiro Ogi, Masashi Kawashita, Koichi Tsukiyama
    • Journal Title

      Chem.Phys.Lett. 421

      Pages: 96-100

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Vibrational excitation of the ν_2 mode of NH_3 by infrared free electron laser2006

    • Author(s)
      Y.Ogi, M.Kawashita, K.Tsukiyama
    • Journal Title

      Chem.Phys.Letters 421

      Pages: 96-100

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Fluorescence lifetimes of the O^1Σ_g^+, R^1Π_g and S^1Δ_g states of H_22005

    • Author(s)
      H.Aita, Y.Ogi, K.Tsukiyama
    • Journal Title

      Journal of Molecular Spectroscopy 232

      Pages: 303-310

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Fluorescence lifetimes of the P^1Σ_g^+, R^1Π_g and S^1Δ_g states of D_22005

    • Author(s)
      H.Aita, T.Yoshinari, Y.Ogi, K.Tsukiyama
    • Journal Title

      Journal of Molecular Spectroscopy 234

      Pages: 130-136

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Fluorescence lifetimes of the O^1Σ_g^+,P^1Σ_g^+,R^1Π_g and S^1Δ_g states of H_22005

    • Author(s)
      Hiroki Aita, Yoshihiro Ogi, Koichi Tsukiyama
    • Journal Title

      J.Molecular Spectroscopy 232

      Pages: 303-310

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Fluorescence lifetimes of the P^1Σ_g^+,R^1Π_g and S^1Δ_g states of D_22005

    • Author(s)
      Hiroki Aita, Toshio Yoshinari, Yoshihiro Ogi, Koichi Tsukiyama
    • Journal Title

      J.Molecular Spectroscopy 234

      Pages: 130-136

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2005 Final Research Report Summary
  • [Journal Article] Fluorescence lifetimes of the O^1Σ_g^+,P^1Σ_g^+,R^1Π_g and S^1Δ_g states of H_22005

    • Author(s)
      H.Aita, Y.Ogi, K.Tsukiyama
    • Journal Title

      Journal of Molecular Spectroscopy 232

      Pages: 303-310

    • Related Report
      2005 Annual Research Report
  • [Journal Article] Fluorescence lifetimes of the P^1Σ_g^+,R^1Π_g and S^1Δ_g states of D_22005

    • Author(s)
      H.Aita, T.Yoshinari, Y.Ogi, K.Tsukiyama
    • Journal Title

      Journal of Molecular Spectroscopy 234

      Pages: 130-136

    • Related Report
      2005 Annual Research Report
  • [Journal Article] The EF, GK, H^1Σ^+_g, I^1Πg, and J^1Δg State of HD :2004

    • Author(s)
      T.Yoshinari, Y.Ogi, et al.
    • Journal Title

      J.Phys.Chem.A 108

      Pages: 7915-7921

    • Related Report
      2004 Annual Research Report
  • [Journal Article] The C'^1A_1' - A^1A_2" band of ND_3 studied by LIASE and TG spectroscopy2004

    • Author(s)
      Y.Ogi, K.Tsukiyama
    • Journal Title

      Chem.Phys. 303

      Pages: 271-278

    • Related Report
      2004 Annual Research Report
  • [Book] 実験化学講座5 化学実験のための基礎技術2005

    • Author(s)
      築山光一 その他
    • Total Pages
      425
    • Publisher
      丸善
    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2005 Annual Research Report 2005 Final Research Report Summary

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Published: 2004-04-01   Modified: 2016-04-21  

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