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Isotope effect in the photodissociation process of nitrous oxide

Research Project

Project/Area Number 11640501
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field Physical chemistry
Research InstitutionJapan Advanced Institute of Science and Technology

Principal Investigator

UMEMOTO Hironobu  Japan Advanced Institute of Science and Technology School of Materials Science Associate Professor, 材料科学研究科, 助教授 (80167288)

Project Period (FY) 1999 – 2000
Project Status Completed (Fiscal Year 2000)
Budget Amount *help
¥3,600,000 (Direct Cost: ¥3,600,000)
Fiscal Year 2000: ¥1,100,000 (Direct Cost: ¥1,100,000)
Fiscal Year 1999: ¥2,500,000 (Direct Cost: ¥2,500,000)
Keywordsnitrous oxide / photodissociation / isotope effect / atmospheric chemistry
Research Abstract

The stratospheric N_2O is enriched in heavy isotopes. In order to explain this isotope anomaly, Yung and Miller have demonstrated, ou the basis of their calculations, that isotopically heavy N_2O, such as ^<14>N^<15>N^<16>O and ^<14>N_2^<18>O, has smaller probability to be photolyzed at wavelengths longer than 200 nm. The peak of the absorption of N_2O is around 180 nm. However, sun light around 180 nm is absorbed by O_2 and less important for the photolysis. Photolysis around 205 nm is more important. Since the absorption coefficient of N_2O changes with the wavelength steeply in this region, a small isotope shift in the wavelength causes a large difference in the absorption coefficient.
In the present work, the photodissociation products of N_2O, N_2(X^1Σ^+_g) and O(^1D_2), were monitored to examine the ^<14>N/^<15>N isotope effect. ^<14>N_2^<16>O, ^<14>N^<15>N^<16>O, and ^<15>N^<14>N^<16>O were photolyzed between 202 and 206 nm. O(^1D_2) and N_2(X ^1Σ^+_g) were monitored by a resonance-enhanced multiphoton ionization technique combined with a time-of-flight mass spectrometric technique. The O(^1D_2) signal was weaker when heavy isotopomers were photolyzed at 205.47 nm. The isotope effect was as large as 10 % for ^4N^<15>N^<16>O, while it was 3 % for ^<15>N^<14>N^<16>O.The absorption coefficients must be smaller for heavy isotopomers. An inverse isotope effect was observed when N_2(X ^1Σ^+_g) was monitored. ^<14>N_2 signal was less than that for ^<14>N^<15>N.There must be an isotope effect in the detection efficiency of rotationally highly excited N_2(X ^1Σ^+_g). The rotational state distributions of N_2(X ^1Σ^+_g) were also measured at two photolysis wavelengths, 205 and 210 nm. It was found that N_2(X ^1Σ^+_g) is highly rotationally excited and that 60 % of the available energy is partitioned into the rotational mode in both cases. No large isotope effect was found in the internal state distributions of N_2(X ^1Σ^+_g).

Report

(3 results)
  • 2000 Annual Research Report   Final Research Report Summary
  • 1999 Annual Research Report
  • Research Products

    (21 results)

All Other

All Publications (21 results)

  • [Publications] H.UMEMOTO: "Reactions of N(2^2D) with CH_3OH and its Isotopomers"J.Phys.Chem.A. 103. 7026-7031 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.UMEMOTO: "^<14>N/^<15>N Isotope Effect in the UV Photodissociation of N_2O"Chem.Phys.Lett.. 314. 267-272 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.UMEMOTO: "Verification of the Insertion Mechanism of N(2^2D) into H-H Bonds by the Vibrational State Distribution Measurement of NH (X^3Σ^-,0【less than or equal】ν"【less than or equal】3)"J.Chem.Phys.. 112. 5762-5766 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.UMEMOTO: "Deactivation Processes of Highly Excited Atomic Nitrogen, N(2p^23p^2S)"Phys.Chem.Chem.Phys.. 2. 3425-3428 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.UMEMOTO: "Production Processes of H (D) Atoms in the Reactions of NO (A ^2Σ^+) with C_2H_2, C_2H_4, H_2O, and their Isotopic Variants"Chem.Phys.. 259. 39-47 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Y.Nozaki: "Identification of Si and SiH in Catalytic Chemical Vapor Deposition of SiH_4 by Laser Induced Fluorescence Spectroscopy"J.Appl.Phys.. 88. 5437-5443 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.Umemoto: "Reactions of N (2^2D) with H_2O and D_2O ; Identification of the Two Exit Channels, NH (ND)+OH (OD) and H (D)+HNO (DNO)"J.Phys.Chem. A. 103, [6]. 700-704 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.Umemoto: "Reactions of N(2^2D) with CH_3OH and its Isotopomers"J.Phys.Chem.A.. 103, [35]. 7026-7031 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.Umemoto: "^<14>N/^<15>N Isotope Effect in the UV Photodissociation of N_2O"Chem.Phys.Lett.. 314, [3-4]. 267-272 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.Umemoto: "Verification of the Insertion Mechanism of N(2^2D) into H-H Bonds by the Vibrational State Distribution Measurement of NH (X^3Σ^-)"J.Chem.Phys.. 112, [13]. 5762-5766 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.Umemoto: "Deactivation Processes of Highly Excited Atomic Nitrogen, N (2p^23p^2S)"Phys.Chem.Chem.Phys.. 2, [15]. 3425-3428 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.Umemoto: "Production Processes of H (D) Atoms in the Reactions of NO (A^2Σ^+) with C_2H_2, C_2H_4, H_2O, and their Isotopic Variants"Chem.Phys.. 259, [1]. 39-47 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Y.Nozaki: "Identification of Si and SiH in Catalytic Chemical Vapor Deposition of SiH_4 by Laser Induced Fluorescence Spectroscopy"J.Appl.Phys.. 88, [9]. 5437-5443 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] H.Umemoto et al.: "Verification of the Insertion Mechanism of N(2^2D) into H-H Bonds by the Vibrational State Distribution Measurement of NH(X^3Σ^-)"J.Chem.Phys.. 112・[13]. 5762-5766 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] H.Umemoto et al.: "Deactivation Processes of Highly Excited Atomic Nitrogen, N(2p^23p^2S)"Phys.Chem.Chem.Phys.. 2・[15]. 3425-3428 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] H.Umemoto et al.: "Production Processes of H(D) Atoms in the Reactions of NO(A^2Σ^+) with C_2H_2,C_2H_4,H_2O, and their Isotopic Variants"Chem.Phys.. 259・[1]. 39-47 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Y.Nozaki et al.: "Identification of Si and SiH in Catalytic Chemical Vapor Deposition of SiH_4 by Laser Induced Fluorescence Spectroscopy"J.Appl.Phys.. 88・[9]. 5437-5443 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] H.UMEMOTO: "Reactions of N(2^2D) with H_2O and D_2O; Identification of the Two Exit Channels,NH(ND)+OH(OD) and H(D)+HNO(DNO)"J.Phys.Chem.A. 103・6. 700-704 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] H.UMEMOTO: "Reactions of N(2^2D) with CH_3OH and its Isotopomers"J.Phys.Chem.A. 103・35. 7026-7031 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] H.UMEMOTO: "^<14>N/^<15>N Isotope Effect in the UV Photodissociation of N_2O"Chem.Phys.Lett.. 314・3-4. 267-272 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] H.UMEMOTO: "Verification of the insertion mechanism of N(2^2D) into H-H bonds by the vibrational state distribution measurement of NH(X^3Σ^-,0【less than or equal】υ"【less than or equal】3)"J.Chem.Phys.. (in press). (2000)

    • Related Report
      1999 Annual Research Report

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Published: 1999-04-01   Modified: 2016-04-21  

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