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Application of Pulse-Shaping and Multi-Pulse-Train for Control of Chemical Reaction in Condensed Phase and Surface

Research Project

Project/Area Number 15350009
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Physical chemistry
Research InstitutionTokyo Institute of Technology

Principal Investigator

WADA Akihide  Tokyo Institute of Technology, Chemical Resources Laboratory, Associate Professor, 資源化学研究所, 助教授 (20202418)

Co-Investigator(Kenkyū-buntansha) KUBOTA Jun  Tokyo Institute of Technology, Chemical Resources Laboratory, Research Associate, 資源化学研究所, 助手 (50272711)
Project Period (FY) 2003 – 2004
Project Status Completed (Fiscal Year 2004)
Budget Amount *help
¥14,800,000 (Direct Cost: ¥14,800,000)
Fiscal Year 2004: ¥5,500,000 (Direct Cost: ¥5,500,000)
Fiscal Year 2003: ¥9,300,000 (Direct Cost: ¥9,300,000)
Keywordspulse train / optimal pulse shaping / adaptive control / control of excitation efficiency / control of reaction / coherent control / low-frequency vibration mode / pulse compression / フェムト秒パルス / 光パルストレイン / 波形整形 / パルスシェイピング / 表面化学 / 超高速分光 / 遠赤外励起
Research Abstract

In order to examine the potentiality of multi pulse train and pulse shaping technique for control of chemical reaction, control of excitation process and excited states of perylene crystal was investigated by optimal pulse shaping technique. We succeeded in controlling the emission spectral feature of an α-perylene crystal ; the intensity of E-emission was increased by a factor of 1.4 without the change of Y-emission intensity. Furthermore, we found a near-infrared pulse shape whose multi-photon excitation efficiency is larger than that of a single femtosecond pulse by a factor of two. It was concluded from these results that pulse train and pulse shaping technique can control excitation process of molecules in condensed phase. In order to extend the application area of the pulse-shaping technique by increasing the pulse energy, the compression of femtosecond pulses obtained from a conventional regenerative amplifier was attempted by X^<(2)>:X^<(2)> process using BBO crystals. It was r … More ealized that the pulse width of 120 fs was narrowed to about 80 fs.
For the search of the molecular system which can be applied by the pulse shaping technique, the time-resolved experiments were carried out on several molecular-adsorbed-surface systems. It was found on isobutene adsorbed zeolite system that a short-lived species is produced by vibrational excitation of isobutene adsorbed OD groups. From the temporal behavior of OD band intensity, the desorption of isobutene takes places after the vibrational relaxation of OD mode finishes and before the system reaches thermal equilibrium. On the c(4×2)-CO/Ni(111) system, it was found that the site-hopping of CO molecule from hollow site to atop site was induced by the irradiation of intense near-infrared pulses. The hopping phenomenon was found to be entirely transient, with the surface returning to the pre-excited state within a few hundred picoseconds without desorption. The transient response of 10 molecular layers of D_2O ice on CO/Pt(111) at 130 K was also investigated under ultra-high vacuum following a near-infrared pump pulse by sum frequency generation (SFG) spectroscopy. It was revealed that the D_2O molecules in the ice crystalline layer formed an amorphous or liquid-like structure in response to the pumping without desorption of D_2O to the gas phase, and the crystals returned to the crystal structure on a sub-nanosecond time scale. Less

Report

(3 results)
  • 2004 Annual Research Report   Final Research Report Summary
  • 2003 Annual Research Report
  • Research Products

    (21 results)

All 2004 2003 Other

All Journal Article (15 results) Publications (6 results)

  • [Journal Article] Optical control of two-photon excitation efficiency of α-perylene crystal by pulse shaping2004

    • Author(s)
      T.Okada, I.Otake, R.Mizoguchi, K.Onda, S.S.Kano, A.Wada
    • Journal Title

      J.Chem.Phys. 121

      Pages: 6386-6391

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Optical control of two-photon excitation efficiency of α-perylene crystal by pulse shaping2004

    • Author(s)
      T.Okada, I.Otake, R.Mizoguchi, K.Onda, S.S.Kano, A.Wada
    • Journal Title

      Journal of Chemical Physics 121

      Pages: 6386-6391

    • Related Report
      2004 Annual Research Report
  • [Journal Article] 和周波発生法による表面化学反応の超高速分光2004

    • Author(s)
      久保田 純, 和田昭英
    • Journal Title

      応用物理 73

      Pages: 1292-1295

    • NAID

      10013651775

    • Related Report
      2004 Annual Research Report
  • [Journal Article] 和周波発生法(SFG)を用いた表面化学反応の超高速分光2004

    • Author(s)
      久保田 純, 和田昭英
    • Journal Title

      真空 47

      Pages: 446-451

    • Related Report
      2004 Annual Research Report
  • [Journal Article] Dynamic Processes of Olefins Adsorbed on Hydroxyl Groups of DM20 Zeolite Excited by Picosecond Infrared Pulses2003

    • Author(s)
      K.Onda, K.Tanabe, H.Noguchi, K.Domen, A.Wada
    • Journal Title

      J.Phys.Chem.B 107

      Pages: 11391-11396

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Optical Control of Excited States of a-Perylene Crystal using Optimized Pulse Shaping Method2003

    • Author(s)
      R.Mizoguchi, S.S.Kano, A.Wada
    • Journal Title

      Chem.Phys.Lett. 379

      Pages: 319-324

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Site-Hopping of Adsorbed CO in c(4x2)-CO/Ni(111) by Laser-Induced Temperature Jump : Time-Resolved Sum-Frequency Generation Observation2003

    • Author(s)
      J.Kubota, E.Yoda, N.Ishizawa, A.Wada, K.Domen, S.S.Kano
    • Journal Title

      J.Phys.Chem.B 107

      Pages: 10329-10332

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Time-resolved Study of D_2O ice crystal on CO/Pt(111) by Ultrashort NIR Laser pumping : Melting and Recrystallization without desorption2003

    • Author(s)
      J.Kubota, A.Wada, S.S.Kano, K.Domen
    • Journal Title

      Chem.Phys.Lett. 377

      Pages: 217-222

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Thinning-Out in Optimized Pulse Shaping Method using Genetic Algorithm2003

    • Author(s)
      R.Mizoguchi, K.Onda, S.S.Kano, A.Wada
    • Journal Title

      Rev.Sci.Inst. 74

      Pages: 2670-2675

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Optical Control of Excited States of ・-Perylene Crystal using Optimized Pulse Shaping Method2003

    • Author(s)
      R.Mizoguchi, S.S.Rano, A.Wada
    • Journal Title

      Chem.Phys.Lett. 379

      Pages: 319-324

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Time-resolved Study of D_2O ice crystal on CO/Pt(111) by Ultra-short NIR Laser pumping : Melting and Recrystallization without desorption2003

    • Author(s)
      J.Kubota, A.Wada, S.S.Kano, K.Domen
    • Journal Title

      Chem.Phys.Lett. 377

      Pages: 217-222

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Structural Change of CO Adsorbed on Pt(111) by Laser Heating : Time-resolved Sum-frequency Generation Study2003

    • Author(s)
      S.Katano, S.Dobashi, J.Kubota, K.Onda, A.Wada, S.S.Kano, K.Domen
    • Journal Title

      Chem.Phys.Lett. 377

      Pages: 601-601

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Vibrational Relaxation of Adsorbate and Adsorbent in the CO-adsorbed DM-20 Zeolite System2003

    • Author(s)
      K.Onda, Y.Iwasawa, A.Wada
    • Journal Title

      Chem.Phys.Lett. 370

      Pages: 437-442

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Second Harmonic Observation of Cu(111) Surface : In situ Measurements during Molecular Adsorption2003

    • Author(s)
      H.Ishida, R.Mizoguchi, K.Onda, C.Hirose, S.S.Kano, A.Wada
    • Journal Title

      Surf.Sci. 526

      Pages: 201-207

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Journal Article] Time-resolved SFG Study of Formate on Ni(111) Surface under Irradiation of Picosecond Laser Pulses2003

    • Author(s)
      H.Noguchi, T.Okada, K.Onda, S.S.Kano, A.Wada, K.Domen
    • Journal Title

      Surf.Sci. 528

      Pages: 183-188

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2004 Final Research Report Summary
  • [Publications] R.Mizoguchi, S.S.Kano, A.Wada: "Optical Control of Excited States of α-Perylene Crystal using Optimized Pulse Shaping Method"Chemical Physics Letters. 379. 314-319 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] R.Mizoguchi, S.S.Kano, A.Wada: "Thinning-Out in Optimized Pulse Shaping Method using Genetic Algorithm"Review of Scienctific Instruments. 72. 2670-2674 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] K.Onda, K.Tanabe, H.Noguchi, K.Domen, A.Wada: "Dynamic Processes of Olefins Adsorbed on Hydroxyl Groups of DM20 Zeolite Excited by Picosecond Infrared Pulses"Journal of Physical Chemistry B. 107. 11391-11396 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] H.Ishida, R.Mizoguchi, K.Onda, C.Hirose, S.S.Kano, A.Wada: "Second Harmonic Observation of Cu(111) Surface : In situ Measurements during Molecular Adsorption"Surface Science. 526. 201-207 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] H.Noguchi, T.Okada, K.Onda, S.S.Kano, A.Wada, K.Domen: "Time-resolved SFG Study of Formate on Ni(111) Surface under Irradiation of Picosecond Laser Pulses"Surface Science. 528. 183-188 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] S.Katano, S.Dobashi, J.Kubota, K.Onda, A.Wada, K.Domen: "Structural Change of CO Adsorbed on Pt(111) by Laser Heating : Time-resolved Sum-frequency Generation Study"Chemical Physics Letters. 377. 601-606 (2003)

    • Related Report
      2003 Annual Research Report

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Published: 2003-04-01   Modified: 2016-04-21  

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