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Wavepacket Dynamics of Ultrafast Chemical Processes

Research Project

Project/Area Number 11166216
Research Category

Grant-in-Aid for Scientific Research on Priority Areas (A)

Allocation TypeSingle-year Grants
Review Section Science and Engineering
Research InstitutionThe University of Tokyo

Principal Investigator

YAMASHITA Koichi  Graduate School of Engineering, Profeesor, 大学院・工学系研究科, 教授 (40175659)

Co-Investigator(Kenkyū-buntansha) NAKAJIMA Tohru  Graduate School of Engineering, Research Associate, 大学院・工学系研究科, 助手 (70292779)
Project Period (FY) 1999 – 2001
Project Status Completed (Fiscal Year 2001)
Budget Amount *help
¥38,400,000 (Direct Cost: ¥38,400,000)
Fiscal Year 2001: ¥6,900,000 (Direct Cost: ¥6,900,000)
Fiscal Year 2000: ¥16,000,000 (Direct Cost: ¥16,000,000)
Fiscal Year 1999: ¥15,500,000 (Direct Cost: ¥15,500,000)
Keywordschirped pulses / laser control / quantum control / chirped coherent Raman / photoinduced-adsorption dynamics / flux correlation function / quantum rate constant / quantum dynamics / 流束相関関数 / 緩和過程 / コヒーレンス / 状態分布制御 / 表面吸着分子 / 光誘起脱離 / パルスレーザー / 波束計算 / 電子励起状態 / CASSCF計算 / ダイナミクス / Si酸化表面 / 光会合反応 / レーザー冷却 / 自然放出 / 誘導放射 / 時間依存シュレシンガー方程式
Research Abstract

1. Molecular Vibrational Cooling via Photoassociation Process :
Wavepacket calculations on the O+H photoassociation reaction with a quadratic-chirped pulse have achieved the vibrational cooling of the product OH molecule.
2. Chirped Coherent Raman Spectroscopy :
On the basis of a second-order perturbation theory, analytical formulas are derived for describing spontaneous and stimulated Raman scatterings of a molecular system in the presence of chirped laser pulse.
3. Photo-stimulated Desorption of Xe from an Oxidized Si(100) Surface :
Ab initio CASSCF calculations for the potential energy surfaces of the Xe/oxidized Si(100) system in the electronic ground and excited states are performed in order to clarify the mechanism of photo-stimulated desorption and the translational energy distribution is analyzed based on wavepacket calculations.
4. Flux-Flux Cross-Correlation Function Approach to Quantum Rate Constants :
We employ a flux-flux cross-correlation approach (CCFA) to calculate quantum thermal rate constants of reactions to which an auto-correlation function approach ACFA) is not adequate to be applied, A combination of closed dividing surfaces and CCFA gives well-defined rate constants for both single and multi-hopping rates.
5. Population Transfer in the Presence of Relaxation :
Achievement of complete population inversion is one of control. In this study, we found that the mechanism important than that of positive-chirp effect for duration of a laser can be arbitrarily determined and chirp rate are chosen. This conclusion demonstrates a possibility of complete population inversion in the presence of ultrafast relaxation.

Report

(4 results)
  • 2001 Annual Research Report   Final Research Report Summary
  • 2000 Annual Research Report
  • 1999 Annual Research Report
  • Research Products

    (26 results)

All Other

All Publications (26 results)

  • [Publications] Mishima, Yamashita: "A Theoretical Study on Chirped Coherent Raman Spectroscopy"J. Phys. Chem.. A105. 2867-2878 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Abe, Yamashita: "Theoretical Study on the Photo-Stimulated Desorption of Xe from an Oxidized Si(001) Surface"Chem. Phys. Lett.. 343. 143-150 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Manz, Naundorf, Yamashita, Zhao: "Quantum Model Simulation of Complete SO->S1 Population Transfer by Means of Intense Laser Pulses with Opposite Chirp"J. Chem. Phys.. 113. 8969-8980 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Nakayama, Yamashita: "Theoretical Study on the Structure of Na+-doped Helium Clusters : Path Integral Monte Carlo Calculations"J. Chem. Phys.. 112. 10966-10975 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Nakayama, Yamashita: "Path Integral Monte Carlo Study on the Structure and Absorption Spectra of A Atoms (Li, Na, K) Attached to Superfluid Helium Clusters"J. Chem. Phys.. 114. 780-791 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Mishima, Yamashita: "A Theoretical Study on Quantum Control of Photodissociation and Photodesorption Dynamics by Femtosecond Chirped Laser Pulses"J. Chem. Phys.. 110. 7756-7769 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Mishima, and K. Yamashita: "A Theoretical Study on Chirped Coherent Raman Spectroscopy"J. Phys. Chem.. A105. 2867-2878 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] A. Abe, and K. Yamashita: "Theoretieal Study on the Photo-Stimulated Desorption of Xe from an Oxidized Si(001) Surface"Chem. Phys. Lett.. 343. 143-150 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] A. Nakayama, and K. Yamashita: "Theoretical Study on the Structure of Na^+-doped Helium Clusters : Path Integral Monte Carlo Calculations"J. Chem. Phys.. 112. 10966-10975 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] J. Manz, H.Naundorf, K. Yamashita, and Y. Zhao: "Quantum Model Simulation of Complete S0_->S1 Population Transfer by Means of Intense Laser Pulses with Opposite Chirp"J. Chem. Phys.. 113. 8969-8980 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] A. Nakayama, and K. Yamashita: "Path Integral Monte Carlo Study on the Structure and Absorption Spectra of Alkali Atoms (Li, Na, K) Attached to Superfluid Helium Clusters"J. Chem. Phys.. 114. 780-791 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Mishima, and K. Yamashita: "A Theoretical Study on Quantum Contol of Photodissociation and Photodesorption Dynamics by Femtosecond Chirped Laser Pulses"J. Chem. Phys.. 110. 7756-7769 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] G.Katz, K.Yamashita, Y.Zeiri, R.Kosloff: "The Fourier Method for Tri-atomic Systems in Quest of the Optimal Coordinate System"Phys. Chem. Chem. Phys.. (印刷中). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] 中山, 山下: "Absorption Spectra of Alkali Atoms (Li, Na, K) Attached to Super fluid Helium Clusters"Spectral Line Shapes. 11. 265-272 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] 三嶋, 山下: "A Theoretical Study on Chirped Coherent Raman Spectroscopy"J. Phys, Chem. A. 105. 2867-2878 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] 阿部, 山下: "Theoretical Study on the Photo-Stimulated Desorption of Xe from an Oxidized Si(001) Surface"Chem. Phys. Lett.. 343. 143-150 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] 島村, 三嶋, 山下: "Laser Control and Manipulation of Molecules"米国化学会(印刷中). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] 中島,田中,山下: "A theoretical study of aluminium chemical vapour deposition using dimethyl aluminium hydride"Surface Science. 444. 99-112 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] 中山,山下: "Theoretical study on the structure of Na^+-doped helium clasters : Path integral Monte Carlo calculations"Journal of Chemical Physics. 112・24. 10966-10975 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] J.Manz,H.Naundorf.山下,Y.Zao: "Quantum model simulation of complete So→Sl population transfer by means of intense laver pulses with opposite chirp"Journal of Chemical Physics. 113・20. 8969-8980 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] 中山,山下: "Path integral Monte Carlo study on the structure and absorption spectra of alkali atoms (Li, Na, K) attached to superfluid helium clustac"Journal of Chemical Physics. 114・2. 780-791 (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] 大脇,亀谷,山下: "Electric Field Effects on the Adsorption, Charge Transfer and Vibrational State at metal Electrodes : A DFT study"Bulletine of Chemical Society of Japan. (印刷中). (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] 大脇,山下: "A DFT study of Electric Field Effects on Protin Transfer Reactions at H^+(H_2O)_2/Pt(III) and Ag (III)"Journal of Electroanalytical Chemistry. (印刷中). (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] 三嶋、山下: "Theoretical Study on Quantum Control of Photodinociation and Photodesorption Dynamics by Femtosecond Chirped Laser Pulses"J. Chem. Phys.. 110. 7756-7769 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] 三嶋、山下: "Quantum Control of Photodissociation Wave Packets"J. Mol. Struc. (Theochem.). 461-462. 483-491 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] 三嶋、山下: "A Theoretical Study on Quantum Control of Photodissociation dynamics by Ultrashort Chirped Laser Pulses"Int. J. Quant. Chem.. 72. 525-532 (1999)

    • Related Report
      1999 Annual Research Report

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Published: 1999-04-01   Modified: 2018-03-28  

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