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Ultrafast Spectroscopy and Interface Femtochemistry of Adsorbed Molecules on a Metal in Liquid

Research Project

Project/Area Number 11450322
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field 工業分析化学
Research InstitutionKYUSHU UNIVERSITY

Principal Investigator

HARATA Akira  Faculty of Matrl. Sci., Kyushu University, Ass. Prof., 大学院・総合理工学研究院, 助教授 (90222231)

Co-Investigator(Kenkyū-buntansha) ISHIOKA Toshio  Faculty of Matrl. Sci., Kyushu University, Research Ass., 大学院・総合理工学研究院, 助手 (60304838)
Project Period (FY) 1999 – 2001
Project Status Completed (Fiscal Year 2001)
Budget Amount *help
¥14,800,000 (Direct Cost: ¥14,800,000)
Fiscal Year 2001: ¥1,400,000 (Direct Cost: ¥1,400,000)
Fiscal Year 2000: ¥4,900,000 (Direct Cost: ¥4,900,000)
Fiscal Year 1999: ¥8,500,000 (Direct Cost: ¥8,500,000)
KeywordsElectrochemical Interface / Femtochemistry / Ultrafast Spectroscopy / Photothermal Phenomena / Nonradiative Processes / Single Crystalline Gold Electrode / Spectro-Electrochemistry / Energy Transfer in Nano-Space / 無幅射過程 / 電気化学
Research Abstract

This study aims to clarify main factors dominating interfacial femtochemistry at a sold/liquid interface. We have applied ultrafast transient reflectivity measurements for investigating ultrafast interaction of photoexcited electrons in metal with molecules adsorbed on the metal immersed in liquid solutions. A well-defined surface of Au(111) was investigated in an aqueous solution of perchloric acid or sulfuric acid, under electrochemical potential control and with/without interface modification by alkanethiols having a long alkyl chain of different lengths.
We successfully developed an experimental setup to observe ultrafast transient reflectivity of metal in liquid with a high precision. Transient reflectivity of the Au(111) surface showed rapid decrease followed by rapid increase and a remaining constant offset for an initial 4 picosecond after photoexcitation. Decay rate constants of the rapid reflectivity change ranged from 3 to 10 (1/ps) depending on the interface conditions but there observed no dependence on excitation light intensity. The rapid decay was attributed to electron relaxation by electron-electron and electron phonon couplings, while the constant offset was due to phonon temperature rise.
The transient reflectivity showed small but apparent dependence on electrochemical potential, kind of solute electrolytes in the liquid side, existence of surface modification, and hydrocarbon chain length of the alkanethiol interface modifiers. The experimental results are considered in connection with atomic and molecular structure of the solid/liquid interface. It is concluded that molecules adsorbed on the interface, including water molecules and adsorbed ions, play significant rolls in dominating ultrafast electron relaxation at the liquid/solid interface.

Report

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

    (24 results)

All Other

All Publications (24 results)

  • [Publications] Akira HARATA, Jyunya TAURA, Takeharu SUGIYAMA: "Heat Transport in Nano-Environments Adjacent to Metal-Liquid Interfaces : Photothermal Study"Analytical Sciences. 17. 197-200 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Takeharu SUGIYAMA, Toshio ISHIOKA, Akira HARATA: "Ultrafast Relaxation at Electrochemical Interfaces of Alkanethiol-Modified Gold Electrodes"Analytical Sciences. 17. 237-240 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Miki SATO, Hiromi AKAGISHI, Akira HARATA, Teiichiro OGAWA: "Polarization and Surface Density Dependence of Pyrenehexadecanoic Acid at the Air-Water Interface under Compression Studied by a Laser Two-Photon Ionization"Langumuir. 17・26. 8167-8171 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Takeharu SUGIYAMA, Toshio ISHIOKA, Akira HARATA, Yoshihiko HATANO: "Femtosecond Time-Resolved Transient Reflectivity at the Au(111) Electrode/Aqueous solution interfaces. The Effects of Laser Photon Impact, Electrochemical Potential Control and Modification by Alkanethiols"Analytical Sciences. 18(in press). (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Takeharu SUGIYAMA, Toshio ISHIOKA, Akira HARATA, Yoshihiko HATANO: "Electrochemical potential-dependence of ultrafast electron thermalization process at Au(111) electrode I aqueous solution interfaces modified with alkanethiols"Journal of Chemical Physics. (in press). (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Akira HARATA, Jyunya TAURA, Takeharu SUGIYAMA: "Heat Transport in Nano-Environments Adjacent to Metal-Liquid Interfaces : Ultrafast Photothermal Study"Analytical Sciences. 17. 197-200 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Takeharu SUGIYAMA, Toshio ISHIOKA, Akira HARATA: "Ultrafast Relaxation at Electrochemical Interfaces of Alkanethiol-Modified Gold Electrodes"Analytical Sciences. 17. 237-240 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Miki SATO, Hiromi AKAGISHI, Akira HARATA, Teiichiro OGAWA: "Polarization and Surface Density Dependence of Pyrenehexadecanoic Acid at the Air-Water Interface under Compression Studied by a Laser Two-Photon Ionization"Langumuir. 17-26. 8167-8171 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Takeharu SUGIYAMA, Toshio ISHIOKA, Akira HARATA, Yoshihiko HATANO: "Femtosecond Time-Resolved Transient Reflectivity at the Au(111) Electrode/Aqueous solution interfaces. The Effects of Laser Photon Impact, Electrochemical Potential Control and Modification by Alkanethiols"Analytical Sciences. 18 (in press). (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Takeharu SUGIYAMA, Toshio ISHIOKA, Akira HARATA, Yoshihiko HATANO: "Electrochemical potential-dependence of ultrafast electron thermalization process at Au(111) electrode/aqueous solution interfaces modified with alkanethiols"Journal of Chemical Physics. (in press). (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Akira HARATA, Jyunya TAURA, Takeharu SUGIYAMA: "Heat Transport in Nano-Environments Adjacent to Metal-Liquid Interfaces : Ultrafast Photothermal Study"Analytical Sciences. 17. 197-200 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] Takeharu SUGIYAMA, Toshio ISHIOKA, Akira HARATA: "Ultrafast Relaxation at Electrochemical Interfaces of Alkanethiol-Modified Gold Electrodes"Analytical Sciences. 17. 237-240 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] Miki SATO, Hiromi AKAGISHI, Akira HARATA, Teiichiro OGAWA: "Polarization and Surface Density Dependence of Pyrenehexadecanoic Acid at the Air-Water Interface under Compression Studied by a Laser Two-Photon Ionization"Langumuir. 17・26. 8167-8171 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] Takeharu SUGIYAMA, Toshio ISHIOKA, Akira HARATA, Yoshihiko HATANO: "Femtosecond Time-Resolved Transient Reflectivity at the Au(111) Electrode/Aqueous solution interfaces. The Effects of Laser Photon Impact, Electrochemical Potential Control, and Modification by Alkanethiols"Analytical Sciences. 18(in press). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] Kazuki ITO,Isao TSUYUMOTO,Akira HARATA and Tsuguo SAWADA: "Ultrafast Energy Transfer of Silver Ultrafine Particles in Aqueous Solutions as Investigated by Ultrafast Lensing Effect Technique."Chemical Physics Letters. 318. 1-6 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Tomohiro MORISHITA,Akihide HIBARA,Tsuguo SAWADA,Isao TSUYUMOTO,and Akira HARATA: "Femtosecond Transient Reflecting Grating Methods and Analysis of the Ultrafast Carrier Dynamics on Si (111) Surfaces."Analytical Sciences. 16. 403-406 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Akira HARATA,Jyunya TAURA and Teiichiro OGAWA: "Heat Conduction in Nano-Environment Observed as Cooling Processes of Colloidal Silver Nanoparticles in Water"Japanese Journal of Applied Physics. 39. 2909-2912 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Akira HARATA and Naonori YAMAGUCHI: "Photothermal Lensing Signal Enhancement by Transient Absorption of Photoexcited States in Liquid Solutions"Analytical Sciences. 16. 743-749 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Valeria TSUKANOVA,Akira HARATA and Teiichiro OGAWA: "Second-Harmonic Probe of Pressure-Induced Structure Ordering within Long-Chain Fluorescence Monomer at the Air/Water Interface"Journal of Chemical Physics. 104・32. 7707-7712 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Akira Harata,Qing Shen.Tsuguo Sawada: "Photothermal Application of Lasers:Study of Fast and Ultrafast Photothermal Phenomena at Metal-Kiquid Interfaces"Annual Rebiew of Physical Chemistry. 50. 193-219 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] Akihide Hibara,Tomohiro Morishita,Isao Tsyumoto,Akira Hrata,Takehiko Kitamori,Tsuguo Sawada: "Direct Measurements of Femtosecond Energy Dissipation Processes of Hot Electrons in a Gold Film"Japanese Journal of Applied Physics. 38. 2983-2987 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] Kenji Katayama,Tsuguo Sawada,Isao Tsuyumoto,Akira Harata: "Picosecond Energy Transfer at Gold/Electrolyte Interfaces Using Transient Reflecting Grating Method under Surface Plasmon Resonance Condition"Bulletin of Chemical Society of Japan. 72・11. 2383-2388 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] S.Ikeda,K.Katayama,T.Sawada,I.Tsuyumoto,A.Harata: "Generation and Observation of GHz Ultrasonic Waves on Liquid Surfaces and a Liquid/Liquid Interface by Transient Reflectiong Grating Method"Jounal of Chemical Physics. 111・20. 9393-9397 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] Gen Furui,Kazuki Ito,Isao Tsuyumoto,Akira Hrata,Tsuguo Sawada: "Mokeculer Dynamics of Auramine/O in Low/Viscosity Solutions as Investigated by an Ultrafast Lensing Effect"Jounal of Physics Chemical A. 103・38. 7575-7579 (1999)

    • Related Report
      1999 Annual Research Report

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

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