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Real Time Observation of Surface Chemical Reaction by Nonlinear Spectroscopy

非线性光谱实时观察表面化学反应

基本信息

批准号：
16072208
负责人：
WADA Akihide
金额：
$ 15.81万
依托单位：
Kobe University (2006)Tokyo Institute of Technology (2004-2005)
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research on Priority Areas
财政年份：
2004
资助国家：
日本
起止时间：
2004 至 2006
项目状态：
已结题

来源：
https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-16072208/
关键词：
surface adsorbed molcule time resolved spectroscopy excited state dynamics sum-freauency generation control of excited state optimized pulse shaping method surface reaction low frequency vibration mode 振動分光和周波発生法反応制御最適化波形整形超高速分

项目摘要

The surface dynamics concerned with thermal excitation can be observed by combining rapid temperature rise induced by irradiation of intense near-infrared (NIR) pulse and vibrational sum-frequency generation (SFG) spectroscopy which is surface sensitive and ultrafast spectroscopic technique. In this study, such time-resolved method was applied to methoxy (CH_3O-)/Ni(111) and C_6H_<12>(cyclohexane)/Ni(111) surface systems. On the C_6H_<12>/Ni(111) system, the irradiation with NIR pulses caused a temporary jump in temperature at the Ni(111) surface and enhanced the intensity of the peak from the high-coverage state, but weakened the peaks from the low-coverage state. It was concluded from the results that the temperature jump excites the cyclohexane molecules from the low-coverage state to the high-coverage state. On the (CH_3O-)/Ni(111) system, the observed temporal profile was reproduced by simulation assuming that the original methoxy in the ground state was in chemical equilibrium wi … More th a new state produced by instantaneous heating. It was concluded from the results that a temperature jump of 250 K induced a change in the molecular orientation or adsorption site of methoxy on the Ni(111) surface without decomposition of methoxy to adsorbed CO and hydrogen. On the control of excitation process of molecules, the optimized pulse shaping technique was applied to increase the emission intensity from perylene molecule induced by two-photon excitation using NIR (wavelength of 800 nm) femtosecond pulse. It was found that the pulse-train-like pulse shape with the pulse interval of about 100 fs showed the emission intensity stronger than that by a single femtosecond pulse. The pulse shapes optimized for crystalline and solution samples were very similar to each other, and the pulse shape effective for the crystalline sample was also effective for the solution sample and vice versa. It was concluded that the mechanism for the efficiency increase was essentially the same for the crystalline and solution samples, and that the intramolecular vibrational modes at around 330 cm^<-1> (oscillation period of about 100 fs) were deeply involved in the excitation process. Less

利用近红外（NIR）脉冲辐射引起的快速升温和振动和频产生（SFG）光谱技术，可以观察到与热激发有关的表面动力学过程。本文将时间分辨方法应用于甲氧基（CH_3O-）/Ni（111）和C_6H_<12>（环己烷）/Ni（111）表面体系。在C_6H_2<12>/Ni（111）体系中，近红外脉冲辐照引起Ni（111）表面温度的暂时性跃变，使高覆盖度态的峰强度增强，而低覆盖度态的峰强度减弱。结果表明，温度跃变使环己烷分子从低覆盖度态激发到高覆盖度态。在（CH_3O-）/Ni（111）体系中，假设基态甲氧基处于化学平衡，通过模拟再现了所观察到的时间分布。 ...更多信息这是一种由瞬时加热产生的新状态。结果表明，250 K的温度跃变导致甲氧基在Ni（111）表面上的分子取向或吸附位置发生变化，而甲氧基没有分解为吸附的CO和H2。在分子激发过程的控制上，采用优化的脉冲整形技术，利用近红外（波长800 nm）飞秒脉冲双光子激发，提高了苝分子的发光强度。结果发现，脉冲串的脉冲形状与约100 fs的脉冲间隔显示的发射强度强于由一个单一的飞秒脉冲。针对结晶和溶液样品优化的脉冲形状彼此非常相似，并且对结晶样品有效的脉冲形状也对溶液样品有效，反之亦然。得出的结论是，对于晶体和溶液样品，效率增加的机制基本上是相同的，并且在约330 cm-1<-1>（振荡周期约为100 fs）处的分子内振动模式深深地参与激发过程。少

项目成果

期刊论文数量（88）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Transfer of Photoenergy in p-Conjugated Polymers. Two Types of Photoluminescence that Involve Energy Transfer along a Polymer Chain

p-共轭聚合物中的光能转移。

DOI：
发表时间：
2005
期刊：
Journal of physical Chemistry B 109
影响因子：
0
作者：
T.Yamamoto;B-L.Lee;I.Nurulla;T.Yasuda;I.Yamaguchi;A.Wada;C.Hirose;M.Tasumi;A.Sakamoto;E.Kobayashi
通讯作者：
E.Kobayashi

最適化波形整形法によるペリレン結晶の励起状態制御

使用优化波形整形方法控制苝晶体的激发态

DOI：
发表时间：
2004
期刊：
影响因子：
0
作者：
Yoshinori Takahashi;Hiroaki Adachi;Tetsuo Taniuchi;Masayuki Takagi;Youichiroh Hosokawa;Shinji Onzuka;Srinivasan Brahadeeswaran;Masashi Yoshimura;Yusuke Mori;Hiroshi Masuhara;Takatomo Sasaki;Hachiro Nakanishi;和田昭英
通讯作者：
和田昭英

ピコ秒レーザーパルス照射による吸着分子の表面ダイナミクス

皮秒激光脉冲照射吸附分子的表面动力学