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

可以通过结合强烈的近红外（NIR）脉冲和振动总和频率产生（SFG）光谱的快速温度升高来观察到与热兴奋有关的表面动力学，该温度升高是表面敏感和超快光谱技术的。在这项研究中，将这种时间分辨的方法应用于方法论（CH_3O-）/Ni（111）和C_6H_ <12>（Cyclohexane）/Ni（111）表面系统。在C_6H_ <12>/Ni（111）系统上，使用NIR脉冲的辐射导致Ni（111）表面的温度暂时升高，并增强了高覆盖状态的峰强度，但从低覆盖状态下却削弱了峰。从结果得出的结论是，温度跳跃使环己烷分子从低覆盖状态激发到高覆盖状态。在（CH_3O-）/Ni（111）系统上，通过模拟复制了观察到的临时轮廓，假设基态的原始方法是在化学平衡的Wi中……更多的是瞬时加热产生的新状态。从结果得出的结论是，250 K的温度跃升引起了Ni（111）表面的分子取向或方法的变化，而没有方法学对吸附的CO和氢的分解。在控制分子的兴奋过程中，采用优化的脉冲成型技术来增加使用NIR（800 nm）fomtsecond脉冲的两光子兴奋感诱导的per骨分子的发射强度。发现脉冲训练脉冲形状的脉冲间隔约为100 fs，显示出比单秒脉冲更强的发射强度。针对晶体和溶液样品优化的脉冲形状彼此非常相似，并且有效的晶体样品对溶液样品也有效，反之亦然。得出的结论是，对于晶体和溶液样品，效率提高的机制基本相同，并且分子内振动模式在330 cm^<-1>>大约330 cm^<-1>（约100 fs的振荡周期）中与兴奋过程深远有关。较少的

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）

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

DOI：
发表时间：
2005
期刊：
表面科学 26
影响因子：
0
作者：
久保田純;和田昭英
通讯作者：
和田昭英

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

SFG 分光法によるPt(111)基板上のTiO2 膜に吸着したフォルメートの観察

SFG 光谱观察 Pt(111) 基底上 TiO2 薄膜吸附的甲酸盐