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

与热激发有关的表面动力学可以通过结合强近红外（NIR）脉冲照射引起的快速温升和表面敏感的超快光谱技术振动和频产生（SFG）光谱来观察。将这种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)表面在C_6H_<12>/Ni(111)系统上，近红外脉冲的照射导致Ni(111)表面温度暂时跃升，增强了高覆盖度状态的峰强度，但减弱了峰的强度。从结果可以看出，温度跳跃将环己烷分子从低覆盖率状态激发到高覆盖率状态。 (CH_3O-)/Ni(111) 系统，通过模拟再现了观察到的时间分布，假设基态的原始甲氧基与瞬时加热产生的新状态处于化学平衡。从结果得出结论。在控制下，250 K 的温度跃变会引起 Ni(111) 表面上甲氧基的分子取向或吸附位点发生变化，而不会分解甲氧基以吸附 CO 和氢气。在分子激发过程中，采用优化的脉冲整形技术来提高近红外（波长800 nm）飞秒脉冲双光子激发引起的苝分子的发射强度，发现具有类似脉冲串的脉冲形状。约100 fs的脉冲间隔显示出比单个飞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，并且脉冲形状对晶体样品有效。对于溶液样品也有效，反之亦然。可以得出结论，晶体样品和溶液样品的效率增加机制基本相同，并且分子内振动模式在330cm^-1（振荡周期）附近。约 100 fs）深入参与了激发过程。

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