Observation of Ultrafast electron dynamics in the molecular frame using quantum rotational wave packet

使用量子旋转波包观察分子框架中的超快电子动力学

• 批准号: 17205004
• 负责人: SUZUKI Toshinori
• 金额: $ 31.28万
• 依托单位: The Institute of Physical and Chemical Research
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (A)
• 财政年份: 2005
• 资助国家: 日本
• 起止时间: 2005 至 2007
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-17205004/
• 关键词: photoelectron spectroscopy; imaging; ultrafast snectroscopy; Nitric Oxide; photoelectron angular distribution; rotational wave nacket; 光電子; 角度分布; 量子欠損; 超高速; 動力学; 光イオン化

Time-resolved photoelectron spectroscopy is a powerful means to probe ultrafast electronic dynamics in the molecule. However, the observation is carried out in the laboratory frame, and the information is always convoluted with the broad molecular axis distribution in the laboratory frame. It is ideal to observe the electronic dynamics in the molecular frame, which requires extraction of photoionization dynamical parameters and recasting the photoelectron angular distribution in the laboratory frame into the distribution in the molecular frame. In the past, photoelectron and photoion coincidence method has been employed to extract such information, however, it is only applicable to dissociative ionization. In the present work, we created a rotational wavepacket motion of a molecule and observed photoionization from various time-dependent axis distribution, from which photoelectron angular distribution in the molecular frame has been extracted. The sample molecule was Nitric Oxide, the … More benchmark system in molecular photoionization study. We prepared a rotational wavepacket in the A state of NO by one-photon absorption from the ground state, and then ionized by another photon from the A state. The measurements were carried out on the integral and differential cross sections, and detailed theoretical analysis was performed. We found that the partial wave of outgoing photoelectron is dominated by p-wave contradicting with the prediction of f-wave by theory. It is also pointed out dic wave has appeared with a reasonable intensity whereas theory does not predict it. The existence of the cbt wave is important for describing directional ejection of an electron into either N-side or 0-side of the molecule. We are planning to collaborate further with theoreticians to elucidate the source of this discrepancy between the experiment and theory, thereby improving our understanding of molecular photoionization dynamics and develop a methodology to probe electronic dynamics in the molecular frame. Less

时间分辨光电子能谱是探测分子中超快电子动力学的有力手段，然而，观察是在实验室框架内进行的，并且信息总是与实验室框架内的宽分子轴分布相混淆。要观察分子框架中的电子动力学，需要提取光电离动力学参数，并将实验室框架中的光电子角分布重新转换为分子框架中的分布。然而，它仅适用于解离电离。在目前的工作中，我们创建了分子的旋转波包运动，并从各种与时间相关的轴分布中观察到光电离，从中得到了分子中的光电子角分布。样品分子是一氧化氮，这是分子光电离研究中的基准系统，我们通过基态的单光子吸收制备了 A 态的旋转波包，并且然后被来自A态的另一个光子电离，对积分截面和微分截面进行了测量，并进行了详细的理论分析，发现出射光电子的部分波以p波为主，这与预测相矛盾。理论上也指出 dic 波的出现是合理的，而强度理论并没有预测它。cbt 波的存在对于描述电子向 N 侧或 0 侧的定向喷射很重要。分子的。我们计划与理论家进一步合作，阐明实验与理论之间差异的根源，从而提高我们对分子光电离动力学的理解，并开发一种在分子框架中探测电子动力学的方法。

项目成果

光電子画像観測法による光イオン化ダイナミクスの研究

利用光电子成像观测方法研究光电离动力学

• 发表时间: 2006
• 作者: Kiyoshi Nishizawa;Mizuki Oku;Keijirou Ohshimo and Toshinori Suzuki;戸田 剛史;Tsuyoshi Ohishi;Yoshiichi Suzuki and Toshinori Suzuki;Masahiro Kou;鈴木 喜一,鈴木 俊法;T. Ohishi;鈴木 喜一,堀尾 琢哉,加藤 吉康,小城 吉寛,高口 博志,鈴木 俊法
• 通讯作者: 鈴木 喜一,堀尾 琢哉,加藤 吉康,小城 吉寛,高口 博志,鈴木 俊法

Determination of photoelectron angular disutributions in the molecular frame by time-resolved photoelectron imaging

通过时间分辨光电子成像测定分子框架中的光电子角分布

• 发表时间: 2005
• 作者: Yoshiichi Suzuki;Takuya Horio;Yoshihiro Ogi;Hiroshi Kohguchi;Toshinori Suzuki;奥 瑞希,大下 慶次郎,岩崎 純史,西澤 潔,鈴木 俊法;武井信裕;鈴木 喜一,鈴木 俊法,;藤本聡;鈴木 喜一,鈴木 俊法;大崎堅;鈴木 俊法;Y. Yamatan;鈴木 俊法;M. Kurita;鈴木 俊法;大崎堅;鈴木 喜一,鈴木 俊法;Y. Yamatani;奥 瑞希,大下 慶次郎,岩崎 純史,西澤 潔,鈴木 俊法;M. Kurita;西澤 潔,大下 慶次郎,鈴木 俊法;赤畑海山;岩崎 純史,;大崎堅;Toshinori Suzuki
• 通讯作者: Toshinori Suzuki

Two-dimensional ion and electron imaging methods in chemical dynamics

化学动力学中的二维离子和电子成像方法

• 发表时间: 2007
• 作者: Takao Fuji;Toshinori Suzuki;Y.Yamatan;日高 洋;Takao Fuji and Toshinori Suzuki;M.Kurita;O. Fukumasa;Toshinori Suzuki;日高 洋;Toshinori Suzuki;O. Fukumasa;O.Fukumasa;日高 洋;Toshinori Suzuki
• 通讯作者: Toshinori Suzuki

3s Rydberg and Cationic States of Pyrazine Studied by Photoelectron Spectroscopy

光电子能谱研究吡嗪的 3s Rydberg 和阳离子态

• 发表时间: 2008
• 期刊: Journal of Physical Chemistry A (In Press)
• 作者: Mizuki Oku;et. al.
• 通讯作者: et. al.

光電子画像観測法の開発と化学反応動力学の展開

光电子图像观察方法的发展和化学反应动力学的发展

• 发表时间: 2007
• 作者: Takao Fuji;Toshinori Suzuki;Y.Yamatan;日高 洋;Takao Fuji and Toshinori Suzuki;M.Kurita;O. Fukumasa;Toshinori Suzuki;日高 洋;Toshinori Suzuki;O. Fukumasa;O.Fukumasa;日高 洋;Toshinori Suzuki;K.Osaki;Toshinori Suzuki;H. Hidaka;T. Toda;Toshinori Suzuki;H. Hidaka;小城 吉寛,高口 博志,莫 宇翔,鈴木 俊法;Y. Yoshihara;小城 吉寛,高口 博志,鈴木 俊法;菊池麻希子;T. Toda;鈴木 俊法;瀧口 愛;K. Akimoto;鈴木 俊法;T. Toda;日高 洋;藤 貴夫,堀尾 琢哉,鈴木 俊法;K. Akimoto;瀧口 愛;鈴木 俊法
• 通讯作者: 鈴木 俊法