Development of a program for the calculation of attosecond time-resolved photoelectron spectra and its application to photo-induced electron transfer reactions

阿秒时间分辨光电子能谱计算程序的开发及其在光诱导电子转移反应中的应用

• 批准号: 16350001
• 负责人: KONO Hirohiko
• 金额: $ 8.06万
• 依托单位: Tohoku University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (B)
• 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/grant/KAKENHI-PROJECT-16350001/
• 关键词: Atomic and molecular physics; Photoelectron spectrum; S-matrix theory; Electronic wave packet; Photoelectron Angular Distribution; Enhanced ionization; Ring current; イオン化; 強レーザー場; 運動量角度分布; 励起状態ダイナミクス; フェムト秒パルス; エタノール; 運動量分布カスプ; フラーレン

Time-resolved photoelectron spectroscopy is useful for probing the dynamics of a molecule that undergoes chemical reactions. To calculate the probability of intense-field-induced ionization or photoelectron spectrum of a time-evolving electronic state as a function of internuclear distances R, we combined wave packet propagation methods for bound electronic state dynamics, such as the time-dependent (TD) adiabatic state approach or the multiconfigurational TD Hartree-Fock method, with the intense-field many-body S-matrix theory. Our new approach was applied to H^+_2. The calculated ionization probability as a function of R is in good agreement with the exact one obtained by an accurate grid point method. Ionization of H: is greatly enhanced at a critical internuclear distance which is much longer than the equilibrium one (known as enhanced ionization). The angular distribution of the photoelectron momentum experimentally observed is reproduced as well. The distribution of the momentum perpendicular to the laser polarization direction has a sharp peak near zero momentum. The "cusp-like" distribution is due to excited state dynamics leading to ionization. We then calculated the photoelectron angular distribution of above-threshold ionization of H_2. We have also calculated the ionization probabilities of polyatomic molecules such as ethanol and water molecule to show that intramolecular electron dynamics is the key to understand the mechanism of enhanced ionization.

时间分辨光电子能谱可用于探测经历化学反应的分子的动力学。为了计算随时间演化的电子态的强场诱导电离或光电子能谱作为核间距离 R 的函数的概率，我们将束缚电子态动力学的波包传播方法（例如时间相关（TD）绝热态方法或多构型 TD Hartree-Fock 方法）与强场多体 S 矩阵理论相结合。我们的新方法应用于 H^+_2。计算出的电离概率作为 R 的函数与通过精确网格点法获得的精确电离概率非常一致。 H 的电离：在比平衡状态长得多的临界核间距离处大大增强（称为增强电离）。还再现了实验观察到的光电子动量的角分布。垂直于激光偏振方向的动量分布在接近零动量时有一个尖峰。 “尖点状”分布是由于激发态动力学导致电离。然后我们计算了 H_2 阈值以上电离的光电子角分布。我们还计算了乙醇和水分子等多原子分子的电离概率，表明分子内电子动力学是理解增强电离机制的关键。

项目成果

Control of π-electron Rotation in Chiral Aromatic Molecules by Nonhelical Laser Pulses

非螺旋激光脉冲控制手性芳香分子中的 π 电子旋转

• 发表时间: 2006
• 期刊: Angew. Chem. Int. Ed. 45(Reviewed)
• 作者: M. Kanno;et. al.
• 通讯作者: et. al.

Ab initio molecular dynamics and wavepacket dynamics of highly charged fullerene cations produced with intense near-infrared laser pulses

• DOI: 10.1016/j.chemphys.2007.04.011
• 发表时间: 2007-09
• 期刊: Chemical Physics
• 影响因子: 2.3
• 作者: K. Nakai;H. Kono;Y. Sato;N. Niitsu;Riadh Sahnoun;Motohiko Tanaka;Y. Fujimura

Time-dependent density functional theory investigation of electric field effects on absorption spectra of meso-meso-linked zinc porphyrin arrays : Role of charge-transfer states

电场对介观-介观连接的锌卟啉阵列吸收光谱影响的时间相关密度泛函理论研究：电荷转移态的作用

• 发表时间: 2005
• 期刊: Journal of Physical Chemistry B 109
• 作者: T.Uemure;S.Saito;Y.Mizutani;K.Tominaga;R.Sahnoun;K.Nakai
• 通讯作者: K.Nakai

Stability limit of highly charged C_<60> cations produced with an intense long-wavelength laser pulse : Calculation of electronic structures by DFT and wavepacket simulation

用强长波长激光脉冲产生的高电荷 C_<60> 阳离子的稳定性极限：通过 DFT 和波包模拟计算电子结构

• 发表时间: 2006
• 期刊: Chemical Physics Letters 430
• 作者: R.Sahnoun;K.Nakai;Y.Sato;H.Kono;Y.Fujimura;M.Tanaka
• 通讯作者: M.Tanaka

Incorporation of a wave packet propagation method into the S-matrix framework : Investigation of the effects of excited state dynamics on intense-field ionization.

将波包传播方法纳入 S 矩阵框架：研究激发态动力学对强场电离的影响。

• 发表时间: 2005
• 期刊: Physical Review A 72・3
• 作者: T.Yoshizawa;M.Mizoguchi;T.Iimori;et al.;Manabu Kanno
• 通讯作者: Manabu Kanno