Quantum control of molecular systems: application to conical intersections and to heterogeneous catalysis

分子系统的量子控制：在锥形交叉点和多相催化中的应用

• 批准号: 256572202
• 负责人: Professor Dr. Hans-Dieter Meyer
• 金额: --
• 依托单位: Institut des Sciences Moléculaires dOrsay - UMR 8214
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2014
• 资助国家: 德国
• 起止时间: 2013-12-31 至 2016-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/256572202?language=en
• 关键词: Quantum; control; molecular; systems; application

Controlling reactivity of a chemical process by selecting reactant internal quantum states, particularly by laser fields, is a central question in chemical dynamics. In this project, we propose the study of two different systems which require a common methodology: (i) the ring-openig of spiropyran, and (ii) the dissociative chemisorption of H2O on transition-metal surfaces.Photochromism is the light-induced reversible transformation of a chemical species between two forms with different absorption spectra. Photochromic materials have given rise to many industrial applications such as optical switches, ophthalmic glasses, optical memories, and non-linear optical devices. Our goal is to show the possibility of controling the ring-opening of spiropyran by laser pulses. The research will be done in close collaboration with experimentalists.The second problem to tackle is the dissociative chemisorption of H2O on transition-metal surfaces, producing chemisorbed H and OH species. This is an important and often obligatory step in many heterogeneous catalytic processes, such as the water-gas shift (WGS) reaction or steam reforming.

通过选择反应物的内部量子态来控制化学过程的反应性，特别是通过激光场来控制，是化学动力学中的一个中心问题。在这个项目中，我们提出了两个不同的系统，需要一个共同的方法来研究：（i）螺吡喃的开环，和（ii）解离化学吸附的H2O过渡金属表面。光致变色是光诱导的两种形式之间的可逆转变具有不同的吸收光谱。光致变色材料已经引起了许多工业应用，诸如光学开关、眼科眼镜、光学存储器和非线性光学器件。 我们的目标是展示用激光脉冲控制螺吡喃开环的可能性。第二个要解决的问题是H2O在过渡金属表面的解离化学吸附，产生化学吸附的H和OH物种。这是许多非均相催化过程中的重要且通常是强制性的步骤，例如水煤气变换（WGS）反应或蒸汽重整。

项目成果

Towards a systematic convergence of Multi-Layer (ML) Multi-Configuration Time-Dependent Hartree nuclear wavefunctions: The ML-spawning algorithm

实现多层 (ML) 多配置瞬态 Hartree 核波函数的系统收敛：ML 生成算法

• DOI: 10.1016/j.chemphys.2016.08.031
• 发表时间: 2016
• 期刊: Chemical Physics
• 影响因子: 2.3
• 作者: D. Mendive-Tapia;T. Firmino;H.-D. Meyer;F. Gatti
• 通讯作者: F. Gatti

Rovibrational spectroscopy using a kinetic energy operator in Eckart frame and the multi-configuration time-dependent Hartree (MCTDH) approach.

使用 Eckart 框架中的动能算子和多配置时间相关 Hartree (MCTDH) 方法的旋转振动光谱

• DOI: 10.1063/1.4895557
• 发表时间: 2014
• 期刊: The Journal of chemical physics
• 作者: K. Sadri;D. Lauvergnat;F. Gatti;H.-D. Meyer
• 通讯作者: H.-D. Meyer

A generalised vibronic-coupling Hamiltonian model for benzopyran.

苯并吡喃的广义振动耦合哈密顿模型

• DOI: 10.1063/1.4861226
• 发表时间: 2014
• 期刊: The Journal of chemical physics
• 作者: L. Joubert-Doriol;B. Lasorne;D. Lauvergnat;H.-D. Meyer;F. Gatti
• 通讯作者: F. Gatti

Resonances of HCO Computed Using an Approach Based on the Multiconfiguration Time-Dependent Hartree Method.

• DOI: 10.1021/acs.jpca.5b04642
• 发表时间: 2015-06
• 期刊: The journal of physical chemistry. A
• 作者: S. Ndengué;R. Dawes;F. Gatti;H. Meyer

Atom-triatom rigid rotor inelastic scattering with the MultiConfiguration Time Dependent Hartree approach

• DOI: 10.1016/j.cplett.2016.12.012
• 发表时间: 2017-01
• 期刊: Chemical Physics Letters
• 影响因子: 2.8
• 作者: S. Ndengué;R. Dawes;F. Gatti;H. Meyer