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.

通过选择反应物内部量子态（特别是通过激光场）来控制化学过程的反应性是化学动力学的核心问题。在这个项目中，我们建议研究需要通用方法的两个不同系统：(i) 螺吡喃的开环，以及 (ii) H2O 在过渡金属表面上的解离化学吸附。光致变色是光诱导的可逆化学物质在具有不同吸收光谱的两种形式之间的转变。光致变色材料已引起许多工业应用，例如光开关、眼镜、光学存储器和非线性光学器件。 我们的目标是展示通过激光脉冲控制螺吡喃开环的可能性。这项研究将与实验人员密切合作进行。要解决的第二个问题是 H2O 在过渡金属表面上的解离化学吸附，产生化学吸附的 H 和 OH 物质。这是许多多相催化过程中重要且通常是必需的步骤，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