Setting benchmarks for modelling gas-surface interactions using coherent control of rotational orientation states
Setting benchmarks for modelling gas-surface interactions using coherent control of rotational orientation states
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DOI：
10.1038/s41467-020-16930-1
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发表时间：
2020-06-19
影响因子：
16.6
通讯作者：
Alexandrowicz, Gil
中科院分区：
文献类型：
--
作者：
Alkoby, Yosef;Chadwick, Helen;Alexandrowicz, Gil
分子-表面碰撞过程中分子量子态的相干演化是迄今为止无法测量的相互作用势的详细描述。本文采用磁控分子束技术研究了旋转取向基态氢分子与氟化锂表面的碰撞。该技术的相干控制特性使我们能够测量旋转投影量子态的复振幅的变化，并使用散射矩阵形式表示它们。我们提取的量子态到态跃迁概率揭示了分子-表面相互作用对分子旋转方向的强烈依赖，并且碰撞翻转旋转方向的概率非常高。我们从实验数据中获得的散射矩阵为理论再现提供了一个超灵敏的基准，指导了H-2与固体表面相互作用的精确理论模型的发展。对分子-表面相互作用的基本和预测性理解是具有挑战性的。在这里，作者报告了一种实验技术，允许直接测量散射矩阵，它报告了分子从表面散射的量子态的相干演化。
The coherent evolution of a molecular quantum state during a molecule-surface collision is a detailed descriptor of the interaction potential which was so far inaccessible to measurements. Here we use a magnetically controlled molecular beam technique to study the collision of rotationally oriented ground state hydrogen molecules with a lithium fluoride surface. The coherent control nature of the technique allows us to measure the changes in the complex amplitudes of the rotational projection quantum states, and express them using a scattering matrix formalism. The quantum state-to-state transition probabilities we extract reveal a strong dependency of the molecule-surface interaction on the rotational orientation of the molecules, and a remarkably high probability of the collision flipping the rotational orientation. The scattering matrix we obtain from the experimental data delivers an ultra-sensitive benchmark for theory to reproduce, guiding the development of accurate theoretical models for the interaction of H-2 with a solid surface. A fundamental and predictive understanding of molecule-surface interactions is challenging to obtain. Here the authors report an experimental technique allowing direct measurement of the scattering matrix, which reports on the coherent evolution of quantum states of a molecule scattering from a surface.