Hartweg Sebastian, Yoder Bruce L, Garcia Gustavo A, Nahon Laurent, Signorell Ruth
Department of Chemistry and Applied Biosciences, Laboratory of Physical Chemistry, ETH Zürich, Vladimir-Prelog-Weg 2, CH-8093 Zürich, Switzerland.
Synchrotron SOLEIL, L'Orme des Merisiers, Saint Aubin BP 48, 91192 Gif sur Yvette, France.
Phys Rev Lett. 2017 Mar 10;118(10):103402. doi: 10.1103/PhysRevLett.118.103402.
We report the first measurements of size-resolved photoelectron angular distributions for the valence orbitals of neutral water clusters with up to 20 molecules. A systematic decrease of the photoelectron anisotropy is found for clusters with up to 5-6 molecules, and most remarkably, convergence of the anisotropy for larger clusters. We suggest the latter to be the result of a local short-range scattering potential that is fully described by a unit of 5-6 molecules. The cluster data and a detailed electron scattering model are used to predict the anisotropy of slow photoelectrons in liquid water. Reasonable agreement with experimental liquid jet data is found.
我们报告了对包含多达20个分子的中性水团簇价轨道的尺寸分辨光电子角分布的首次测量。对于包含多达5 - 6个分子的团簇,发现光电子各向异性有系统地降低,最显著的是,较大团簇的各向异性趋于收敛。我们认为后者是由一个由5 - 6个分子组成的单元完全描述的局部短程散射势导致的。利用团簇数据和详细的电子散射模型来预测液态水中慢光电子的各向异性。发现与实验液体射流数据有合理的一致性。