Barnes Jonathan V, Borgeaud Dit Avocat Dominique P, Simmen Edith, Yang Huanyu, Yoder Bruce L, Signorell Ruth
Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 2, Zürich 8093, Switzerland.
J Phys Chem A. 2023 Oct 19;127(41):8544-8555. doi: 10.1021/acs.jpca.3c03820. Epub 2023 Oct 5.
Using a pulsed Stern-Gerlach deflection experiment, we present the results of a comparative study on the magnetic properties of neutral sodium-doped solvent clusters Na(Sol) with = 1-4 (Sol: HO, NH, CHOH, CHOCH). Experimental deflection ratios are compared with values calculated from molecular dynamics simulations. NaNH and NaHO are deflected as a spin 1/2 system, consistent with spin transitions occurring on a time scale significantly longer than 100 μs. For all other clusters, reduced deflection is observed. The observed magnetic deflection behavior is correlated to the number of thermally populated rotational states in the clusters. We discuss that spin-rotational couplings allow for avoided crossings and a reduction in the effective magnetic moment of the cluster. This work attempts to understand the evolution of magnetic properties in isolated weakly bound clusters and is relevant to diamagnetic and paramagnetic species expected to exist in solvated electron systems.
通过脉冲斯特恩-盖拉赫偏转实验，我们展示了对中性钠掺杂溶剂团簇Na(Sol)（Sol = HO、NH、CHOH、CH OCH）磁性的比较研究结果。将实验偏转率与分子动力学模拟计算的值进行了比较。NaNH和NaHO作为自旋1/2系统发生偏转，这与在明显长于100 μs的时间尺度上发生的自旋跃迁一致。对于所有其他团簇，观察到偏转减小。观察到的磁偏转行为与团簇中热占据的转动状态数相关。我们讨论了自旋-转动耦合允许避免交叉并降低团簇的有效磁矩。这项工作试图理解孤立弱束缚团簇中磁性的演变，并且与预计存在于溶剂化电子系统中的抗磁性和顺磁性物种相关。
