Ang Xu, Yujie Ma, Dong Yan, Fangfang Li, Fei Song, Ti Zhou, Zihan Yuan, Xiyu Liu, Jiaxing Liu, Fengyan Wang
{"title":"通过与稀有气体原子的高能量碰撞对钇的自旋轨道激发进行成像。","authors":"Ang Xu, Yujie Ma, Dong Yan, Fangfang Li, Fei Song, Ti Zhou, Zihan Yuan, Xiyu Liu, Jiaxing Liu, Fengyan Wang","doi":"10.1021/acs.jpclett.4c01924","DOIUrl":null,"url":null,"abstract":"<p><p>The energy required for spin-orbit excitation plays a critical role in understanding translational-to-electronic energy conversion, particularly in chemical reactions involving changes in spin states. This is particularly important for transition metal atoms possessing <i>d</i>-orbitals, which result in multiple spin-orbit split energy levels at low energies. The accurate identification and characterization of spin-orbit transitions in such species require advanced experimental techniques and theoretical support. In this study, the spin-orbit excited collisions of Y(<sup>2</sup>D<sub>3/2</sub>) with rare gas atoms Ne, Ar, and Kr leading to Y(<sup>2</sup>D<sub>5/2</sub>) were observed using laser-ablated crossed-beam and time-sliced ion velocity mapping imaging techniques. Through a comparison of the forward angular distributions of Y(<sup>2</sup>D<sub>3/2</sub>) to the backward and sideway scattering distributions of Y(<sup>2</sup>D<sub>5/2</sub>) from elastic and inelastic collisions of Y(<sup>2</sup>D) with rare gas atoms, this study reveals that the spin-orbit electronic excitation occurs with high collision energy and low impact parameters from backward and sideway collisions. The effectiveness of the spin-orbit excitation process is strongly dependent on the collision energy or temperature, suggesting that energy requirements of the process have to be considered in chemical reactions involving changes in spin states.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"8721-8727"},"PeriodicalIF":4.6000,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Imaging Spin-Orbit Excitation of Yttrium through High-Energy Collisions with Rare Gas Atoms.\",\"authors\":\"Ang Xu, Yujie Ma, Dong Yan, Fangfang Li, Fei Song, Ti Zhou, Zihan Yuan, Xiyu Liu, Jiaxing Liu, Fengyan Wang\",\"doi\":\"10.1021/acs.jpclett.4c01924\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>The energy required for spin-orbit excitation plays a critical role in understanding translational-to-electronic energy conversion, particularly in chemical reactions involving changes in spin states. This is particularly important for transition metal atoms possessing <i>d</i>-orbitals, which result in multiple spin-orbit split energy levels at low energies. The accurate identification and characterization of spin-orbit transitions in such species require advanced experimental techniques and theoretical support. In this study, the spin-orbit excited collisions of Y(<sup>2</sup>D<sub>3/2</sub>) with rare gas atoms Ne, Ar, and Kr leading to Y(<sup>2</sup>D<sub>5/2</sub>) were observed using laser-ablated crossed-beam and time-sliced ion velocity mapping imaging techniques. Through a comparison of the forward angular distributions of Y(<sup>2</sup>D<sub>3/2</sub>) to the backward and sideway scattering distributions of Y(<sup>2</sup>D<sub>5/2</sub>) from elastic and inelastic collisions of Y(<sup>2</sup>D) with rare gas atoms, this study reveals that the spin-orbit electronic excitation occurs with high collision energy and low impact parameters from backward and sideway collisions. The effectiveness of the spin-orbit excitation process is strongly dependent on the collision energy or temperature, suggesting that energy requirements of the process have to be considered in chemical reactions involving changes in spin states.</p>\",\"PeriodicalId\":62,\"journal\":{\"name\":\"The Journal of Physical Chemistry Letters\",\"volume\":\" \",\"pages\":\"8721-8727\"},\"PeriodicalIF\":4.6000,\"publicationDate\":\"2024-08-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry Letters\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.jpclett.4c01924\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/8/20 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry Letters","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpclett.4c01924","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/8/20 0:00:00","PubModel":"Epub","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
自旋轨道激发所需的能量对于理解平移到电子的能量转换起着至关重要的作用,尤其是在涉及自旋状态变化的化学反应中。这对于拥有 d 轨道的过渡金属原子尤为重要,因为 d 轨道会在低能量时产生多个自旋轨道分裂能级。要准确识别和表征此类物质的自旋轨道跃迁,需要先进的实验技术和理论支持。在这项研究中,利用激光照射交叉光束和时间切片离子速度映射成像技术,观察了 Y(2D3/2)与稀有气体原子 Ne、Ar 和 Kr 的自旋轨道激发碰撞导致的 Y(2D5/2)。通过比较 Y(2D)与稀有气体原子的弹性和非弹性碰撞产生的 Y(2D3/2)前向角分布与 Y(2D5/2)后向和侧向散射分布,该研究揭示了后向和侧向碰撞产生的自旋轨道电子激发具有碰撞能量高、碰撞参数低的特点。自旋轨道激发过程的有效性与碰撞能量或温度密切相关,这表明在涉及自旋态变化的化学反应中必须考虑该过程的能量要求。
Imaging Spin-Orbit Excitation of Yttrium through High-Energy Collisions with Rare Gas Atoms.
The energy required for spin-orbit excitation plays a critical role in understanding translational-to-electronic energy conversion, particularly in chemical reactions involving changes in spin states. This is particularly important for transition metal atoms possessing d-orbitals, which result in multiple spin-orbit split energy levels at low energies. The accurate identification and characterization of spin-orbit transitions in such species require advanced experimental techniques and theoretical support. In this study, the spin-orbit excited collisions of Y(2D3/2) with rare gas atoms Ne, Ar, and Kr leading to Y(2D5/2) were observed using laser-ablated crossed-beam and time-sliced ion velocity mapping imaging techniques. Through a comparison of the forward angular distributions of Y(2D3/2) to the backward and sideway scattering distributions of Y(2D5/2) from elastic and inelastic collisions of Y(2D) with rare gas atoms, this study reveals that the spin-orbit electronic excitation occurs with high collision energy and low impact parameters from backward and sideway collisions. The effectiveness of the spin-orbit excitation process is strongly dependent on the collision energy or temperature, suggesting that energy requirements of the process have to be considered in chemical reactions involving changes in spin states.
期刊介绍:
The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.