Photoinduced nonadiabatic dynamics in quartet Na3 and K3 formed using helium nanodroplet isolation
Photoinduced nonadiabatic dynamics in quartet Na3 and K3 formed using helium nanodroplet isolation
复制标题
使用氦纳米液滴隔离形成的四重奏 Na3 和 K3 中的光诱导非绝热动力学
DOI：
10.1063/1.1418248
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发表时间：
2001
影响因子：
4.4
通讯作者：
M. Gutowski
中科院分区：
文献类型：
--
作者：
J. Reho;J. Higgins;M. Nooijen;K. Lehmann;G. Scoles;M. Gutowski
氦纳米液滴分离用于产生货车德瓦尔斯结合的四重态碱金属三聚体（Na 3和K 3），其选择性超过相应的化学结合的双重三聚体。频率分辨的激发和发射光谱揭示了非绝热自旋翻转过程中的电子激发态的存在。共观察到4个四重态到四重态的电子跃迁：Na 3的24 E ′，1 4 E <$1 4A 2 ′跃迁和 K3的14A 1 ″，2 4 E ′ <$1 4A 2 ′跃迁. 时间分辨光谱表明，Na 3中的系间穿越时间从0-0带激发后的1.4 ns降低到较高电子振动能级（3，5/2）的约400 ps。共振四重荧光的分析表明，激发的电子态振动冷却的时间尺度上，是可比的，但比，系统间的交叉时间慢。
Helium nanodroplet isolation is used to produce van der Waals-bound quartet state alkali trimers (Na3 and K3) selectively over the corresponding chemically bound doublet trimers. Frequency-resolved excitation and emission spectroscopy reveals the presence of nonadiabatic spin–flip processes in the electronically excited states. A total of four quartet to quartet electronic transitions are observed: the 2 4E′,1 4E←1 4A2′ transitions of Na3 and the 1 4A1″,2 4E′←1 4A2′ transitions of K3. Time-resolved spectroscopy reveals that intersystem crossing times in Na3 decrease from 1.4 ns after excitation of the 0–0 band to approximately 400 ps for the higher vibronic levels (3,5/2). Analysis of the resonant quartet fluorescence reveals that the excited electronic state cools vibrationally on a time scale that is comparable to, but slower than, the intersystem crossing time.