Departament ECM, Facultat de Física and IN2UB, Universitat de Barcelona, Diagonal 645, 08028 Barcelona, Spain.
Phys Chem Chem Phys. 2013 Nov 14;15(42):18388-400. doi: 10.1039/c3cp52221k.
The dynamics following the photoexcitation of Ag atoms in (4)He nanodroplets via the 5p (2)P1/2 ← 5s (2)S1/2 and 5p (2)P3/2 ← 5s (2)S1/2 transitions has been investigated in a joint experimental and theoretical effort. It has been experimentally found that upon excitation to the (2)P1/2 state, the Ag atoms are ejected with a speed distribution peaking at about 55 m s(-1). When Ag is excited to the (2)P3/2 state, a rich phenomenology is found. While a fraction of the impurities remains solvated, the impurities that are ejected from the droplets either as Ag or AgHe have speed distributions similar, but not identical, to those found for excitation to the (2)P1/2 state. The experimental findings are qualitatively analyzed within a three-dimensional, time-dependent density functional approach for the helium droplet. The dynamics of the Ag-(4)He1000 system has been followed for several tens of picoseconds, long enough to observe AgHe exciplex formation and the departure of the photoexcited Ag atom from the helium droplet.
通过 5p (2)P1/2 ← 5s (2)S1/2 和 5p (2)P3/2 ← 5s (2)S1/2 跃迁,研究了(4)He 纳米液滴中 Ag 原子光激发后的动力学。实验发现,当激发到(2)P1/2 态时,Ag 原子以约 55 m s(-1)的速度分布被逐出。当 Ag 被激发到(2)P3/2 态时,会发现丰富的现象。虽然一部分杂质仍然被溶剂化,但从液滴中逐出的杂质无论是 Ag 还是 AgHe,其速度分布与激发到(2)P1/2 态时相似,但不完全相同。实验结果通过氦液滴的三维时变密度泛函方法进行了定性分析。对 Ag-(4)He1000 体系进行了几十皮秒的动力学跟踪,足以观察到 AgHe 激基复合物的形成和光激发的 Ag 原子从氦液滴中逸出。