Iablonskyi D, Nagaya K, Fukuzawa H, Motomura K, Kumagai Y, Mondal S, Tachibana T, Takanashi T, Nishiyama T, Matsunami K, Johnsson P, Piseri P, Sansone G, Dubrouil A, Reduzzi M, Carpeggiani P, Vozzi C, Devetta M, Negro M, Calegari F, Trabattoni A, Castrovilli M C, Faccialà D, Ovcharenko Y, Möller T, Mudrich M, Stienkemeier F, Coreno M, Alagia M, Schütte B, Berrah N, Kuleff A I, Jabbari G, Callegari C, Plekan O, Finetti P, Spezzani C, Ferrari E, Allaria E, Penco G, Serpico C, De Ninno G, Nikolov I, Diviacco B, Di Mitri S, Giannessi L, Prince K C, Ueda K
Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 980-8577 Sendai, Japan.
Department of Physics, Graduate School of Science, Kyoto University, 606-8502 Kyoto, Japan.
Phys Rev Lett. 2016 Dec 30;117(27):276806. doi: 10.1103/PhysRevLett.117.276806.
Ne clusters (∼5000 atoms) were resonantly excited (2p→3s) by intense free electron laser (FEL) radiation at FERMI. Such multiply excited clusters can decay nonradiatively via energy exchange between at least two neighboring excited atoms. Benefiting from the precise tunability and narrow bandwidth of seeded FEL radiation, specific sites of the Ne clusters were probed. We found that the relaxation of cluster surface atoms proceeds via a sequence of interatomic or intermolecular Coulombic decay (ICD) processes while ICD of bulk atoms is additionally affected by the surrounding excited medium via inelastic electron scattering. For both cases, cluster excitations relax to atomic states prior to ICD, showing that this kind of ICD is rather slow (picosecond range). Controlling the average number of excitations per cluster via the FEL intensity allows a coarse tuning of the ICD rate.
在费米实验室,氖团簇(约5000个原子)被强自由电子激光(FEL)辐射共振激发(2p→3s)。这种多重激发的团簇可以通过至少两个相邻激发原子之间的能量交换进行无辐射衰变。受益于种子FEL辐射的精确可调谐性和窄带宽,对氖团簇的特定位置进行了探测。我们发现,团簇表面原子的弛豫通过一系列原子间或分子间库仑衰变(ICD)过程进行,而体原子的ICD还会受到周围激发介质通过非弹性电子散射的影响。对于这两种情况,团簇激发在ICD之前弛豫到原子态,这表明这种ICD相当缓慢(皮秒范围)。通过FEL强度控制每个团簇的平均激发数,可以对ICD速率进行粗略调节。