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Time-resolved measurement of interatomic Coulombic decay induced by two-photon double excitation of Ne2

The hitherto unexplored two-photon doubly excited states [Ne*(2p−13s)]2 were experimentally identified using the seeded, fully coherent, intense extreme ultraviolet free-electron laser FERMI. These states undergo ultrafast interatomic Coulombic decay (ICD), which predominantly produces singly ionized dimers.  T. Takanashi et al. Physical Review Letters, Vol. 118 - 3, pp. 033202 (2017)

Stimulated by the developments of XUV FELs, a new class of ICD (Interatomic or intermolecular Coulombic decay) processes in multiply excited clusters was recently predicted theoretically. In these processes, transfer of the de-excitation energy from one of the excited atoms in a cluster results in the ionization of another excited atom. This mechanism plays a central role in the creation of ions when clusters are exposed to moderate-intensity laser pulses of photon energies insufficient for a single-photon ionization. Recently, such a process was indirectly observed in helium droplets. At the same time, ab initio dynamical calculations propose an efficient scheme for production of the doubly excited Ne dimers by a single intense XUV pulse and predict respective ICD rates and electron spectra.
In this work, by using the fully coherent XUV pulses from the seeded free-electron laser FERMI, we have unambiguously identified the two-photon doubly excited [Ne(2p13s)]2 states of the Ne dimer. The presently realized pump-probe scheme enabled direct access to the time evolution of ICD of these states. In particular, measuring the yield of Ne+2 ions as a function of time delay between the pump XUV and probe UV pulses, we were able to determine the corresponding ICD transition rates (lifetimes). The experimental lifetimes of the short- and long-lived doubly excited states [Ne(2p13s)]2, obtained with the help of the model dynamical calculations, are in good agreement with the previously reported ab initio values. We believe that the presently realized scheme involving the XUV FEL pump and femtosecond UV probe pulses may become a powerful tool for future real-time dynamical investigations of ultrafast relaxation processes of excited systems and mechanisms of energy and charge transfer in media.
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Time-resolved measurement of interatomic Coulombic decay induced by two-photon double excitation of Ne2
Takanashi Tsukasa, Golubev N.V., Callegari Carlo, Fukuzawa Hironobu, Motomura Koji, Iablonskyi Denys, Kumagai Yoshiaki, Mondal Subhendu, Tachibana Tetsuya, Nagaya Kiyonobu, Nishiyama Toshiyuki, Matsunami K., Johnsson Per, Piseri Paolo, Sansone Giuseppe, Dubrouil Antoine, Reduzzi Maurizio, Carpeggiani Paolo Antonio, Vozzi Caterina, Devetta Michele, Negro Matteo, Faccialà Davide, Calegari Francesca, Trabattoni Andrea, Castrovilli Mattea Carmen, Ovcharenko Yevheniy, Mudrich Marcel, Stienkemeier Frank, Coreno Marcello, Alagia Michele, Schütte Bernd, Berrah Nora, Plekan Oksana, Finetti Paola, Spezzani Carlo, Ferrari Eugenio, Allaria Enrico, Penco Giuseppe, Serpico Claudio, De Ninno Giovanni, Diviacco Bruno, Di Mitri Simone, Giannessi Luca, Jabbari G., Prince Kevin Charles, Cederbaum Lorenz S., Demekhin Philipp, Kuleff Alexander, Ueda Kiyoshi. Physical Review Letters, Vol. 118 - 3, pp. 033202 (2017)
doi: 10.1103/PhysRevLett.118.033202
Last Updated on Thursday, 13 April 2017 12:32