Photodissociation dynamics of ionic argon pentamer

Abstract

Photodissociation of the ionized argon pentamer, Ar + 5 , is studied using an extended diatomicsin-molecules interaction model with the inclusion of the spin-orbit coupling and various dynamical approaches. A thorough comparison with the experimental data available in the literature is presented, including photofragment abundances and their kinetic and internal energy distributions.New predictions are reported for ultra-violet photoexcitation energies, a range that has not been studied before either experimentally or theoretically.

Electron diffraction as a structure tool for charged and neutral nanoclusters formed in superfluid helium droplets

“…We note here that our work on Ar N + is the first experimental report on the structures of Ar clusters. The dissociative nature of the cluster 89,100–102 and the lack of high resolution spectral features 82,84,89 make ED perhaps the only choice in this case.…”

Non-adiabatic dynamics combining Ehrenfest, decoherence, and multiscale approaches applied to ionic rare-gas clusters photodissociation, post-ionization fragmentation, and collisions

“…Note also that alternative names like hemiquantal method [14,16,22,23,24,25,26,27] and semiclassical method [19,28,29,20,30,21,31] were also used in our previous studies.…”

Photodissociation of medium-sized argon cluster cations in the visible region

“…In the specific case of rare-gas cluster cations, it means that partial charges may be produced on separate fragments. Nevertheless, previous simulations on small rare-gas cluster cations [27][28][29]38 have clearly shown that realistic predictions can be obtained even if a purely mean-field method is employed provided heavily averaged quantities are considered (fragments abundance, mean kinetic energy released, etc.) and if partial charges are properly treated as quantum probabilities that the positive charge resides on a particular fragment.…”

“…A lot of experiments were performed at that time focusing on their photoabsorption spectrum over a broad range of photon energies and cluster sizes [2][3][4] as well as subsequent, post-absorption dynamics. 2,[4][5][6][7][8][9][10][11][12][13][14][15][16][17][18] Up to now, however, calculations on the rare-gas cluster cation photodynamics have not exceeded the smallest cluster sizes [19][20][21][22][23][24][25][26][27][28][29] or very short simulation times. 30,31 As a consequence, most of the experimental photodissociation data obtained for Ar N + clusters have still been waiting for their appropriate theoretical interpretation even though simple and computationally cheap interaction models based on the diatomics-in-molecules approach (DIM) 32 exist for Ar N +33 (and also for other rare gases 1,33 ) for quite a long time.…”

“…28 Thirdly, though the DIM approach is an inherently pairwise additive, the most significant three-body contributions (induced dipole -induced dipole interactions and dispersion three-body forces) can also be easily taken into account. 1,37 It is the main intention of the present paper to extend the preceding calculations on the photodissociation dynamics of small Ar N + (typically with N r 5) [19][20][21][22][23][24][25][26][27][28][29] or extremely short-time simulations 30,31 is considered here since most of the experimental photodissociation data have been published for Ar N + for this photon energy or for energies from a close vicinity. The main focus of the present study is on the sizes, abundance and stability of photofragments, and short-time fragmentation kinetics.…”