A comprehensive study of Interatomic Coulombic Decay in argon dimers: Extracting R-dependent absolute decay rates from the experiment

Abstract

In this work we present a comprehensive and detailed study of Interatomic Coulombic Decay (ICD) occurring after irradiating argon dimers with XUV-synchrotron radiation. A manifold of different decay channels is observed and the corresponding initial and final states are assigned.Additionally, the effect of nuclear dynamics on the ICD electron spectrum is examined for one specific decay channel. The internuclear distance-dependent width Γ(R) of the decay is obtained from the measured energy distribution employing a classical nuclear dynamics model.

Using principal component analysis for neural network high-dimensional potential energy surface

“…Their work, as well as others, could undoubtedly demonstrate that ICD represents an important contribution to the relaxation of excited Ar 2 . [12][13][14][15][16][17][18][19] A resonant process of energy-transfer in Ar 2 , which happens below the energy threshold for ICD, has been reported by Mizuno et al 20 Therefore, a 3s −1 hole created by photoionization is filled by a 3p electron at the same site while the released energy is transferred to the neutral neighbor, which, in turn, becomes electronically excited, but not ionized like in ICD.…”

Tracing charge transfer in argon dimers by XUV-pump IR-probe experiments at FLASH

“…Their work, as well as others, could undoubtedly demonstrate that ICD represents an The Journal of Chemical Physics ARTICLE scitation.org/journal/jcp important contribution to the relaxation of excited Ar 2 . [12][13][14][15][16][17][18][19] A resonant process of energy-transfer in Ar 2 , which happens below the energy threshold for ICD, has been reported by Mizuno et al 20 Therefore, a 3s −1 hole created by photoionization is filled by a 3p electron at the same site while the released energy is transferred to the neutral neighbor, which, in turn, becomes electronically excited, but not ionized like in ICD. Besides mechanisms that involve only transfer of energy, excited Ar 2 may also relax via pathways which in addition comprise charge transfer (CT) from one site to its neighbor.…”

Interatomic and Intermolecular Coulombic Decay

“…Early experiments on ICD using the COLTRIMS technique can be found, for example, in refs ( 2 , 8 , 15 , 16 , 29 , 57 , 58 , 60 , 187 − 189 , 198 , 215 , and 296 − 303 ); later work in refs ( 23 , 28 , 196 , 203 , 205 , 245 , 247 , 248 , and 304 − 315 ); and most recent work in refs ( 54 , 107 , 192 , 201 , 249 , 250 , 259 , and 316 − 324 )…”

“… 198 The time-dependent theory for nuclear wave packet dynamics was also applied in refs ( 199 ) and ( 200 ) to compute electron and KER spectra of ICD after resonant Auger decay in Ar 2 and ArKr, and theoretical predictions of those works on Ar dimers were later verified in independent experiments. 201 , 202 …”

“…A single decay channel of NeAr dimers was examined and the KER of the transition Ne( 2+ (2 s –1 2 p –11 P )Ar to Ne 2+ (2 p –21 D )–Ar + (3 p –1 )) was used such that by adapting Γ( R ) the theoretical results matched the distribution obtained in the experiment. 196 Rist and co-workers 201 examined experimentally shakeup-induced ICD of Ar 2 and identified a decay channel which turned out to be suitable for a direct extraction of Γ( R ) from the measured data without the need of any theoretical modeling. Although the extraction procedure treated the decay incoherently, the coherent treatment by full theoretical modeling yielded matching results.…”