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Collisions, Ionization and Reactions Inside Helium Nanodroplets Close to Zero K

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Collisions, Ionization and Reactions Inside Helium Nanodroplets Close to Zero K Cold Physics and Chemistry: Collisions, Ionization and Reactions inside Helium Nanodroplets Close to Zero K. A. Mauracher1, O. Echt2, A.M. Ellis3, S. Yang3, D.K. Bohme4, J. Postler1, A. Kaiser1, S. Denifl1 and P. Scheier1,* 1Institut für Ionenphysik und Angewandte Physik, Leopold-Franzens-Universität Innsbruck, Technikerstr. 25, A-6020 Innsbruck, Austria 2Department of Physics, University of New Hampshire, Durham, USA 3Department of Chemistry, University of Leicester, University Road, Leicester LE1 7RH, United Kingdom 4Department of Chemistry, York University, Toronto, Ontario M3J 1P3, Canada *Corresponding author: [email protected] Contents Contents .................................................................................................................................................. 1 1 Introduction ..................................................................................................................................... 4 2 Formation and size distributions of helium nanodroplets .............................................................. 5 Mass spectra of pristine helium nanodroplets........................................................................ 8 3 Pickup of atoms and molecules (dopants) .................................................................................... 12 Collision dynamics in helium nanodroplets ........................................................................... 13 Growth of unusual structures ............................................................................................... 14 Multicenter growth of metallic nanoclusters ........................................................................ 15 Core-shell nanoclusters ......................................................................................................... 16 Growth on the edge of helium nanodroplets ....................................................................... 16 Growth of large clusters ........................................................................................................ 17 Manipulation of dopants ....................................................................................................... 18 4 Nanoparticles and nanowires ........................................................................................................ 18 Large helium nanodroplets ................................................................................................... 18 Soft Landing ........................................................................................................................... 19 Deposition experiments: metallic nanoparticles................................................................... 20 Deposition experiments: nanowires and vortices ................................................................. 23 5 Ionization of pure helium nanodroplets........................................................................................ 26 Charge localization and transport in a helium nanodroplet ................................................. 26 Formation of a strongly bound ionic core ............................................................................. 27 1 + Threshold energies of small Hen ions ................................................................................... 28 The possibility of multiple ionization of helium nanodroplets via free electrons ................. 30 Photoionization of undoped helium nanodroplets ............................................................... 31 + The special behavior of He4 .................................................................................................. 32 6 Helium anions ................................................................................................................................ 32 Negatively charged helium nanodroplets ............................................................................. 32 Atomic and molecular helium anions in helium nanodroplets ............................................. 33 Quantum chemical considerations of anionic helium species .............................................. 35 6.3.1 Formation of anionic species ......................................................................................... 35 6.3.2 Anionic species in helium nanodroplets, the ratio .................................................... 36 The importance of helium anions in helium nanodroplets ................................................... 38 6.4.1 Single charge transfer from He* to dopants ................................................................ 38 6.4.2 Double charge transfer from He* to dopants .............................................................. 39 6.4.3 He+ subthreshold formation via He* ............................................................................ 40 6.4.4 Multiple ionization events via He*............................................................................... 40 7 Ionization of doped helium nanodroplets ..................................................................................... 41 Charge transfer from He+ ...................................................................................................... 41 Penning ionization ................................................................................................................. 42 Magic numbers in positively charged dopant cluster distributions ...................................... 45 Photoionization of doped helium nanodroplets ................................................................... 46 Multiple-ionization of dopants .............................................................................................. 47 Sequential Penning ionization ............................................................................................... 51 8 Solvation of ions in helium nanodroplets ...................................................................................... 52 Size and structure of snowballs ............................................................................................. 52 Solvation dynamics ................................................................................................................ 57 9 Anions from doped HNDs .............................................................................................................. 59 Electron attachment to the nucelobases thymine and adenine ........................................... 61 Electron attachment to TNT and nitromethane .................................................................... 64 Anions formed upon electron attachment to chloroform in He droplets ............................ 65 Dissociative electron attachment to acetic and amino acids ................................................ 68 Anions formed upon electron attachment to water clusters in He droplets ........................ 68 High resolution electron attachment to carbon dioxide clusters in HNDs ........................... 70 10 Chemical reactions .................................................................................................................... 72 Neutral reactions ................................................................................................................... 72 Intra-droplet and intra-cluster ion-molecule reactions ........................................................ 75 10.2.1 Ionization initiated by electron and dissociative electron transfer to He+.................... 75 2 10.2.2 Dynamics of ionization initiated by electron and dissociative electron transfer to He+ 76 10.2.3 “Self” and “mixed” ion-molecule reactions: experimental strategies .......................... 77 10.2.4 Intra-cluster reactions with H2, CH4 ............................................................................... 78 10.2.5 Intra-cluster reactions of alcohols ................................................................................. 80 10.2.6 Intra-cluster reactions with co-embedded dopants: C60/ H2O and C60/NH3 .................. 81 10.2.7 Intra-cluster reactions with co-embedded Na and SF6: self-assembly of salt nanocrystals ................................................................................................................................... 82 10.2.8 Reactions of He* with fullerenes: formation of multiply-charged ions and ion/ion reactions with cations. .................................................................................................................. 82 11 Spectroscopic investigations of highly reactive molecules, clusters and ions .......................... 83 Free radicals .......................................................................................................................... 83 Clusters and complexes ......................................................................................................... 85 11.2.1 Molecular clusters ......................................................................................................... 85 11.2.2 Molecular complexes .................................................................................................... 87 11.2.3 Molecular ions ............................................................................................................... 90 12 Adsorption on fullerenes and fullerene aggregates .................................................................. 93 Adsorption on C60 and C70 .....................................................................................................
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