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Lawrence Berkeley National Laboratory Recent Work Lawrence Berkeley National Laboratory Recent Work Title Photoionization and photofragmentation of singly charged positive and negative Sc3 N@ C80 endohedral fullerene ions Permalink https://escholarship.org/uc/item/0b15m4tn Journal Physical Review A, 99(6) ISSN 2469-9926 Authors Müller, A Martins, M Kilcoyne, ALD et al. Publication Date 2019-06-03 DOI 10.1103/PhysRevA.99.063401 Peer reviewed eScholarship.org Powered by the California Digital Library University of California 1 Photoionization and photofragmentation of singly charged positive and negative 2 Sc3N@C80 endohedral fullerene ions 1, ∗ 2 3 4 1 5 5 6 3 A. M¨uller, M. Martins, A. L. D. Kilcoyne, R. A. Phaneuf, J. Hellhund, A. Borovik Jr., K. Holste, S. Bari, 5 6 5 2 7 6 5 4 T. Buhr, S. Klumpp, A. Perry-Sassmannshausen, S. Reinwardt, S. Ricz, K. Schubert, and S. Schippers 1 5 Institut f¨urAtom- und Molek¨ulphysik,Justus-Liebig-Universit¨atGießen, 6 Leihgesterner Weg 217, 35392 Giessen, Germany 2 7 Institut f¨urExperimentalphysik, Universit¨atHamburg, 8 Luruper Chaussee 149, 22761 Hamburg, Germany 3 9 Advanced Light Source, Lawrence Berkeley National Laboratory, 10 1 Cyclotron Road, M.S. 7R0222, Berkeley, CA 94720-8229, USA 4 11 Department of Physics, University of Nevada, Reno, NV 89557-0058, USA 5 12 I. Physikalisches Institut, Justus-Liebig-Universit¨atGießen, 13 Heinrich-Buff-Ring 16, 35392 Giessen, Germany 6 14 Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg, Germany 7 15 Institute for Nuclear Research, Hungarian Academy of Sciences, P.O. Box 51, 4001 Debrecen, Hungary 16 (Dated: April 6, 2019) + − Photoprocesses of the endohedral fullerene ions Sc3N@C80 and Sc3N@C80 in the gas phase have been investigated in the photon energy ranges 30 - 50 eV and 280 - 420 eV. Single and double ionization as well as single ionization accompanied by the release of a C2 dimer were observed as a function of the photon energy for the positive parent ion and double detachment was measured for the negative parent ion. The emphasis of the experiments was on the specific effects of the encapsulated trimetallic nitride cluster Sc3N on the observed reactions. Clear evidence of photoexcitation near the Sc L edge is obtained with the dominating contributions visible in the one- and two-electron-removal channels. K-vacancy production in the encapsulated central nitrogen atom is seen in the single + ionization of Sc3N@C80 but is much less pronounced in the photoionization-with-fragmentation channel. Comparison of the cross sections near the carbon K edge with the corresponding channels + measured previously in the photoionization of Lu3N@C80 reveal strong similarities. Previously + predicted sharp resonance features in the ionization of Sc3N@C80 ions below the Sc M edge are not confirmed. The experiments are accompanied by quantum-chemistry calculations in the Hartree- Fock approximation and by model calculations employing density functional theory (DFT). 17 I. INTRODUCTION 39 of the nature and applicability of fullerenes and endohe- 40 dral fullerenes is associated with their response to electro- 41 18 The first experimental evidence for the existence of magnetic radiation [7{10]. The references given in recent 42 publications [11{15] provide an overview of experimental 19 soccer-ball-shaped C60 molecules [1] initiated an im- 43 20 mensely growing activity in several different fields of sci- research in the field of photoionization and photofrag- 44 21 ence. Almost in parallel with the exploration of the new mentation of fullerenes. Investigating many-particle sys- 45 22 class of spherical carbon structures, it was speculated tems such as molecules, clusters and fullerenes by observ- 46 23 and then realized that the carbon spheres can host and ing fine structure near atomic inner-shell photoabsorp- 47 24 isolate single atoms or molecules and even clusters of tion edges is particularly elucidating. Examples of mea- 48 25 atoms that can only be stabilized inside a spherical or surements employing gas-phase near-edge x-ray absorp- 49 26 nearly spherical carbon shell [2,3]. Research on such tion fine structure (NEXAFS) spectroscopy of nanopar- 50 27 carbon cages with encapsulated atoms, i.e., endohedral ticles, biopolymers, and ionic species have been provided 51 28 fullerenes, was spurred by scientific interest in the be- in a recent overview article [16]. 29 havior of these intriguing nanoscale objects and by the 52 Most of the work on photoprocesses involving 30 perspectives of their usefulness in many diverse fields of 53 fullerenes and endohedral fullerenes is theoretical ([8, 17] 31 applications ranging from medical treatment to the de- 54 and references therein) because experiments are ham- 32 velopment of efficient solar cells and the realization of 55 pered by the limited availability of pure fullerene sam- 33 qubits in a spin quantum computer. All these aspects 56 ples. The problem of sample purity can be overcome 34 have been reviewed many times. Here, only a few ref- 57 by employing mass-selective preparation of fullerene tar- 35 erences to recent reviews on endohedral fullerenes are 58 gets. This is possible by producing beams of electri- 36 provided [4{6]. 59 cally charged fullerenes and passing them through mass- 37 One research direction among the wide and diverse sci- 60 over-charge filters. When beams of fullerene ions are 38 entific endeavours aiming at the detailed understanding 61 made to interact with photon beams for studying pho- 62 toionization and photofragmentation, the advantage of 63 pure-target preparation is accompanied by the possibil- ∗ [email protected] 64 ity of measuring absolute cross sections [10]. During the 2 1 0 0 S c N @ C + 3 8 0 2 + 2 + 7 ) C 6 0 2 + 8 0 C A + 0 S c N @ C p 3 8 0 3 8 @ ( + t C N 8 3 + 7 n C 6 0 6 0 c @ e C r + 4 S 4 N r 2 7 + 7 3 @ u 3 + C c C c N C + S + 4 0 7 0 2 + 3 @ n C @ 3 + 2 + C 2 + C 8 4 c o 2 + 7 0 5 6 N I S C C N C 3 6 0 5 0 7 0 C 3 7 8 c 2 + + c + 2 0 S + + C C S 6 2 C 5 6 + 5 0 C C C 6 6 7 4 7 8 0 3 0 0 4 0 0 5 0 0 6 0 0 7 0 0 8 0 0 9 0 0 1 0 0 0 1 1 0 0 M a s s / c h a r g e FIG. 1. (color online) Magnetically analyzed mass-per-charge spectrum of positive ions extracted from an ECR ion source while evaporating a Sc3N@C80-containing fullerene sample into the plasma chamber of the source. 65 last one and a half decades, photon-ion merged-beams 101 II. EXPERIMENT 66 experiments were carried out with positively and neg- 67 atively charged fullerene ions [13, 14, 18{20] and with + 102 The experiments were carried out at two different 68 positively charged endohedral fullerenes Sc3N@C80 [21], + + + 103 synchrotron-radiation sources during several beam-time 69 Ce@C82 [22], Xe@C60 [23, 24] and Lu3N@C80 [15]. 104 periods at each of the facilities. The photon-ion merged- 105 beams technique [10] was employed both at the Ad- 106 vanced Light Source (ALS) in Berkeley and at PETRA 70 The focus of this communication is on gas-phase exper- q 107 III in Hamburg. Two permanent experimental installa- 71 iments with Sc3N@C80 in charge states q = ±1. A wide 108 tions were used, namely, the PIPE (Photon-Ion Spec- 72 range of photon energies is covered which include the re- 109 trometer at PETRA III) endstation [30, 31] of beam- 73 gions of Sc M-shell and L-shell absorption edges as well 110 line P04 [32] and the IPB (Ion-Photon Beamline) endsta- 74 as the K edges of C and N. Previous experimental studies 111 tion [33] of beamline 10.0.1. at the ALS. Several of the 75 of photoprocesses involving the Sc L edge together with 112 most recent publications of the present collaboration on 76 the N K and the C K edges in neutral Sc3N@C80 com- 113 photoprocesses of ions studied at the endstations at the 77 prise the observation of photo-electrons [25], of photoab- 114 ALS [13, 34{37] and at PETRA III [38{43] illustrate the 78 sorption [26, 27], of core-level photoemission [26] and of 115 experimental capabilities and the latest developments. 79 momentum-resolved multi-coincidence spectra [12]. Pi- + 80 oneering work on Sc3N@C80 ions [21] investigated the 116 The basic concepts of the endstations used for the 81 influence of the Sc3N cluster on the photoionization of 117 present experiments are very similar. The desired ions + 82 the Sc3N@C80 parent ions in the energy range of ap- 118 are produced by a suitable ion source. The extracted 83 proximately 30 to 50 eV. The latter experiment stimu- 119 ions are accelerated by a voltage of 6 kV. The ion beam + 84 lated theoretical work on photoionization of Sc3N@C80 120 is dispersed in a magnetic field and ions of a given mass 85 ions [28, 29] in which excess cross sections were arising 121 and charge are selected for further transportation to the 86 from the encapsulated atoms compared to the cross sec- 122 photon-ion merged-beams region. Product ions are sepa- 87 tion for the C80 carbon shell. A particularly intrigu- 123 rated from the parent ion beam by a second magnet and 88 ing prediction was made by Korol and Solov'yov [28] of 124 directed to a single-particle detector.
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