Cation and Anion Formation in F 1s-Excited SF6-Clusters
-
Christian Grunewald
Abstract
Cation and anion formation from molecular SF6 and SF6 clusters is reported in the F 1s-excitation regime (680–720 eV) using tunable synchrotron radiation. Stable products are identified by mass spectrometry, while the tunablility of the soft X-rays source is used to determine mechanistic details on the formation of the detected charged products. Characteristic differences are observed between product formation from the isolated molecule as well as from clusters for both, cations and anions. Specifically, dication formation, such as SF22+, is only observed for molecular precursors, which are formed with high efficiency at the F 1s → t2g-transition. SF6− is efficiently formed from clusters upon F 1s → t1u-transition. Mechanistic details on the formation of stable products are discussed.
Dedicated to: Prof. Dr. Friedrich Temps on the occasion of his 65th birthday.
Acknowledgement
We thank E. Serdaroglu for his help during the experiments. Financial support by DFG (Funder Id: http://dx.doi.org/10.13039/501100001659, RU420/8-1 and Funder Id: http://dx.doi.org/10.13039/501100001659, Graduiertenkolleg 1582-TP A1) is gratefully acknowledged.
References
1. J. L. Dehmer, J. Chem. Phys. 56 (1972) 4496.10.1063/1.1677895Suche in Google Scholar
2. E. Hudson, D. A. Shirley, M. Domke, G. Remmers, A. Puschmann, T. Mandel, C. Xue, G. Kaindl, Phys. Rev. A 47 (1993) 361.10.1103/PhysRevA.47.361Suche in Google Scholar PubMed
3. A. P. P. Natalense, R. R. Lucchese, J. Chem. Phys. 111 (1999) 5344.10.1063/1.479794Suche in Google Scholar
4. R. E. Lavilla, R. D. Deslattes, J. Chem. Phys. 44 (1966) 4399.10.1063/1.1726649Suche in Google Scholar
5. T. A. Ferrett, D. W. Lindle, P. A. Heimann, H. G. Kerkhoff, U. E. Becker, D. A. Shirley, Phys. Rev. A 34 (1986) 1916.10.1103/PhysRevA.34.1916Suche in Google Scholar PubMed
6. P. Decleva, G. Fronzoni, A. Kivimaki, J. A. Ruiz, S. Svensson, J. Phys. B – At. Mol. Opt. Phys. 42 (2009) 055102.10.1088/0953-4075/42/5/055102Suche in Google Scholar
7. G. Prümper, Y. Tamenori, A. De Fanis, U. Hergenhahn, M. Kitajima, M. Hoshino, H. Tanaka, K. Ueda, J. Phys. B – At. Mol. Opt. Phys. 38 (2005) 1.10.1088/0953-4075/38/1/001Suche in Google Scholar
8. M. N. Piancastelli, W. C. Stolte, R. Guillemin, A. Wolska, S. W. Yu, M. M. Sant’Anna, D. W. Lindle, J. Chem. Phys. 122 (2005) 094312.10.1063/1.1855314Suche in Google Scholar PubMed
9. C. Strahlman, R. Sankari, A. Kivimäki, R. Richter, M. Coreno, R. Nyholm, Rev. Sci. Instrum. 87 (2016) 013109.10.1063/1.4940425Suche in Google Scholar PubMed
10. S. W. J. Scully, R. A. Mackie, R. Browning, K. F. Dunn, C. J. Latimer, J. Phys. B 35 (2002) 2703.10.1088/0953-4075/35/12/306Suche in Google Scholar
11. M. Stener, D. Toffoli, G. Fronzoni, P. Decleva, J. Chem. Phys. 124 (2006) 114306.10.1063/1.2178799Suche in Google Scholar PubMed
12. R. Feifel, J. H. D. Eland, L. Storchi, F. Tarantelli, J. Chem. Phys. 122 (2005) 144309.10.1063/1.1872837Suche in Google Scholar PubMed
13. K. Mitsuke, T. Kondow, K. Kuchitsu, J. Phys. Chem. 90 (1986) 1552.10.1021/j100399a019Suche in Google Scholar
14. J. Stöhr, NEXAFS Spectroscopy, Springer Ser. Surf. Sci. 25, Springer, Berlin (1992).10.1007/978-3-662-02853-7Suche in Google Scholar
15. E. Rühl, Int. J. Mass Spectrom. 229 (2003) 117.10.1016/j.ijms.2003.08.006Suche in Google Scholar
16. R. Flesch, A. A. Pavlychev, J. J. Neville, J. Blumberg, M. Kuhlmann, W. Tappe, F. Senf, O. Schwarzkopf, A. P. Hitchcock, E. Rühl, Phys. Rev. Lett. 86 (2001) 3767.10.1103/PhysRevLett.86.3767Suche in Google Scholar PubMed
17. A. A. Pavlychev, R. Flesch, E. Rühl, Phys. Rev. A 70 (2004) 015201.10.1103/PhysRevA.70.015201Suche in Google Scholar
18. I. L. Bradeanu, R. Flesch, N. Kosugi, A. A. Pavlychev, E. Rühl, Phys. Chem. Chem. Phys. 8 (2006) 1906.10.1039/B517199GSuche in Google Scholar
19. R. Flesch, E. Serdaroglu, F. Blobner, P. Feulner, X. O. Brykalova, A. A. Pavlychev, N. Kosugi, E. Rühl, Phys. Chem. Chem. Phys. 14 (2012) 9397.10.1039/c2cp23451cSuche in Google Scholar PubMed
20. I. L. Bradeanu, N. Kosugi, R. Flesch, E. Rühl, J. Phys. Chem. A 112 (2008) 9192.10.1021/jp802068hSuche in Google Scholar PubMed
21. R. Flesch, E. Serdaroglu, X. O. Brykalova, E. I. Kan, E. S. Klyushina, Y. S. Krivosenko, A. A. Pavlychev, E. Rühl, J. Chem. Phys. 138 (2013) 144302.10.1063/1.4798975Suche in Google Scholar PubMed
22. R. Flesch, N. Kosugi, I. L. Bradeanu, J. J. Neville, E. Rühl, J. Chem. Phys. 121 (2004) 8343.10.1063/1.1804180Suche in Google Scholar PubMed
23. A. A. Pavlychev, E. Rühl, J. Electron Spectrosc. Relat. Phenom. 106 (2000) 207.10.1016/S0368-2048(99)00078-XSuche in Google Scholar
24. A. A. Pavlychev, X. O. Brykalova, D. A. Mistrov, R. Flesch, E. Rühl, J. Electron Spectrosc. Relat. Phenom. 166 (2008) 45.10.1016/j.elspec.2008.06.001Suche in Google Scholar
25. I. Luzon, M. Nagler, V. Chandrasekaran, O. Heber, D. Strasser, J. Phys. Chem. A 120 (2016) 221.10.1021/acs.jpca.5b09967Suche in Google Scholar PubMed
26. A. Lindblad, M. Winkler, M. Tchaplyguine, G. Öhrwall, S. Svensson, O. Björneholm, Surf. Sci. 603 (2009) 433.10.1016/j.susc.2008.11.032Suche in Google Scholar
27. R. Flesch, N. Kosugi, A. Knop-Gericke, E. Rühl, Z. Phys. Chem. 228 (2014) 387.10.1515/zpch-2014-0509Suche in Google Scholar
28. E. Rühl, R. Flesch, J. Chem. Phys. 121 (2004) 5322.10.1063/1.1784780Suche in Google Scholar PubMed
29. W. C. Wiley, I. H. McLaren, Rev. Sci. Instrum. 26 (1955) 1150.10.1063/1.1715212Suche in Google Scholar
30. W. L. Jolly, K. D. Bomben, C. J. Eyermann, At. Data Nucl. Data Tab. 31 (1984) 433.10.1016/0092-640X(84)90011-1Suche in Google Scholar
31. R. W. Shaw, T. X. Carroll, T. D. Thomas, J. Am. Chem. Soc. 95 (1973) 5870.10.1021/ja00799a006Suche in Google Scholar
32. M. Sasanuma, E. Ishiguro, T. Hayaisha, H. Masuko, Y. Morioka, T. Nakajima, M. Nakamura, J. Phys. B 12 (1979) 4057.10.1088/0022-3700/12/24/012Suche in Google Scholar
33. K. Hiraoka, A. Shimizu, A. Minamitsu, M. Nasu, S. Fujimaki, S. Yamabe, J. Am. Soc. Mass Spectrom. 6 (1995) 1137.10.1016/1044-0305(95)00583-8Suche in Google Scholar PubMed
34. E. Rühl, C. Heinzel, H. Baumgärtel, M. Lavollée, P. Morin, Z. Phys. D 31 (1994) 245.10.1007/BF01445002Suche in Google Scholar
35. E. Rühl, H. W. Jochims, Z. Phys. Chem. 195 (1996) 137.10.1524/zpch.1996.195.Part_1_2.137Suche in Google Scholar
36. L. G. Christophorou, J. K. Olthoff, J. Phys. Chem. Ref. Data 29 (2000) 267.10.1063/1.1288407Suche in Google Scholar
37. M. Fenzlaff, R. Gerhard, E. Illenberger, J. Chem. Phys. 88 (1988) 149.10.1063/1.454646Suche in Google Scholar
38. B. L. Henke, P. Lee, T. J. Tanaka, R. L. Shimabukuro, At. Data Nucl. Data Tab. 27 (1982) 1.10.1016/0092-640X(82)90002-XSuche in Google Scholar
39. O. Björneholm, F. Federmann, F. Fössing, T. Möller, Phys. Rev. Lett. 74 (1995) 3017.10.1103/PhysRevLett.74.3017Suche in Google Scholar PubMed
40. J. C. Creasey, I. R. Lambert, R. P. Tuckett, K. Codling, L. J. Frasinski, P. A. Hatherly, M. Stankiewicz, J. Chem. Soc. Faraday Trans. 87 (1991) 1287.10.1039/ft9918701287Suche in Google Scholar
41. E. Rühl, A. P. Hitchcock, P. Morin, M. Lavollée, J. Chim. Phys. 92 (1995) 521.10.1051/jcp/1995920521Suche in Google Scholar
42. L. Journel, R. Guillemin, A. Haouas, P. Lablanquie, F. Penent, J. Palaudoux, L. Andric, M. Simon, D. Ceolin, T. Kaneyasu, J. Viefhaus, M. Braune, W. B. Li, C. Elkharrat, F. Catoire, J. C. Houver, D. Dowek, Phys. Rev. A 77 (2008) 042710.10.1103/PhysRevA.77.042710Suche in Google Scholar
© 2020 Walter de Gruyter GmbH, Berlin/Boston
Artikel in diesem Heft
- Frontmatter
- Preface
- Congratulations to Friedrich Temps: a multifaceted career in Physical Chemistry
- Time-Resolved Measurements and Master Equation Modelling of the Unimolecular Decomposition of CH3OCH2
- Direct Kinetic Measurements and Master Equation Modelling of the Unimolecular Decomposition of Resonantly-Stabilized CH2CHCHC(O)OCH3 Radical and an Upper Limit Determination for CH2CHCHC(O)OCH3 + O2 Reaction
- Elevated pressure low-temperature oxidation of linear five-heavy-atom fuels: diethyl ether, n-pentane, and their mixture
- Nucleation of soot: experimental assessment of the role of polycyclic aromatic hydrocarbon (PAH) dimers
- On the influence of water on urea condensation reactions: a theoretical study
- Comparison of detailed reaction mechanisms for homogeneous ammonia combustion
- Simplified Representation of Multichannel Thermal Unimolecular Reactions. II. Refined Parametrization of Formaldehyde Dissociation
- Cation and Anion Formation in F 1s-Excited SF6-Clusters
- Barrier to internal rotation, symmetry and carbonyl reactivity in methyl 3,3,3-trifluoropyruvate
- Shock-tube study of the decomposition of octamethylcyclotetrasiloxane and hexamethylcyclotrisiloxane
- Vibrational sum-frequency generation study of molecular structure, sterical constraints and nonlinear optical switching contrast of mixed alkyl-azobenzene self-assembled monolayers
- Aqueous Contact Ion Pairs of Phosphate Groups with Na+, Ca2+ and Mg2+ – Structural Discrimination by Femtosecond Infrared Spectroscopy and Molecular Dynamics Simulations
- Solvent-dependent photochemical dynamics of a phenoxazine-based photoredox catalyst
- The geometry relaxation and photodeactivation from the S2 state of dibenzofuran studied by ultrafast spectroscopy
- Approaching black-box calculations of pump-probe fragmentation dynamics of polyatomic molecules
- Full-Dimensional Photodynamics of Bistable Proton Transfer Switches
- Thermal Isomerization of [Co(acac)2(N3)(py)] in Liquid Solution Studied by Time-Resolved Fourier-Transform Infrared Spectroscopy
Artikel in diesem Heft
- Frontmatter
- Preface
- Congratulations to Friedrich Temps: a multifaceted career in Physical Chemistry
- Time-Resolved Measurements and Master Equation Modelling of the Unimolecular Decomposition of CH3OCH2
- Direct Kinetic Measurements and Master Equation Modelling of the Unimolecular Decomposition of Resonantly-Stabilized CH2CHCHC(O)OCH3 Radical and an Upper Limit Determination for CH2CHCHC(O)OCH3 + O2 Reaction
- Elevated pressure low-temperature oxidation of linear five-heavy-atom fuels: diethyl ether, n-pentane, and their mixture
- Nucleation of soot: experimental assessment of the role of polycyclic aromatic hydrocarbon (PAH) dimers
- On the influence of water on urea condensation reactions: a theoretical study
- Comparison of detailed reaction mechanisms for homogeneous ammonia combustion
- Simplified Representation of Multichannel Thermal Unimolecular Reactions. II. Refined Parametrization of Formaldehyde Dissociation
- Cation and Anion Formation in F 1s-Excited SF6-Clusters
- Barrier to internal rotation, symmetry and carbonyl reactivity in methyl 3,3,3-trifluoropyruvate
- Shock-tube study of the decomposition of octamethylcyclotetrasiloxane and hexamethylcyclotrisiloxane
- Vibrational sum-frequency generation study of molecular structure, sterical constraints and nonlinear optical switching contrast of mixed alkyl-azobenzene self-assembled monolayers
- Aqueous Contact Ion Pairs of Phosphate Groups with Na+, Ca2+ and Mg2+ – Structural Discrimination by Femtosecond Infrared Spectroscopy and Molecular Dynamics Simulations
- Solvent-dependent photochemical dynamics of a phenoxazine-based photoredox catalyst
- The geometry relaxation and photodeactivation from the S2 state of dibenzofuran studied by ultrafast spectroscopy
- Approaching black-box calculations of pump-probe fragmentation dynamics of polyatomic molecules
- Full-Dimensional Photodynamics of Bistable Proton Transfer Switches
- Thermal Isomerization of [Co(acac)2(N3)(py)] in Liquid Solution Studied by Time-Resolved Fourier-Transform Infrared Spectroscopy
