Investigating the Rydberg states and photodissociation dynamics of Kr2 using velocity map imaging

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Autoren

  • Cailum M.K. Stienstra
  • Neville J.A. Coughlan
  • Alexander Haack
  • Patrick J.J. Carr
  • Jeff Crouse
  • Joshua Featherstone
  • W. Scott Hopkins

Externe Organisationen

  • University of Waterloo
Forschungs-netzwerk anzeigen

Details

OriginalspracheEnglisch
Seiten (von - bis)505-515
Seitenumfang11
FachzeitschriftCanadian journal of chemistry
Jahrgang101
Ausgabenummer8
PublikationsstatusVeröffentlicht - Aug. 2023
Extern publiziertJa

Abstract

Although the krypton dimer, Kr2, is a prototypical weakly bound van der Waals complex in its ground electronic state, the excited states of Kr2 exhibit many and various interactions. Resonance-enhanced multiphoton ionization and velocity map imaging provide an avenue to explore the electronic structure and photofragmentation dynamics of Kr2 in the vacuum ultraviolet region. By monitoring photofragmentation product channels and recoil anisotropy distributions, one can gain insights into excited state symmetries and lifetimes, which can aid in interpreting spectroscopy. Here, we study the spectroscopy and photodissociation dynamics of Kr2 in the 91 000–94 500 cm−1 region. We record and assign photofragment product channels for 32 vibronic bands corresponding to seven electronic transitions. We also identify two previously unobserved vibronic band systems, which we assign as the Kr2 5p [5/2]3 1g ← X0+gand 5p [3/2]20+g←X0+g transitions. Velocity map images show photofragments arising from predissociation of the neutral Rydberg states and from dissociative photoionization at the n > 2 photon level. We also observe variation in branching ratios between the predissociative and dissociative photoionization channels depending on the lifetime of the intermediate; longer lived states favour higher dissociative photoionization yields and exhibit β6 anisotropy parameters for predissociation product channels, indicating “rotational smearing” of the product angular distributions.

ASJC Scopus Sachgebiete

Zitieren

Investigating the Rydberg states and photodissociation dynamics of Kr2 using velocity map imaging. / Stienstra, Cailum M.K.; Coughlan, Neville J.A.; Haack, Alexander et al.
in: Canadian journal of chemistry, Jahrgang 101, Nr. 8, 08.2023, S. 505-515.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Stienstra, CMK, Coughlan, NJA, Haack, A, Carr, PJJ, Crouse, J, Featherstone, J & Scott Hopkins, W 2023, 'Investigating the Rydberg states and photodissociation dynamics of Kr2 using velocity map imaging', Canadian journal of chemistry, Jg. 101, Nr. 8, S. 505-515. https://doi.org/10.1139/cjc-2022-0283
Stienstra, C. M. K., Coughlan, N. J. A., Haack, A., Carr, P. J. J., Crouse, J., Featherstone, J., & Scott Hopkins, W. (2023). Investigating the Rydberg states and photodissociation dynamics of Kr2 using velocity map imaging. Canadian journal of chemistry, 101(8), 505-515. https://doi.org/10.1139/cjc-2022-0283
Stienstra CMK, Coughlan NJA, Haack A, Carr PJJ, Crouse J, Featherstone J et al. Investigating the Rydberg states and photodissociation dynamics of Kr2 using velocity map imaging. Canadian journal of chemistry. 2023 Aug;101(8):505-515. doi: 10.1139/cjc-2022-0283
Stienstra, Cailum M.K. ; Coughlan, Neville J.A. ; Haack, Alexander et al. / Investigating the Rydberg states and photodissociation dynamics of Kr2 using velocity map imaging. in: Canadian journal of chemistry. 2023 ; Jahrgang 101, Nr. 8. S. 505-515.
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title = "Investigating the Rydberg states and photodissociation dynamics of Kr2 using velocity map imaging",
abstract = "Although the krypton dimer, Kr2, is a prototypical weakly bound van der Waals complex in its ground electronic state, the excited states of Kr2 exhibit many and various interactions. Resonance-enhanced multiphoton ionization and velocity map imaging provide an avenue to explore the electronic structure and photofragmentation dynamics of Kr2 in the vacuum ultraviolet region. By monitoring photofragmentation product channels and recoil anisotropy distributions, one can gain insights into excited state symmetries and lifetimes, which can aid in interpreting spectroscopy. Here, we study the spectroscopy and photodissociation dynamics of Kr2 in the 91 000–94 500 cm−1 region. We record and assign photofragment product channels for 32 vibronic bands corresponding to seven electronic transitions. We also identify two previously unobserved vibronic band systems, which we assign as the Kr2 5p [5/2]3 1g ← X0+gand 5p [3/2]20+g←X0+g transitions. Velocity map images show photofragments arising from predissociation of the neutral Rydberg states and from dissociative photoionization at the n > 2 photon level. We also observe variation in branching ratios between the predissociative and dissociative photoionization channels depending on the lifetime of the intermediate; longer lived states favour higher dissociative photoionization yields and exhibit β6 anisotropy parameters for predissociation product channels, indicating “rotational smearing” of the product angular distributions.",
keywords = "krypton dimer, photofragment imaging, REMPI spectroscopy, Rydberg states, time-of-flight spectrometry, VMI",
author = "Stienstra, {Cailum M.K.} and Coughlan, {Neville J.A.} and Alexander Haack and Carr, {Patrick J.J.} and Jeff Crouse and Joshua Featherstone and {Scott Hopkins}, W.",
note = "Funding Information: WSH acknowledges funding from the Canadian Foundation for Innovation (CFI), Ontario Research Fund (ORF), and Natural Sciences and Engineering Research Council (NSERC) of Canada in the form of a Discovery Grant. CMKS acknowledges financial support from NSERC in the form of a Canadian Graduate Scholarship. NJAC acknowledges financial support from the NSERC Banting postdoctoral fellowship program. AH gratefully acknowledges this work being funded by the Deutsche Forschungsgemeinschaft (DFG; German Research Foundation; 449651261). Canadian Foundation for Innovation, Ontario Research Fund, Natural Sciences and Engineering Research Council of Canada, Deutsche Forschungsgemeinschaft (DFG; German Research Foundation). ",
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volume = "101",
pages = "505--515",
journal = "Canadian journal of chemistry",
issn = "0008-4042",
publisher = "National Research Council of Canada",
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Download

TY - JOUR

T1 - Investigating the Rydberg states and photodissociation dynamics of Kr2 using velocity map imaging

AU - Stienstra, Cailum M.K.

AU - Coughlan, Neville J.A.

AU - Haack, Alexander

AU - Carr, Patrick J.J.

AU - Crouse, Jeff

AU - Featherstone, Joshua

AU - Scott Hopkins, W.

N1 - Funding Information: WSH acknowledges funding from the Canadian Foundation for Innovation (CFI), Ontario Research Fund (ORF), and Natural Sciences and Engineering Research Council (NSERC) of Canada in the form of a Discovery Grant. CMKS acknowledges financial support from NSERC in the form of a Canadian Graduate Scholarship. NJAC acknowledges financial support from the NSERC Banting postdoctoral fellowship program. AH gratefully acknowledges this work being funded by the Deutsche Forschungsgemeinschaft (DFG; German Research Foundation; 449651261). Canadian Foundation for Innovation, Ontario Research Fund, Natural Sciences and Engineering Research Council of Canada, Deutsche Forschungsgemeinschaft (DFG; German Research Foundation).

PY - 2023/8

Y1 - 2023/8

N2 - Although the krypton dimer, Kr2, is a prototypical weakly bound van der Waals complex in its ground electronic state, the excited states of Kr2 exhibit many and various interactions. Resonance-enhanced multiphoton ionization and velocity map imaging provide an avenue to explore the electronic structure and photofragmentation dynamics of Kr2 in the vacuum ultraviolet region. By monitoring photofragmentation product channels and recoil anisotropy distributions, one can gain insights into excited state symmetries and lifetimes, which can aid in interpreting spectroscopy. Here, we study the spectroscopy and photodissociation dynamics of Kr2 in the 91 000–94 500 cm−1 region. We record and assign photofragment product channels for 32 vibronic bands corresponding to seven electronic transitions. We also identify two previously unobserved vibronic band systems, which we assign as the Kr2 5p [5/2]3 1g ← X0+gand 5p [3/2]20+g←X0+g transitions. Velocity map images show photofragments arising from predissociation of the neutral Rydberg states and from dissociative photoionization at the n > 2 photon level. We also observe variation in branching ratios between the predissociative and dissociative photoionization channels depending on the lifetime of the intermediate; longer lived states favour higher dissociative photoionization yields and exhibit β6 anisotropy parameters for predissociation product channels, indicating “rotational smearing” of the product angular distributions.

AB - Although the krypton dimer, Kr2, is a prototypical weakly bound van der Waals complex in its ground electronic state, the excited states of Kr2 exhibit many and various interactions. Resonance-enhanced multiphoton ionization and velocity map imaging provide an avenue to explore the electronic structure and photofragmentation dynamics of Kr2 in the vacuum ultraviolet region. By monitoring photofragmentation product channels and recoil anisotropy distributions, one can gain insights into excited state symmetries and lifetimes, which can aid in interpreting spectroscopy. Here, we study the spectroscopy and photodissociation dynamics of Kr2 in the 91 000–94 500 cm−1 region. We record and assign photofragment product channels for 32 vibronic bands corresponding to seven electronic transitions. We also identify two previously unobserved vibronic band systems, which we assign as the Kr2 5p [5/2]3 1g ← X0+gand 5p [3/2]20+g←X0+g transitions. Velocity map images show photofragments arising from predissociation of the neutral Rydberg states and from dissociative photoionization at the n > 2 photon level. We also observe variation in branching ratios between the predissociative and dissociative photoionization channels depending on the lifetime of the intermediate; longer lived states favour higher dissociative photoionization yields and exhibit β6 anisotropy parameters for predissociation product channels, indicating “rotational smearing” of the product angular distributions.

KW - krypton dimer

KW - photofragment imaging

KW - REMPI spectroscopy

KW - Rydberg states

KW - time-of-flight spectrometry

KW - VMI

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U2 - 10.1139/cjc-2022-0283

DO - 10.1139/cjc-2022-0283

M3 - Article

AN - SCOPUS:85167823457

VL - 101

SP - 505

EP - 515

JO - Canadian journal of chemistry

JF - Canadian journal of chemistry

SN - 0008-4042

IS - 8

ER -