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Fluorescence emission from photo-fragments after resonant S 2p excitations in H2S
KTH, School of Engineering Sciences (SCI), Physics, Atomic and Molecular Physics.
KTH, School of Engineering Sciences (SCI), Physics, Atomic and Molecular Physics.
CNR-INFM, Laboratorio Nazionale TASC.
KTH, School of Engineering Sciences (SCI), Physics, Atomic and Molecular Physics.ORCID iD: 0000-0001-7389-5501
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2007 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 9, no 3, 389-395 p.Article in journal (Refereed) Published
Abstract [en]

Visible-UV fluorescence emission of gas-phase hydrogen sulfide, H2S, has been studied at the S 2p edge with synchrotron radiation excitation. Dispersed fluorescence measurements in the wavelength range 300 - 900 nm were taken at several photon energies corresponding to the excitations of the S 2p electrons to the unoccupied molecular and Rydberg orbitals. The spectra reveal fluorescence from the H, S, S+, HS and HS+ photo-fragments. H is found to be the strongest emitter at Rydberg excitations, while the emission from S+ is dominant at the molecular resonances and above the S 2p ionization thresholds. The intensities of hydrogen Lyman-alpha (122 nm), Balmer-alpha (656 nm), Balmer-beta (486 nm) transitions as well as the visible-UV total fluorescence yield (300 - 900 nm) and the total ion yield were measured by scanning the photon energy in small steps across the S 2p edge. The different Balmer lines show some sensitivity to the specific core excitations, which is, however, not so strong as that recently observed in the water molecule.

Place, publisher, year, edition, pages
2007. Vol. 9, no 3, 389-395 p.
Keyword [en]
X-RAY EXCITATION, DECAY CHANNELS, PHOTOELECTRON-SPECTROSCOPY, AUGER DECAY, MOLECULES, PHOTOIONIZATION, STATES, ATOMS
National Category
Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:kth:diva-7998DOI: 10.1039/b610199bISI: 000243204200008Scopus ID: 2-s2.0-33845962796OAI: oai:DiVA.org:kth-7998DiVA: diva2:13200
Note
QC 20100916Available from: 2008-02-20 Created: 2008-02-20 Last updated: 2017-12-14Bibliographically approved
In thesis
1. Synchrotron radiation studies of gas phase molecules: from hydrogen to DNA sugars
Open this publication in new window or tab >>Synchrotron radiation studies of gas phase molecules: from hydrogen to DNA sugars
2008 (English)Doctoral thesis, comprehensive summary (Other scientific)
Abstract [en]

This thesis summarises experimental results on the molecular spectroscopy of gas phase molecules excited by synchrotron radiation in the VUV and soft X-ray regions. We have used three different detection techniques, photon induced fluorescence spectroscopy, photoionisation mass spectroscopy and near edge X-ray absorption fine structure spectroscopy to study molecular deuterium, hydrogen sulphide, ammonia, methanol, pyridine, pyridazine, pyrimidine, pyrazine, s-triazine, and 2-deoxy-D-ribose, the last one also known as the DNA sugar. Out of this variety of techniques and molecules we have shown that: (1) high resolution dispersed fluorescence allows us to identify vibrational and rotational bands in molecular deuterium, as well as to estimate the predissociation probability of the same molecule [paper I]; (2) the main species fluorescing after core excitation of methane, ammonia [paper III], hydrogen sulphide [paper II], pyridine, pyrimidine and s-triazine is H Balmer α, followed by fluorescence from ionised species, molecular bands and Balmer β, γ , δ; (3) the Rydberg enhancement seen in fluorescence measurements of water [Melero et al. PRL 96 (2006) 063003], corroborated later in H2S [paper II], NH3 [paper III] and CH4 [paper III] and postulated as general behaviour for molecules formed by low-Z atoms, is also seen in larger organic cyclic molecules, e.g. azabenzenes; (4) when dissociative ionisation of pyridine, pyridazine, pyrimidine, pyrazine, s-triazine and 2-deoxy-D-ribose occurs, concerted bond rearrangement and nuclear motion takes place as opposed to stepwise dissociation [papers V and VI].

Place, publisher, year, edition, pages
Stockholm: KTH, 2008. x, 56 p.
Series
Trita-FYS, ISSN 0280-316X ; 2008:1
Keyword
KTH thesis, synchrotron radiation, gas phase, bio molecules
National Category
Atom and Molecular Physics and Optics
Identifiers
urn:nbn:se:kth:diva-4640 (URN)978-91-7178-852-8 (ISBN)
Public defence
2008-03-13, FA31, Albanova, Roslagstullabacken 21, Stockholm, 10:15
Opponent
Supervisors
Note
QC 20100916Available from: 2008-02-20 Created: 2008-02-20 Last updated: 2010-09-16Bibliographically approved
2. Flourescence properties of trendy molecules studied with synchrotron radiation
Open this publication in new window or tab >>Flourescence properties of trendy molecules studied with synchrotron radiation
2006 (English)Licentiate thesis, comprehensive summary (Other scientific)
Abstract [en]

This thesis summarises the experimental results on molecular spectroscopy of gas phase molecules using synchrotron radiation in the UV- VUV and soft-X rays regions. The results of applying Photon Induced Fluorescence Spectroscopy (PIFS) to D2, H2S, H2O and pyrimidine are presented and discussed. Both inner and outer shell excitations of free molecules lead to different relaxation processes. However, a common result is that when the molecule breaks and the resulting neutral fragments are left in an excited state, they might fluoresce in the UV- Vis range. PIFS technique has two main advantages, it permits to detect neutral fragments and to identify the fluorescing species. From this fact, we can infer dissociation channels and trace back the electronic processes that led to the fluorescence. For these molecules we have analysed and interpreted both dispersed and undispersed fluorescence. What motivates our work is the lack of fluorescence studies and in a more general sense, to contribute to the knowledge of important molecules for life such as water and pyrimidine.

Place, publisher, year, edition, pages
Stockholm: KTH, 2006. ix, 47 p.
Series
Trita-FYS, ISSN 0280-316X ; 2006.57
National Category
Physical Sciences
Identifiers
urn:nbn:se:kth:diva-4148 (URN)91-7178-428-4 (ISBN)
Presentation
2006-10-09, Sal FA31, AlbaNova universitetscentrum, Roslagstullsb 21, Stockholm, 10:00
Opponent
Supervisors
Note
QC 20101125Available from: 2006-10-13 Created: 2006-10-13 Last updated: 2010-11-25Bibliographically approved

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