Core-Level Spectroscopy of 2-Thiouracil at the Sulfur L1- and L2,3-Edges Utilizing a SASE Free-Electron Laser

Lever, Fabiano; Mayer, Dennis; Metje, Jan; Alisauskas, Skirmantas; Calegari, Francesca; Düsterer, Stefan; Feifel, Raimund; Niebuhr, Mario; Manschwetus, Bastian; Kuhlmann, Marion; Mazza, Tommaso; Robinson, Matthew Scott; Squibb, Richard J.; Trabattoni, Andrea; Wallner, Måns; Wolf, Thomas J. A.; Gühr, Markus

doi:10.3390/molecules26216469

Title: Core-Level Spectroscopy of 2-Thiouracil at the Sulfur L1- and L2,3-Edges Utilizing a SASE Free-Electron Laser

Abstract

In this paper, we report X-ray absorption and core-level electron spectra of the nucleobase derivative 2-thiouracil at the sulfur L₁- and L_2,3-edges. We used soft X-rays from the free-electron laser FLASH2 for the excitation of isolated molecules and dispersed the outgoing electrons with a magnetic bottle spectrometer. We identified photoelectrons from the 2p core orbital, accompanied by an electron correlation satellite, as well as resonant and non-resonant Coster–Kronig and Auger–Meitner emission at the L₁- and L_2,3-edges, respectively. We used the electron yield to construct X-ray absorption spectra at the two edges. The experimental data obtained are put in the context of the literature currently available on sulfur core-level and 2-thiouracil spectroscopy.

Authors:

Lever, Fabiano;

; Metje, Jan; Alisauskas, Skirmantas; Calegari, Francesca; Düsterer, Stefan; Feifel, Raimund;

; Manschwetus, Bastian; Kuhlmann, Marion; Mazza, Tommaso; Robinson, Matthew Scott; Squibb, Richard J.;

; Wallner, Måns;

; Gühr, Markus

Publication Date:: 2021-10-26

Research Org.:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Volkswagen Foundation; Federal Ministry of Education and Research (BMBF); German Research Foundation (DFG); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; European Research Council (ERC); Swedish Research Council (VR); Knut and Alice Wallenberg Foundation

OSTI Identifier:: 1828079

Alternate Identifier(s):: OSTI ID: 1877676; OSTI ID: 1878586

Grant/Contract Number:: NA; AC02-76SF00515; GU 1478/1-1; 637756

Resource Type:: Published Article

Journal Name:: Molecules

Additional Journal Information:: Journal Name: Molecules Journal Volume: 26 Journal Issue: 21; Journal ID: ISSN 1420-3049

Publisher:: MDPI AG

Country of Publication:: Switzerland

Language:: English

Subject:: 47 OTHER INSTRUMENTATION; X-ray; photoelectron; sulfur; thiouracil; nucleobases; Coster–Kronig; Auger–Meitner; NEXAFS; FLASH

Citation Formats


                    Lever, Fabiano, Mayer, Dennis, Metje, Jan, Alisauskas, Skirmantas, Calegari, Francesca, Düsterer, Stefan, Feifel, Raimund, Niebuhr, Mario, Manschwetus, Bastian, Kuhlmann, Marion, Mazza, Tommaso, Robinson, Matthew Scott, Squibb, Richard J., Trabattoni, Andrea, Wallner, Måns, Wolf, Thomas J. A., and Gühr, Markus. Core-Level Spectroscopy of 2-Thiouracil at the Sulfur L1- and L2,3-Edges Utilizing a SASE Free-Electron Laser.  Switzerland: N. p., 2021. 
Web.  doi:10.3390/molecules26216469.

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                    Lever, Fabiano, Mayer, Dennis, Metje, Jan, Alisauskas, Skirmantas, Calegari, Francesca, Düsterer, Stefan, Feifel, Raimund, Niebuhr, Mario, Manschwetus, Bastian, Kuhlmann, Marion, Mazza, Tommaso, Robinson, Matthew Scott, Squibb, Richard J., Trabattoni, Andrea, Wallner, Måns, Wolf, Thomas J. A., & Gühr, Markus. Core-Level Spectroscopy of 2-Thiouracil at the Sulfur L1- and L2,3-Edges Utilizing a SASE Free-Electron Laser.  Switzerland.  https://doi.org/10.3390/molecules26216469

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                    Lever, Fabiano, Mayer, Dennis, Metje, Jan, Alisauskas, Skirmantas, Calegari, Francesca, Düsterer, Stefan, Feifel, Raimund, Niebuhr, Mario, Manschwetus, Bastian, Kuhlmann, Marion, Mazza, Tommaso, Robinson, Matthew Scott, Squibb, Richard J., Trabattoni, Andrea, Wallner, Måns, Wolf, Thomas J. A., and Gühr, Markus. Tue .  
"Core-Level Spectroscopy of 2-Thiouracil at the Sulfur L1- and L2,3-Edges Utilizing a SASE Free-Electron Laser".  Switzerland.  https://doi.org/10.3390/molecules26216469.

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@article{osti_1828079,

  title        = {Core-Level Spectroscopy of 2-Thiouracil at the Sulfur L1- and L2,3-Edges Utilizing a SASE Free-Electron Laser},

  author       = {Lever, Fabiano and Mayer, Dennis and Metje, Jan and Alisauskas, Skirmantas and Calegari, Francesca and Düsterer, Stefan and Feifel, Raimund and Niebuhr, Mario and Manschwetus, Bastian and Kuhlmann, Marion and Mazza, Tommaso and Robinson, Matthew Scott and Squibb, Richard J. and Trabattoni, Andrea and Wallner, Måns and Wolf, Thomas J. A. and Gühr, Markus},

  abstractNote = {In this paper, we report X-ray absorption and core-level electron spectra of the nucleobase derivative 2-thiouracil at the sulfur L1- and L2,3-edges. We used soft X-rays from the free-electron laser FLASH2 for the excitation of isolated molecules and dispersed the outgoing electrons with a magnetic bottle spectrometer. We identified photoelectrons from the 2p core orbital, accompanied by an electron correlation satellite, as well as resonant and non-resonant Coster–Kronig and Auger–Meitner emission at the L1- and L2,3-edges, respectively. We used the electron yield to construct X-ray absorption spectra at the two edges. The experimental data obtained are put in the context of the literature currently available on sulfur core-level and 2-thiouracil spectroscopy.},

  doi          = {10.3390/molecules26216469},

  journal      = {Molecules},

  number       = 21,

  volume       = 26,

  place        = {Switzerland},

  year         = {2021},

  month        = {10}

}

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Title: Core-Level Spectroscopy of 2-Thiouracil at the Sulfur L1- and L2,3-Edges Utilizing a SASE Free-Electron Laser

Abstract

Citation Formats

Non-invasive online wavelength measurements at FLASH2 and present benchmark journal, January 2018

Flash II: Perspectives and challenges journal, April 2011

Simulated and Experimental Time-Resolved Photoelectron Spectra of the Intersystem Crossing Dynamics in 2-Thiouracil journal, November 2018

On the decay of the triplet state of thionucleobases journal, January 2017

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URSA-PQ: A Mobile and Flexible Pump-Probe Instrument for Gas Phase Samples at the FLASH Free Electron Laser journal, November 2020

Photophysics and Photochemistry of Canonical Nucleobases’ Thioanalogs: From Quantum Mechanical Studies to Time Resolved Experiments journal, June 2017

Photo-cross-linking and high-resolution mass spectrometry for assignment of RNA-binding sites in RNA-binding proteins journal, August 2014

Femtosecond Time-Resolved Photoelectron Spectroscopy journal, April 2004

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The tautomeric equilibria of thio analogues of nucleic acid bases. Part 3. Ultraviolet photoelectron spectra of 2-thiouracil and its methyl derivatives journal, January 1990

Ultrafast X-ray Auger probing of photoexcited molecular dynamics journal, June 2014

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Increase in the photoreactivity of uracil derivatives by doubling thionation journal, January 2015

Carbon and oxygen kll and sulfur lmm auger spectra of ocs journal, January 1990

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A Static Picture of the Relaxation and Intersystem Crossing Mechanisms of Photoexcited 2-Thiouracil journal, August 2015

The resonant Auger effect journal, January 2000

Spatial Factors for Triplet Fusion Reaction of Singlet Oxygen Photosensitization journal, October 2017

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Probing ultrafast ππ*/nπ* internal conversion in organic chromophores via K-edge resonant absorption journal, June 2017

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Ionization and fragmentation of OCS and CS2 after photoexcitation around the sulfur 2p edge journal, August 1997

Normal and resonant Auger spectroscopy of isocyanic acid, HNCO journal, July 2018

Transient resonant Auger–Meitner spectra of photoexcited thymine journal, January 2021

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Shake-up transitions in S 2p, S 2s and F 1s photoionization of the SF 6 molecule journal, February 2009

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Flash II: Perspectives and challenges
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Simulated and Experimental Time-Resolved Photoelectron Spectra of the Intersystem Crossing Dynamics in 2-Thiouracil
journal, November 2018

On the decay of the triplet state of thionucleobases
journal, January 2017

Intersystem crossing dynamics in singly substituted thiouracil studied by time-resolved photoelectron spectroscopy: Micro-environmental effects due to sulfur position
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URSA-PQ: A Mobile and Flexible Pump-Probe Instrument for Gas Phase Samples at the FLASH Free Electron Laser
journal, November 2020

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journal, June 2017

Photo-cross-linking and high-resolution mass spectrometry for assignment of RNA-binding sites in RNA-binding proteins
journal, August 2014

Femtosecond Time-Resolved Photoelectron Spectroscopy
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journal, January 2020

Efficient DNA interstrand crosslinking by 6-thioguanine and UVA radiation
journal, August 2011

Magnetic field paralleliser for 2π electron-spectrometer and electron-image magnifier
journal, April 1983

The tautomeric equilibria of thio analogues of nucleic acid bases. Part 3. Ultraviolet photoelectron spectra of 2-thiouracil and its methyl derivatives
journal, January 1990

Ultrafast X-ray Auger probing of photoexcited molecular dynamics
journal, June 2014

Core-level spectroscopy and dynamics of free molecules
journal, January 2011

Experimental strategies for optical pump – soft x-ray probe experiments at the LCLS
journal, April 2014

Increase in the photoreactivity of uracil derivatives by doubling thionation
journal, January 2015

Carbon and oxygen kll and sulfur lmm auger spectra of ocs
journal, January 1990

Observing Femtosecond Fragmentation Using Ultrafast X-ray-Induced Auger Spectra
journal, July 2017

Tautomerism in 4-Hydroxypyrimidine, S -Methyl-2-thiouracil, and 2-Thiouracil
journal, December 2010

Direct observation of electron dynamics in the attosecond domain
journal, July 2005

A Static Picture of the Relaxation and Intersystem Crossing Mechanisms of Photoexcited 2-Thiouracil
journal, August 2015

The resonant Auger effect
journal, January 2000

Spatial Factors for Triplet Fusion Reaction of Singlet Oxygen Photosensitization
journal, October 2017

Electron shake-up and correlation satellites and continuum shake-off distributions in X-Ray photoelectron spectra of the rare gas atoms
journal, January 1988

4-thiothymidine sensitization of DNA to UVA offers potential for a novel photochemotherapy
journal, January 2012

Probing ultrafast ππ/nπ internal conversion in organic chromophores via K-edge resonant absorption
journal, June 2017

Photochemical and Photodynamical Properties of Sulfur-Substituted Nucleic Acid Bases,
journal, September 2018

Novel DNA lesions generated by the interaction between therapeutic thiopurines and UVA light
journal, March 2007

Simultaneous operation of two soft x-ray free-electron lasers driven by one linear accelerator
journal, June 2016

Role of Postreplicative DNA Mismatch Repair in the Cytotoxic Action of Thioguanine
journal, August 1996

Ionization and fragmentation of OCS and CS2 after photoexcitation around the sulfur 2p edge
journal, August 1997

Normal and resonant Auger spectroscopy of isocyanic acid, HNCO
journal, July 2018

Transient resonant Auger–Meitner spectra of photoexcited thymine
journal, January 2021

Photoactivation of DNA thiobases as a potential novel therapeutic option
journal, July 2001

Tracing the 267 nm-Induced Radical Formation in Dimethyl Disulfide Using Time-Resolved X-ray Absorption Spectroscopy
journal, February 2019

2-Thiouracil intersystem crossing photodynamics studied by wavelength-dependent photoelectron and transient absorption spectroscopies
journal, January 2017

Shake-up transitions in S 2p, S 2s and F 1s photoionization of the SF ₆ molecule
journal, February 2009