Untersuchung unabhängiger N‐H‐ und N‐C‐Bindungsverformungen auf ultrakurzen Zeitskalen mit resonanter inelastischer Röntgenstreuung

Eckert, Sebastian; Norell, Jesper; Miedema, Piter S.; Beye, Martin; Fondell, Mattis; Quevedo, Wilson; Kennedy, Brian; Hantschmann, Markus; Pietzsch, Annette; Van Kuiken, Benjamin E.; Ross, Matthew; Minitti, Michael P.; Moeller, Stefan P.; Schlotter, William F.; Khalil, Munira; Odelius, Michael; Föhlisch, Alexander

doi:10.1002/ange.201700239

Untersuchung unabhängiger N‐H‐ und N‐C‐Bindungsverformungen auf ultrakurzen Zeitskalen mit resonanter inelastischer Röntgenstreuung

Journal Article · Fri Apr 07 00:00:00 EDT 2017 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.201700239· OSTI ID:1352453

^[1]; Norell, Jesper ^[2]; ^[3]; ^[3]; Fondell, Mattis ^[3]; Quevedo, Wilson ^[3]; Kennedy, Brian ^[3]; Hantschmann, Markus ^[3]; ^[3]; ^[4]; ^[4]; Minitti, Michael P. ^[5]; Moeller, Stefan P. ^[5]; Schlotter, William F. ^[5]; ^[4]; ^[2]; ^[1]

Institut für Physik und Astronomie Universität Potsdam Karl-Liebknecht-Str. 24/25 14476 Potsdam Deutschland, Institute for Methods and Instrumentation for Synchrotron Radiation Research Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Albert-Einstein-Str. 15 12489 Berlin Deutschland
Department of Physics Stockholm University AlbaNova University Center 10691 Stockholm Schweden
Institute for Methods and Instrumentation for Synchrotron Radiation Research Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Albert-Einstein-Str. 15 12489 Berlin Deutschland
Department of Chemistry University of Washington Seattle WA 98195 USA
LCLS SLAC National Accelerator Laboratory 2575 Sand Hill Road Menlo Park CA 94025 USA

Abstract

Die Femtosekundendynamik nach resonanten Photoanregungen mit optischen und Röntgenpulsen ermöglicht eine selektive Verformung von chemischen N‐H‐ und N‐C‐Bindungen in 2‐Thiopyridon in wässriger Lösung. Die Untersuchung der orbitalspezifischen elektronischen Struktur und ihrer Dynamik auf ultrakurzen Zeitskalen mit resonanter inelastischer Röntgenstreuung an der N1s‐Resonanz am Synchrotron und dem Freie‐Elektronen‐Laser LCLS in Kombination mit quantenchemischen Multikonfigurationsberechnungen erbringen den direkten Nachweis dieser kontrollierten photoinduzierten Molekülverformungen und ihrer ultrakurzen Zeitskala.

View Journal Article

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515; SC0002190

OSTI ID:: 1352453

Alternate ID(s):: OSTI ID: 1352455

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 22 Vol. 129; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (25)

Molcas 8: New capabilities for multiconfigurational quantum chemical calculations across the periodic table : Molcas 8 Aquilante, Francesco; Autschbach, Jochen; Carlson, Rebecca K. Journal of Computational Chemistry, Vol. 37, Issue 5 https://doi.org/10.1002/jcc.24221	journal	November 2015
Molecular structures and protonation state of 2-Mercaptopyridine in aqueous solution Eckert, S.; Miedema, P. S.; Quevedo, W. Chemical Physics Letters, Vol. 647 https://doi.org/10.1016/j.cplett.2016.01.050	journal	March 2016
Intersystem Crossing Pathways in the Noncanonical Nucleobase 2-Thiouracil: A Time-Dependent Picture Mai, Sebastian; Marquetand, Philipp; González, Leticia The Journal of Physical Chemistry Letters, Vol. 7, Issue 11 https://doi.org/10.1021/acs.jpclett.6b00616	journal	May 2016
Energies and alkylations of tautomeric heterocyclic compounds: old problems - new answers Beak, Peter Accounts of Chemical Research, Vol. 10, Issue 5 https://doi.org/10.1021/ar50113a006	journal	May 1977
The restricted active space self-consistent-field method, implemented with a split graph unitary group approach Malmqvist, Per Aake.; Rendell, Alistair.; Roos, Bjoern O. The Journal of Physical Chemistry, Vol. 94, Issue 14 https://doi.org/10.1021/j100377a011	journal	July 1990
Solvent effects on protomeric equilibriums: quantitative correlation with an electrostatic hydrogen-bonding model Beak, Peter; Covington, Johnny B. Journal of the American Chemical Society, Vol. 100, Issue 12 https://doi.org/10.1021/ja00480a069	journal	June 1978
Convergent Proton-Transfer Photocycles Violate Mirror-Image Symmetry in a Key Melanin Monomer Olsen, Seth; Riesz, Jennifer; Mahadevan, Indu Journal of the American Chemical Society, Vol. 129, Issue 21 https://doi.org/10.1021/ja069280u	journal	May 2007
Superior Photoprotective Motifs and Mechanisms in Eumelanins Uncovered Corani, Alice; Huijser, Annemarie; Gustavsson, Thomas Journal of the American Chemical Society, Vol. 136, Issue 33 https://doi.org/10.1021/ja501499q	journal	August 2014
2,4-Dithiothymine as a Potent UVA Chemotherapeutic Agent Pollum, Marvin; Jockusch, Steffen; Crespo-Hernández, Carlos E. Journal of the American Chemical Society, Vol. 136, Issue 52 https://doi.org/10.1021/ja510611j	journal	December 2014
UV-Induced Proton Transfer between DNA Strands Zhang, Yuyuan; de La Harpe, Kimberly; Beckstead, Ashley A. Journal of the American Chemical Society, Vol. 137, Issue 22 https://doi.org/10.1021/jacs.5b03914	journal	June 2015
Displacement of protomeric equilibriums by self-association: hydroxypyridine-pyridone and mercaptopyridine-thiopyridone isomer pairs Beak, Peter; Covington, Johnny B.; Smith, Stanley G. The Journal of Organic Chemistry, Vol. 45, Issue 8 https://doi.org/10.1021/jo01296a002	journal	April 1980
Excited-State Dynamics in 6-Thioguanosine from the Femtosecond to Microsecond Time Scale Reichardt, Christian; Guo, Cao; Crespo-Hernández, Carlos E. The Journal of Physical Chemistry B, Vol. 115, Issue 12 https://doi.org/10.1021/jp112018u	journal	March 2011
Resonance Raman Spectroscopic and Theoretical Investigation of the Excited State Proton Transfer Reaction Dynamics of 2-Thiopyridone Du, Rui; Liu, Chong; Zhao, Yanying The Journal of Physical Chemistry B, Vol. 115, Issue 25 https://doi.org/10.1021/jp203185a	journal	June 2011
Ultrafast Proton Dynamics in Aqueous Amino Acid Solutions Studied by Resonant Inelastic Soft X-ray Scattering Blum, M.; Odelius, M.; Weinhardt, L. The Journal of Physical Chemistry B, Vol. 116, Issue 46 https://doi.org/10.1021/jp302958j	journal	November 2012
Information Content in O[1s] K-edge X-ray Emission Spectroscopy of Liquid Water Odelius, Michael The Journal of Physical Chemistry A, Vol. 113, Issue 29 https://doi.org/10.1021/jp903096k	journal	July 2009
Photochemistry of Pheomelanin Building Blocks and Model Chromophores: Excited-State Intra- and Intermolecular Proton Transfer El Nahhas, Amal; Pascher, Torbjörn; Leone, Loredana The Journal of Physical Chemistry Letters, Vol. 5, Issue 12 https://doi.org/10.1021/jz500720g	journal	June 2014
Orbital-specific mapping of the ligand exchange dynamics of Fe(CO)5 in solution Wernet, Ph.; Kunnus, K.; Josefsson, I. Nature, Vol. 520, Issue 7545 https://doi.org/10.1038/nature14296	journal	April 2015
Increase in the photoreactivity of uracil derivatives by doubling thionation Pollum, M.; Jockusch, S.; Crespo-Hernández, C. E. Phys. Chem. Chem. Phys., Vol. 17, Issue 41 https://doi.org/10.1039/C5CP04822B	journal	January 2015
Probing hydrogen bonding orbitals: resonant inelastic soft X-ray scattering of aqueous NH ₃ Weinhardt, L.; Ertan, E.; Iannuzzi, M. Physical Chemistry Chemical Physics, Vol. 17, Issue 40 https://doi.org/10.1039/C5CP04898B	journal	January 2015
The restricted active space followed by second-order perturbation theory method: Theory and application to the study of CuO2 and Cu2O2 systems Malmqvist, Per Åke; Pierloot, Kristine; Shahi, Abdul Rehaman Moughal The Journal of Chemical Physics, Vol. 128, Issue 20 https://doi.org/10.1063/1.2920188	journal	May 2008
Communication: The dark singlet state as a doorway state in the ultrafast and efficient intersystem crossing dynamics in 2-thiothymine and 2-thiouracil Pollum, Marvin; Crespo-Hernández, Carlos E. The Journal of Chemical Physics, Vol. 140, Issue 7 https://doi.org/10.1063/1.4866447	journal	February 2014
Dynamics of the OH group and the electronic structure of liquid alcohols Schreck, Simon; Pietzsch, Annette; Kunnus, Kristjan Structural Dynamics, Vol. 1, Issue 5 https://doi.org/10.1063/1.4897981	journal	September 2014
X-ray resonant scattering involving dissociative states Gelmukhanov, Faris; Ågren, Hans Physical Review A, Vol. 54, Issue 1 https://doi.org/10.1103/PhysRevA.54.379	journal	July 1996
Spatial Quantum Beats in Vibrational Resonant Inelastic Soft X-Ray Scattering at Dissociating States in Oxygen Pietzsch, A.; Sun, Y. -P.; Hennies, F. Physical Review Letters, Vol. 106, Issue 15 https://doi.org/10.1103/PhysRevLett.106.153004	journal	April 2011
Resonant inelastic x-ray scattering studies of elementary excitations Ament, Luuk J. P.; van Veenendaal, Michel; Devereaux, Thomas P. Reviews of Modern Physics, Vol. 83, Issue 2 https://doi.org/10.1103/RevModPhys.83.705	journal	June 2011

Similar Records

Schalten in Metall‐organischen Gerüsten

Journal Article · Sun Dec 01 19:00:00 EST 2019 · Angewandte Chemie · OSTI ID:1576806

Modellierung, Simulation und Implementierung von Zellen für die solargetriebene Wasserspaltung

Journal Article · Wed Oct 05 20:00:00 EDT 2016 · Angewandte Chemie · OSTI ID:1401229

Untersuchung unabhängiger N‐H‐ und N‐C‐Bindungsverformungen auf ultrakurzen Zeitskalen mit resonanter inelastischer Röntgenstreuung

Citation Formats

References (25)

Similar Records

Related Subjects