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Following Metal-to-Ligand Charge-Transfer Dynamics with Ligand and Spin Specificity Using Femtosecond Resonant Inelastic X-ray Scattering at the Nitrogen K-Edge

Jay, Raphael (author)
Uppsala universitet,Institutionen för fysik och astronomi,Univ Potsdam, Inst Phys & Astron, D-14476 Potsdam, Germany.
Eckert, Sebastian (author)
Univ Potsdam, Inst Phys & Astron, D-14476 Potsdam, Germany.;Uppsala Univ, Dept Phys & Astron, S-5120 Uppsala, Sweden.;Helmholtz Zentrum Berlin Mat & Energie, Inst Methods & Instrumentat Synchrotron Radiat Re, D-12489 Berlin, Germany.
Van Kuiken, Benjamin E. (author)
European XFEL, D-22869 Schenefeld, Germany.
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Ochmann, Miguel (author)
Univ Hamburg, Dept Phys, D-22761 Hamburg, Germany.;Ctr Free Electron Laser Sci, D-22761 Hamburg, Germany.
Hantschmann, Markus (author)
Uppsala universitet,Institutionen för fysik och astronomi,Univ Potsdam, Inst Phys & Astron, D-14476 Potsdam, Germany.;Uppsala Univ, Dept Phys & Astron, S-5120 Uppsala, Sweden.;Helmholtz Zentrum Berlin Mat & Energie, Inst Methods & Instrumentat Synchrotron Radiat Re, D-12489 Berlin, Germany.
Cordones, Amy A. (author)
Lawrence Berkeley Natl Lab, Ultrafast Xray Sci Lab, Chem Sci Div, Berkeley, CA 94720 USA.;SLAC Natl Accelerator Lab, Stanford PULSE Inst, Menlo Pk, CA 94025 USA.
Cho, Hana (author)
Lawrence Berkeley Natl Lab, Ultrafast Xray Sci Lab, Chem Sci Div, Berkeley, CA 94720 USA.;Pusan Natl Univ, Dept Chem, Busan 46241, South Korea.;Pusan Natl Univ, Chem Inst Funct Mat, Busan 46241, South Korea.
Hong, Kiryong (author)
Pusan Natl Univ, Dept Chem, Busan 46241, South Korea.;Pusan Natl Univ, Chem Inst Funct Mat, Busan 46241, South Korea.
Ma, Rory (author)
Univ Hamburg, Dept Phys, D-22761 Hamburg, Germany.;Ctr Free Electron Laser Sci, D-22761 Hamburg, Germany.;Pohang Accelerator Lab, Pohang 37673, Gyeongbuk, South Korea.;Pusan Natl Univ, Dept Chem, Busan 46241, South Korea.;Pusan Natl Univ, Chem Inst Funct Mat, Busan 46241, South Korea.
Lee, Jae Hyuk (author)
Lawrence Berkeley Natl Lab, Ultrafast Xray Sci Lab, Chem Sci Div, Berkeley, CA 94720 USA.
Dakovski, Georgi L. (author)
SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA.
Turner, Joshua J. (author)
SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA.;Stanford Univ, Stanford Inst Mat & Energy Sci, Stanford, CA 94305 USA.
Minitti, Michael P. (author)
SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA.
Quevedo, Wilson (author)
Helmholtz Zentrum Berlin Mat & Energie, Inst Methods & Instrumentat Synchrotron Radiat Re, D-12489 Berlin, Germany.
Pietzsch, Annette (author)
Helmholtz Zentrum Berlin Mat & Energie, Inst Methods & Instrumentat Synchrotron Radiat Re, D-12489 Berlin, Germany.
Beye, Martin (author)
Helmholtz Zentrum Berlin Mat & Energie, Inst Methods & Instrumentat Synchrotron Radiat Re, D-12489 Berlin, Germany.;DESY, D-22607 Hamburg, Germany.
Kim, Tae Kyu (author)
Yonsei Univ, Dept Chem, Seoul 03722, South Korea.
Schoenlein, Robert W. (author)
Lawrence Berkeley Natl Lab, Ultrafast Xray Sci Lab, Chem Sci Div, Berkeley, CA 94720 USA.
Wernet, Philippe, 1971- (author)
Uppsala universitet,Kemisk och biomolekylär fysik,Uppsala Univ, Dept Phys & Astron, S-5120 Uppsala, Sweden.
Foehlisch, Alexander (author)
Univ Potsdam, Inst Phys & Astron, D-14476 Potsdam, Germany.;Uppsala Univ, Dept Phys & Astron, S-5120 Uppsala, Sweden.;Helmholtz Zentrum Berlin Mat & Energie, Inst Methods & Instrumentat Synchrotron Radiat Re, D-12489 Berlin, Germany.
Huse, Nils (author)
Univ Hamburg, Dept Phys, D-22761 Hamburg, Germany.;Ctr Free Electron Laser Sci, D-22761 Hamburg, Germany.
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 (creator_code:org_t)
2021-07-14
2021
English.
In: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 12:28, s. 6676-6683
Related links:
https://urn.kb.se/re...
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https://doi.org/10.1...
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  • Journal article (peer-reviewed)
Abstract Subject headings
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  • We demonstrate for the case of photoexcited [Ru(2,2'-bipyridine)(3)](2+) how femtosecond resonant inelastic X-ray scattering (RIXS) at the ligand K-edge allows one to uniquely probe changes in the valence electronic structure following a metal-to-ligand charge-transfer (MLCT) excitation. Metal-ligand hybridization is probed by nitrogen-1s resonances providing information on both the electron-accepting ligand in the MLCT state and the hole density of the metal center. By comparing to spectrum calculations based on density functional theory, we are able to distinguish the electronic structure of the electron-accepting ligand and the other ligands and determine a temporal upper limit of (250 +/- 40) fs for electron localization following the charge-transfer excitation. The spin of the localized electron is deduced from the selection rules of the RIXS process establishing new experimental capabilities for probing transient charge and spin densities.

Subject headings

NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)
NATURVETENSKAP  -- Kemi -- Teoretisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Theoretical Chemistry (hsv//eng)

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