Real-Time Observation of Surface Bond Breaking with an X-ray Laser

被引:174
作者
Dell'Angela, M. [1 ,2 ]
Anniyev, T. [3 ]
Beye, M. [3 ,4 ]
Coffee, R. [5 ]
Foehlisch, A. [4 ,6 ]
Gladh, J. [7 ]
Katayama, T. [3 ]
Kaya, S. [3 ]
Krupin, O. [5 ,8 ]
LaRue, J. [3 ]
Mogelhoj, A. [9 ,10 ]
Nordlund, D. [11 ]
Norskov, J. K. [9 ,12 ]
Oberg, H. [7 ]
Ogasawara, H. [11 ]
Ostrom, H. [7 ]
Pettersson, L. G. M. [7 ]
Schlotter, W. F. [5 ]
Sellberg, J. A. [3 ,7 ]
Sorgenfrei, F. [1 ,2 ]
Turner, J. J. [5 ]
Wolf, M. [13 ]
Wurth, W. [1 ,2 ]
Nilsson, A. [3 ,7 ,9 ,11 ]
机构
[1] Univ Hamburg, D-22761 Hamburg, Germany
[2] Ctr Free Electron Laser Sci, D-22761 Hamburg, Germany
[3] SLAC Natl Accelerator Lab, SIMES, Menlo Pk, CA 94025 USA
[4] Mat & Energie GmbH, Helmholtz Zentrum Berlin, Inst Methods & Instrumentat Synchrotron Radiat Re, D-12489 Berlin, Germany
[5] SLAC Natl Accelerator Lab, Linac Coherent Light Source, Menlo Pk, CA 94025 USA
[6] Univ Potsdam, Inst Phys & Astron, D-14476 Golm, Germany
[7] Stockholm Univ, AlbaNova Univ Ctr, Dept Phys, SE-10691 Stockholm, Sweden
[8] European Xray Free Electron Laser XFEL GmbH, D-22761 Hamburg, Germany
[9] SLAC Natl Accelerator Lab, Sustainable Energy Catalysis SUNCAT Ctr Interface, Menlo Pk, CA 94025 USA
[10] Tech Univ Denmark, Dept Phys, Ctr Atom Scale Mat Design CAMD, DK-2800 Lyngby, Denmark
[11] SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA
[12] Stanford Univ, Dept Chem Engn, SUNCAT Ctr Interface Sci & Catalysis, Stanford, CA 95305 USA
[13] Max Planck Gesell, Fritz Haber Inst, D-14195 Berlin, Germany
关键词
EMISSION SPECTROSCOPY; DESORPTION-KINETICS; MOLECULAR-MOTION; METAL-SURFACES; CO; DYNAMICS; ADSORPTION; RU(001);
D O I
10.1126/science.1231711
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
We used the Linac Coherent Light Source free-electron x-ray laser to probe the electronic structure of CO molecules as their chemisorption state on Ru(0001) changes upon exciting the substrate by using a femtosecond optical laser pulse. We observed electronic structure changes that are consistent with a weakening of the CO interaction with the substrate but without notable desorption. A large fraction of the molecules (30%) was trapped in a transient precursor state that would precede desorption. We calculated the free energy of the molecule as a function of the desorption reaction coordinate using density functional theory, including van der Waals interactions. Two distinct adsorption wells-chemisorbed and precursor state separated by an entropy barrier-explain the anomalously high prefactors often observed in desorption of molecules from metals.
引用
收藏
页码:1302 / 1305
页数:5
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