Femtochemistry at Metal Surfaces:  Nonadiabatic Reaction Dynamics

Frischkorn, Christian; Wolf, Martin

doi:10.1021/cr050161r

Cited by 329 publications

(377 citation statements)

References 169 publications

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“…Various spectroscopic techniques have been used to probe chemical reactions at interfaces. Since surface chemical reactions involve structural changes, many spectroscopic techniques, such as electron energy loss spectroscopy (EELS), [5][6][7][8] infrared (IR) spectroscopy, 9,10 Raman spectroscopy 9,11,12 and sum frequency generation (SFG) spectroscopy [12][13][14] have been widely used to probe vibrational structures and their changes in surface chemical reactions. In addition, scanning tunnelling microscopy (STM) has also been utilized to study surface chemical reactions by exploiting its ability to probe changes in electronic structure and large geometric changes of species reacting at a surface.…”

Section: Introductionmentioning

confidence: 99%

Surface photochemistry probed by two-photon photoemission spectroscopy

Zhou

Ren

et al. 2012

Energy Environ. Sci.

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Two-photon photoemission (2PPE) has been widely used in the study of electronic structure and dynamics of unoccupied electronic states on different types of surfaces and interfaces. Since 2PPE probes electronically excited states, it should be sensitive to surface excited electronic structure changes that accompany surface chemical reactions. Therefore, this method could potentially be used to study the kinetics and dynamics of surface chemical reactions as well as surface photocatalysis. In this article, we briefly review recent progress made in the study of surface photochemistry and photocatalysis using the time-dependent 2PPE (TD-2PPE) method. A few examples are given to demonstrate the application of this method in probing surface photochemistry and photocatalysis, particularly photocatalysis of methanol on TiO 2 surfaces. Since many problems associated with surface photochemistry and surface photocatalysis are related to energy and environmental issues, the 2PPE technique could have important applications in the study of the fundamental problems in energy and environmental sciences.

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Section: Introductionmentioning

confidence: 99%

Surface photochemistry probed by two-photon photoemission spectroscopy

Zhou

Ren

et al. 2012

Energy Environ. Sci.

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“…This method is a well-known technique in the field of mass spectroscopy developed by John B. Fenn and Koichi Tanaka to whom the chemistry Nobel prize 2002 [16] was awarded. Desorption from metallic surfaces with the help of femtosecond laser pulses is essentially triggered by excited electrons within the metallic substrate [17,18]. On femtosecond time scale, electrons obey a nonequilibrium energy distribution [19,20].…”

Section: Introductionmentioning

confidence: 99%

“…Higher occupied electron states in the substrate enable electron transfer to the adsorbate, thus inducing chemical reactions, i.e., desorption. On the femto-to picosecond time scale, also an enhanced electron temperature, as compared to the lattice, can induce desorption [17,18]. In contrast, for nanosecond irradiation heating proceeds slowly and electronic nonequilibrium plays no role.…”

Section: Introductionmentioning

confidence: 99%

Influence of fs-laser desorption on target normal sheath accelerated ions

Hoffmeister

Bellei

Harres

et al. 2013

Phys. Rev. ST Accel. Beams

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We report on the effects of fs-laser desorption on the ion acceleration induced by the target normal sheath acceleration (TNSA) mechanism. The experiment was performed at the Lawrence Livermore National Laboratory (LLNL) using the 100 TW Callisto laser of the Jupiter Laser Facility (JLF). Thin metal foils (Au, Cu, and Al) with thicknesses ranging from 10 to 20 m were irradiated by a variable number of low intensity ($ 10 12 W=cm 2 ) laser pulses, the last one arriving 100 ms before the main pulse. With these short pulses water vapor and hydrocarbon contaminations could stepwise be removed from the target surface. Substantial modifications of the TNSA-ion energy spectra were observed such as diminished proton energy and intensity, the absence of low-charged ion states, increased particle numbers for C 4þ and O 6þ ions in the higher energetic part of their particle spectra as well as the acceleration of target ions. The controlled application of fs-laser desorption on the laser-ion acceleration thus strongly influences the ion spectra and offers the possibility of selecting a targeted range of ion species for the acceleration to higher energies due to the systematic removal of contamination layers.

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“…Since these original studies, the field of femtochemistry has rapidly evolved and it is not the aim of this perspective to review this development. Rather, the reader is referred to a number of excellent articles, reviews and books that have appeared over the years (3)(4)(5)(6)(7)(8)(9)(10)(11)(12)(13)(14)(15).…”

Section: Introductionmentioning

confidence: 99%

Electronic structure in real time: mapping valence electron rearrangements during chemical reactions

Wernet

2011

Phys. Chem. Chem. Phys.

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The interest in following the evolution of the valence electronic structure of atoms and molecules during chemical reactions on a femtosecond time scale is discussed. By explicitly mapping the occupied part of the electronic structure with femtosecond pump-probe schemes one essentially follows the electrons making the bonds while the bonds change. This holds the key to unprecedented insight into chemical bonding in short-lived intermediates and reveals the coupled motion of electrons and nuclei. Examples from the recent literature on small molecules and anionic clusters in the gas phase and on atoms and molecules on surfaces using lab-based femtosecond laser methods are used to demonstrate the case. They highlight how the evolution of the valence electronic structure can be probed with time-resolved photoelectron spectroscopy with ultraviolet (UV) probe photon energies of up to 6 eV. It is shown how new insight can be gained by extending the probing wavelength into the vacuumultraviolet (VUV) region to photon energies of 20 eV and more by accessing the whole occupied valence electronic structure with time-resolved VUV photoelectron spectroscopy.Finally, the importance of soft x-ray free-electron lasers with probe photon energies of several hundred eV and femtosecond pulses and in particular the key role of femtosecond timeresolved soft x-ray emission spectroscopy or resonant inelastic x-ray scattering for mapping the electronic structure during chemical reactions is discussed.2

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Femtochemistry at Metal Surfaces: Nonadiabatic Reaction Dynamics

Cited by 329 publications

References 169 publications

Surface photochemistry probed by two-photon photoemission spectroscopy

Surface photochemistry probed by two-photon photoemission spectroscopy

Influence of fs-laser desorption on target normal sheath accelerated ions

Electronic structure in real time: mapping valence electron rearrangements during chemical reactions

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