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7 Sep 2012

Volume 137, Issue 9, Articles (09xxxx)

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J. Chem. Phys. 137, 091706 (2012); http://dx.doi.org/10.1063/1.4746803 (10 pages)

Zhanyu Ning and John C. Polanyi
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Preface: Special Topic Section on Photochemistry at Surfaces

Horia Metiu

J. Chem. Phys. 137, 091501 (2012); http://dx.doi.org/10.1063/1.4746797 (1 page)

Online Publication Date: 4 September 2012

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This Special Topic Section on Photochemistry at Surfaces contains invited essays by several leading scientists in the field. These essays present personal perspectives on the field and provide an overview of promising areas for future research on photo-initiated processes at surfaces using advanced experimental techniques. The authors focus on fundamental aspects of the field, which also has significant future applications in photovoltaic solar cells and photocatalytic water splitting.
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82.50.-m Photochemistry
82.65.+r Surface and interface chemistry; heterogeneous catalysis at surfaces

Electron stimulated desorption, DIET, and photochemistry at surfaces: A personal recollection

John T. Yates, Jr.

J. Chem. Phys. 137, 091701 (2012); http://dx.doi.org/10.1063/1.4746798 (10 pages)

Online Publication Date: 4 September 2012

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A personal recollection of the beginning of the field of photochemistry on surfaces is given.
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82.65.+r Surface and interface chemistry; heterogeneous catalysis at surfaces
68.43.Rs Electron stimulated desorption
79.20.La Photon- and electron-stimulated desorption
82.20.Tr Kinetic isotope effects including muonium
82.50.-m Photochemistry

Electronically induced surface reactions: Evolution, concepts, and perspectives

Dietrich Menzel

J. Chem. Phys. 137, 091702 (2012); http://dx.doi.org/10.1063/1.4746799 (13 pages) | Cited 1 time

Online Publication Date: 4 September 2012

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This is a personal account of the development of the title subject which is the broader field encompassing surface photochemistry. It describes the early times when the main interest centered on desorption induced by slow electrons, follows its evolution in experiment (use of synchrotron radiation and connections to electron spectroscopies; use of lasers) and mechanisms, and briefly mentions the many different subfields that have evolved. It discusses some practically important aspects and applications and ends with an account of an evolving new subfield, the application to photochemistry on nanoparticles.
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82.65.+r Surface and interface chemistry; heterogeneous catalysis at surfaces
68.43.Rs Electron stimulated desorption
79.20.La Photon- and electron-stimulated desorption
82.50.-m Photochemistry

The road to hot electron photochemistry at surfaces: A personal recollection

J. W. Gadzuk

J. Chem. Phys. 137, 091703 (2012); http://dx.doi.org/10.1063/1.4746800 (14 pages) | Cited 1 time

Online Publication Date: 4 September 2012

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A very important part of contemporary fs-laser surface photochemistry (SPC) is based on a proposed mechanism in which a laser pulse incident upon an adsorbate-covered surface photoexcites substrate electrons which in turn inelastically scatter from atoms and molecules (chemists may call them “reactants”) in or on the surface. The present narrative outlines my own very personal SPC saga that began with early exposure to the wonders of and fascination with inelastic resonant electron scattering from gas phase atoms and molecules that dominated the Atomic and Electron Physics activities at NBS (now NIST) in 1968 when I arrived. How this lead to a fundamental understanding of important aspects of SPC is the focus of this essay.
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82.65.+r Surface and interface chemistry; heterogeneous catalysis at surfaces
82.50.-m Photochemistry

Photoexcitation of adsorbates on metal surfaces: One-step or three-step

Hrvoje Petek

J. Chem. Phys. 137, 091704 (2012); http://dx.doi.org/10.1063/1.4746801 (11 pages) | Cited 1 time

Online Publication Date: 4 September 2012

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In this essay we discuss the light-matter interactions at molecule-covered metal surfaces that initiate surface photochemistry. The hot-electron mechanism for surface photochemistry, whereby the absorption of light by a metal surface creates an electron-hole pair, and the hot electron scatters through an unoccupied resonance of adsorbate to initiate nuclear dynamics leading to photochemistry, has become widely accepted. Yet, ultrafast spectroscopic measurements of molecule-surface electronic structure and photoexcitation dynamics provide scant support for the hot electron mechanism. Instead, in most cases the adsorbate resonances are excited through photoinduced substrate-to-adsorbate charge transfer. Based on recent studies of the role of coherence in adsorbate photoexcitation, as measured by the optical phase and momentum resolved two-photon photoemission measurements, we examine critically the hot electron mechanism, and propose an alternative description based on direct charge transfer of electrons from the substrate to adsorbate. The advantage of this more quantum mechanically rigorous description is that it informs how material properties of the substrate and adsorbate, as well as their interaction, influence the frequency dependent probability of photoexcitation and ultimately how light can be used to probe and control surface femtochemistry.
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82.65.+r Surface and interface chemistry; heterogeneous catalysis at surfaces
68.43.Mn Adsorption kinetics
82.20.Hf Product distribution
82.30.Fi Ion-molecule, ion-ion, and charge-transfer reactions
82.50.Pt Multiphoton processes
82.53.St Femtochemistry of adsorbed molecules

Toward photochemistry of integrated heterogeneous systems

Yoshiyasu Matsumoto

J. Chem. Phys. 137, 091705 (2012); http://dx.doi.org/10.1063/1.4746802 (6 pages)

Online Publication Date: 4 September 2012

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This paper begins with describing the excitation mechanisms in surface photochemistry and nuclear dynamics of adsorbate induced by electronic excitation. An illustrative example is Cs adsorbate on a Cu(111) surface. This adsorption system shows drastic changes in the electronic structure with coverage; this allows us to examine different types of electronic excitations that stimulate nuclear motions of Cs. Remarks are made on challenges in photoinduced processes at well-defined surfaces: direct observations of adsorbate-substrate vibrational modes and photoinduced reactions between adsorbates. Then, the paper addresses some issues in more complex systems: metal-liquid interfaces and powdered photocatalysts of metal oxides. Photochemistry and photoinduced nuclear dynamics at metal-liquid interfaces have not been well explored. Studies on this subject may make it possible to bridge the gap between surface photochemistry and electrochemistry. Photocatalysis with powdered catalysts has been extensively studied and is still an active area, but our understanding of the mechanism of photocatalysis is far from satisfactory. Although complicated, the highly integrated systems provide an opportunity to extend our knowledge of surface photochemistry.
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82.65.+r Surface and interface chemistry; heterogeneous catalysis at surfaces
68.43.Mn Adsorption kinetics
82.20.Hf Product distribution
82.50.-m Photochemistry

Surface aligned reaction

Zhanyu Ning and John C. Polanyi

J. Chem. Phys. 137, 091706 (2012); http://dx.doi.org/10.1063/1.4746803 (10 pages) | Cited 3 times

Online Publication Date: 4 September 2012

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This paper reflects on three decades during which the study of surface aligned reaction (SAR) has advanced. The objective in SAR, which in considerable part still lies ahead, is the simultaneous control of atomic and molecular “collision energies, collision angles, and impact parameter.” Following a discussion of the benefits of such an approach we review the progress made, and, as a stimulus to experiment, present new calculations of SAR dynamics for bimolecular reaction at a metal surface. It seems reasonable to suppose that we are now entering a decade in which a combination of scanning tunneling microscopy and femtosecond laser spectroscopy will bring the full realisation of SAR.
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82.65.+r Surface and interface chemistry; heterogeneous catalysis at surfaces
78.47.J- Ultrafast spectroscopy (<1 psec)
68.49.Df Molecule scattering from surfaces (energy transfer, resonances, trapping)
79.20.Rf Atomic, molecular, and ion beam impact and interactions with surfaces
82.20.Fd Collision theories; trajectory models
82.53.-k Femtochemistry
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