Infrared-laser-induced photodesorption of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi mathvariant="normal">NH</mml:mi></mml:mrow><mml:mrow><mml:mn>3</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math>and<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi mathvariant="normal">ND</mml:mi></mml:mrow><mml:mrow><mml:mn>3</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math>adsorbed on s

Hussla, Ingo; Seki, H.; Chuang, T. J.; Gortel, Zbigniew W.; Kreuzer, H. J.; Piercy, P.

doi:10.1103/physrevb.32.3489

Cited by 108 publications

(27 citation statements)

References 28 publications

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“…In the first case, either infrared (IR) 17 or, more commonly, ultraviolet/visible (UV/vis) photons 1 couple directly to the dipole or transition dipole moment of the adsorbate-substrate complex. For weakly bound adsorbates, the black body radiation at ambient temperatures suffices to induce direct desorption.…”

Section: Mechanisms Of Photodesorptionmentioning

confidence: 99%

“…17 Using a master equation, which took phonon and electronic damping and molecular dipole coupling into account, it was argued 17 that the desorption mechanism is a thermal process arising from "resonant heating". Accordingly, the N-H bond serves as an "antenna" that directs radiation energy, via surface phonons, to the molecule-surface bond, to break it.…”

Section: Intramolecular Resonant Excitation and Predesorptionmentioning

confidence: 99%

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Quantum Dynamical Approach to Ultrafast Molecular Desorption from Surfaces

2006

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Section: Mechanisms Of Photodesorptionmentioning

confidence: 99%

Section: Intramolecular Resonant Excitation and Predesorptionmentioning

confidence: 99%

Quantum Dynamical Approach to Ultrafast Molecular Desorption from Surfaces

2006

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“…Damping of the incident vibrational energy is necessary for trapping only if significant mechanical coupling exists between the incident molecule's vibration and the translation degree of freedom along the surface normal (V-T coupling). Unsuccessful attempts 23,24 to achieve isotope selective desorption by vibrational excitation of physisorbed molecules from insulator and metal surfaces showed that vibration/translation coupling is often negligible compared to the coupling to the surface modes, even for insulators such as NaCl. 23 The lack of isotope selectivity and the observation of a laser fluence threshold for vibrational pre-desorption were interpreted in terms of a resonant heating mechanism 25 where the substrate temperature is raised due to vibrational energy transfer from internal modes of the adsorbate to surface vibrations (phonons) leading to thermal desorption.…”

Section: B Insensitivity Of Sticking To Vibrational Excitationmentioning

confidence: 99%

The sticking probability of D2O-water on ice: Isotope effects and the influence of vibrational excitation

Hundt

Bisson

Beck

2012

The Journal of Chemical Physics

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The present study measures the sticking probability of heavy water (D 2 O) on H 2 O-and on D 2 O-ice and probes the influence of selective OD-stretch excitation on D 2 O sticking on these ices. Molecular beam techniques are combined with infrared laser excitation to allow for precise control of incident angle, translational energy, and vibrational state of the incident molecules. For a translational energy of 69 kJ/mol and large incident angles (θ ≥ 45 • ), the sticking probability of D 2 O on H 2 O-ice was found to be 1% lower than on D 2 O-ice. OD-stretch excitation by IR laser pumping of the incident D 2 O molecules produces no detectable change of the D 2 O sticking probability (<10 −3 ). The results are compared with other gas/surface systems for which the effect of vibrational excitation on trapping has been probed experimentally.

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“…So far, there has been only indirect experimental confirmation of the calculated transient temperature jump. 5,8 Because of the rapidity of the heating and cooling in pulsed laser excitation, which is typically several nanoseconds in duration, direct probing of the surface-temperature history has proven to be difficult.Here, we introduce a technique based on resonant second-harmonic generation (SHG) that is capable of ultrafast measurement of surface temperature. SHG has recently been exploited in many studies because of its sensitivity to changes at an interface.…”

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confidence: 99%

Can Pulsed Laser Excitation of Surfaces Be Described by a Thermal Model?

et al. 1988

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In using pulsed laser excitation of surfaces to induce desorption or reaction of adsorbed molecules, it has generally been assumed that the absorbed energy is rapidly randomized, and a thermal model can be used to calculate the surface-temperature change. In this work, the transient temperature jump on a Ag(llO) surface induced by an 8-nsec laser pulse is directly monitored with a psec probe pulse. The probe is based on a temperature-dependent second-harmonic-generation effect. The experiment provides the first direct evidence that the heat-diffusion model can correctly predict the magnitude and the time evolution of the temperature on the surface. PACS numbers: 79.20.Ds, 42.65.Ky, 68.35.Md The use of lasers to induce and probe chemical and physical processes on surfaces is a subject of much recent interest in surface science. x There are a few unique advantages in using lasers to excite an adsorbate/substrate system to induce surface reactions. The initial excitation is mode specific and may lead to the possibility of nonstatistical reaction channels. In many cases, however, thermalization of the initial excitation may be fast compared to the reaction rate, and all reactions would then proceed under thermal conditions. Even for this latter case of equilibration of the initially absorbed energy, the rapid (>10 10 deg/sec) temperature rise caused by pulsed laser excitation can change the relative yields of products coming from competing chemical pathways. The latter advantage has been demonstrated in studies of surface reactions. 2 In order to correctly interpret the events following pulsed laser excitation of surfaces, it is essential to know the time scale of thermalization from the initially excited mode, and the resultant surface-temperature increase. An accurate account of the temperature evolution on the surface is essential to properly determine the kinetic parameters of the surface process.Many surface studies have used powerful nanosecond laser pulses to excite metal substrates in order to induce surface processes. 2 " 9 In all cases, the transient temperature jump at the surface is not experimentally determined, but is calculated by a classical heat-diffusion model. 10 ' 11 This model assumes that the energy absorbed into a specific mode thermalizes instantaneously and that the transfer of heat from the surface to the bulk can be treated by use of bulk heat-diffusion constants. Furthermore, several working assumptions have been widely used to reduce the complexity of the calculation, such as that higher-order terms in the heat-transfer equation can be neglected.For excitation of metals using light from the near ir to the uv, intraband or interband electronic transitions are involved. Several femtosecond experiments have been performed recently for a variety of metals, where the rates of electron relaxation through electron-phonon collisions where shown to be of the order of several picoseconds. 12 " 15 Therefore, it is reasonable to assume that, on a nanosecond time scale, thermal equilibrium is est...

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Infrared-laser-induced photodesorption ofNH3andND3adsorbed on s

Cited by 108 publications

References 28 publications

Quantum Dynamical Approach to Ultrafast Molecular Desorption from Surfaces

Quantum Dynamical Approach to Ultrafast Molecular Desorption from Surfaces

The sticking probability of D2O-water on ice: Isotope effects and the influence of vibrational excitation

Can Pulsed Laser Excitation of Surfaces Be Described by a Thermal Model?

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