Desorption induced by femtosecond laser pulses

Prybyla, J. A.; Heinz, Tony F.; Misewich, J.; Loy, M. M. T.; Glownia, J. H.

doi:10.1103/physrevlett.64.1537

Cited by 260 publications

(132 citation statements)

References 28 publications

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“…The most detailed experimental probes of such mechanisms are pumpprobe measurements, where two laser pulses with a variable delay are used to excite electronic transitions in a molecule and then probe the progress of the chemical reaction that ensues on femtosecond timescales. In the field of femtochemistry, such techniques have been invaluable for tracking reaction mechanisms or even for changing the branching ratios of different processes [104][105][106][107][108][109][110][111][112][113][114][115]. These techniques are now becoming useful to probe the highly non-equilibrium processes driven by plasmonic hot carriers [36,39,116].…”

Section: Molecular Injection: Plasmon-enhanced Catalysis and Femtochementioning

confidence: 99%

Plasmonic hot carrier dynamics in solid-state and chemical systems for energy conversion

2016

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Surface plasmons provide a pathway to efficiently absorb and confine light in metallic nanostructures, thereby bridging photonics to the nano scale. The decay of surface plasmons generates energetic 'hot' carriers, which can drive chemical reactions or be injected into semiconductors for nano-scale photochemical or photovoltaic energy conversion. Novel plasmonic hot carrier devices and architectures continue to be demonstrated, but the complexity of the underlying processes make a complete microscopic understanding of all the mechanisms and design considerations for such devices extremely challenging. Here, we review the theoretical and computational efforts to understand and model plasmonic hot carrier devices. We split the problem into three steps: hot carrier generation, transport and collection, and review theoretical approaches with the appropriate level of detail for each step along with their predictions. We identify the key advances necessary to complete the microscopic mechanistic picture and facilitate the design of the next generation of devices and materials for plasmonic energy conversion.

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Section: Molecular Injection: Plasmon-enhanced Catalysis and Femtochementioning

confidence: 99%

Plasmonic hot carrier dynamics in solid-state and chemical systems for energy conversion

2016

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“…4 It is by no means trivial that the desorption rate should follow a power law and calculating the exponent of a particular system is a major challenge of any DIMET model.…”

Section: Dimet Desorption Ratesmentioning

confidence: 99%

“…Photoinduced desorption had already been observed for a few adsorbate systems 1,2 using lowintensity nanosecond laser pulses, but high-intensity femtosecond laser pulses have been shown to induce desorption in a large class of adsorbate systems [3][4][5][6][7][8][9][10] and induce chemical reactions which cannot proceed by thermal heating. 11 The mechanism attributed to these reactions is excitation of substrate electrons by the laser pulse.…”

Section: Introductionmentioning

confidence: 99%

Hot-electron-mediated desorption rates calculated from excited-state potential energy surfaces

2009

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We present a model for desorption induced by ͑multiple͒ electronic transitions ͓DIET ͑DIMET͔͒ based on potential energy surfaces calculated with the delta self-consistent field extension of density-functional theory. We calculate potential energy surfaces of CO and NO molecules adsorbed on various transition-metal surfaces and show that classical nuclear dynamics does not suffice for propagation in the excited state. We present a simple Hamiltonian describing the system with parameters obtained from the excited-state potential energy surface and show that this model can describe desorption dynamics in both the DIET and DIMET regimes and reproduce the power-law behavior observed experimentally. We observe that the internal stretch degree of freedom in the molecules is crucial for the energy transfer between the hot electrons and the molecule when the coupling to the surface is strong.

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“…9 In the case of desorption induced by multiple electronic transitions (DIMET) the intensity of the desorbate signal is known to increase nonlinearly with laser intensity. 10 This is thought to be a signature of the multielectron nature of the adsorbate excitation prior to desorption. In the case of DIMET there is a correlation between the desorbate kinetic energy and the incident laser intensity.…”

Section: Introductionmentioning

confidence: 99%

Femtosecond Near-Infrared Laser Desorption of Multilayer Benzene on Pt{111}: A Molecular Newton's Cradle?

et al. 2000

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Velocity distributions resulting from the intense, near-IR laser desorption of multilayers of benzene adsorbed on Pt{111} are reported as a function of laser intensity, which was varied by changing fluence and pulse width. The velocity distributions as a function of intensity show characteristics of both thermally and electronically induced desorption. Changing the pulse width from the subpicosecond to the subnanosecond regime only results in a small quantitative change in the velocity distributions, suggesting a similar desorption mechanism for laser pulse duration spanning 3 orders of magnitude. Possible mechanisms are discussed and a new mechanism is proposed in which the process is initiated by a thermally assisted DIET excitation in the chemisorbed layer, and followed by energy transfer from the Pt-benzene interface to the outermost benzene layers via a molecular Newton's cradle mechanism.

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Desorption induced by femtosecond laser pulses

Cited by 260 publications

References 28 publications

Plasmonic hot carrier dynamics in solid-state and chemical systems for energy conversion

Plasmonic hot carrier dynamics in solid-state and chemical systems for energy conversion

Hot-electron-mediated desorption rates calculated from excited-state potential energy surfaces

Femtosecond Near-Infrared Laser Desorption of Multilayer Benzene on Pt{111}: A Molecular Newton's Cradle?

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