Localized Multiphoton Emission of Femtosecond Electron Pulses from Metal Nanotips

Ropers, Claus; Solli, Daniel R.; Schulz, C. P.; Lienau, Christoph; Elsaesser, Thomas

doi:10.1103/physrevlett.98.043907

Cited by 369 publications

(425 citation statements)

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“…Applications are diverse and include surface enhanced Raman scattering [1,2], second [3,4] and third [5,6] harmonic generation, two-photon photoluminescence [59,60], continuum generation [61] or localized multiphoton photoemission [7,8]. Recently, even higher nonlinear effects such as above-threshold and strong-field photoemission and acceleration were observed in plasmonic and other nanostructures [12,62,63,17,15,64], closing the gap to strong-field and attosecond physics.…”

Section: Methodsmentioning

confidence: 99%

“…7 Most likely, surface plasmon polaritons are induced at the inner walls of the hollow waveguide by an incident, linearly polarized light field and propagate towards the narrowed end of the taper (see Figs. 1.9(a) and 1.12).…”

Section: Tapered Hollow Waveguidesmentioning

confidence: 99%

“…This allows for the study of numerous linear and nonlinear optical processes such as surface-enhanced Raman scattering [1,2], second [3,4] and third [5,6] harmonic generation, and multiphoton photoemission [7,8] using low-energy laser pulses with high (MHz) repetition rates. The rapidly increasing number of reports about the enhancement of optical phenomena in nanoantennas, -waveguides, -tips, -spheres, -particles, and rough surfaces impressively illustrate the growing importance of nano-optics in the natural sciences.…”

Section: Introductionmentioning

confidence: 99%

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Extreme-ultraviolet light generation in plasmonic nanostructures

et al. 2013

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The present (cumulative) thesis examines fundamentals of nanostructure-enhanced extreme-ultraviolet light generation in noble gases using two different nanostructure geometries for local field-enhancement. Specifically, resonant antennas and tapered hollow waveguide nanostructures are utilized to enhance low-energy femtosecond laser pulses, which in turn induce light emission from excited xenon, argon and neon atoms and ions. Spectral analysis of this radiation reveals that coherent high-order harmonic generation is not feasible under the examined conditions, contrary to former expectations and reports. Instead, the spectral characteristics unequivocally identify that incoherent fluorescence from multiphoton excited and strong-field ionized gas atoms is the predominant process in such schemes. Furthermore, novel nanostructure-enhanced effects are reported such as surface-enhanced fifth-order harmonic generation (from bow-tie nanoantennas) and the formation of a bistable nanoplasma (in a hollow waveguide). These effects offer intriguing links between nonlinear nano-optics, plasma dynamics and extreme-ultraviolet radiation.v vi

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Section: Methodsmentioning

confidence: 99%

Section: Tapered Hollow Waveguidesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Extreme-ultraviolet light generation in plasmonic nanostructures

et al. 2013

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“…It allows for quantum coherent control of chemical reactions [2] on the nanoscale, quantum information processing, provides a tool for nano-photonic circuit analysis, and, with the high field compression, new avenues for extreme nonlinear optics such as higher harmonic generation [12] or femtosecond electron pulse generation [32].…”

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confidence: 99%

Femtosecond Nanofocusing with Full Optical Waveform Control

et al. 2011

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The spatial confinement and temporal control of an optical excitation on nanometer length scales and femtosecond time scales has been a long-standing challenge in optics. It would provide spectroscopic access to the elementary optical excitations in matter on their natural length and time scales [1] and enable applications from ultrafast nano-opto-electronics to single molecule quantum coherent control [2]. Previous approaches have largely focused on using surface plasmon polariton (SPP) resonant nanostructures [3] or SPP waveguides [4, 5] to generate nanometer localized excitations. However, these implementations generally suffer from mode mismatch [6] between the far-field propagating light and the near-field confinement. In addition, the spatial localization in itself may depend on the spectral phase and amplitude of the driving laser pulse thus limiting the degrees of freedom available to independently control the nano-optical waveform. Here we utilize femtosecond broadband SPP coupling, by laterally chirped fan gratings, onto the shaft of a monolithic noble metal tip, leading to adiabatic SPP compression and localization at the tip apex [7, 8]. In combination with spectral pulse shaping [9, 10] with feedback on the intrinsic nonlinear response of the tip apex, we demonstrate the continuous micro-to nano-scale self-similar mode matched transformation of the propagating femtosecond SPP field into a 20 nm spatially and 16 fs temporally confined light pulse at the tip apex.Furthermore, with the essentially wavelength and phase independent 3D focusing mechanism we show the generation of arbitrary optical waveforms nanofocused at the tip. This unique femtosecond nano-torch with high nano-scale power delivery in free space and full spectral and temporal control opens the door for the extension of the powerful nonlinear and ultrafast vibrational and electronic spectroscopies to the 2 nanoscale [11, 12].In order to achieve the goal of an efficient nanometer confined femtosecond light source with independent spatial localization and temporal control of the optical field, and which can freely be manipulated in 3D, the use of the unique properties of surface plasmon polaritons (SPP's) has long been discussed as a potential solution. It is well established that the strong surface field localization and size and shape dependent resonances of SPP's as electromagnetic surface waves associated with collective charge density oscillations at noble metal-dielectric interfaces allow for sub-wavelength spatial control of even broadband optical fields [13]. Elegant solutions to overcome the SPP diffraction limit [14] and achieve nano-focusing based on interference of localized SPP modes exist in the form of specially arranged cascaded, percolated, or self-similar chains of metal nanostructures as optical antennas [3,15,16]. However, the achievable optical waveforms at the nano-focus are often constrained by the phase relationship between the spectral modes already necessary to achieve the 3D nano-focusing [5]. This limits ...

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“…Recently, the optically induced emission of ultrafast electron bursts from single metallic nanostructures attracts substantial interest [1,2]. Due to the high-order nonlinearity of the emission process, such electron bursts are expected to have durations much shorter than a single field cycle.…”

Section: Introductionmentioning

confidence: 99%