Ultrafast Strong-Field Photoemission from Plasmonic Nanoparticles

Dombi, Péter; Hörl, Anton; Rácz, Péter; Márton, István; Trügler, Andreas; Krenn, Joachim R.; Hohenester, Ulrich

doi:10.1021/nl304365e

Cited by 259 publications

(253 citation statements)

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“…Hundreds of nJ were demonstrated experimentally ( [6] and this work), and our concept can be combined with divided-pulse approaches [11]. Perceived applications range from ultrafast electron diffraction with single-electron pulses at MHz repetition rates [12,13] to various experiments in ultrafast plasmonics performed with long-cavity oscillators [14]. Many other fields of research may also benefit from the mechanisms and perspectives reported here.…”

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confidence: 78%

Conversion of chirp in fiber compression

et al. 2014

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Focusing positively chirped femtosecond pulses into nonlinear fibers provides significant spectral broadening and compression at higher pulse energies than achievable conventionally because self-focusing and damage are avoided. Here, we investigate the transfer of input to output chirp in such an arrangement. Our measurements show that the group delay dispersion of the output pulse, originating from the nonlinearities, is considerably reduced as compared to the initial value, by about a factor of 10. The mechanism of chirp reduction is understood by an interplay of selfphase modulation with initial chirp within the fiber. A simple model calculation based on this picture yields satisfactory agreement with the observations and predicts significant chirp reduction for input pulses up to the μJ regime. In practice, the reduction of chirp observed here allows for compressing the spectrally broadened intense pulses by ultrabroadband dispersive multilayer mirrors of quite moderate dispersion. Spectral broadening and pulse compression in fibers can be extended to significantly higher pulse energies by (1) using large-mode-area photonic crystal fibers [1][2][3][4][5][6] in combination with (2) chirping the input pulses [6,1]. The latter approach is particularly promising for upscaling the pulse energy because the nonlinear broadening mechanisms in the fiber scale with the pulse's peak intensity, whereas damaging effects caused by self-focusing scale with the peak power. Experiments show that chirped pulses at higher energy can provide the same amount of broadening as short pulses of lower energy [6]. Positive chirp was applied to generate 350 nJ, 16 fs pulses at a repetition rate of 5.1 MHz in this way [6]. Negatively chirped input can also result in some improvements [1], although the fiber's dispersion tends to compress the propagating pulses in a nondesired way. A central aspect of chirped broadening with practical relevance is the amount of output chirp that is generated at the high input-chirps required for making full use of the advantage of chirped broadening. Will the output chirp be low enough so that efficient compression schemes such as chirped mirrors are still practically applicable?Here we report an experimental investigation of how the input chirp converts to an output chirp during broadening in a large-mode-area fiber. The concept of our measurement is depicted in Fig. 1. A long-cavity Ti:sapphire oscillator [7] (Scientific XL, Femtolasers GmbH) provides 55 fs pulses at a central wavelength of 795 nm with ∼500 nJ of pulse energy at a repetition rate of 5.1 MHz. The system's internal prism compressor is used for inducing a well-defined group delay dispersion (D in ); this stretches the pulses in time to a duration τ in . An aspheric lens (f ≈ 40 mm) is used to focus the chirped pulses into a large-mode-area fiber (LMA-25, Thorlabs) for nonlinear broadening. The output beam is collimated with another lens (f ≈ 20 mm). The output pulses have a group delay dispersion D out and a duration τ out . The output pu...

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confidence: 78%

Conversion of chirp in fiber compression

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“…In this regime, the quantum nature of the interaction opens a new paradigm for utilizing optical gap antennas beyond the control of electromagnetic fields at the nanometer length scale [16,17]. For instance, incoming photons can exchange energy with tunneling charges modifying thus the conductance of the barrier [18,19] and strong-field effects were recently reported [20,21]. Therefore, adopting metal-based optical antennas as a disruptive technological vehicle may provide advanced functional devices to interface nanoscale electronics and photonics.…”

Section: Optical Rectificationmentioning

confidence: 99%

Nonlinear Photon-Assisted Tunneling Transport in Optical Gap Antennas

et al. 2014

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This supplementary material provides additional details about thermal effects observed in optical rectennas, and describes the observed correlation between the photocurrent and the nonlinearity of the conductance when irradiated with increasing laser intensities. I. THERMAL EFFECTSThermal effects can drastically influence the conduction properties of a laser irradiated tunneling jonction as reviewed by S. Grafström in Ref. [1]. Among possible processes resulting from photon absorption in the metal and subsequent Joule heating, let us mention thermal expansion of the gold leads, thermally-assisted field emission and thermovoltage arising from a temperature difference of the two sides of the rectenna feedgap when the laser is irradiating either one [2]. While it is difficult to completely rule out a potential heatrelated increased conductance in the results shown in the main manuscript, heat processes are providing well defined characteristics when the sample is scanned through the focus such as a contrast reversal of the current [3]. We did observe evidence for thermal currents in a rectenna consisted of an electromigrated Ti/Au stack. The ∼5 nm thick Ti layer acts a seed layer between the glass substrate and the gold layer. In the main manuscript, a Cr layer was systematically used instead of Ti and the results discussed below were never reproduced with Cr/Au rectennas. II. OPTICAL RECTIFICATIONWithin the assumptions discussed by Mayer and co-workers in Ref. [6], the classical picture of the rectified current is given by AbstractWe introduce strongly-coupled optical gap antennas to interface optical radiation with current-

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“…051401 Recent advances in nanoscience and nanotechnologies are creating new avenues for designing and making nanometerscale metal structures which respond to irradiation with electromagnetic radiation by creating a tunable induced electric field near the metal surface [1,2]. This induced "plasmonic" field originates in the incident-field-driven coherent collective motion of conduction electrons which, when stimulated near its natural resonance (plasmon) frequency, generate a very large induced polarization in subwavelength-size structures on substrate surfaces [3][4][5][6][7][8][9] and isolated nanoparticles [10]. Near metallic nanospheres and for linearly polarized incident radiation [10][11][12][13][14][15][16], the oscillating induced polarization gives rise to oscillating plasmonic fields with dipole-like angular distribution oriented along the polarization direction of the incident radiation [17].…”

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Retrieving plasmonic near-field information: A quantum-mechanical model for streaking photoelectron spectroscopy of gold nanospheres

Saydanzad

Thumm

2016

Phys. Rev. A

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Streaked photoemission from nanostructures is characterized by size-and material-dependent nanometer-scale variations of the induced nanoplasmonic response to the electronic field of the streaking pulse and thus holds promise of allowing photoelectron imaging with both subfemtosecond temporal and nanometer spatial resolution. In order to scrutinize the driven collective electronic dynamics in 10-200-nm-diameter gold nanospheres, we calculated the plasmonic field induced by streaking pulses in the infrared and visible spectral range and developed a quantum-mechanical model for streaked photoemission by extreme ultraviolet pulses. Our simulated photoelectron spectra reveal a significant amplitude enhancement and phase shift of the photoelectron streaking trace relative to calculations that exclude the induced plasmonic field. Both are most pronounced for streaking pulses tuned to the plasmon frequency and retrace the plasmonic electromagnetic field enhancement and phase shift near the nanosphere surface. DOI: 10.1103/PhysRevA.94.051401 Recent advances in nanoscience and nanotechnologies are creating new avenues for designing and making nanometerscale metal structures which respond to irradiation with electromagnetic radiation by creating a tunable induced electric field near the metal surface [1,2]. This induced "plasmonic" field originates in the incident-field-driven coherent collective motion of conduction electrons which, when stimulated near its natural resonance (plasmon) frequency, generate a very large induced polarization in subwavelength-size structures on substrate surfaces [3-9] and isolated nanoparticles [10]. Near metallic nanospheres and for linearly polarized incident radiation [10][11][12][13][14][15][16], the oscillating induced polarization gives rise to oscillating plasmonic fields with dipole-like angular distribution oriented along the polarization direction of the incident radiation [17].Strong plasmonic field enhancement effects are linked to the local dielectric properties of the nanostructure and form the underlying physical phenomenon in established surfaceenhanced Raman spectroscopy (SERS) [18] and various prototype and suggested applications, such as attosecond nanoplasmonic-field microscopy [3] and nanoplasmonically enhanced photocatalysis [19] and light harvesting [20]. The detailed understanding of plasmonic excitations in solids requires imaging techniques that resolve their spatiotemporal evolution [3,16]. While ultrafast laser technology is available in many laboratories worldwide, allowing the resolution of various aspects of the electronic dynamics during the infrared (IR)-pulse-streaked extreme ultraviolet (XUV) photoionization of gaseous atoms with a precision of about 10 as [21], a promising emerging line of attosecond science targets the electronic dynamics in solids, biomolecules, and nanostructures [2,22]. These highly time-resolved investigations on solid targets address effects that are absent in isolated atoms in the gas phase, such as the propagation of photoexcite...

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Ultrafast Strong-Field Photoemission from Plasmonic Nanoparticles

Cited by 259 publications

References 35 publications

Conversion of chirp in fiber compression

Conversion of chirp in fiber compression

Nonlinear Photon-Assisted Tunneling Transport in Optical Gap Antennas

Retrieving plasmonic near-field information: A quantum-mechanical model for streaking photoelectron spectroscopy of gold nanospheres

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