Few-Femtosecond Plasmon Dephasing of a Single Metallic Nanostructure from Optical Response Function Reconstruction by Interferometric Frequency Resolved Optical Gating

Anderson, Alexandria; Deryckx, Kseniya S.; Xu, Xiaoji G.; Steinmeyer, Günter; Raschke, Markus B.

doi:10.1021/nl101090s

Cited by 135 publications

(136 citation statements)

References 47 publications

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“…[4][5][6][7][8] This role continues for understanding the ultrafast electron dynamics of metals. [9][10][11][12][13][14][15] Silver in particular assume a special status due to its high optical conductivity and wide range of applications from mirrors to plasmonics and optical metamaterials.…”

Section: Introductionmentioning

confidence: 99%

Optical dielectric function of silver

et al. 2015

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The dielectric function of silver is a fundamental quantity related to its electronic structure and describes its optical properties. However, results published over the past six decades are in part inconsistent and exhibit significant discrepancies. The measurement is experimentally challenging with the values of dielectric function spanning over five orders of magnitude from the mid-infrared to the visible/ultraviolet spectral range. Using broadband spectroscopic ellipsometry, we determine the complex valued dielectric function of evaporated and template stripped polycrystalline silver films from 0.05 eV (λ = 25 µm) to 4.14 eV (λ = 300 nm) with a statistical uncertainty of less than 1%. From Drude analysis of the 0.1 -3 eV range, values of the plasma frequency ω p = 8.9 ± 0.2 eV, dielectric function at infinite frequency ∞ = 5 ± 2, and relaxation time τ = 1/Γ = 17 ± 3 fs are obtained, with the absolute uncertainties estimated from systematic errors and experimental repeatability. Further analysis based on the extended Drude model reveals an increase in τ with decreasing frequency in agreement with Fermi liquid theory, and extrapolates to τ 22 fs for zero frequency. A deviation from simple Fermi liquid behavior is suggested at energies below 0.1 eV (λ = 12 µm) with the onset of a further increase in τ connecting to the DC value from transport measurements of ∼ 40 fs. The results are consistent with a wide range of optical and plasmonic experiments throughout the infrared and visible/ultraviolet spectral range. The influence of grain boundaries, defect scattering, and surface oxidation is discussed. The results are compared with our previous measurements of the dielectric function of gold [Phys. Rev. B 86, 235147 (2012)].

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Section: Introductionmentioning

confidence: 99%

Optical dielectric function of silver

et al. 2015

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“…[4][5][6][7] However, there are two fundamental limitations on the confinement of light in the femtosecond and nanometer regimes: on the one hand, femtosecond pulses are prone to becoming distorted in the phase domain while propagating through dispersive elements, such as lenses or objectives. Such distortions typically result in a stretched pulse: i.e., longer than the Fourier limit.…”

Section: Introductionmentioning

confidence: 99%

Phase control of femtosecond pulses on the nanoscale using second harmonic nanoparticles

et al. 2014

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Investigations of ultrafast processes occurring on the nanoscale require a combination of femtosecond pulses and nanometer spatial resolution. However, controlling femtosecond pulses with nanometer accuracy is very challenging, as the limitations imposed both by dispersive optics on the time duration of a pulse and by the spatial diffraction limit on the focusing of light must be overcome simultaneously. In this paper, we provide a universal method that allows full femtosecond pulse control in subdiffraction-limited areas. We achieve this aim by exploiting the intrinsic coherence of the second harmonic emission from a single nonlinear nanoparticle of deep subwavelength dimensions. The method is proven to be highly sensitive, easy to use, quick, robust and versatile. This approach allows measurements of minimal phase distortions and the delivery of tunable higher harmonic light in a nanometric volume. Moreover, the method is shown to be compatible with a wide range of particle sizes, shapes and materials, allowing easy optimization for any given sample. This method will facilitate the investigation of light-matter interactions on the femtosecond-nanometer level in various areas of scientific study.

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“…The MIIPS-optimized pulses are then characterized via interferometric frequency resolved optical gating (IFROG) [25] and the pulse transient is reconstructed with phase and amplitude information from the DC portion of the spectrogram using a standard FROG retrieval algorithm. The pulse replicas as required for the IFROG autocorrelation measurements are themselves generated with the pulse shaper.…”

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“…While the tips used in our off-resonant experiments shown here typically exhibit SPP resonances in the vicinity of 650 nm, the use of localized tip SPP's with measured dephasing times of up to T 2 ≃ 20 fs [25] can provide additional capability for tailoring the optical waveform with higher field enhancement, albeit at the expense of minimal pulse duration.…”

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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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Few-Femtosecond Plasmon Dephasing of a Single Metallic Nanostructure from Optical Response Function Reconstruction by Interferometric Frequency Resolved Optical Gating

Cited by 135 publications

References 47 publications

Optical dielectric function of silver

Optical dielectric function of silver

Phase control of femtosecond pulses on the nanoscale using second harmonic nanoparticles

Femtosecond Nanofocusing with Full Optical Waveform Control

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