Nanoscale chemical mapping using three-dimensional adiabatic compression of surface plasmon polaritons

Angelis, Francesco De; Das, Gobind; Candeloro, Patrizio; Patrini, M.; Galli, Mattéo; Bek, Alpan; Lazzarino, Marco; Maksymov, Ivan S.; Liberale, Carlo; Andreani, Lucio Claudio; Fabrizio, E. Di

doi:10.1038/nnano.2009.348

Cited by 367 publications

(308 citation statements)

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“…As a result, SPPs can be focused beyond the diffraction limit in three dimensions on a sub-wavelength spot, with drastically enhanced optical intensity [12][13][14] . The effect of SPP adiabatic nanofocusing has been confirmed, studied and also tested for nanometre-scale microscopy in a series of earlier experiments [15][16][17][18][19] .In our investigation, this intriguing phenomenon of SPP adiabatic nanofocusing is used to generate ultrashort extreme ultraviolet (EUV) pulses directly from near-infrared (NIR) pulses. As depicted in Fig.…”

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confidence: 69%

Plasmonic generation of ultrashort extreme-ultraviolet light pulses

et al. 2011

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Ultrashort extreme-ultraviolet pulses are a key tool in timeresolved spectroscopy for the investigation of electronic motion in atoms 1,2 , molecules 3 and solids 4 . High-harmonic generation is a well-established process for producing ultrashort extreme-ultraviolet pulses by direct frequency upconversion of femtosecond near-infrared pulses [5][6][7] . However, elaborate pump-probe experiments performed on the attosecond timescale 8,9 require continuous efforts to improve the spatiotemporal coherence and also the repetition rate of the generated pulses. Here, we demonstrate a three-dimensional metallic waveguide for the plasmonic generation of ultrashort extreme-ultraviolet pulses by means of field enhancement using surface-plasmon polaritons. The intensity enhancement factor reaches a peak of ∼350, allowing generation up to the 43rd harmonic in xenon gas, with a modest incident intensity of ∼1 3 10 11 W cm -2 . The pulse repetition rate is maintained as high as 75 MHz without external cavities. The plasmonic waveguide is fabricated on a cantilever microstructure and is therefore suitable for near-field spectroscopy with nanometre-scale lateral selectivity.Surface-plasmon polaritons (SPPs) are described as the electromagnetic wave propagating along a metal-dielectric interface that results from coupling between incident photons and surface plasmons 10,11 . In nanostructured tapered waveguides, SPPs can be controlled to adiabatically follow the geometric shape of the waveguide and asymptotically stop at the tip of the taper where the local crosssectional dimension becomes infinitesimally small 12,13 . As a result, SPPs can be focused beyond the diffraction limit in three dimensions on a sub-wavelength spot, with drastically enhanced optical intensity [12][13][14] . The effect of SPP adiabatic nanofocusing has been confirmed, studied and also tested for nanometre-scale microscopy in a series of earlier experiments [15][16][17][18][19] .In our investigation, this intriguing phenomenon of SPP adiabatic nanofocusing is used to generate ultrashort extreme ultraviolet (EUV) pulses directly from near-infrared (NIR) pulses. As depicted in Fig. 1, a three-dimensional waveguide was devised to concentrate the incident NIR pulses into a sub-wavelength spot, allowing highharmonic generation of EUV light pulses to take place with high spatiotemporal coherence. The waveguide is a metallic nanostructure made of silver and has a hollow hole that takes the shape of a tapered cone with its elliptical cross-section decreasing from the inlet aperture (minor-axis diameter, 2 mm) to the exit aperture (minor-axis diameter, 100 nm). The incident NIR pulses are focused on the inlet aperture at a repetition rate of 75 MHz with a moderate intensity of 1 × 10 11 W cm 22 . While each NIR pulse propagates through the tapered hole towards the exit aperture, the electric field intensity inside the hole undergoes a substantial boost that is sustained by the SPPs driven by the incident NIR pulse. Consequently, high-harmonic EUV pulses are generate...

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confidence: 69%

Plasmonic generation of ultrashort extreme-ultraviolet light pulses

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“…Without loss of generality we choose to work around 740 nm, which corresponds to an optimal base radius of 195 nm. The tip has a radius of curvature of 5 nm, which is a realistic value for state of the art nanofabrication [36]. If not otherwise stated, the FDTD mesh has a discretization of 1 nm.…”

Section: Metal Nanoconesmentioning

confidence: 99%

“…Furthermore, such antenna architecture is fully compatible with scanning probe technology [36]. Nanofocusing relies on the propagation of surface plasmon polaritons (SPPs) along a metal nanowire [37].…”

Section: Introductionmentioning

confidence: 99%

Light scattering under nanofocusing: Towards coherent nanoscopies

Mohammadi

Agio

2012

Optics Communications

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We investigate light scattering under nanofocusing in the context of coherent spectroscopy. We discuss the different mechanisms that may enhance the signal in extinction and how these depend on nanofocusing as well as on the probed system. We find that nanofocusing may improve the detection sensitivity by orders of magnitude under realistic conditions, enabling scanning implementations of coherent spectroscopy at the nanoscale.

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“…This light source with arbitrary waveform control at the nanoscale is of a fundamentally new quality compared to both conventional far-and near-field sources. It allows for the systematic extension of near background-free scanning probe microscopy [22,26,30] to the nanoscale implementation of many forms of nonlinear and ultrafast spectroscopies for spatio-temporal imaging [31].…”

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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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Nanoscale chemical mapping using three-dimensional adiabatic compression of surface plasmon polaritons

Cited by 367 publications

References 31 publications

Plasmonic generation of ultrashort extreme-ultraviolet light pulses

Plasmonic generation of ultrashort extreme-ultraviolet light pulses

Light scattering under nanofocusing: Towards coherent nanoscopies

Femtosecond Nanofocusing with Full Optical Waveform Control

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