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Light Amplification and Nonlinear Microscopy by Stimulated Raman Scattering

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Light Amplification and Nonlinear Microscopy by Stimulated Raman Scattering Light Amplification and Nonlinear Microscopy by Stimulated Raman Scattering M. A. Ferrara1, A. D’Arco1,2, M. Indolfi1, N. Brancati3, L. Zeni2 and L. Sirleto1 1National Research Council (CNR) - Institute for Microelectronics and Microsystems, I-80131 Napoli, Italy 2Second University of Naples (SUN), Department of Information Engineering, I-81031 Aversa, Italy 3National Research Council (CNR) – Istituto di Calcolo e Reti ad Alte Prestazioni, I-80131 Napoli, Italy Keywords: Nanophotonics, Biophotonics, Nonlinear Optics, Stimulated Raman Scattering. Abstract: The Stimulated Raman Scattering has important connections with nanophotonics and biophotonics. Concerning nanophotonics, one of the most recent challenges is the investigation of ‘nonlinear optical phenomena at nanoscale’. Among them, stimulated Raman scattering is one of the most interesting, due to its significant implications from both fundamental and applicative point of view. In this paper, comparison among experimental investigations of stimulated Raman scattering in amorphous silicon nanoparticles and in silicon micro- and nano-crystals, at the wavelengths of interest for telecommunications, are reported. In addition, concerning biophotonics, first, the implementation of femtosecond Stimulated Raman Spectroscopy (f-SRS), as a single point of scanning microscopy, is described. Then, the integration of f-SRS in a laser scanning microscope and label free imaging of polystyrene-beads are demonstrated. 1 INTRODUCTION The "ideal" material for Raman amplification should have wide, flat and high Raman gain into all In silicon photonics and silicon nanophotonics, the range of interest in telecommunications (from amplification and light emission are still the most 1270 to 1650 nm). Unfortunately, as a general rule, challenging goals to get. In Stimulated Raman due to the physics behind the Raman effect, there is Scattering (SRS), a pump laser beam enters a a tradeoff for Raman amplification. In nature, we nonlinear medium and spontaneous generation and have material, for example silicon, with high Raman amplification lead to a beam at a frequency different efficiency and small bandwidth, and material, for from the pump. Raman amplification, demonstrated example silica, with a large bandwidth but with in the early 1970s, is an interesting approach for small amplification (see figure 1). The above- optical amplification, because it is only restricted by mentioned tradeoff is a fundamental limitation the pump wavelength and Raman active modes of towards the realization of micro-/nano-sources with the gain medium (Shen and Bloembergen, 1965). large emission spectra. Therefore, the investigation Raman lasing can be achieved by using SRS of new materials possessing both large Raman gain phenomenon, which permits, in principle, the coefficients and spectral bandwidth is becoming amplification in a wide interval of wavelengths, mandatory in order to satisfy the increasing from the ultraviolet to the infrared (Stolen, 2004). telecommunications demands (Refi, 1999). In order SRS is used in tunable laser development, high to overcome these limitations, a possible option is to energy pulse compression, etc. Considering bulk consider nanocomposite and nanostructured semiconductors, lasing by SRS was first discovered materials. in GaP (Nishizawa and Suto, 1980), whereas SRS Raman scattering in electrons-confined and from spherical droplets and microspheres, with photons confined materials is a fascinating research diameters 5-20 µm, has been observed using both field of great importance from both fundamental and pulsed and continuous wave probe beams (Spillane applicative point of view. Concerning the et al., 2002). Raman lasers have been also fundamental one, there have been a number of demonstrated in silicon micro-waveguides (Rong et investigations both experimental and theoretical, but al., 2005). the question is still "open" (Gaponenko et al., 2002), while from an applicative point of view, there are some important prospective, for example to realize are sensitive to the same molecular vibrations micro/nano source, with improved performances, probed in spontaneous Raman spectroscopy, but based on SRS. unlike linear Raman spectroscopy, CRS techniques The phenomenon of strong resonant and local exhibit a nonlinear dependence on the incoming enhancement of visible electro-magnetic (EM) light fields and produce coherent radiation. In CRS, radiation when incident on the surface of metallic two collinear laser beams (pump and probe) at particles and films resulting from surface plasmon different frequencies excite the sample. When the resonances, continues to attract significant attention difference in frequencies is equal to a molecular for fundamental and applied interests (Kawata, vibration, a stimulated and coherent excitation of 2009). However, the possibility of EM radiation molecular bond vibration modes (third order non- enhancement from semiconducting and insulating linear process) occur and a significant increase of materials, particularly in silicon, is noteworthy for Raman signal is observed. This latter property has silicon-based optoelectronic applications owing to popularized CRS as a microscopy modality, as it is the potential for monolithically integrating photonic intimately related to the technique’s strong optical technology and semiconductor electronics (Cao et signals that enable fast imaging applications. CRS al., 2006). Except for a report of SRS from microscopy makes it possible to achieve images individual single walled carbon nanotubes (Zhang et based on vibrational Raman contrast at imaging al., 2006), and the observation of SRS from speeds much faster than attained with conventional semiconductor nanowires (Wu et al., 2009), we find Raman microscopes. Clearly, this attribute is very no other evidence for this important nonlinear optic attractive for biological imaging, where imaging effect in nanostructured materials. speed is an important experimental parameter In biophotonics, confocal and multiphotons (Ploetz et al., 2007; Freudiger et al., 2008; Ozeki et fluorescence microscopy are important and powerful al., 2009; Nandakumar et al., 2009; Fu et al., 2013). techniques for imaging of biological samples. CRS includes two techniques: coherent anti- However, these microscopic techniques show some Stokes Raman scattering (CARS) and SRS. We note limitations, indeed, they require chemical labels that that a CARS spectrum is different from its could interfere with biological functionalities; corresponding spontaneous Raman spectrum due to additionally the photo-bleaching introduces artefacts a non-resonant background, which complicates and limits the measurement repeatability. Therefore, spectral assignment, causes difficulties in image it is necessary to introduce and implement a new interpretation, and limits detection sensitivity (Ploetz multiphotons microscopy technique suited for real et al., 2007; Freudiger et al., 2008; Ozeki et al., time imaging with high three dimensional spatial 2009; Nandakumar et al., 2009). resolution and chemical specificity of unlabeled The recent development of SRS microscopy living cells. Raman microscopy can be used as a overcame these limitations and provided better contrast mechanism based on vibrational properties. imaging contrast mechanism (vibrational) contrast. A typical Raman spectrum makes available SRS eliminates the non-resonant background information on the molecular and chemical structure problem because the generated third order SRS of the sample, offering an intrinsic chemical nonlinear polarization is directly heterodyne mixed selectivity. Nevertheless, linear Raman microscopy and amplified by the input beam with the exact same is limited to weak signals, so, to obtain an image phase, therefore always resulting in a zero non- acquisition times are very long. resonant contribution. Definitely, SRS is free from It is worth noting that, due to the recent the non-resonant background, exhibiting an identical femtoseconds laser technological development, spectrum as the spontaneous Raman it is linearly nonlinear techniques have found application in soft proportional to the concentration of the analyte, and matter and in particular in biological materials. therefore it allows straightforward quantification. In Femtoseconds laser allows to obtain an average such situations, it is natural to consider the power, incident onto the sample, lower than the application of SRS to biological microscopy. When photodamage limit and a high enough pump peak SRS microscopy was proposed (Ploetz et al., 2007; power to ensure the triggering of the nonlinear Freudiger et al., 2008; Ozeki et al., 2009), two effects. In addition, the range of pulses wavelengths, transform-limited picosecond (ps) lasers with narrow generated into the range between 680 nm and 1300 spectral bandwidth were used to excite a single nm, permits to work in the window of water Raman-active vibrational mode for fast imaging transparency, significantly reducing the absorption. with high spectral resolution. With this ps–ps Coherent Raman Scattering (CRS) techniques excitation sources it is not possible to distinguish mixed chemical species with overlapped Raman the broadening and the shift of spontaneous Raman bands in the sample because other vibrational modes emission, more than the half of C-band could be of the sample are not excited. However, in many live cover using silicon quantum dots, without biological and biomedical applications, simultaneous implementing
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