Frequency modulation stimulated Raman scattering scheme for real-time background correction with a single light source.

A frequency modulation (FM) scheme for stimulated Raman scattering (SRS) is presented with a single fiber-based light source. Pulse-to-pulse wavelength-switching allows real-time subtraction of parasitic signals leaving only the resonant SRS signal with a noise reduction of up to 30 % compared to digital subtraction schemes, leading effectively to a contrast improvement by a factor of up to 8.3. The wide tuning range of the light source from 1500 cm-1 to 3000 cm-1 and the possibility to separately adjust the resonant and the nonresonant wavenumber for every specimen allow to investigate a variety of samples with high contrast and high signal-to-noise ratio, e. g., for medical diagnostics.

Multi-color stimulated Raman scattering with a frame-to-frame wavelength-tunable fiber-based light source.

We present multi-color imaging by stimulated Raman scattering (SRS) enabled by an ultrafast fiber-based light source with integrated amplitude modulation and frame-to-frame wavelength tuning. With a relative intensity noise level of -153.7 dBc/Hz at 20.25 MHz the light source is well suited for SRS imaging and outperforms other fiber-based light source concepts for SRS imaging. The light source is tunable in under 5 ms per arbitrary wavelength step between 700 cm-1 and 3200 cm-1, which allows for addressing Raman resonances from the fingerprint to the CH-stretch region. Moreover, the compact and environmentally stable system is predestined for fast multi-color assessments of medical or rapidly evolving samples with high chemical specificity, paving the way for diagnostics and sensing outside of specialized laser laboratories.

Toward integrated synchronously pumped optical parametric oscillators in silicon nitride.

We present a tunable, hybrid waveguide-fiber optical parametric oscillator (OPO) synchronously pumped by an ultra-fast fiber laser exploiting four-wave mixing (FWM) generated in silicon nitride waveguides. Parametric oscillation results in a 35 dB enhancement of the idler spectral power density in comparison to spontaneous FWM, with the ability of wide wavelength tuning over 86 nm in the O-band. Measurements of the oscillation threshold and the efficiency of the feedback loop reveal how an integration of the OPO on a single silicon nitride chip can be accomplished at standard repetition rates of pump lasers in the order of 100 MHz.

High-sensitivity frequency modulation CARS with a compact and fast tunable fiber-based light source.

Frequency modulation (FM) coherent anti-Stokes Raman scattering (CARS) is presented, using a compact as well as fast and widely tunable fiber-based light source. With this light source, Raman resonances between 700cm-1 and 3200cm-1 can be addressed via wavelength tuning within only 5 ms, which allows for FM CARS measurements with frame-to-frame wavelength switching. Moreover, the functionality for high-sensitivity FM CARS measurements was integrated by means of fiber optics to keep a stable and reliable operation. The light source accomplished FM CARS measurements with a 40 times enhanced sensitivity at a lock-in amplifier (LIA) bandwidth of 1 Hz. For fast imaging with frame-to-frame wavelength switching at a LIA bandwidth of 1 MHz, an 18-fold contrast enhancement could be verified, making this light source ideal for routine and out-of-lab FM CARS measurements for medical diagnostics or environmental sensing.

Optical parametric amplification in silicon nitride waveguides for coherent Raman imaging.

We present tunable waveguide-based optical parametric amplification by four-wave mixing (FWM) in silicon nitride waveguides, with the potential to be set up as an all-integrated device, for narrowband coherent anti-Stokes Raman scattering (CARS) imaging. Signal and idler pulses are generated via FWM with only 3 nJ pump pulse energy and stimulated by using only 4 mW of a continuous-wave seed source, resulting in a 35 dB enhancement of the idler spectral power density in comparison to spontaneous FWM. By using waveguides with different widths and tuning the wavelength of the signal wave seed, idler wavelengths covering the spectral region from 1.1 µm up to 1.6 µm can be generated. The versatility of the chip-based FWM light source is demonstrated by acquiring CARS images.

Spontaneous four-wave mixing in silicon nitride waveguides for broadband coherent anti-Stokes Raman scattering spectroscopy.

We present a light source for coherent anti-Stokes Raman scattering (CARS) based on broadband spontaneous four-wave mixing, with the potential to be further integrated. By using 7 mm long silicon nitride waveguides, which offer tight mode confinement and a high nonlinear refractive index coefficient, broadband signal and idler pulses were generated with 4 nJ of input pulse energy. In comparison to fiber-based experiments, the input energy and the waveguide length were reduced by two orders of magnitude, respectively. The idler and residual pump pulses were used for CARS measurements, enabling chemically selective and label-free spectroscopy over the entire fingerprint region, with an ultrafast fiber-based pump source at 1033 nm wavelength. The presented simple light source paves the path towards cost-effective, integrated lab-on-a-chip CARS applications.

Photochemical preparation of gold nanoparticle decorated cyclodextrin vesicles with tailored plasmonic properties.

We report a photochemical strategy for the preparation of plasmonic vesicles by the in situ formation of gold nanoparticles at the surface of cyclodextrin host vesicle templates decorated with photoactive guest polymers. Upon irradiation with UV light, these carefully designed polymer shells undergo a Norrish type I reaction to generate reducing radicals for the in situ reduction of gold salts and simultaneously provide a stabilizing matrix allowing for a dense decoration with discrete gold seeds. In a highly controlled growth procedure the gold particle size can be adjusted between 3 and 28 nm resulting in an increasing interparticle plasmonic coupling as revealed by a pronounced redshift of the surface plasmon resonance (SPR) band and an enhanced absorption at wavelengths above 600 nm. This unique combination of cyclodextrin vesicles capable of specifically recognizing guest molecules with a plasmonic particle shell displaying multiple interparticle gaps acting as electromagnetic hotspots shows great potential for surface-enhanced Raman scattering (SERS) applications.

Density matrix study of ground state depletion towards sub-diffraction-limited spontaneous Raman scattering spectroscopy.

The suppression of Raman scattering is of high interest for the achievement of sub-diffraction-limited resolution in Raman scattering spectroscopy and microscopy. We present density matrix calculations of the suppression of spontaneous Raman scattering via ground state depletion in a level system based on the molecule tris(bipyridine)ruthenium(ii). This particular molecule has been earlier used for an experimental demonstration of the suppression of spontaneous Raman scattering, allowing us to successfully verify the validity of our numerical calculations by a comparison to the experimental results. We investigate the required level of detail of the molecule model as well as the influence of certain molecule and pulse parameters on the Raman scattering suppression. It was found that pulses with a duration longer than the lifetime of the electronic states allow for a high suppression of the Raman scattering. Pulses shorter than the coherence lifetime between the ground state and electronic states lead to a similarly high suppression but also accomplish the suppression with more than one order of magnitude lower pulse energy fluence. Additionally, using a laser wavelength that is in resonance with one of the electronic transitions of the sample should allow suppressing the Raman scattering with four to six orders of magnitude lower pulse energy fluence.

Rapid spectro-polarimetry to probe molecular symmetry in multiplex coherent anti-Stokes Raman scattering.

We present the simultaneous detection of the spectrum and the complete polarization state of a multiplex coherent anti-Stokes Raman scattering signal with a fast division-of-amplitude spectro-polarimeter. The spectro-polarimeter is based on a commercial imaging spectrograph, a birefringent wedge prism, and a segmented polarizer. Compared to the standard rotating-retarder fixed-analyzer spectro-polarimeter, only a single measurement is required and an up to 21-fold reduced acquisition time is shown. The measured Stokes parameters allow us to differentiate between vibrational symmetries and to determine the depolarization ratio ρ by data post-processing.