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-window sparse spectral sampling stimulated Raman scattering microscopy.

Stimulated Raman scattering (SRS) is a nondestructive and rapid technique for imaging of biological and clinical specimens with label-free chemical specificity. SRS spectral imaging is typically carried out either via broadband methods, or by tuning narrowband ultrafast light sources over narrow spectral ranges thus specifically targeting vibrational frequencies. We demonstrate a multi-window sparse spectral sampling SRS (S4RS) approach where a rapidly-tunable dual-output all-fiber optical parametric oscillator is tuned into specific vibrational modes across more than 1400 cm-1 during imaging. This approach is capable of collecting SRS hyperspectral images either by scanning a full spectrum or by rapidly tuning into select target frequencies, hands-free and automatically, across the fingerprint, silent, and high wavenumber windows of the Raman spectrum. We further apply computational techniques for spectral decomposition and feature selection to identify a sparse subset of Raman frequencies capable of sample discrimination. Here we have applied this novel method to monitor spatiotemporal dynamic changes of active pharmaceutical ingredients in skin, which has particular relevance to topical drug product delivery.

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.

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.

Portable all-fiber dual-output widely tunable light source for coherent Raman imaging.

We present a rapidly tunable dual-output all-fiber light source for coherent Raman imaging, based on a dispersively matched mode-locked laser pumping a parametric oscillator. Output pump and Stokes pulses with a maximal power of 170 and 400 mW, respectively, and equal durations of 7 ps could be generated. The tuning mechanism required no mechanical delay line, enabling all-electronic arbitrary wavelength switching across more than 2700 cm - 1 in less than 5 ms. The compact setup showed a reliable operation despite mechanical shocks of more than 25 m / s 2 and is, thus, well suited for operation in a mobile cart. Imaging mouse and human skin tissue with both the portable light source and a commercial laboratory-bound reference system yielded qualitatively equal results and verified the portable light source being well suited for coherent Raman microscopy.

Low-power broadband all-optical switching via intermodal cross-phase modulation in integrated optical waveguides.

We demonstrate the potential of all-optical switches in integrated waveguides based on intermodal cross-phase modulation between transverse modes. For this purpose, the differential phase between two transverse modes of a probe beam was altered by cross-phase modulation with a control beam propagating only in the fundamental mode. A switching behavior was accomplished by spatially filtering the resulting multimode interference of the probe modes, which changed depending on the control beam power. All-optical switching with a contrast of 82% at 1280 nm over a frequency range of 4.4 THz at 1.6 nJ was achieved, representing an improvement of the product of necessary power and waveguide length by a factor of nearly 2000 compared to similar experiments in graded-index fibers. Additionally, we show that the center wavelength of the switch can be tailored by changing the cross-sectional geometry of the waveguide or the involved probe modes.

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.

Optical parametric chirped pulse oscillation.

A concept to flexibly adjust the spectral bandwidth of the output pulses of a fiber optical parametric oscillator is presented. By adjusting the chirp of the pump pulses appropriate to the chirp of the resonant pulses, the energy of the output pulses can be transferred into a user-defined spectral bandwidth. For this concept of optical parametric chirped pulse oscillation, we present numerical simulations of a parametric oscillator, which is able to convert pump pulses with a spectral bandwidth of 3.3 nm into output pulses with an adjustable spectral bandwidth between 9 and 0.05 nm. Combined with a wavelength tunability between 1200 and 1300 nm and pulse energies of up to 100 nJ, the concept should allow to adapt a single all-fiber parametric oscillator to a variety of applications, e.g., in multimodal nonlinear microscopy.

Stabilization of High Oxidation State Upconversion Nanoparticles by N-Heterocyclic Carbenes.

The stabilization of high oxidation state nanoparticles by N-heterocyclic carbenes is reported. Such nanoparticles represent an important subset in the field of nanoparticles, with different and more challenging requirements for suitable ligands compared to elemental metal nanoparticles. N-Heterocyclic carbene coated NaYF4 :Yb,Tm upconversion nanoparticles were synthesized by a ligand-exchange reaction from a well-defined precursor. This new photoactive material was characterized in detail and employed in the activation of photoresponsive molecules by low-intensity near-infrared light (λ=980 nm).

Two-octave spanning supercontinuum generation in stoichiometric silicon nitride waveguides pumped at telecom wavelengths.

We demonstrate supercontinuum generation in stoichiometric silicon nitride (Si3N4 in SiO2) integrated optical waveguides, pumped at telecommunication wavelengths. The pump laser is a mode-locked erbium fiber laser at a wavelength of 1.56 µm with a pulse duration of 120 fs. With a waveguide-internal pulse energy of 1.4 nJ and a waveguide with 1.0 µm × 0.9 µm cross section, designed for anomalous dispersion across the 1500 nm telecommunication range, the output spectrum extends from the visible, at around 526 nm, up to the mid-infrared, at least to 2.6 µm, the instrumental limit of our detection. This output spans more than 2.2 octaves (454 THz at the -30 dB level). The measured output spectra agree well with theoretical modeling based on the generalized nonlinear Schrödinger equation. The infrared part of the supercontinuum spectra shifts progressively towards the mid-infrared, well beyond 2.6 µm, by increasing the width of the waveguides.

Near-infrared photoswitching of cyclodextrin-guest complexes using lanthanide-doped LiYF4 upconversion nanoparticles.

This communication reports a new type of supramolecular cyclodextrin-guest complexes using cyclodextrin coated upconversion nanoparticles as hosts and monovalent and divalent azobenzenes and arylazopyrazoles as guests. A potentially biocompatible photocontrol of the interaction by isomerization of the azobenzene or arylazopyrazole was achieved by laser irradiation at 980 nm and a very low light intensity of 0.22 W cm-2.

Ultrafast, all-optical control of modal phases in a few-mode fiber for all-optical switching.

The phase differences between the transverse modes of an optical fiber can be altered all-optically by intermodal cross-phase modulation. In this Letter, we experimentally demonstrate this effect with ultrashort laser pulses. An ultrashort probe pulse, guided in both modes of a two-mode fiber, is co-propagating and temporally overlapping with an ultrashort control pulse, guided in the fundamental mode only and centered at a separate wavelength. The use of ultrashort pulses allows for a notable phase shift at a 33-fold reduced control pulse energy and a 173-fold reduced fiber length, compared to previous experiments. A total phase shift of 0.285π between the two probe modes was achieved at a 9 nJ control pulse energy in a 19 cm long two-mode graded-index fiber. Additionally, the capability of this scheme to switch ultrashort pulses in an all-optical manner was investigated. A modulation depth of 50% was achieved, limited by temporal nonlinear effects.

Electronically and rapidly tunable fiber-integrable optical parametric oscillator for nonlinear microscopy.

We present a fiber-based optical parametric oscillator (FOPO) pumped by a fiber-coupled laser diode. The FOPO consisted of a photonic crystal fiber to convert the pump pulses via four-wave mixing and a dispersive resonator formed by a single-mode fiber. Via dispersion filtering, output pulses with a bandwidth of about 3 nm, a temporal duration of about 8 ps and a pulse energy of up to 22 nJ could be generated. By changing the repetition frequency of the pump laser diode by about ±1 kHz, the wavelength of the output pulses could be tuned between 1130 and 1310 nm within 8 µs, without the need to change the length of the resonator. Therewith, the FOPO should especially be suited for hyperspectral imaging, while its all-electronic control constitutes a promising approach to a turnkey and alignment-free light source.

Ultrafast two-color all-optical transverse mode conversion in a graded-index fiber.

We report on experimental conversion of picosecond probe pulses from the fundamental mode (LP01) to the next higher-order mode (LP11) by optically induced transient long-period gratings in a graded-index fiber using subpicosecond control pulses. In contrast to former experiments, the temporally synchronized control (1030 nm) and probe pulses (1250 nm) were easily distinguishable by their wavelengths, allowing for the first direct observation of such an ultrafast transverse mode conversion. Despite a nonperfect pulse duration ratio between control and probe pulses as well as an unavoidable excitation of unwanted higher-order modes, a clear energy conversion of 18% between the LP01-mode and the LP11-mode was observed at 2.3 times lower control pulse energies compared to previous experiments.

Ultrafast, low-power, all-optical switching via birefringent phase-matched transverse mode conversion in integrated waveguides.

We demonstrate the potential of birefringence-based, all-optical, ultrafast conversion between the transverse modes in integrated optical waveguides by modelling the conversion process by numerically solving the multi-mode coupled nonlinear Schroedinger equations. The observed conversion is induced by a control beam and due to the Kerr effect, resulting in a transient index grating which coherently scatters probe light from one transverse waveguide mode into another. We introduce birefringent phase matching to enable efficient all-optically induced mode conversion at different wavelengths of the control and probe beam. It is shown that tailoring the waveguide geometry can be exploited to explicitly minimize intermodal group delay as well as to maximize the nonlinear coefficient, under the constraint of a phase matching condition. The waveguide geometries investigated here, allow for mode conversion with over two orders of magnitude reduced control pulse energy compared to previous schemes and thereby promise nonlinear mode switching exceeding efficiencies of 90% at switching energies below 1 nJ.

On-chip visible-to-infrared supercontinuum generation with more than 495 THz spectral bandwidth.

We report ultra-broadband supercontinuum generation in high-confinement Si3N4 integrated optical waveguides. The spectrum extends through the visible (from 470 nm) to the infrared spectral range (2130 nm) comprising a spectral bandwidth wider than 495 THz, which is the widest supercontinuum spectrum generated on a chip.

Experimental realization of femtosecond transverse mode conversion using optically induced transient long-period gratings.

We present the experimental realization of transverse mode conversion in an optical fiber via an optically induced long-period grating. The transient gratings are generated by femtosecond laser pulses, exploiting the Kerr effect to translate intensity patterns emerging from multimode interference into a spatial refractive index modulation. Since these modulations exist only while the pump beam is present, they can be used for optical switching of transverse modes. As only a localized part of the grating was written at a time and the probe beam was co-propagating with the pump beam the required pulse energies could be reduced to 120 nJ which is about a factor of 600 lower than in previous quasi-continuous-wave experiments. Accompanying numerical simulations allow a better understanding of the involved effects and show excellent agreement to the experimental results.

Toward an all-optically stabilized frequency comb based on a mode-locked fiber laser.

We present an erbium-doped mode-locked fiber laser comprising two all-optical control mechanisms acting on the carrier envelope offset (CEO)-frequency as well as the repetition frequency. The laser's repetition frequency is stabilized via optically pumping a distinct ytterbium-doped fiber module. By proving that additionally controlling the pump power of the erbium-doped gain fiber acts sufficiently complementary on the laser's CEO-frequency compared with repetition frequency stabilization, we demonstrate the feasibility of this concept for an all-optically controlled frequency comb in an all-fiber setup.

Optical repetition rate stabilization of a mode-locked all-fiber laser.

We designed an all-fiber mode-locked Erbium laser with optically stabilized repetition rate of 31.4 MHz. The stabilization was achieved by changing the refractive index of an Ytterbium-doped fiber in the resonator via optical pumping at a wavelength of 978 nm; and for long-term stability the local temperature of the fiber was additionally controlled with a thermo-electric element. The repetition rate was stabilized over 12 hours, and an Allan deviation of 2.5 × 10⁻¹² for an averaging time of 1 s could be achieved.

Spectrally resolving single-shot polarimeter.

We demonstrate a spectrally resolving single-shot polarimeter. The system consists of a commercial imaging spectrograph, modified by a birefringent wedge and a segmented polarizer. The physical operating principle and limitations of the apparatus as well as preliminary polarimetric measurements on the emission of random lasers are reported.