Highly efficient and widely tunable Si3N4 waveguide-based optical parametric oscillator.

We demonstrate an efficient and widely tunable synchronously pumped optical parametric oscillator (OPO) exploiting four-wave mixing (FWM) in a silicon nitride (Si3N4) waveguide with inverted tapers. At a pump pulse duration of 2 ps, the waveguide-based OPO (WOPO) exhibited a high external pump-to-idler conversion efficiency of up to -7.64 dB at 74% pump depletion and a generation of up to 387 pJ output idler pulse energy around 1.13 µm wavelength. Additionally, the parametric oscillation resulted in a 64 dB amplification of idler power spectral density in comparison to spontaneous FWM, allowing for a wide idler wavelength tunability of 191 nm around 1.15 µm. Our WOPO represents a significant improvement of conversion efficiency as well as output energy among χ3 WOPOs, rendering an important step towards a highly efficient and widely tunable chip-based light source for, e.g., coherent anti-Stokes Raman scattering.

Toward integrated tantalum pentoxide optical parametric oscillators.

We present a hybrid waveguide-fiber optical parametric oscillator (OPO) exploiting degenerate four-wave mixing in tantalum pentoxide. The OPO, pumped with ultrashort pulses at 1.55 µm wavelength, generated tunable idler pulses with up to 4.1 pJ energy tunable center wavelength between 1.63 µm and 1.68 µm. An upper bound for the total tolerable cavity loss of 32 dB was found, rendering a chip-integrated OPO feasible as a compact and robust light source.

Longitudinal to transversal conversion of mode-locked states in an empty optical resonator.

A longitudinal mode-locked state can be converted to a transverse mode-locked state by exploiting the spectral and spatial filtering of an empty optical resonator. Carrier and amplitude modulation sidebands were simultaneously transmitted by the conversion resonator, yielding phase-locked superpositions of up to five transverse modes. Equivalently, an amplitude-modulated beam was converted into a beam that periodically moved across the transverse plane. Precise control over the spatial beam shape during oscillation was gained by independently altering the set of transverse modes and their respective powers, which demonstrated an increased level of control in the generation of transverse mode-locked states.

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.

Higher-order mode supercontinuum generation in dispersion-engineered liquid-core fibers.

Supercontinuum generation enabled a series of key technologies such as frequency comb sources, ultrashort pulse sources in the ultraviolet or the mid-infrared, as well as broadband light sources for spectroscopic methods in biophotonics. Recent advances utilizing higher-order modes have shown the potential to boost both bandwidth and modal output distribution of supercontinuum sources. However, the strive towards a breakthrough technology is hampered by the limited control over the intra- and intermodal nonlinear processes in the highly multi-modal silica fibers commonly used. Here, we investigate the ultrafast nonlinear dynamics of soliton-based supercontinuum generation and the associated mode coupling within the first three lowest-order modes of accurately dispersion-engineered liquid-core fibers. By measuring the energy-spectral evolutions and the spatial distributions of the various generated spectral features polarization-resolved, soliton fission and dispersive wave formation are identified as the origins of the nonlinear broadening. Measured results are confirmed by nonlinear simulations taking advantage of the accurate modeling capabilities of the ideal step-index geometry of our liquid-core platform. While operating in the telecommunications domain, our study allows further advances in nonlinear switching in emerging higher-order mode fiber networks as well as novel insights into the sophisticated nonlinear dynamics and broadband light generation in pre-selected polarization states.

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.

Rotational motion and rheotaxis of human sperm do not require functional CatSper channels and transmembrane Ca2+ signaling.

Navigation of sperm in fluid flow, called rheotaxis, provides long-range guidance in the mammalian oviduct. The rotation of sperm around their longitudinal axis (rolling) promotes rheotaxis. Whether sperm rolling and rheotaxis require calcium (Ca2+ ) influx via the sperm-specific Ca2+ channel CatSper, or rather represent passive biomechanical and hydrodynamic processes, has remained controversial. Here, we study the swimming behavior of sperm from healthy donors and from infertile patients that lack functional CatSper channels, using dark-field microscopy, optical tweezers, and microfluidics. We demonstrate that rolling and rheotaxis persist in CatSper-deficient human sperm. Furthermore, human sperm undergo rolling and rheotaxis even when Ca2+ influx is prevented. Finally, we show that rolling and rheotaxis also persist in mouse sperm deficient in both CatSper and flagellar Ca2+ -signaling domains. Our results strongly support the concept that passive biomechanical and hydrodynamic processes enable sperm rolling and rheotaxis, rather than calcium signaling mediated by CatSper or other mechanisms controlling transmembrane Ca2+ flux.

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.

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.

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.