Quasi-periodic spectro-temporal pulse breathing in a femtosecond-pumped tellurite graded-index multimode fiber.

We report on the multidimensional characterization of femtosecond pulse nonlinear dynamics in a tellurite glass graded-index multimode fiber. We observed novel multimode dynamics of a quasi-periodic pulse breathing which manifests as a recurrent spectral and temporal compression and elongation enabled by an input power change. This effect can be assigned to the power dependent modification of the distribution of excited modes, which in turn modifies the efficiency of involved nonlinear effects. Our results provide indirect evidence of periodic nonlinear mode coupling occurring in graded-index multimode fibers thanks to the modal four-wave-mixing phase-matched via Kerr-induced dynamic index grating.

Some aspects about time broadening in fluorescence up-conversion measurements.

Several aspects contributing to the temporal broadening in the measurement of ultrafast fluorescence by means of up-conversion wave mixing are presented: the characteristics of the sample, those of the collection optics, and the wave mixing with the gate pulse in a non-linear crystal. It is concluded that these contributions are emission wavelength dependent and can be as important as the pulse durations in determining the instrument response function in this technique.

Spontaneous versus Stimulated Surface-Enhanced Raman Scattering of Liquid Water.

We have observed for the first time the surface-enhanced (SE) signal of water in an aqueous dispersion of silver nanoparticles in spontaneous (SERS) and femtosecond stimulated Raman (SE-FSRS) processes with different wavelengths of the Raman pump (515, 715, and 755 nm). By estimating the fraction of water molecules that interact with the metal surface, we have calculated enhancement factors (EF): 4.8 × 106 for SERS and (3.6-3.7) × 106 for SE-FSRS. Furthermore, we have tested the role of simultaneous plasmon resonance and Raman resonance conditions for the aν 1 + bν3 overtone mode of water (755 nm) in SE-FSRS signal amplification. When the wavelength of the Raman pump is within the plasmon resonance of the metal nanoparticles, the Raman resonance has a negligible effect on the EF. However, the Raman resonance with the aν 1 + bν3 mode strongly enhances the signal of the fundamental OH stretching mode of water.

Raman-induced pulse destabilization and bistability in an all-normal dispersion oscillator.

We report the experimental study of spectral modulations induced by a stimulated Raman scattering process in an all-fiber all-normal dispersion oscillator. With the use of dispersive Fourier transform, we recorded a series of single-shot spectra of consecutive laser pulses. The data indicate that the Raman process destabilizes the long-wavelength part of the laser pulse spectrum without disrupting the single-pulse generation regime. Our experiments revealed also that the oscillator displayed bistable operation for high pump powers. Two stable dissipative soliton mode-locked states were observed, together with output power hysteresis.

Ultra low-noise coherent supercontinuum amplification and compression below 100 fs in an all-fiber polarization-maintaining thulium fiber amplifier.

We report an ultra-low noise, polarization-maintaining, ultrafast Thulium-doped all-fiber chirped pulse amplifier, seeded by a polarized all-normal dispersion (ANDi) supercontinuum (SC) driven by an ultrafast Erbium-fiber laser. The system comprises only polarization-maintaining fibers and delivers 96 fs pulses with 350 mW output power at 100 MHz, centered at 1900 nm. The integrated relative intensity noise (RIN) in the range of 10 Hz - 10 MHz is only 0.047% at the amplifier output, which is virtually identical to the RIN of the Erbium-fiber laser driving the SC. Therefore, neither the SC generation nor the amplification process introduce significant excess noise. The RIN of our system is an order of magnitude lower than similar systems previously seeded with Raman solitons. This highlights the superior noise properties of ANDi SC and their potential as ultra-low noise seed sources for broadband, high power ultrafast fiber amplifiers and frequency combs.

Nonlinear refractive index measurement by SPM-induced phase regression.

Herewith, we describe how intensity and phase of the ultrashort pulse retrieved with second-harmonic frequency-resolved optical gating (SHG FROG) can be utilized for measurement of the nonlinear refractive index (n 2). Through comparison with available literature, we show that our method surpasses Z-scan in terms of precision by a factor of two, and thus, constitutes an interesting alternative. We present results for various materials: fused silica, calcite, YVO 4, BiBO, CaF 2, and YAG at 1030 nm. Unlike the Z-scan, the use of this method is not restricted to free-space geometry, but due to its characteristics, it can be used in integrated waveguides or photonic crystal fibers as well.

A Seedless Method for Gold Nanoparticle Growth inside a Silica Matrix: Fabrication of Materials Capable of Third-Harmonic Generation in the Near-Infrared.

A composite in which gold nanoparticles (AuNPs) approximately 10 nm in size are embedded in amorphous transparent silica matrix has been produced. The synthetic protocol uses HAuCl4 as the Au ion source, tetraethoxysilane (TEOS) as the SiO2 precursor, and l-ascorbic acid (AA) as the reducing agent. AA is employed before the sol-gel process in an amount sufficient only for reduction of Au3+ ions to Au+ . By using a cationic surfactant, benzylcetyldimethylammonium chloride hydrate (BDAC) and/or cetyltrimethylammonium bromide (CTAB), the Au+ ions are encapsulated within metalomicelles, which prevents them from being reduced to Au0 and enables their homogeneous distribution in the gel. Reduction of Au+ to Au0 and the growth of the AuNPs occurs at room temperature during the gelation, and arises from the release of EtOH during the hydrolysis of TEOS. The composites contain 0.027 wt % of Au. They exhibit nonlinear optical behavior characterized by the third-order nonlinear refraction index, n2 , in the range 3.6-5.7×10-16  cm2 W-1 at λ=1.030 µm. The composites are capable of effective third-harmonic generation of ultrashort near-IR (210 fs, 1.030 µm) laser pulse through a direct third-order mechanism.

Noncollinear and nonlinear pulse propagation.

A novel method for numerical modelling of noncollinear and nonlinear interaction of femtosecond laser pulses is presented. The method relies on a separate treatment of each of the interacting pulses by it's own rotated unidirectional pulse propagation equation (UPPE). We show that our method enables accurate simulations of the interaction of pulses travelling at a mutual angle of up to 140°. The limit is imposed by the unidirectionality principal. Additionally, a novel tool facilitating the preparation of noncollinear propagation initial conditions - a 3D Fourier transform based rotation technique - is presented. The method is tested with several linear and nonlinear cases and, finally, four original results are presented: (i) interference of highly chirped pulses colliding at mutual angle of 120°, (ii) optical switching through cross-focusing of perpendicular beams (iii) a comparison between two fluorescence up-conversion processes in BBO with large angles between the input beams and (iv) a degenerate four-wave mixing experiment in a boxcar configuration.

Nonlinear polarization evolution of ultrashort pulses in polarization maintaining fibers.

We examine properties of an ultrashort laser pulse propagating through an artificial Saturable Absorber based on Nonlinear Polarization Evolution device which has been realized with Polarization Maintaining fibers only (PM NPE). We study and compare in-line and Faraday Mirror geometries showing that the latter is immune to errors in the PM NPE construction. Experimental results for the transmission measurements of the PM NPE setup for different input linear polarization angles and various input pulse powers are presented. We show that PM NPE topology is of crucial importance for controlling the properties of the output pulse as it rules the contribution of cross-phase modulation to an overall nonlinear phase change. We also demonstrate an excellent agreement between the numerical model and experimental results.

Full 3D modelling of pulse propagation enables efficient nonlinear frequency conversion with low energy laser pulses in a single-element tripler.

Although new optical materials continue to open up access to more and more wavelength bands where femtosecond laser pulses can be generated, light frequency conversion techniques are still indispensable in filling the gaps on the ultrafast spectral scale. With high repetition rate, low pulse energy laser sources (oscillators) tight focusing is necessary for a robust wave mixing and the efficiency of broadband nonlinear conversion is limited by diffraction as well as spatial and temporal walk-off. Here we demonstrate a miniature third harmonic generator (tripler) with conversion efficiency exceeding 30%, producing 246 fs UV pulses via cascaded second order processes within a single laser beam focus. Designing this highly efficient and ultra compact frequency converter was made possible by full 3-dimentional modelling of propagation of tightly focused, broadband light fields in nonlinear and birefringent media.

Ultrafast laser mode-locked using nonlinear polarization evolution in polarization maintaining fibers.

We demonstrate an all-fiber ultrafast ytterbium laser oscillator mode-locked by means of a nonlinear polarization evolution (NPE) method realized in polarization-maintaining (PM) fibers. A sequence of the PM fiber pieces is shown to perform NPE action while maintaining a required temporal overlap of the ordinary and extraordinary pulses propagating through it. We present details of simple numerical simulations showing the advantage of the proposed scheme of segmented PM fibers. The laser utilizing the above mentioned design which generates ultrashort pulses at a 20.54 MHz repetition rate with the dechirped pulse duration around 150 fs and a pulse energy of 0.85 nJ is also presented.

Spectral compression of femtosecond pulses using chirped volume Bragg gratings.

In this Letter, we demonstrate a 360 fold spectral bandwidth reduction of femtosecond laser pulses using the method of sum frequency generation of pulses with opposite chirps. The reduction has been achieved in a compact setup in which a single chirped volume Bragg grating replaces conventional stretcher and compressor units. Starting with 180 fs pulses, we have obtained, with a 30% overall efficiency, pulses longer than 100 ps with the spectral bandwidth of 0.23 cm-1 (7 GHz). We also discuss our method on theoretical grounds.

Dynamics of intermolecular interactions in CCl4via the isotope effect by femtosecond time-resolved spectroscopy.

We report our study on the ultrafast dynamics of intermolecular interactions in liquid CCl4. A transient transmission time domain signal, obtained in the 40 ps delay range, exhibits beating at the difference frequency of the totally symmetric stretching vibrations of the tetrachloride isotopologues. We show that the spectra obtained as the windowed Fourier transform of different parts of the time domain signal in the range of this totally symmetric vibration, split due to the isotope effect, carry the information about the dynamics of the coherently excited, coupled molecules. We use a simple theoretical model in order to prove that the intermolecular interaction influences the relative amplitudes of the isotopologue peaks in the spectrum. Moreover, we demonstrate that the pump induced coherence in the system leads to additional strengthening of the interaction, which can be observed in the spectra obtained from the experimental time domain signal.

Identification of the Excited-State C═C and C═O Modes of trans-ß-Apo-8'-carotenal with Transient 2D-IR-EXSY and Femtosecond Stimulated Raman Spectroscopy.

Assigning the vibrational modes of molecules in the electronic excited state is often a difficult task. Here we show that combining two nonlinear spectroscopic techniques, transient 2D exchange infrared spectroscopy (T2D-IR-EXSY) and femtosecond stimulated Raman spectroscopy (FSRS), the contribution of the C═C and C═O modes in the excited-state vibrational spectra of trans-ß-apo-8'-carotenal can be unambiguously identified. The experimental results reported in this work confirm a previously proposed assignment based on quantum-chemical calculations and further strengthen the role of an excited state with charge-transfer character in the relaxation pathway of carbonyl carotenoids. On a more general ground, our results highlight the potentiality of nonlinear spectroscopic methods based on the combined use of visible and infrared pulses to correlate structural and electronic changes in photoexcited molecules.

Simple all-PM-fiber laser mode-locked with a nonlinear loop mirror.

In this Letter, we present a figure-eight all-PM-fiber laser oscillator design with a nonlinear optical loop mirror as an artificial saturable absorber. Unlike previous constructions using the same mode-locking technique, our cavity is constructed entirely of polarization-maintaining (PM) fibers, making the oscillator more resistant to thermal and mechanical perturbations. Two simple and robust laser configurations that differ by the output coupling ratio (70% or 30%) are presented. The first configuration delivers high energy pulses of 3.5 nJ, and the second configuration delivers pulses of 1.6 nJ at a common repetition rate of 15 MHz. In either configuration, the pulsed operation is stable, and the laser operates in a single pulse train regime, even for pump powers approaching twice the power required for mode-locking. We have also observed that, at higher intracavity powers, stimulated Raman scattering plays a significant role.

Automodulations in an extended cavity, passively modelocked Ti:Sapphire oscillator--period doubling and chaos.

An extended cavity Ti:Sapphire oscillator exhibits stable operation for positively chirped pulses, while in the negative chirp regime multiple pulses are present in the cavity. At the border of these regimes automodulations, being an effect of the interplay between population inversion, laser medium polarization and the laser pulse field, appear. Two particular instabilities: period doubling and chaotic behavior of the pulse train envelope are observed. Complex temporal evolution of the pulse spectrum within the modulation period is investigated.