Self-starting mode-locking in an all-PM Yb-doped fiber laser oscillator enabled by a 3x3 nonlinear optical lossy loop mirror.

Ultrafast fiber oscillators based on loop mirror saturable absorbers often suffer from a problematic self-starting mode-locking operation. It is usually necessary to provide an additional phase shift in the loop, guaranteeing repeatable initiation of the pulsed regime. 3x3 even splitting ratio fiber couplers have recently introduced a required phase shift in an all-fiber loop mirror architecture. Until now, mode-locking induced by a 3x3 fiber coupler has been associated only with nonlinear amplifying loop mirrors. Here, we present a self-starting ultrafast dispersion-managed all-polarization-maintaining Yb-doped oscillator that utilizes a nonlinear optical lossy loop mirror instead. We show three ways of inserting asymmetric losses in a loop via a variable optical attenuator, a fiber coupler, and a very simple lossy splice. Complete characterization of all output ports of the oscillator proves significant spectral and temporal breathing of the pulse when circulating through the net normal dispersion cavity, which can deliver nJ-level pulse energy. The system guarantees excellent stability, low noise and performance comparable to nonlinear amplifying loop mirrors while being simpler, cheaper, and providing more usable output ports with different pulse characteristics.

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.

SERS-PLSR Analysis of Vaginal Microflora: Towards the Spectral Library of Microorganisms.

The accurate identification of microorganisms belonging to vaginal microflora is crucial for establishing which microorganisms are responsible for microbial shifting from beneficial symbiotic to pathogenic bacteria and understanding pathogenesis leading to vaginosis and vaginal infections. In this study, we involved the surface-enhanced Raman spectroscopy (SERS) technique to compile the spectral signatures of the most significant microorganisms being part of the natural vaginal microbiota and some vaginal pathogens. Obtained data will supply our still developing spectral SERS database of microorganisms. The SERS results were assisted by Partial Least Squares Regression (PLSR), which visually discloses some dependencies between spectral images and hence their biochemical compositions of the outer structure. In our work, we focused on the most common and typical of the reproductive system microorganisms (Lactobacillus spp. and Bifidobacterium spp.) and vaginal pathogens: bacteria (e.g., Gardnerella vaginalis, Prevotella bivia, Atopobium vaginae), fungi (e.g., Candida albicans, Candida glabrata), and protozoa (Trichomonas vaginalis). The obtained results proved that each microorganism has its unique spectral fingerprint that differentiates it from the rest. Moreover, the discrimination was obtained at a high level of explained information by subsequent factors, e.g., in the inter-species distinction of Candida spp. the first three factors explain 98% of the variance in block Y with 95% of data within the X matrix, while in differentiation between Lactobacillus spp. and Bifidobacterium spp. (natural flora) and pathogen (e.g., Candida glabrata) the information is explained at the level of 45% of the Y matrix with 94% of original data. PLSR gave us insight into discriminating variables based on which the marker bands representing specific compounds in the outer structure of microorganisms were found: for Lactobacillus spp. 1400 cm-1, for fungi 905 and 1209 cm-1, and for protozoa 805, 890, 1062, 1185, 1300, 1555, and 1610 cm-1. Then, they can be used as significant marker bands in the analysis of clinical subjects, e.g., vaginal swabs.

First events in the coil-to-globule transition of PVME in water: An ultrafast temperature jump - time-resolved elastic light scattering study.

HYPOTHESIS: The coil-to-globule transition is an essential phenomenon in protein and polymer solutions. Late stages of such transitions, >1 µs, have been thoroughly studied. Yet, the initial ones are a matter of speculations. Here, we present the first observation of a sub-nanosecond stage of the coil-to-globule transition of poly (vinyl methyl ether), PVME, in water. EXPERIMENTS: The detection of an early stage of the coil-to-globule transition has been possible thanks to a novel experimental approach - time-resolved elastic light scattering study, following an ultrafast temperature jump. We identified a molecular process active in the observed stage of the transition with use of broadband dielectric spectroscopy. FINDINGS: In the experiment's time window, from a few ps to around 600 ps, we observed an increase in the light scattering intensity 300-400 ps after the temperature jump that heated the sample above its lower critical solution temperature (LCST). The observed time coincides with the time of segmental relaxation of PVME, determined by broadband dielectric spectroscopy in the temperature range of the LCST of the PVME/water mixture. This coincidence strongly suggests that the observed herein stage of coil-to-globule transition is the rapid formation of local nuclei along the polymer chain. Those nuclei may grow and aggregate in later stages of the process, which are out of our experimental time window.

Low noise, self-referenced all polarization maintaining Ytterbium fiber laser frequency comb: erratum.

We provide a corrected figure of our previous publication [Opt. Express25, 18017 (2017)10.1364/OE.25.018017].

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.

Diverse nature of femtosecond laser ablation of poly(L-lactide) and the influence of filamentation on the polymer crystallization behaviour.

Over the past few years we have witnessed growing interest in ultrafast laser micromachining of bioresorbable polymers for fabrication of medical implants and surface modification. In this paper we show that surface structuring of poly(L-lactide) with 300 fs laser pulses at 515 and 1030 nm wavelength leads to formation of defects inside the polymer as a result of laser beam filamentation. Filament-induced channels have diameter around 1 µm and length of hundreds of micrometers. SEM images of microchannels cross-sections are presented. The influence of wavelength and pulse spacing on bulk modification extent was investigated and parameters limiting filamentation were determined. We show that filamentation can be used for controlling properties of PLLA. The presence of filament-induced modifications such as empty microchannels and pressure wave-induced stress lead to increased ability of polymer to crystallize at lower temperature. Crystallization behaviour and crystal morphology after laser treatment was investigated in details using different analytical techniques such as WAXD, DSC and FTIR/ATR. Hydrolytic degradation experiment was performed. Presented method can be applied for controllable, spatially distributed modification of polymer crystallinity, crystalline phase structure and hydrolytic degradation profile.

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.

Low noise, self-referenced all polarization maintaining Ytterbium fiber laser frequency comb.

We report the implementation of a self-referenced optical frequency comb generated by a passively mode-locked all polarization maintaining (PM) Yb fiber laser based on a nonlinear amplifying loop mirror (NALM). After spectral broadening the optical spectrum spans from 650 nm to 1400 nm, allowing for the generation of an optical octave and carrier envelope offset frequency (fceo) stabilization through a conventional f-2f interferometer. We demonstrate for the first time the stabilization of the fceo of such a PM Yb system with an in-loop fractional frequency stability scaled to an optical frequency of low 10-19 at 1 second averaging time, offering a great potential for applications in optical atomic clock metrology.

Influence of the excitation light intensity on the rate of fluorescence quenching reactions: pulsed experiments.

The effect of multiple light excitation events on bimolecular photo-induced electron transfer reactions in liquid solution is studied experimentally. It is found that the decay of fluorescence can be up to 25% faster if a second photon is absorbed after a first cycle of quenching and recombination. A theoretical model is presented which ascribes this effect to the enrichment of the concentration of quenchers in the immediate vicinity of fluorophores that have been previously excited. Despite its simplicity, the model delivers a qualitative agreement with the observed experimental trends. The original theory by Burshtein and Igoshin (J. Chem. Phys., 2000, 112, 10930-10940) was created for continuous light excitation though. A qualitative extrapolation from the here presented pulse experiments to the continuous excitation conditions lead us to conclude that in the latter the order of magnitude of the increase of the quenching efficiency upon increasing the light intensity of excitation, must also be on the order of tens of percent. These results mean that the rate constant for photo-induced bimolecular reactions depends not only on the usual known factors, such as temperature, viscosity and other properties of the medium, but also on the intensity of the excitation light.

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.

High-accuracy reference standards for two-photon absorption in the 680-1050 nm wavelength range.

Degenerate two-photon absorption (2PA) of a series of organic fluorophores is measured using femtosecond fluorescence excitation method in the wavelength range, λ2PA = 680-1050 nm, and ~100 MHz pulse repetition rate. The function of relative 2PA spectral shape is obtained with estimated accuracy 5%, and the absolute 2PA cross section is measured at selected wavelengths with the accuracy 8%. Significant improvement of the accuracy is achieved by means of rigorous evaluation of the quadratic dependence of the fluorescence signal on the incident photon flux in the whole wavelength range, by comparing results obtained from two independent experiments, as well as due to meticulous evaluation of critical experimental parameters, including the excitation spatial- and temporal pulse shape, laser power and sample geometry. Application of the reference standards in nonlinear transmittance measurements is discussed.

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.

Symmetry Breaking in Platinum Acetylide Chromophores Studied by Femtosecond Two-Photon Absorption Spectroscopy.

We study instantaneous two-photon absorption (2PA) in a series of nominally quasi-centrosymmetric trans-bis(tributylphosphine)-bis-(4-((9,9-diethyl-7-ethynyl-9H-fluoren-2-yl) ethynyl)-R)-platinum complexes, where 11 different substituents, R = N(phenyl)2(NPh2), NH2, OCH3, t-butyl, CH3, H, F, CF3, CN, benzothiazole, and NO2, represent a range of electron-donating (ED) and electron-withdrawing (EW) strengths, while the Pt core acts as a weak ED group. We measure the 2PA cross section in the 540-810 nm excitation wavelength range by complementary femtosecond two-photon excited fluorescence (2PEF) and nonlinear transmission (NLT) methods and compare the obtained values to those of the Pt-core chromophore and the corresponding noncentrosymmetric side group (ligand) chromophores. Peak 2PA cross sections of neutral and ED-substituted Pt complexes occur at S0 → Sn transitions to higher energy states, above the lowest-energy S0 → S1 transition, and the corresponding values increase systematically with increasing ED strength, reaching maximum value, σ2 ∼ 300 GM (1 GM = 10-50 cm4 s), for R = NPh2. At transition energies overlapping with the lowest-energy S0 → S1 transition in the one-photon absorption (1PA) spectrum, the same neutral and ED-substituted Pt complexes show weak 2PA, σ2 < 30-100 GM, which is in agreement with the nearly quadrupolar structure of these systems. Surprisingly, EW-substituted Pt complexes display a very different behavior, where the peak 2PA of the S0 → S1 transition gradually increases with increasing EW strength, reaching values σ2 = 700 GM for R = NO2, while in the S0 → Sn transition region the peak 2PEF cross section decreases. We explained this effect by breaking of inversion symmetry due to conformational distortions associated with low energy barrier for ground-state rotation of the ligands. Our findings are corroborated by theoretical calculations that show large increase of the permanent electric dipole moment change in the S0 → S1 transition when ligands with strong EW substituents are twisted by 90° relative to the planar chromophore. Our NLT results in the S0 → S1 transition region are quantitatively similar to those obtained from the 2PEF measurement. However, at higher transition energy corresponding to S0 → Sn transition region, the NLT method yields effective multiphoton absorption stronger than the 2PEF measurement in the same systems. Such enhancement is observed in all Pt complexes as well as in all ligand chromophores studied, and we tentatively attribute this effect to nearly saturated excited-state absorption (ESA), which may occur if 2PA from the ground state is immediately followed by strongly allowed 1PA to higher excited states.

Phenylene vinylene platinum(II) acetylides with prodigious two-photon absorption.

The linear and nonlinear optical properties of a series of linear and cross-conjugated platinum(II) acetylide complexes that contain extended p-(phenylene vinylene) chromophores are reported. The complexes exhibit very high femtosecond two-photon absorption (2PA) cross section values (σ(2) up to 10,000 GM), as measured by nonlinear transmission (NLT) and two-photon excited fluorescence (2PEF) methods. The large 2PA cross sections span a broad range of wavelengths, 570-810 nm, and they overlap with the triplet excited state absorption. Spectral coincidence of high cross section 2PA and triplet absorption is a key feature giving rise to efficient dual-mode optical power limiting (OPL).

Primary role of the chromophore bond length alternation in reversible photoconversion of red fluorescence proteins.

Rapid photobleaching of fluorescent proteins can limit their use in imaging applications. The underlying kinetics is multi-exponential and strongly depends on the local chromophore environment. The first, reversible, step may be attributed to a rotation around one of the two exocyclic C-C bonds bridging phenol and imidazolinone groups in the chromophore. However it is not clear how the protein environment controls this motion - either by steric hindrances or by modulating the electronic structure of the chromophore through electrostatic interactions. Here we study the first step of the photobleaching kinetics in 13 red fluorescent proteins (RFPs) with different chromophore environment and show that the associated rate strongly correlates with the bond length alternation (BLA) of the two bridge bonds. The sign of the BLA appears to determine which rotation is activated. Our results present experimental evidence for the dominance of electronic effects in the conformational dynamics of the RFP chromophore.