Design criteria for ultrafast optical parametric amplifiers

open2noOptical parametric amplifiers (OPAs) exploit second-order nonlinearity to transfer energy from a fixed frequency pump pulse to a variable frequency signal pulse, and represent an easy way of tuning over a broad range the frequency of an otherwise fixed femtosecond laser system. OPAs can also act as broadband amplifiers, transferring energy from a narrowband pump to a broadband signal and thus considerably shortening the duration of the pump pulse. Due to these unique properties, OPAs are nowadays ubiquitous in ultrafast laser laboratories, and are employed by many users, such as solid state physicists, atomic/molecular physicists, chemists and biologists, who are not experts in ultrafast optics. This tutorial paper aims at providing the non-specialist reader with a self-consistent guide to the physical foundations of OPAs, deriving the main equations describing their performance and discussing how they can be used to understand their most important working parameters (frequency tunability, bandwidth, pulse energy/repetition rate scalability, control over the carrier-envelope phase of the generated pulses). Based on this analysis, we derive practical design criteria for OPAs, showing how their performance depends on the type of the nonlinear interaction (crystal type, phase-matching configuration, crystal length), on the characteristics of the pump pulse (frequency, duration, energy, repetition rate) and on the OPA architecture.Manzoni, C.; Cerullo, G.Manzoni, Cristian; Cerullo, GIULIO NICOL

Probing equilibrium glass flow up to exapoise viscosities

Glasses are out-of-equilibrium systems aging under the crystallization threat. During ordinary glass formation, the atomic diffusion slows down rendering its experimental investigation impractically long, to the extent that a timescale divergence is taken for granted by many. We circumvent here these limitations, taking advantage of a wide family of glasses rapidly obtained by physical vapor deposition directly into the solid state, endowed with different "ages" rivaling those reached by standard cooling and waiting for millennia. Isothermally probing the mechanical response of each of these glasses, we infer a correspondence with viscosity along the equilibrium line, up to exapoise values. We find a dependence of the elastic modulus on the glass age, which, traced back to temperature steepness index of the viscosity, tears down one of the cornerstones of several glass transition theories: the dynamical divergence. Critically, our results suggest that the conventional wisdom picture of a glass ceasing to flow at finite temperature could be wrong.Comment: 4 figures and 1 supplementary figur

Characterization of femtosecond laser written waveguides for integrated biochemical sensing

Fluorescence detection is known to be one of the most sensitive among the different optical sensing techniques. This work focuses on excitation and detection of fluorescence emitted by DNA strands labeled with fluorescent dye molecules that can be excited at a specific wavelength. Excitation occurs via optical channel waveguides written with femtosecond laser pulses applied coplanar with a microfluidic channel on a glass chip. The waveguides are optically characterized in order to facilitate the design of sensing structures which can be applied for monitoring the spatial separation of biochemical\ud species as a result of capillary electrophoresis

Resonant optical control of the structural distortions that drive ultrafast demagnetization in Cr2_2O3_3

We study how the color and polarization of ultrashort pulses of visible light can be used to control the demagnetization processes of the antiferromagnetic insulator Cr$_2$O$_3$. We utilize time-resolved second harmonic generation (SHG) to probe how changes in the magnetic and structural state evolve in time. We show that, varying the pump photon-energy to excite either localized transitions within the Cr or charge transfer states, leads to markedly different dynamics. Through a full polarization analysis of the SHG signal, symmetry considerations and density functional theory calculations, we show that, in the non-equilibrium state, SHG is sensitive to {\em both} lattice displacements and changes to the magnetic order, which allows us to conclude that different excited states couple to phonon modes of different symmetries. Furthermore, the spin-scattering rate depends on the induced distortion, enabling us to control the timescale for the demagnetization process. Our results suggest that selective photoexcitation of antiferromagnetic insulators allows fast and efficient manipulation of their magnetic state.Comment: 7 pages, 5 figure

Optical sensing in microchip capillary electrophoresis by femtosecond laser written waveguides

Capillary electrophoresis separation in an on-chip integrated microfluidic channel is typically monitored with bulky, bench-top optical excitation/detection instrumentation. Optical waveguides allow confinement and transport of light in the chip directing it to a small volume of the microfluidic channel and collecting the emitted/transmitted radiation. However, the fabrication of optical waveguides or more complex photonic components integrated with the microfluidic channels is not a straightforward process, since it requires a localized increase of the refractive index of the substrate.\ud Recently, a novel technique has emerged for the direct writing of waveguides and photonic circuits in transparent glass substrates by focused femtosecond laser pulses.\ud In this work we demonstrate the integration of femtosecond laser written optical waveguides into a commercial microfluidic chip. We fabricate high quality waveguides intersecting the microchannels at arbitrary positions and use them to optically address with high spatial selectivity their content. In particular, we apply our technique to integrate optical detection in microchip capillary electrophoresis. Waveguides are inscribed at the end of the separation channel in order to optically excite the different plugs reaching that point; fluorescence from the labelled biomolecules crossing the waveguide output is efficiently collected at a 90° angle by a high numerical aperture optical fiber. The sensitivity of the integrated optical detection system was first evaluated filling the chip with a dye solution, obtaining a minimum detectable concentration of 40 pM. \ud After dynamic coating of the microchannels with an EPDMA polymer we demonstrate electrophoresis of an oligonucleotide plug with concentration down to 1 nM and wavelength-selective monitoring of on-chip separation of three fluorescent dyes. Work is in progress on separation and detection of fluorescent-labeled DNA fragments, targeting specific, diagnostically relevant regions of a template DNA, for application to the detection of chromosome aberrations

Fluorescence monitoring of capilarry electrophoresis separation in a lab-on-a-chip with monolithically integrated waveguides

Femtosecond-laser-written optical waveguides were monolithically integrated into a commercial lab-on-a-chip to intersect a microfluidic channel. Laser excitation through these waveguides confines the excitation window to a width of 12 μm, enabling high-spatial-resolution monitoring of different fluorescent analytes, during their migration/separation in the microfluidic channel by capillary electrophoresis. Wavelength-selective monitoring of the on-chip separation of fluorescent dyes is implemented as a proof-of-principle. We envision well-controlled microfluidic plug formation, waveguide excitation, and a low limit of detection to enable monitoring of extremely small quantities with high spatial resolution

Laser-driven quantum magnonics and THz dynamics of the order parameter in antiferromagnets

The impulsive generation of two-magnon modes in antiferromagnets by femtosecond optical pulses, so-called femto-nanomagnons, leads to coherent longitudinal oscillations of the antiferromagnetic order parameter that cannot be described by a thermodynamic Landau-Lifshitz approach. We argue that this dynamics is triggered as a result of a laser-induced modification of the exchange interaction. In order to describe the oscillations we have formulated a quantum mechanical description in terms of magnon pair operators and coherent states. Such an approach allowed us to} derive an effective macroscopic equation of motion for the temporal evolution of the antiferromagnetic order parameter. An implication of the latter is that the photo-induced spin dynamics represents a macroscopic entanglement of pairs of magnons with femtosecond period and nanometer wavelength. By performing magneto-optical pump-probe experiments with 10 femtosecond resolution in the cubic KNiF$_3$ and the uniaxial K$_2$NiF$_4$ collinear Heisenberg antiferromagnets, we observed coherent oscillations at the frequency of 22 THz and 16 THz, respectively. The detected frequencies as a function of the temperature ideally fit the two-magnon excitation up to the N\'eel point. The experimental signals are described as dynamics of magnetic linear dichroism due to longitudinal oscillations of the antiferromagnetic vector.Comment: 25 pages, 10 figure

Wide-range optical spin orientation in Ge from near-infrared to visible light

Ge-based spin-photodiodes have been employed to investigate the spectral dependence of optical spin orientation in germanium, in the range 400-1550 nm. We found the expected maximum in the spin polarization of photocarriers for excitation at the direct gap in Γ (1550 nm) and a second sizable peak due to photogeneration in the L valleys (530 nm). Data suggest distinct spin depolarization mechanisms for excitation at Γ and L, with shorter spin relaxation times whether the X point is involved. These devices can be used as integrated photon-helicity detectors over a wide spectral range

Scaling-Up Techniques for the Nanofabrication of Cell Culture Substrates via Two-Photo Polymerization for Industrial-Scale Expansion of Stem Cells

Stem-cell-based therapies require a high number (106–109) of cells, therefore in vitro expansion is needed because of the initially low amount of stem cells obtainable from human tissues. Standard protocols for stem cell expansion are currently based on chemically-defined culture media and animal-derived feeder-cell layers, which expose cells to additives and to xenogeneic compounds, resulting in potential issues when used in clinics. The two-photon laser polymerization technique enables three-dimensional micro-structures to be fabricated, which we named synthetic nichoids. Here we review our activity on the technological improvements in manufacturing biomimetic synthetic nichoids and, in particular on the optimization of the laser-material interaction to increase the patterned area and the percentage of cell culture surface covered by such synthetic nichoids, from a low initial value of 10% up to 88% with an optimized micromachining time. These results establish two-photon laser polymerization as a promising tool to fabricate substrates for stem cell expansion, without any chemical supplement and in feeder-free conditions for potential therapeutic uses