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Second harmonic generation (SHG) microscopy is an important optical imaging technique in a variety of applications. This article describes the history and physical principles of SHG microscopy and its more advanced variants, as well as their strengths and weaknesses in biomedical applications. It also provides an overview of SHG and advanced SHG imaging in neuroscience and microtubule imaging and how these methods can aid in understanding microtubule formation, structuration, and involvement in neuronal function. Finally, we offer a perspective on the future of these methods and how technological advancements can help make SHG microscopy a more widely adopted imaging technique.

Tumors, their microenvironment, and the mechanisms by which collagen morphology changes throughout cancer progression have recently been a topic of interest. Second harmonic generation (SHG) and polarization second harmonic (P-SHG) microscopy are label-free, hallmark methods that can highlight this alteration in the extracellular matrix (ECM). This article uses automated sample scanning SHG and P-SHG microscopy to investigate ECM deposition associated with tumors residing in the mammary gland. We show two different analysis approaches using the acquired images to distinguish collagen fibrillar orientation changes in the ECM. Lastly, we apply a supervised deep-learning model to classify naïve and tumor-bearing mammary gland SHG images. We benchmark the trained model using transfer learning with the well-known MobileNetV2 architecture. By fine-tuning the different parameters of these models, we show a trained deep-learning model that suits such a small dataset with 73% accuracy.

Roaming dynamics in real time Roaming is distinct from conventional reaction channels because of the unusual geometries that chemical systems use to bypass the minimum energy pathway. It is a relatively new phenomenon that is usually determined in experiments through spectroscopic characterization of the roaming products. Using a combination of time-resolved Coulomb explosion imaging and quasiclassical trajectory analysis, Endo et al. report real-time observation of individual fragments of the prototypical reaction of deuterated formaldehyde (D 2 CO) dissociation as they roam on ultrafast time scales. They show that roaming not only occurs several orders of magnitude earlier than previously expected but also that it can terminate in a radical (D + DCO) rather than the well-known molecular (D 2 + CO) product channel. Science , this issue p. 1072

In this work, we demonstrate the sensitivity of the frequency-resolved optical switching (FROSt) technique to detect a small amount of spectral phase shift for the precise characterization of ultrashort laser pulses. We characterized fs pulses centered at 1.75 µm that are spectrally broadened up to 700 nm of bandwidth in a hollow-core fiber and subsequently compressed down to 2.3 optical cycle duration by propagation in the air at atmospheric pressure. By inserting thin fused silica windows of different thicknesses in the beam path, we accurately retrieve group delay dispersion (GDD) variations as small as 10 fs2. Such GDD variations correspond to a change of the pulse duration of only 0.2 fs for a Fourier transform limited 2-cycle pulse at 1.75 µm (i.e., 11.8 fs). The capability to measure such tiny temporal variations thus demonstrates that the FROSt technique has sufficient sensitivity to precisely characterize single-cycle pulses.

We report on an optical architecture delivering sub-120 femtosecond laser pulses of 20 µJ tunable from 5.5 µm to 13 µm in the mid-infrared range (mid-IR). The system is based on a dual-band frequency domain optical parametric amplifier (FOPA) optically pumped by a Ti:Sapphire laser and amplifying 2 synchronized femtosecond pulses each with a widely tunable wavelength around 1.6 and 1.9 µm respectively. These amplified pulses are then combined in a GaSe crystal to produce the mid-IR few-cycle pulses by means of difference frequency generation (DFG). The architecture provides a passively stabilized carrier-envelope phase (CEP) whose fluctuations has been characterized to 370 mrad RMS.

We experimentally demonstrate the formation of multidimensional solitary states (MDSS) in N2O-filled hollow-core fiber (HCF), driven by ultraviolet (UV) sub-picosecond pulses.

A Frequency Resolved Optical Gating instrument accepting s or p polarized input pulses ranging from 205 nm to 2000 nm, durations from 2 cycles to 100 ps, and nano-Joule energies is presented.

We present advanced features of the frequency resolved optical switching technique: (i) temporal characterization of an IR supercontinuum, (ii) a high precision on group delay dispersion, (iii) characterization of pulses independently of their polarization direction.

We show that frequency resolved optical switching (FROSt) can be used to characterize high repetition rate laser sources. We characterize supercontinuum pulses extending from 1.2 µm to 1.8 µm up to 500 kHz.

The use of ultrashort laser pulses with long wavelengths as drivers is a relevant strategy for scaling high harmonic generation (HHG) to higher photon energies. Here, stimulated Raman scattering enhanced by the formation of multidimensional solitary states in a molecular gas‐filled hollow‐core fiber as the mechanism to produce a versatile HHG driver is reported on. This recently discovered method allows to red shift and to compress conventional subpicosecond laser pulses with a simple experimental apparatus, ultimately increasing the generated photon energy, while assuring a high photon flux. The adaptability, simplicity, and stability of this method make it attractive for tailoring HHG sources to individual applications at specific photon energies. Measurements of resonant magnetic scattering in a cobalt/platinum multilayer sample are presented as a demonstration of the relevance of this approach for photon‐hungry applications in the extreme ultraviolet.

Multidimensional solitary states generated by intermodal stimulated Raman scattering in a gas-filled hollow-core fiber form red-shifted, few-cycle pulses after propagation thought glass. These pulses, when used to drive the high harmonic generation process, allow for tailoring the extreme ultraviolet source to specific photon-demanding applications.

High harmonic generation (HHG) in gasses has become a method of choice among table-top extreme ultraviolet (XUV) sources. In order to push the harmonic cut-off towards higher photon energies, many strategies can be implemented, including red-shifting and compressing the driver pulses. Here, we propose a new approach for tuning the red-shift of sub-picosecond driver pulses and compressing them to few-cycle durations in a single stage. This method uses newly discovered multidimensional solitary states (MDSS) pulses as a spatio-temporal engineered source based on the nonlinear Raman process in gas-filled hollow-core fibres (HCF) [1] . It has a few key advantages: 1) The MDSS pulses exhibit a negative quadratic spectral phase and can be compressed by simple propagation through glass. 2) In contrast with commonly-used optical parametric amplifiers, a small redshift can be obtained, allowing to reach a target XUV photon energy while minimizing the detrimental effects of long driver wavelengths on HHG efficiency. We apply our method to X-ray Resonant Magnetic Scattering (XRMS) measurements on a cobalt/platinum ferromagnet, an application that requires a high photon flux at the M 2,3 edge of cobalt (60 eV).

For a decade, a number of ultrafast science applications [1] - [3] involve high-field coherent radiation in the mid-infrared region, motivating the development of such laser sources. In this context, we have designed an optical setup able to generate few-cycle pulses around 10 µm, with 20 µJ of energy per pulse providing carrier-to-envelop phase (CEP) stability and control [4] . As depicted in figure 1 , the laser source is based on a frequency domain optical parametric amplifier (FOPA) [5] , coupled with intrapulse difference frequency generation (DFG). From an incident pulse of 45 fs at 800 nm, two spectral bands around 1.8 µm are amplified and shaped in the FOPA before being converted to the mid-infrared by DFG.

We have used the FERMI free-electron laser to perform time-resolved photoelectron imaging experiments on a complex group of resonances near 15.38 eV in the absorption spectrum of molecular nitrogen, N2, under jet-cooled conditions. The new data complement and extend the earlier work of Fushitani et al. [Opt. Express 27, 19702–19711 (2019)], who recorded time-resolved photoelectron spectra for this same group of resonances. Time-dependent oscillations are observed in both the photoelectron yields and the photoelectron angular distributions, providing insight into the interactions among the resonant intermediate states. In addition, for most states, we observe an exponential decay of the photoelectron yield that depends on the ionic final state. This observation can be rationalized by the different lifetimes for the intermediate states contributing to a particular ionization channel. Although there are nine resonances within the group, we show that by detecting individual photoelectron final states and their angular dependence, we can identify and differentiate quantum pathways within this complex system.

Using time-resolved Coulomb explosion imaging (CEI) in an ultraviolet (UV) pump near infrared (NIR) probe experiment, we directly image the different dissociation dynamics in the formaldehyde molecule. Different pathways are distinguished from each other, despite their statistical nature. To extract such dynamics, hidden in a statistical background, calls for an elimination of noise. In our approach, we take advantage of CEI being a quasi-background-free technique., International Conference of Computational Methods in Sciences and Engineering ICCMSE 2020, April 29 – May 3, 2020, Crete, Greece (Virtual), Series: AIP Conference Proceedings

A Frequency Resolved Optical Gating instrument accepting s or p polarized input pulses ranging from 205 nm to 2000 nm, durations from 2 cycles to 100 ps, and nano-Joule energies is presented.

We report the generation of a 100 keV electron beam by direct laser acceleration using longitudinal electric fields in low-density gas. This configuration is a viable pathway for ultrafast electron experiments and relativistic electron production.

International audience; We demonstrate experimentally that the frequency resolved optical switching (FROSt) method is independent of the polarization direction of the pulse to be characterized. In this perspective, it is employed to characterize two or three co-propagating pulses linearly polarized in orthogonal directions, enabling to retrieve simultaneously their temporal intensity and phase profiles together with their group delay. This technique is also applied to track a simple nonlinear process involving different polarization states: type-I second harmonic generation (SHG). We are able to characterize the depleted fundamental pulse along with the generated second-harmonic pulse, thus demonstrating that the FROSt technique is a practical and powerful tool to observe nonlinear processes both in the temporal and spectral domains even if it involves different polarization states.

International audience; The frequency-resolved optical switching (FROSt) method developed for ultrashort pulse characterization is implemented for single-shot measurements. In this basic demonstration, the delay axis of the spectrogram is spatially encoded by the pump beam having a small incident angle with the photoexcited material. We present the calibration procedure for spectrograms acquired in single-shot and the temporal characterization of 44 fs pulses with central wavelength at 800 nm both in scanning and single-shot FROSt configurations. The retrieved pulses are compared by means of the root-mean-square field error. Finally, the pulses are propagated through a known dispersive material to measure the added group-delay dispersion.

Nonlinear parametric processes involving ultrashort pulses are typically carried out in time domain, which mathematically corresponds to a convolution of their frequency spectra. In contrast, this spectral convolution changes into a multiplication operation when performing the nonlinear interaction in frequency domain. Here, we extend the scope of frequency-domain nonlinear optics by demonstrating its ability to perform a temporal convolution. Through this approach, nonlinear optical operations that are inaccessible in time domain can be realised: specific optical information can be coherently advanced by picoseconds within a pulse sequence—a newly generated second harmonic pulse carries the amplitude and phase information of two input pulses. This central pulse is isolated when using an input field consisting of two cross-polarized input pulses in combination with type-II second harmonic generation. The effects of nonlinear temporal convolution can be viewed from the aspect of signal processing and pulse shaping, where the nonlinear interaction in the parametric crystal plays the role of a dynamic linear optical filter—in contrast to conventional static filters—with a shaping mask instantaneously adapting to the laser field.

We demonstrate an efficient approach for enhancing the spectral broadening of long laser pulses and for efficient frequency redshifting by exploiting the intrinsic temporal properties of molecular alignment inside a gas-filled hollow-core fiber (HCF). We find that laser-induced alignment with durations comparable to the characteristic rotational time scale T R o t A l i g n enhances the efficiency of redshifted spectral broadening compared to noble gases. The applicability of this approach to Yb lasers with (few hundred femtoseconds) long pulse duration is illustrated, for which efficient broadening based on conventional Kerr nonlinearity is challenging to achieve. Furthermore, this approach proposes a practical solution for high energy broadband long-wavelength light sources, and it is attractive for many strong field applications.

We establish time-resolved high harmonic generation (tr-HHG) as a powerful spectroscopy for photoinduced dynamics in strongly correlated materials through a detailed investigation of the insulator-to-metal transitions in vanadium dioxide. We benchmark our technique by comparing our measurements to established momentum-resolved ultrafast electron diffraction, and theoretical density functional calculations. Tr-HHG allows distinguishing of individual dynamic channels, including a transition to a thermodynamically hidden phase. In addition, the HHG yield is shown to be modulated at a frequency characteristic of a coherent phonon in the equilibrium monoclinic phase over a wide range of excitation fluences. These results demonstrate that tr-HHG is capable of tracking complex dynamics in solids through its sensitivity to the band structure., 20 pages and 4 figures main text, 8 pages and 4 figures supplementary information

A conventional hollow core fiber (HCF) scheme is implemented to investigate spectral broadening of Titanium:Sapphire (Ti-Sa) femtosecond laser pulses in saturated hydrocarbon molecules compared to unsaturated ones. While the saturated molecules exhibit a spectral broadening similar to noble gases, for the unsaturated ones with π bonds, broadening towards blue is restrained. Numerical simulations underpin that it is a combination of group velocity dispersion (GVD) and Raman scattering which limits the spectral broadening for the unsaturated molecules. Compression of low energy ∼40fs pulses to ∼8fs using saturated hydrocarbons is demonstrated, suggesting the feasibility of this media for high repetition rate laser pulse compression.

As a photoexcited molecule breaks apart, we can see not just where the fragments are but also whether they are departing from the beaten path.

Ultrafast demagnetization, a phenomenon of utmost interest in the context of optical control of magnetically recorded data, has been extensively studied in a variety of different materials. However, only a limited number of studies have investigated the impact of the pump laser wavelength on the process, and only within a narrow spectral range. Performing resonant scattering experiment at the cobalt ${M}_{2,3}$ edges, using extreme ultraviolet radiation photons from a high harmonic source, we studied the ultrafast demagnetization dynamics of Co/Pt multilayers by tuning the pump wavelength to 0.4, 0.8, and 1.8 \ensuremath{\mu}m. We show that the degree of demagnetization at short time scale (100s of fs) is stronger at longer wavelengths. This is explained by the wavelength dependence of both the laser induced heating of the electrons (${T}_{e}\ensuremath{\propto}{\ensuremath{\lambda}}^{2}$) and the spatial distribution of the electromagnetic energy deposited into the multilayer sample.

We present a novel approach for measuring the carrier-envelope phase (CEP) stability of a laser source by employing the process of high harmonic generation (HHG) in solids. HHG in solids driven by few-cycle pulses is very sensitive to the waveform of the driving pulse, therefore enabling to track the shot-to-shot CEP fluctuations of a laser source. This strategy is particularly practical for pulses at long central wavelength up to the mid-infrared spectral range where usual techniques used in the visible or near-infrared regions are challenging to transpose. We experimentally demonstrate this novel tool by measuring the CEP fluctuations of a mid-infrared laser source centered at 9.5~μm.

“Roamers” are directly observed in the prototypical roaming reaction in the formaldehyde molecule. Despite their statistical nature, roaming is well discriminated from the radical- and molecular dissociation channels, using Coulomb explosion imaging and theoretical modeling., International Conference on Ultrafast Phenomena 2020, Nov. 16-19, 2020, Washington, D.C.

We report the control of tunnel ionization in lithium niobate (${\mathrm{LiNbO}}_{3}$) using phase-controlled two-color laser fields. Through a macroscopic observable of high contrast, we disclose the crucial contribution of the microscopic spontaneous polarization of the ferroelectric material to the ionization rate: as the relative two-color phase is varied, the ablated area of ${\mathrm{LiNbO}}_{3}$ is modulated by 35% when the laser and crystal polarization directions are parallel. Rotating the sample by ${180}^{\ensuremath{\circ}}$ around the laser propagation axis leads to an out-of-phase modulation. We use a two-band model to highlight the key contribution of the material's spontaneous polarization for the symmetry breaking of the ionization rate. Our results open new perspectives for the direct control of ionization dynamics in solids by tailoring the electric field of femtosecond laser pulses.

Here, we report the first time observation of the formation of highly-stable multidimensional solitary states (MDSS) in gas-filled Hollow-core fibers. The MDSS have broadband red-shifted spectra with an uncommon negative quadratic spectral phase at output, originating from Raman enhancement due to the strong intermodal nonlinear interactions.

A conventional hollow-core fiber (HCF) scheme is implemented to investigate the effect of group velocity dispersion (GVD) and Raman scattering in spectral broadening in molecular gases for low energy pulse compression application.

We present a novel, to the best of our knowledge, approach for scaling the peak power of mid-infrared laser pulses with few-cycle duration and carrier-to-envelope phase stabilization. Using frequency domain optical parametric amplification (FOPA), selective amplification is performed on two spectral slices of broadband pulses centered at 1.8 µm wavelength. In addition to amplification, the Fourier plane is used for specific pulse shaping to control both the relative polarization and the phase/delay between the two spectral slices of the input pulses. At the output of the FOPA, intrapulse difference frequency generation provides carrier–envelope phase stabilized two-cycle pulses centered at 9.5 µm wavelength with 25.5 µJ pulse energy. The control of the carrier–envelope phase is demonstrated through the dependence of high-harmonic generation in solids. This architecture is perfectly adapted to be scaled in the future to high average and high peak powers using picosecond ytterbium laser technologies.

Physical review / B 101(21), 214311 (1-6) (2020). doi:10.1103/PhysRevB.101.214311, Laser micromachining techniques using femtosecond laser pulses are employed for the fabrication of a wide range of devices, from optical waveguides and fiber Bragg gratings to microfluidic systems. In this perspective, it is important to characterize how transparent materials respond to the high-intensity laser field in order to fully understand and control the strong-field ionization process at the core of such techniques. Here, we characterize the laser polarization dependence of $y$-cut and $x$-cut ferroelectric lithium niobate (LiNbO$_3$) upon ionization. Using linearly polarized 1800-nm femtosecond pulses, we perform single-shot laser-induced ablation measurements to obtain a macroscopic observable with a large contrast compared to all-optical techniques. In the tunnel ionization regime, the crystal orientation can be correlated with the structural symmetry/asymmetry of the material. This is revealed through a variation of the ablated area when the laser polarization is rotated with respect to the c axis of the crystal. It is further found that ablation is more pronounced when the laser polarization is oriented towards angular regions containing Nb-O bonds of the unit cell, identifying the main chemical bonds contributing to the ionization of the material. The experimental results are supported by numerical simulations based on a two-band model for LiNbO$_3$., Published by Inst., Woodbury, NY

We extend time-resolved high harmonic spectroscopy to solid-state systems by investigating the dynamics of the insulator-to-metal phase transition in the strongly correlated material, VO2, revealing all electronic states involved.

A high harmonics source is used to perform x-ray resonant magnetic scattering on magnetic samples. The dynamics of laser-induced ultrafast demagnetization are probed and longer pump wavelengths are found to increase the initial quenching levels.

In conventional laser-scanning microscopy, images are formed by acquiring the signal from pixel to pixel. Here, we report more than one order of magnitude reduction in acquisition time of Interferometric Second Harmonic Generation (I-SHG) by scanning the phase within each pixel, to characterize the relative polarity of various samples. Using an electro-optic phase-scanner, we show that the phase-shift patterns required for interferometry can be applied at each pixel during the scanning of the sample, allowing single-scan I-SHG (1S-ISHG) measurements. Requiring exposure times comparable to standard SHG intensity images, the additional phase information of the signal can thus be retrieved in parallel to its amplitude at the time-scale of seconds. Moreover, slower modulations can be used to enhance the precision of the phase measurement, without any spatial or temporal shift between interferograms, in contrast to conventional frame phase-shifting I-SHG (standard I-SHG). This continues to extend I-SHG to dynamical processes, and opens it to large-scale studies, as well as to imaging samples where the signal-to-noise ratio is an issue.

To generalize the applicability of the temporal characterization technique called “tunneling ionization with a perturbation for the time-domain observation of an electric field” (TIPTOE), the technique is examined in the multicycle regime over a broad wavelength range, from the UV to the IR range. The technique is rigorously analyzed first by solving the time-dependent Schrödinger equation. Then, experimental verification is demonstrated over an almost 5-octave wavelength range at 266, 1800, 4000 and 8000 nm by utilizing the same nonlinear medium – air. The experimentally obtained dispersion values of the materials used for the dispersion control show very good agreement with the ones calculated using the material dispersion data and the pulse duration results obtained for 1800 and 4000 nm agree well with the frequency-resolved optical gating measurements. The universality of TIPTOE arises from its phase-matching-free nature and its unprecedented broadband operation range.

Pulse compression based on non-linear propagation in a gas-filled hollow core fiber (HCF) is amongst the common techniques to generate few-cycle laser pulses [1]. Although very efficient, the major disadvantage of this method is the need to use expensive noble gases like krypton or xenon to compress low energy pulses [2–4]. Our latest results confirm that certain molecular gases, hydrofluorocarbons, represent an affordable and efficient alternative to the traditional atomic gases [5,6]. Such gases bear the potential to generalize HCF compression to high repetition rate, low intensity laser systems [7].