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The established paradigm to create valley states, excitations at local band extrema ("valleys"), is through selective occupation of specific valleys via circularly polarized laser pulses. Here we show a second way exists to create valley states, not by valley population imbalance but by "light-shaping" in momentum space, i.e. controlling the shape of the distribution of excited charge at each valley. While noncontrasting in valley charge, such valley states are instead characterized by a valley current, identically zero at one valley and finite and large at the other. We demonstrate that these (i) are robust to quantum decoherence, (ii) allow lossless toggling of the valley state with successive femtosecond laser pulses, and (iii) permit valley contrasting excitation both with and without a gap. Our findings open a route to robust ultrafast and switchable valleytronics in a wide scope of 2d materials, bringing closer the promise of valley-based electronics.

The modification of the surface topography at the micro- and nanoscale is a widely established as one of the best ways to engineering the surface of materials, to improve the tribological performances of materials in terms of load capacity and friction. The present paper reviews the state of the art on laser surface texturing by exploiting the technique of direct laser writing for tailoring the coefficient of friction, highlighting the effect of the textures' arrangement on the lubricated conformal and non-conformal contact behavior.

The field of valleytronics considers the creation and manipulation of "valley states", charge excitations characterized by a particular value of the crystal momentum in the Brillouin zone. Here we show, using the example of minimally gapped (≤40 meV) graphene, that there exist lightforms that create almost perfect valley contrasting current states (up to ∼80% valley purity) in the absence of a valley contrasting charge excitation. These "momentum streaked" THz waveforms act by deforming the excited state population in momentum space such that current flows at one valley yet is blocked at the conjugate valley. This approach both unlocks the potential of graphene as a materials platform for valleytronics, as gaps of 10-40 meV are robustly found in useful experimental contexts such as graphene/hBN systems, while simultaneously providing a tool toward ultrafast light control of valley currents in diverse minimally gapped matter, including many topological insulator systems.

Femtosecond laser material processing (FLMP) was used to make an X-ray mask in a 500 µm thick tungsten sheet without the use of any chemical etch methods. The laser produced an 800 nm wavelength at a 1 kHz repetition rate and a pulse width of 100 fs. The laser beam arrival at the tungsten sheet was synchronized to a computer numerically controlled (CNC) stage that allowed for motion in the XYZθ directions. The X-ray mask design was made using CAD/CAM software (Alphacam 2019 R1) and it consisted of linear, circular, and 45° angle features that covered an area of 10 mm × 10 mm. A total of 70 laser beam passes at a moderate laser energy of 605.94 J/cm 2 were used to make through-cut features into the tungsten sheet. The morphology of the top view (laser incident, LS) images showed cleaner and smoother cut edges relative to the bottom view (laser exit, LE) images. It was found that the size dimensions of the through-cut features on the LE surfaces were better aligned with the CAD dimensions than those of the LS surfaces. The focused laser beam produced inclined cut surfaces as the beam made the through cut from the LS to the LE of the tungsten sheet. The circular features at the LS surface deviated toward being oval-like on the LE surface, which could be compensated for in future CAD designs. The dependence of the CNC processing speed on the thickness of the etch depth was determined to have a third-order exponential decay relationship, thereby producing a theoretical model that will be useful for future investigators to predict the required experimental parameters needed to achieve a known etch depth in tungsten. This is the first study that has demonstrated the capability of using a femtosecond laser to machine through-cut an X-ray mask in a 500 µm thick tungsten sheet with no involvement of a wet etch or any other such supporting process.

Advanced coloration methods are of pivotal importance in science, technology, and engineering. However, 3D structural colors that are critical for emerging multidimensional information representation and recording are rarely achievable. Here, a facile voxel-level programmable 3D structural coloration in the bulk lithium niobate (LiNbO 3 ) crystal is reported. This is achieved by engineering wavelength-selective interference between ordinary (O) and extraordinary (E) light in the crystal matrix. To induce effective phase contrast between O and E light for establishing the highly localized interference across the visible band, the presence of a pulse-internal-coupling effect is revealed in the single-pulse ultrafast laser-crystal interaction and an ultrafast-laser-induced micro-amorphization (MA) strategy is thus developed to manipulate local matrix structure. Consequently, micro-nanoscale colorful voxels can be fast inscribed into any spatial position of the crystal matrix in one step. It is demonstrated that the colors can be flexibly manipulated and quickly extracted in 3D space. Multidimensional MA-color data storage with large capacity, high writing and readout speed, long lifetime, and excellent stability under harsh conditions is achieved. The present principle enables multifunctional 3D structural coloration devices inside high-refractive-index transparent dielectrics and can serve as a general platform to innovate next-generation information optics., (© 2023 Wiley-VCH GmbH.)

Significance: Two-photon microscopy is used routinely for in vivo imaging of neural and vascular structures and functions in rodents with a high resolution. Image quality, however, often degrades in deeper portions of the cerebral cortex. Strategies to improve deep imaging are therefore needed. We introduce such a strategy using the gating of high repetition rate ultrafast pulse trains to increase the signal level., Aim: We investigate how the signal generation, signal-to-noise ratio (SNR), and signal-to-background ratio (SBR) improve with pulse gating while imaging in vivo mouse cerebral vasculature., Approach: An electro-optic modulator with a high-power (6 W) 80 MHz repetition rate ytterbium fiber amplifier is used to create gates of pulses at a 1 MHz repetition rate. We first measure signal generation from a Texas Red solution in a cuvette to characterize the system with no gating and at a 50%, 25%, and 12.5% duty cycle. We then compare the signal generation, SNR, and SBR when imaging Texas Red-labeled vasculature using these conditions., Results: We find up to a 6.73-fold increase in fluorescent signal from a cuvette when using a 12.5% duty cycle pulse gating excitation pattern as opposed to a constant 80 MHz pulse train at the same average power. We verify similar increases for in vivo imaging to that observed in cuvette testing. For deep imaging, we find that pulse gating results in a 2.95-fold increase in the SNR and a 1.37-fold increase in the SBR on average when imaging mouse cortical vasculature at depths ranging from 950 to 1050    μ m ., Conclusions: We demonstrate that a pulse gating strategy can either be used to limit heating when imaging superficial brain regions or used to increase signal generation in deep regions. These findings should encourage others to adopt similar pulse gating excitation schemes for imaging neural structures through two-photon microscopy., (© 2023 The Authors.)

Nanomaterials are widely used in the fields of sensors, optoelectronics, biophotonics and ultrafast photonics due to their excellent mechanical, thermal, optical, electrical and magnetic properties. Particularly, owing to their nonlinear optical properties, fast response time and broadband operation, nanomaterials are ideal saturable absorption materials in ultrafast photonics, which contribute to the improvement of laser performance. Therefore, nanomaterials are of great importance to applications in wavelength-tunable broadband pulsed lasers. Herein, we review the integration and applications of nanomaterials in wavelength-tunable broadband ultrafast photonics. Firstly, the two integration methods, which are direct coupling and evanescent field coupling, and their characteristics are introduced. Secondly, the applications of nanomaterials in wavelength-tunable broadband lasers are summarized. Finally, the development of nanomaterials and broadband tunable lasers is reviewed and discussed., (© 2023 IOP Publishing Ltd.)

Superficial modifications on silicon wafers produced by single-shot focused femtosecond laser irradiation having a 1030 nm wavelength and 300 fs pulse duration were experimentally and theoretically analyzed. The laser fluence window when the amorphous silicon phase develops, resulting in a ring-like modification shape, was experimentally estimated to be between 0.26 J/cm2 and 0.40 J/cm2 and was independent of the silicon dopant type and laser focusing conditions; however, the window was narrower when compared to results reported for shorter pulse durations. In addition, we present a simplified numerical model that can explain and predict the formation of these patterns based on the caloric coefficients of silicon and the energy distribution of the deposited material.

Metallic micro/nano structures with special physicochemical properties have undergone rapid development owing to their broad applications in micromachines and microdevices. Ultrafast laser processing is generally accepted as an effective technology for functional structures manufacture, however, the controllable fabrication of specific metallic micro/nano structures remains a challenge. Here, this work proposes a novel strategy of laser induced transient solid-liquid transition to fabricate unique structures. Through modulating the transient state of metal from solid to liquid phase using the initial pulse excitation, the subsequent ultrafast pulse-induced recoil pressure can suppress the plasma emission and removal of liquid phase metals, resulting in the controllable fabrication of coffee-ring structures. The solid-liquid transition dynamics, which related with the transient reflectivity and plasma intensity, are revealed by established two temperature model coupled with molecular dynamics model. The coffee-ring structure exhibits tunable structure color owing to various optical response, which can be used for color printing with large scale and high resolution. This work provides a promising strategy for fabricating functional micro/nano structures, which can greatly broaden the potential applications., (© 2022 Wiley-VCH GmbH.)

Multiphoton excitation of fluorescence has many potential advantages over resonant (one-photon) excitation, but the method has not found widespread use for ultrasensitive applications. We recently described an approach to the multiphoton excitation of single molecules that uses a pulse shaper to compress and tailor pulses from an ultrafast broadband laser in order to optimise the brightness and signal-to-background ratio following non-linear excitation. Here we provide a detailed description of the setup and illustrate its use and potential by optimising two-photon fluorescence of a common fluorophore, rhodamine 110, at the single-molecule level. We also show that a DNA oligonucleotide labelled with a fluorescent nucleobase analogue, tC, can be detected using two-photon FCS, whereas one-photon excitation causes rapid photobleaching. The ability to improve the signal-to-background ratio and to reduce the incident power required to attain a given brightness can be applied to the multiphoton excitation of any fluorescent species, from small molecules with low multiphoton cross sections to the brightest nanoparticles., (Creative Commons Attribution license.)

Ultrafast laser ablation is widely used as a versatile method for accurate micro-machining of polymers, glasses and metals for a variety of industrial and biomedical applications. We report on the use of a novel process parameter, the modulation of the laser pulse energy during the multi-scan texturing of surfaces. We show that this new and straightforward control method allows us to attain higher and lower roughness (Ra) values than the conventional constant pulse energy irradiation sequence. This new multi-scanning laser ablation strategy was conducted on metals that are commonly used in the biomedical industry, such as stainless steel, titanium, brass and silver samples, using a linear (increasing or decreasing) gradient of pulse energy, i.e., varying the pulse energy across successive laser scans. The effects of ablation were studied in terms of roughness, developed interfacial area ratio, skewness and ablation efficiency of the processed surfaces. Significantly, the investigation has shown a global trend for all samples that the roughness is minimum when a decreasing energy pulse sequence is employed, i.e., the irradiation sequence ends up with the applied laser fluences close to threshold laser fluences and is maximum with increasing energy distribution. Scanning electron microscopy (SEM) and atomic force microscopy (AFM) analysis on single craters with the three different energy deposition conditions revealed a chaotic and random material redistribution in the cases of uniform and increasing energy distributions and the presence of regular laser-induced periodic surface structures (LIPSS) at the bottom of the ablation region in the case of decreasing energy distribution. It is also shown that the ablation efficiency of the ablated surfaces does not significantly change between the three cases. Therefore, this novel energy control strategy permits the control of the roughness of the processed surfaces without losing the ablation efficiency.

Significance: The creation of subepithelial voids within scarred vocal folds via ultrafast laser ablation may help in localization of injectable biomaterials toward a clinically viable therapy for vocal fold scarring., Aim: We aim to prove that subepithelial voids can be created in a live animal model and that the ablation process does not engender additional scar formation. We demonstrate localization and long-term retention of an injectable biomaterial within subepithelial voids., Approach: A benchtop nonlinear microscope was used to create subepithelial voids within healthy and scarred cheek pouches of four Syrian hamsters. A model biomaterial, polyethylene glycol tagged with rhodamine dye, was then injected into these voids using a custom injection setup. Follow-up imaging studies at 1- and 2-week time points were performed using the same benchtop nonlinear microscope. Subsequent histology assessed void morphology and biomaterial retention., Results: Focused ultrashort pulses can be used to create large subepithelial voids in vivo. Our analysis suggests that the ablation process does not introduce any scar formation. Moreover, these studies indicate localization, and, more importantly, long-term retention of the model biomaterial injected into these voids. Both nonlinear microscopy and histological examination indicate the presence of biomaterial-filled voids in healthy and scarred cheek pouches 2 weeks postoperation., Conclusions: We successfully demonstrated subepithelial void formation, biomaterial injection, and biomaterial retention in a live animal model. This pilot study is an important step toward clinical acceptance of a new type of therapy for vocal fold scarring. Future long-term studies on large animals will utilize a miniaturized surgical probe to further assess the clinical viability of such a therapy.

A high concentration of Er 3+ without clustering issues is essential in an Er-doped waveguide amplifier as it is needed to produce a high gain and low noise signal. Ultrafast laser plasma doping is a technique that facilitates the blending of femtosecond laser-produced plasma from an Er-doped TeO 2 glass with a substrate to form a high Er 3+ concentration layer. The influence of substrate temperature on the morphological, structural, and optical properties was studied and reported in this paper. Analysis of the doped substrates using scanning electron microscopy (SEM) confirmed that temperatures up to approximately 400 °C are insufficient for the incoming plasma plume to modify the strong covalent bonds of silica (SiO 2 ), and the doping process could not take place. The higher temperature used caused the materials from Er-doped tellurite glass to diffuse deeper (except Te with smaller concentration) into silica, which created a thicker film. SEM images showed that Er-doped tellurite glass was successfully diffused in the Si 3 N 4 . However, the doping was not as homogeneous as in silica.

We report an increase in terahertz (THz) radiation efficiency due to FeCo/WSe 2 structures in the reflection geometry. This can be attributed to an absorption increase in the alloy FeCo layer at the input FeCo/WSe 2 interface due to constructive interference, as well as to the backward transport of hot carriers from FeCo to WSe 2 . In contrast to the transmission geometry, the THz generation efficiency in the reflection is much less dependent on the magnetic layer thickness. Our results suggest a cheap and efficient way to improve the characteristics of THz spintronic emitters with the conservation of a full set of their important properties.

Owing to their extraordinary physical and chemical properties, two-dimensional (2D) materials have aroused extensive attention and have been widely used in photonic and optoelectronic devices, catalytic reactions, and biomedicine. In particular, 2D materials possess a unique bandgap structure and nonlinear optical properties, which can be used as saturable absorbers in ultrafast lasers. Here, we mainly review the top-down and bottom-up methods for preparing 2D materials, such as graphene, topological insulators, transition metal dichalcogenides, black phosphorus, and MXenes. Then, we focus on the ultrafast applications of 2D materials at the typical operating wavelengths of 1, 1.5, 2, and 3 μm. The key parameters and output performance of ultrafast pulsed lasers based on 2D materials are discussed. Furthermore, an outlook regarding the fabrication methods and the development of 2D materials in ultrafast photonics is also presented.

This paper reports on nonlinear spectral broadening of 1.1 ps pulses in a gas-filled multi-pass cell to generate sub-100 fs optical pulses at 1030 nm and 515 nm at pulse energies of 0.8 mJ and 225 µJ, respectively, for pump-probe experiments at the free-electron laser FLASH. Combining a 100 kHz Yb:YAG laser with 180 W in-burst average power and a post-compression platform enables reaching simultaneously high average powers and short pulse durations for high-repetition-rate FEL pump-probe experiments., (open access.)

Since the first experimental discovery of graphene 16 years ago, many other 2D layered nanomaterials have been reported. However, the majority of 2D nanostructures suffer from relatively complicated fabrication processes that have bottlenecked their development and their uptake by industry for practical applications. Here, the recent progress in sensing, photonic, and (opto-)electronic applications of PtSe 2 , a 2D layered material that is likely to be used in industries benefiting from its high air-stability and semiconductor-technology-compatible fabrication methods, is reviewed. The advantages and disadvantages of a range of synthesis methods for PtSe 2 are initially compared, followed by a discussion of its outstanding properties, and industrial and commercial advantages. Research focused on the broadband nonlinear photonic properties of PtSe 2 , as well as reports of its use as a saturable absorber in ultrafast lasers, are then reviewed. Additionally, the advances that have been achieved in a range of PtSe 2 -based field-effect transistors, photodetectors, and sensors are summarized. Finally, a conclusion on these results along with the outlook for the future is presented., (© 2020 Wiley-VCH GmbH.)

The quantum cascade laser has evolved to be a compact, powerful source of coherent mid-infrared light; however, its fast gain dynamics strongly restricts the formation of ultrashort pulses. As such, the shortest pulses reported so far were limited to a few picoseconds with some hundreds of milliwatts of peak power, strongly narrowing their applicability for time-resolved and nonlinear experiments. Here we demonstrate an approach capable of producing near-transform-limited subpicosecond pulses with several watts of peak power. Starting from a frequency-modulated phase-locked state, ultrashort high-peak-power pulses are generated via spectral filtering, gain modulation-induced spectral broadening and external pulse compression. We assess their temporal nature by means of a novel asynchronous sampling method, coherent beat note interferometry and interferometric autocorrelation. These results open new pathways for nonlinear physics in the mid-infrared., Competing Interests: Competing interestsThe authors declare no competing interests., (© The Author(s) 2021.)

High-order harmonic generation (HHG) is currently utilized for developing compact table-top radiation sources to provide highly coherent extreme ultraviolet (XUV) and soft X-ray pulses; however, the low repetition rate of fundamental lasers, which is typically in the multi-kHz range, restricts the area of application for such HHG-based radiation sources. Here, we demonstrate a novel method for realizing a MHz-repetition-rate coherent XUV light source by utilizing intracavity HHG in a mode-locked oscillator with an Yb:YAG thin disk laser medium and a 100-m-long ring cavity. We have successfully implemented HHG by introducing two different rare gases into two separate foci and picking up each HH beam. Owing to the two different HH beams generated from one cavity, this XUV light source will open a new route to performing a time-resolved measurement with an XUV-pump and XUV-probe scheme at a MHz-repetition rate with a femtosecond resolution., Competing Interests: Conflict of interestThe authors declare that they have no conflict of interest., (© The Author(s) 2020.)

By proposing an atomically thick dielectric coating on a metal nanoemitter, we theoretically show that the optical field tunneling of ultrafast-laser-induced photoemission can occur at an ultralow incident field strength of 0.03 V/nm. This coating strongly confines plasmonic fields and provides secondary field enhancement beyond the geometrical plasmon field enhancement effect, which can substantially reduce the barrier and enable more efficient photoemission. We numerically demonstrate that a 1 nm thick layer of SiO 2 around a Au-nanopyramid will enhance the resonant photoemission current density by 2 orders of magnitude, where the transition from multiphoton absorption to optical field tunneling is accessed at an incident laser intensity at least 10 times lower than that of the bare nanoemitter. The effects of the coating properties such as refractive index, thickness, and geometrical settings are studied, and tunable photoemission is numerically demonstrated by using different ultrafast lasers. Our approach can also directly be extended to nonmetal emitters, to-for example-2D material coatings, and to plasmon-induced hot carrier generation.

Laser processing of gold nanorods (Au NRs) relying on light-matter interaction provides great opportunities in various potential applications. Unveiling the light-induced structure change is a crucial goal in order to control the shape and related properties for practical application. However, the internal atomic structure control of metallic NRs has long been a challenge. Here, the concept of internal atomic structure tailored with light is demonstrated and Au NRs with various internal atomic structures including point defects, twin structures, and polycrystalline nanospheres are fabricated. Experimental characterization and theoretical simulation show that light-induced localized energy deposition and dynamic stresses distribution give rise to atomic structure change. Au NRs with internal defects show enhanced potential to improve activity. The concept of light tailoring of internal atomic structure represents a promising strategy for the rational design of metallic NRs to boost wide applications., (© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Micro/nanoprocessing of graphene surfaces has attracted significant interest for both science and applications due to its effective modulation of material properties, which, however, is usually restricted by the disadvantages of the current fabrication methods. Here, by exploiting cylindrical focusing of a femtosecond laser on graphene oxide (GO) films, we successfully produce uniform subwavelength grating structures at high speed along with a simultaneous in situ photoreduction process. Strikingly, the well-defined structures feature orientations parallel to the laser polarization and significant robustness against distinct perturbations. The proposed model and simulations reveal that the structure formation is based on the transverse electric (TE) surface plasmons triggered by the gradient reduction of the GO film from its surface to the interior, which eventually results in interference intensity fringes and spatially periodic interactions. Further experiments prove that such a regular structured surface can cause enhanced optical absorption (>20%) and an anisotropic photoresponse (~0.46 ratio) for the reduced GO film. Our work not only provides new insights into understanding the laser-GO interaction but also lays a solid foundation for practical usage of femtosecond laser plasmonic lithography, with the prospect of expansion to other two-dimensional materials for novel device applications., Competing Interests: Conflict of interestThe authors declare that they have no conflict of interest., (© The Author(s) 2020.)

Mode-locked fibre lasers (MLFLs) are fundamental building blocks of many photonic systems used in industrial, scientific and biomedical applications. To date, 1-2 μm MLFLs have been well developed; however, passively mode-locked fibre lasers in the visible region (380-760 nm) have never been reported. Here, we address this challenge by demonstrating an all-fibre visible-wavelength passively mode-locked picosecond laser at 635 nm. The 635 nm mode-locked laser with an all-fibre figure-eight cavity uses a Pr/Yb codoped ZBLAN fibre as the visible gain medium and a nonlinear amplifying loop mirror as the mode-locking element. First, we theoretically predict and analyse the formation and evolution of 635 nm mode-locked pulses in the dissipative soliton resonance (DSR) regime by solving the Ginzburg-Landau equation. Then, we experimentally demonstrate the stable generation of 635 nm DSR mode-locked pulses with a pulse duration as short as ~96 ps, a radio-frequency signal-to-noise ratio of 67 dB and a narrow spectral bandwidth of <0.1 nm. The experimental results are in excellent agreement with our numerical simulations. In addition, we also observe 635 nm noise-like pulse operation with a wide (>1 nm) and modulated optical spectrum. This work represents an important step towards miniaturized ultrafast fibre lasers in the visible spectral region., Competing Interests: Conflict of interestThe authors declare that they have no conflict of interest., (© The Author(s) 2020.)

The development of ultra-intense and ultra-short light sources is currently a subject of intense research driven by the discovery of novel phenomena in the realm of relativistic optics, such as the production of ultrafast energetic particle and radiation beams for applications. It has been a long-standing challenge to unite two hitherto distinct classes of light sources: those achieving relativistic intensity and those with pulse durations approaching a single light cycle. While the former class traditionally involves large-scale amplification chains, the latter class places high demand on the spatiotemporal control of the electromagnetic laser field. Here, we present a light source producing waveform-controlled 1.5-cycle pulses with a 719 nm central wavelength that can be focused to relativistic intensity at a 1 kHz repetition rate based on nonlinear post-compression in a long hollow-core fiber. The unique capabilities of this source allow us to observe the first experimental indications of light waveform effects in laser wakefield acceleration of relativistic energy electrons., Competing Interests: Conflict of interestT.N. and P.S. hold a patent on the stretched HCF design. Patent owner: Laser-Laboratorium Göttingen eV (37077 Göttingen, DE); inventors: Peter Simon, Tamas Nagy; patent no.: DE102007048769B3; status: granted; aspect: the described pulse compressor incorporates a type of hollow waveguide described in the above German patent. The remaining authors declare that they have no conflict of interest., (© The Author(s) 2020.)

The 2018 Nobel Prize in Physics was awarded to Arthur Ashkin (prize share ½), Gérard Mourou (prize share ¼), and Donna Strickland (prize share ¼) for "groundbreaking inventions in the field of laser physics." This feature article summarizes the development of "optical tweezers and their application to biological systems" by Arthur Ashkin, as well as the Mourou/Strickland method of "generating high-intensity, ultrashort optical pulses" known as chirped pulse amplification. Further developments are also briefly discussed.

Here, a single-step, biomimetic approach for the realization of omnidirectional transparent antireflective glass is reported. In particular, it is shown that circularly polarized ultrashort laser pulses produce self-organized nanopillar structures on fused silica (SiO 2 ). The laser-induced nanostructures are selectively textured on the glass surface in order to mimic the spatial randomness, pillar-like morphology, as well as the remarkable antireflection properties found on the wings of the glasswing butterfly, Greta oto, and various Cicada species. The artificial structures exhibit impressive antireflective properties, both in the visible and infrared frequency ranges, which are remarkably stable over time. Accordingly, the laser-processed glass surfaces show reflectivity smaller than 1% for various angles of incidence in the visible spectrum for s-p linearly polarized configurations. However, in the near-infrared spectrum, the laser-textured glass shows higher transmittance compared to the pristine. It is envisaged that the current results will revolutionize the technology of antireflective transparent surfaces and impact numerous applications from glass displays to optoelectronic devices., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Experimental methods that use free-electron laser (FEL) sources that can deliver short X-ray pulses below a 10 fs pulse duration and traditional optical lasers are ideal tools for pump-probe experiments. However, these new methods also come with a unique set of challenges, such as how to accurately determine temporal overlap between two sources at the femtosecond scale and how to correct for the pulse-to-pulse beam property fluctuations of the FEL light derived from the self-amplified spontaneous emission process. Over the past several years of performing pump-probe experiments at the Linac Coherent Light Source (LCLS), new methods and tools have been developed to improve the ways experimental timing is measured, monitored and scanned. The aim of this article is to present an overview of the most commonly used techniques at LCLS to perform pump-probe-type experiments., (open access.)

User operation at the European X-ray Free-Electron Laser Facility started at the SASE1 undulator beamline in fall 2017. The majority of the experiments utilize optical lasers (mostly ultrafast) for pump-probe-type measurements in combination with X-ray pulses. This manuscript describes the purpose-developed pump-probe laser system as installed at SASE1, implemented features and plans for further upgrades.

Conventional temporal focusing-based multiphoton excitation microscopy (TFMPEM) can offer widefield optical sectioning with an axial excitation confinement of a few microns. To improve the axial confinement of TFMPEM, a binary computer-generated Fourier hologram (CGFH) via a digital-micromirror-device (DMD) was implemented to intrinsically improve the axial confinement by filling the back-focal aperture of the objective lens. Experimental results show that the excitation focal volume can be condensed and the axial confinement improved about 24% according to the DMD holography. In addition, pseudouniform MPE can be achieved using two complementary CGFHs with rapid pulse-width modulation switching via the DMD. Furthermore, bioimaging of CV-1 in origin with SV40 genes-7 cells demonstrates that the TFMPEM with binary DMD holography can improve image quality by enhancing axial excitation confinement and rejecting out-of-focus excitation., ((2018) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE).)

Few-layer black phosphorus (BP) which exhibits excellent optical and electronic properties, has great potential applications in nanodevices. However, BP inevitably suffers from the rapid degradation in ambient air because of the high reactivity of P atoms with oxygen and water, which greatly hinders its wide applications. Herein, we demonstrate the electrostatic functionalization as an effective way to simultaneously enhance the stability and dispersity of aqueous phase exfoliated few-layer BP. The poly dimethyldiallyl ammonium chloride (PDDA) is selected to spontaneously and uniformly adsorb on the surface of few-layer BP via electrostatic interaction. The positive charge-center of the N atom of PDDA, which passivates the lone-pair electrons of P, plays a critical role in stabilizing the BP. Meanwhile, the PDDA could serve as hydrophilic ligands to improve the dispersity of exfoliated BP in water. The thinner PDDA-BP nanosheets can stabilize in both air and water even after 15 days of exposure. Finally, the uniform PDDA-BP-polymer film was used as a saturable absorber to realize passive mode-locking operations in a fiber laser, delivering a train of ultrafast pulses with the duration of 1.2 ps at 1557.8 nm. This work provides a new way to obtain highly stable few-layer BP, which shows great promise in ultrafast optics application.

The spectral dispersion of ultrashort pulses allows the simultaneous focusing of light in both space and time, which creates so-called spatiotemporal foci. Such space-time coupling may be combined with the existing holographic techniques to give a further dimension of control when generating focal light fields. In the present study, it is shown that a phase-only hologram placed in the pupil plane of an objective and illuminated by a spatially chirped ultrashort pulse can be used to generate three-dimensional arrays of spatio-temporally focused spots. By exploiting the pulse front tilt generated at focus when applying simultaneous spatial and temporal focusing (SSTF), it is possible to overlap neighboring foci in time to create a smooth intensity distribution. The resulting light field displays a high level of axial confinement, with experimental demonstrations given through two-photon microscopy and the non-linear laser fabrication of glass., Competing Interests: The authors declare no conflict of interest.

Ultrafast lasers have become increasingly important as research tools in laboratories and commercial enterprises suggesting laser safety, personal protection and awareness become ever more important. Laser safety eyewear are typically rated by their optical densities (OD) over various spectral ranges, but these measurements are usually made using low power, large beam size, and continuous beam conditions. These measurement scenarios are vastly different than the high power, small beam size, and pulsed laser beam conditions where ultrafast lasers have extremely high peak powers and broad spectra due to the short pulse durations. Many solid-state lasers are also tunable over a broad wavelength range, further complicating the selection of adequate laser safety eyewear. Eighteen laser eyewear filter samples were tested under real-world conditions using a Ti:Sapphire regenerative amplifier with output pulses centered at 800 nm running from 2 Hz to 1 KHz repetition rate. The typical maximum peak laser irrandiance employed was ca. 3 TW/cm 2 (800 nm wavelength, 450 uJ/pulse with 80 fs FWHM pulse duration) or less when damage occurred, depending on the sample. While many samples maintained their integrity under these test conditions, many plastic samples showed signs of failure which reduced their OD, in some cases transmitting 4 to 5 orders of magnitude higher than expected. In general, glass filters performed significantly better than plastic filters, exhibiting less physical damage to the substrate and less absorber degradation.

Low-dimensional (LD) materials demonstrate intriguing optical properties, which lead to applications in diverse fields, such as photonics, biomedicine and energy. Due to modulation of electronic structure by the reduced structural dimensionality, LD versions of metal, semiconductor and topological insulators (TIs) at the same time bear distinct nonlinear optical (NLO) properties as compared with their bulk counterparts. Their interaction with short pulse laser excitation exhibits a strong nonlinear character manifested by NLO absorption, giving rise to optical limiting or saturated absorption associated with excited state absorption and Pauli blocking in different materials. In particular, the saturable absorption of these emerging LD materials including two-dimensional semiconductors as well as colloidal TI nanoparticles has recently been utilized for Q-switching and mode-locking ultra-short pulse generation across the visible, near infrared and middle infrared wavelength regions. Beside the large operation bandwidth, these ultrafast photonics applications are especially benefit from the high recovery rate as well as the facile processibility of these LD materials. The prominent NLO response of these LD materials have also provided new avenues for the development of novel NLO and photonics devices for all-optical control as well as optical circuits beyond ultrafast lasers., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

In this work, we present all epi-direction detected images of an unstained mouse retina using multiphoton microscopy with a sub-50 fs Yb-fiber laser centered at 1.07 μm. This wavelength is particularly interesting as the fundamental wavelength is transparent to the anterior segment of the eye and the higher harmonics are above DNA-damaging UV wavelengths. We present a characterization of the multimodal signals emitted from the different retinal layers, as well as from the choroid and the sclera. By characterizing native multiphoton signals from the retina, we move closer to having Yb-fiber considered for in vivo diagnosis of retinal disease through multiphoton microscopy as well as for corrective therapies.

Two-color multiphoton microscopy through wavelength mixing of synchronized lasers has been shown to increase the spectral window of excitable fluorophores without the need for wavelength tuning. However, most currently available dual output laser sources rely on the costly and complicated optical parametric generation approach. In this report, we detail a relatively simple and low cost diamond Raman laser pumped by a ytterbium fiber amplifier emitting at 1055 nm, which generates a first Stokes emission centered at 1240 nm with a pulse width of 100 fs. The two excitation wavelengths of 1055 and 1240 nm, along with the effective two-color excitation wavelength of 1140 nm, provide an almost complete coverage of fluorophores excitable within the range of 1000-1300 nm. When compared with 1055 nm excitation, two-color excitation at 1140 nm offers a 90% increase in signal for many far-red emitting fluorescent proteins (for example, tdKatushka2). We demonstrate multicolor imaging of tdKa-tushka2 and Hoechst 33342 via simultaneous two-color two-photon, and two-color three-photon microscopy in engineered 3D multicellular spheroids. We further discuss potential benefits and applications for two-color three-photon excitation. In addition, we show that this laser system is capable of in vivo imaging in mouse cortex to nearly 1 mm in depth with two-color excitation., Competing Interests: Conflict Of Interest: The authors declare no conflict of interest.

Molybdenum disulfide (MoS2 ) and tungsten disulfide (WS2 ), two representative transition metal dichalcogenide materials, have captured tremendous interest for their unique electronic, optical, and chemical properties. Compared with MoS2 and WS2 , molybdenum ditelluride (MoTe2 ) and tungsten ditelluride (WTe2 ) possess similar lattice structures while having smaller bandgaps (less than 1 eV), which is particularly interesting for applications in the near-infrared wavelength regime. Here, few-layer MoTe2 /WTe2 nanosheets are fabricated by a liquid exfoliation method using sodium deoxycholate bile salt as surfactant, and the nonlinear optical properties of the nanosheets are investigated. The results demonstrate that MoTe2 /WTe2 nanosheets exhibit nonlinear saturable absorption property at 1.55 μm. Soliton mode-locking operations are realized separately in erbium-doped fiber lasers utilizing two types of MoTe2 /WTe2 -based saturable absorbers, one of which is prepared by depositing the nanosheets on side polished fibers, while the other is fabricated by mixing the nanosheets with polyvinyl alcohol and then evaporating them on substrates. Numerous applications may benefit from the nonlinear saturable absorption features of MoTe2 /WTe2 nanosheets, such as visible/near-infrared pulsed laser, materials processing, optical sensors, and modulators., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

We review the recent developments in the field of ultrafast Cherenkov fiber lasers. Two essential properties of such laser systems - broad wavelength tunability and high efficiency of Cherenkov radiation wavelength conversion are discussed. The exceptional performance of the Cherenkov fiber laser systems are highlighted - dependent on the realization scheme, the Cherenkov lasers can generate the femtosecond output tunable across the entire visible and even the UV range, and for certain designs more than 40 % conversion efficiency from the pump to Cherenkov signal can be achieved. The femtosecond Cherenkov laser with all-fiber architecture is presented and discussed. Operating in the visible range, it delivers 100-200 fs wavelength-tunable pulses with multimilliwatt output power and exceptionally low noise figure an order of magnitude lower than the traditional wavelength tunable supercontinuum-based femtosecond sources. The applications for Cherenkov laser systems in practical biophotonics and biomedical applications, such as bio-imaging and microscopy, are discussed.

Multiphoton laser scanning microscopy commonly relies on bulky and expensive femtosecond lasers. We integrated a novel minimal-footprint Ti:sapphire oscillator, pumped by a frequency-doubled distributed Bragg reflector tapered diode laser, into a clinical multiphoton tomograph and evaluated its imaging capability using different biological samples, i.e. cell monolayers, corneal tissue, and human skin. With the novel laser, the realization of very compact Ti:sapphire-based systems for high-quality multiphoton imaging at a significantly size and weight compared to current systems will become possible., (© 2015 Wiley Periodicals, Inc.)

Light-induced material phase transitions enable the formation of shapes and patterns from the nano- to the macroscale. From lithographic techniques that enable high-density silicon circuit integration, to laser cutting and welding, light-matter interactions are pervasive in everyday materials fabrication and transformation. These noncontact patterning techniques are ideally suited to reshape soft materials of biological relevance. We present here the use of relatively low-energy (< 2 nJ) ultrafast laser pulses to generate 2D and 3D multiscale patterns in soft silk protein hydrogels without exogenous or chemical cross-linkers. We find that high-resolution features can be generated within bulk hydrogels through nearly 1 cm of material, which is 1.5 orders of magnitude deeper than other biocompatible materials. Examples illustrating the materials, results, and the performance of the machined geometries in vitro and in vivo are presented to demonstrate the versatility of the approach.

Ultrafast optical lasers play an essential role in exploiting the unique capabilities of recently commissioned X-ray free-electron laser facilities such as the Linac Coherent Light Source (LCLS). Pump-probe experimental techniques reveal ultrafast dynamics in atomic and molecular processes and reveal new insights in chemistry, biology, material science and high-energy-density physics. This manuscript describes the laser systems and experimental methods that enable cutting-edge optical laser/X-ray pump-probe experiments to be performed at LCLS.

Using picosecond time-resolved photoelectron imaging, we have studied the intramolecular vibrational energy redistribution (IVR) dynamics that occur following the excitation of the 3(1)5(1) level, which lies 2068 cm(-1) above the S1 origin in p-difluorobenzene. Our technique, which has superior time resolution to that of earlier studies but retains sufficient energy resolution to identify the behavior of individual vibrational states, enables us to determine six distinct beating periods in photoelectron intensity, only one of which has been observed previously. Analysis shows that the IVR dynamics are restricted among only a handful of vibrational levels, despite the relatively high excitation energy. This is deduced to be a consequence of the high symmetry and rigid structure of p-difluorobenzene.