Light-Shaping of Valley States.

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.

Giant and Controllable Valley Currents in Graphene by Double Pumped THz Light.

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.

Pulse train gating to improve signal generation for in vivo two-photon fluorescence microscopy.

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 µm. 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.

Femtosecond Laser Machining of an X-ray Mask in a 500 Micron-Thick Tungsten Sheet.

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/cm2 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.

Wavelength-tunable broadband lasers based on nanomaterials.

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.

3D Imprinting of Voxel-Level Structural Colors in Lithium Niobate Crystal.

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 (LiNbO3 ) 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.

Pulse train gating to improve signal generation for in vivo two-photon fluorescence microscopy.

Significance: Two-photon microscopy is used routinely for in vivo imaging of neural and vascular structure and function 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 gates of high repetition rate ultrafast pulse trains to increase signal level. Aim: We investigate how 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 is used with a high-power (6 W) 80 MHz repetition rate ytterbium fiber amplifier 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 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. We verify similar increases for in vivo imaging to that observed in cuvette testing. For deep imaging we find pulse gating to result in a 2.95-fold increase in SNR and a 1.37-fold increase in SBR on average when imaging mouse cortical vasculature at depths ranging from 950 µm to 1050 µm. 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 structure through two-photon microscopy.

Thermodynamical Analysis of the Formation of α-Si Ring Structures on Silicon Surface.

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.

Ultrafast Laser Patterning of Metals Commonly Used in Medical Industry: Surface Roughness Control with Energy Gradient Pulse Sequences.

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.

Pulse-shaped broadband multiphoton excitation for single-molecule fluorescence detection in the far field.

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.

Laser Induced Coffee-Ring Structure through Solid-Liquid Transition for Color Printing.

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.

Tailoring the Coefficient of Friction by Direct Laser Writing Surface Texturing.

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.

In vivo hamster cheek pouch subepithelial ablation, biomaterial injection, and localization: pilot study.

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.

Effect of Substrate Temperature on Morphological, Structural, and Optical Properties of Doped Layer on SiO2-on-Silicon and Si3N4-on-Silicon Substrate.

A high concentration of Er3+ 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 TeO2 glass with a substrate to form a high Er3+ 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 (SiO2), 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 Si3N4. However, the doping was not as homogeneous as in silica.

Femtosecond pulses from a mid-infrared quantum cascade laser.

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.

Increasing the Efficiency of a Spintronic THz Emitter Based on WSe2/FeCo.

We report an increase in terahertz (THz) radiation efficiency due to FeCo/WSe2 structures in the reflection geometry. This can be attributed to an absorption increase in the alloy FeCo layer at the input FeCo/WSe2 interface due to constructive interference, as well as to the backward transport of hot carriers from FeCo to WSe2. 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.

Recent Progress of Two-Dimensional Materials for Ultrafast Photonics.

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.

60 fs, 1030†nm FEL pump-probe laser based on a multi-pass post-compressed Yb:YAG source.

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.

Layered PtSe2 for Sensing, Photonic, and (Opto-)Electronic Applications.

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 PtSe2 , 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 PtSe2 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 PtSe2 , 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 PtSe2 -based field-effect transistors, photodetectors, and sensors are summarized. Finally, a conclusion on these results along with the outlook for the future is presented.

Opening a new route to multiport coherent XUV sources via intracavity high-order harmonic generation.

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.