Femtosecond Pulsed Laser Beam Research Articles

An innovative detection technique for capillary electrophoresis: Localized terahertz emission-time domain spectroscopy

Terahertz (THz) time-domain spectroscopy (TDS) is a recently emerging analysis method which can provide unique information on molecular vibration and rotation induced by inter/intra-molecular interactions. Although the application of THz-TDS to high-performance microscale separation methods like capillary electrophoresis (CE) has been anticipated, it has been hindered due to the diffraction limit of THz wave (typically, hundreds µm). In order to realize CE-THz-TDS, in this study, we placed a narrow open-tubular capillary on the surface of a GaAs semiconductor substrate as a “localized” THz-emitter. By focusing femtosecond pulsed laser beams at the surface of a gallium arsenide (GaAs) substrate closest to the capillary, THz waves were locally generated to pass through the capillary, so that THz absorbance spectra were obtained from the capillary which has narrower inner diameter than the diffraction limit. As a typical result from acetic acid analysis in the CE-THz-TDS platform, information on the refractive index and extinction coefficient was obtained, which showed non-linear and linear concentration dependence, respectively, similar to conventional THz-TDS using large liquid cells. Finally, CE-THz-TDS analysis of several carboxylic acids was demonstrated. Two acids were successfully separated and detected with THz-TDS, where their electrophoretic mobility values were estimated as close to those obtained with conventional contactless conductivity detection. Our proposed CE-THz-TDS showed the potential for the systematic analysis of inter/intra-molecular weak interactions like hydrogen bonds, which are unable to obtain with conventional detectors.

Nanoscale local modification of PMMA refractive index by tip-enhanced femtosecond pulsed laser irradiation

Tip-enhanced optical effects have enabled a wide palette of nanoscale investigation techniques and recently they were successfully used to modify and manipulate matter with nanoscale spatial resolution. We contribute to this latter area by reporting a viable method to modify the refractive index of polymethyl methacrylate (PMMA). Local surface changes of the refractive index are accomplished by focusing a femtosecond pulsed near-infrared laser beam on the apex of a metalized nanosized tip, traditionally used in scanning probe microscopy (SPM). The refractive index is changed over a circular area with diameter <200 nm under 790 nm illumination, representing a four-fold increase in resolution compared to the current state-of-the-art. These results are obtained at low laser pulse energies (<0.5 nJ), which represents a two orders of magnitude advantage over previously reported methods. Besides enabling modifications of the refractive index with high lateral resolution, this method can pave the way towards other important applications such the fabrication of photonic crystal lattices and surface waveguides.

Terahertz shaping technology based on coherent beam combining

The generation of terahertz (THz) waves by focusing a femtosecond pulsed laser beam at a distance is able to overcome the strong absorption properties of air and has rapidly attracted the attention of industry. However, the poor directionality of the THz wave radiation generated by this method is not conducive to THz wave applications. By controlling the morphology of the ultrafast laser-excited plasma filament and its electron density distribution through coherent beam combining technology, we achieve direct THz beam shaping and are able to obtain THz wave radiation of Gaussian or arbitrary transverse distribution. The novel experimental approach proposed in this paper opens up the research field of direct THz wave shaping using plasma. Moreover, it innovates multi-parameter convergence algorithms and, by doing so, has the potential to find beam patterns with higher energy conversion efficiency and break the energy limit of THz waves emitted by lasers at high power.

I-design terahertz microfluidic chip for attomole-level sensing

We developed a nonlinear optical crystal-based compact terahertz (THz)-microfluidic chip with several I-design meta-atoms for attomole (amol)-level sensing of trace amounts of solution samples. The I-design meta-atom consists of a metallic strip with a micometer-sized gap sandwiched by other metallic strips. It is periodically arrayed in a row of 1 × 5 units. A point THz source locally generated by optical rectification at the irradiation spot of a femtosecond-pulse laser beam induces a tightly confined electric-field mode at the gap regions and modifies the resonance frequency when a microchannel fabricated along the space between the metallic strips is filled with solutions. Using this chip, we could detect minute changes in the concentration of trace amounts of ethanol- and glucose-water solutions and mineral water by measuring the shift in the resonance frequencies. We succeeded in detecting 472 amols of solutes in solutions less than 100 picoliters using an effective sensing area of 0.10 λ THz × 0.57 λ THz, which indicates an improvement of approximately one order of magnitude compared to the performance of existing chips. This technique compactifies THz-microfluidic chips with high sensitivity and would accelerate the development of microfluidics integrated with THz technology, such as lab-on-a-chip devices and THz micro total analysis systems.

Label-Free Super-Resolution Microscopy By Means of Transient Absorption Saturation

In recent decades, super-resolution optical microscopy has become an attractive research topic that typically has been developed based on fluorescent labelling that becomes the essential tool for breaking diffraction-limited in biological imaging. However, deep tissue and label-free imaging remain challenging, especially for tick and highly scattering biological specimens [1]. With the development of ultrashort pulse laser sources, non-linear optical (NLO) light-matter interaction has acquired a central role in optical microscopy for label-free imaging due to efficient signal generation in the non-linear process [2]. The advantages of NLO approaches include the reduction of scattering due to the use of near-infrared radiation, which enables high penetration depth and reduces the aberrations introduced by the specimen [1]. Non-linear interaction comprises the generation of sum frequencies, high-harmonic generation (SHG/ THG), Raman scattering, two-photon fluorescence and others [3]. Transient absorption, also known as pump-probe microscopy is a non-linear optical imaging technique that can probe the dynamics of the excited states. [1]. In this work, we perform super-resolution label-free imaging using our custom-built near-infrared pump-probe microscope. Two femtosecond pulsed laser beams, generated by an OPO pumped by a Ti:sapphire laser (Chameleon Ultra II and compact OPO Coherent), are coupled into a commercial laser scanning confocal microscope (Nikon A1 MP). We explore the saturation of transient absorption using a doughnut-shaped beam in the STED-like approach to saturate the absorption [3] and forward SHG and SFG processes to achieve label-free imaging at an improved spatial resolution. [1] Astratov V. (2019). “Label-Free Super-Resolution Microscopy”. Springer Nature.[2] Sheppard. C.J.R. (2020). Multiphoton Microscopy: a personal historical review with some future prediction. Biomed. Opt.[3]Zanini, G. et al. 2019. Label-Free Optical Nanoscopy of Single-Layer Graphene. ACS Nano.

Two-photon fluorescence-assisted laser ablation of non-planar metal surfaces: fabrication of optical apertures on tapered fibers for optical neural interfaces.

We propose a feedback-assisted direct laser writing method to perform laser ablation of fiber optic devices in which their light-collection signal is used to optimize their properties. A femtosecond-pulsed laser beam is used to ablate a metal coating deposited around a tapered optical fiber, employed to show the suitability of the approach to pattern devices with a small radius of curvature. During processing, the same pulses generate two-photon fluorescence in the surrounding environment and the signal is monitored to identify different patterning regimes over time through spectral analysis. The employed fs beam mostly interacts with the metal coating, leaving almost intact the underlying silica and enabling fluorescence to couple with a specific subset of guided modes, as verified by far-field analysis. Although the method is described here for tapered optical fibers used to obtain efficient light collection in the field of optical neural interfaces, it can be easily extended to other waveguide-based devices and represents a general approach to support the implementation of a closed-loop laser ablation system of fiber optics.

Solution-based green amplified spontaneous emission from colloidal perovskite nanocrystals exhibiting high stability

Solution-based optical amplification affords a host of benefits ranging from flexibility in the choice of cavity size and shape to high photostability afforded by the constant replenishment of gain media. Works reporting solution-based optical amplification in colloidal semiconductor nanocrystals, however, remain sparse due to the difficulty in achieving high particle number densities required for sustained optical gain. In this work, we demonstrate highly stable amplified spontaneous emission (ASE) from a solution of green-emitting CsPbBr3 perovskite nanocrystals dispersed in a nonpolar solvent after a facile postsynthesis processing step. This processing step not only allows for the purification of nanocrystals from their growth solution, but also allows for long-term colloidal stability at high particle concentrations. Although it is widely reported that perovskite nanocrystals suffer from poor chemical stability, our nanocrystal solutions retain their ASE properties despite long-term storage in excess of five months under ambient conditions. Photostability tests show steady ASE intensities in excess of three hours under constant photoexcitation from a femtosecond pulsed laser beam (&amp;gt;107 shots), far exceeding those of thin films by an order of magnitude. This work opens the possibility of harnessing colloidal CsPbBr3 nanocrystals as highly robust, solution-based optical gain media.

The influence of the ionization regime on femtosecond laser beam machining mono-crystalline diamond

Diamond is widely used in a series of industrial and scientific applications, including the micro-electro-mechanical systems, optical elements, ultra-precision machining tools, etc. Femtosecond laser beam machining is promising for high precision and high accuracy machining diamond material for its famous non-thermal machining regime. Initially, the laser ablation threshold was determined for the low and high laser fluence stage, respectively. Then, the ionization regime of femtosecond pulsed laser beam machining mono-crystalline diamond with different laser power was discussed. The influence of the ionization regime on laser machining also was analyzed basing on Raman analysis and laser machined surface topography. The laser ablation threshold was 0.29 J/cm2 for the low laser fluence stage and 2.35 J/cm2 for the high laser fluence stage, respectively. The calculation of the Keldysh parameter indicated that the multi-photon ionization prevailed in the low laser fluence stage while the tunneling ionization became dominant in the high laser fluence stage. The transition of the ionization regime from the multi-photon ionization to the tunneling ionization occurred around the laser fluence 3.2 J/cm2. Graphitization of diamond material was discovered on laser machined diamond surface by means of Raman analysis. Graphitization would be enhanced by the tunneling ionization regime in the high laser fluence stage. A strong surface cracking tendency was also observed in laser machining in the high fluence stage.

Modelling periodic structure formation on 100Cr6 steel after irradiation with femtosecond-pulsed laser beams

We investigate the periodic structure formation upon intense femtosecond pulsed irradiation of chrome steel (100Cr6) for linearly polarised laser beams. The underlying physical mechanism of the laser-induced periodic structures is explored, their spatial frequency is calculated and theoretical results are compared with experimental observations. The proposed theoretical model comprises estimations of electron excitation, heat transfer, relaxation processes, and hydrodynamics-related mass transport. Simulations describe the sequential formation of sub-wavelength ripples and supra-wavelength grooves. In addition, the influence of the laser wavelength on the periodicity of the structures is discussed. The proposed theoretical investigation offers a systematic methodology towards laser processing of steel surfaces with important applications.

Influence of femtosecond pulsed laser irradiation on bismuth germanium oxide single crystal properties

High quality bismuth germanium oxide single crystals were irradiated by a femtosecond pulsed laser beam of increasing power. Analyses performed on irradiated and unirradiated samples showed significant changes in transmittance, transmission spectra, sample color, Raman spectra, X-ray diffraction (XRD) pattern, Verdet constant, magneto-optical property, and absorption coefficient. After irradiation, the transmission spectra values increased whereas anisotropy detected in the transmission spectra of unirradiated samples disappeared. The change of color caused by irradiation was noticeable to the naked eye. The XRD measurements confirmed structural changes induced by laser irradiation, i.e., the laser-beam-incident side of the sample became almost amorphous, whereas the side opposite to the incident can be indexed to the Bi12GeO20 compound. Irradiation caused increase of Raman spectra peaks with the exception of crystal peaks of type E, which disappeared. The femtosecond pulsed laser irradiation can be used to improve bismuth germanium oxide single crystal optical properties.

Micro-modification in Borosilicate Glass Using Femtosecond Laser

Direct laser writing technique has gained popularity on account of its application potential for achieving micro-modification inside various glasses, crystals and transparent media. Such modification is an important requirement for efficient guidance of waves for modern communication technology and integrated optical devices. When a focused ultrashort laser beam gets absorbed in a transparent material via nonlinear absorption, it will lead to permanent modification in the optical properties of the solid within the focused volume. This phenomenon has been used to modify the optical property of borosilicate glass using 45 femtosecond pulse laser beam at 3 kHz repetition rate. Refractive index of the material changed along the beam path enabling writing of an optical waveguide. Structural modification in the laser treated area is confirmed on the basis of the results obtained from Raman and Fourier Transform Infrared spectra. Written waveguide structure supported guidance of HeNe laser beam at 633 nm and its transmitted profile were used to calculate the change in refractive index of the laser exposed area. An increased refractive index by 0.5 x 10-4 in the laser treated region was measured compared with surrounding glass.

3D microfabrication of single-wall carbon nanotube/polymer composites by two-photon polymerization lithography

We present a method to develop single-wall carbon nanotube (SWCNT)/polymer composites into arbitrary three-dimensional micro/nano structures. Our approach, based on two-photon polymerization lithography, allows one to fabricate three-dimensional SWCNT/polymer composites with a minimum spatial resolution of a few hundreds nm. A near-infrared femtosecond pulsed laser beam was focused onto a SWCNT-dispersed photo resin, and the laser light solidified a nanometric volume of the resin. The focus spot was three-dimensionally scanned, resulting in the fabrication of arbitrary shapes of SWCNT/polymer composites. SWCNTs were uniformly distributed throughout the whole structures, even in a few hundreds nm thick nanowires. Furthermore, we also found an intriguing phenomenon that SWCNTs were self-aligned in polymer nanostructures, promising improvements in mechanical and electrical properties. Our method has great potential to open up a wide range of applications such as micro- and nanoelectromechanical systems, micro/nano actuators, sensors, and photonics devices based on CNTs.

Optical trapping and polarization-controlled scattering of dielectric spherical nanoparticles by femtosecond laser pulses

Abstract We present optical trapping behavior of 50-nm-sized polystyrene beads, suspended in water medium, by femtosecond pulsed laser beam. In addition to a higher number of nanoparticles trapped at the focal spot by the ultrashort laser pulses compared with that by continuous-wave laser, the nanoparticles are scattered out of the focal spot by the laser pulses to the surrounding area. The scattered particles form a partially opened folding fan-shaped bright locus in two opposite directions, in an alternating manner, perpendicular to the laser polarization. To understand those phenomena, we analyzed radiation (gradient and scattering) force of femtosecond laser pulses and their temporal force exerted on the dielectric spherical nanoparticles by taking into account the impulsive peak power and the axial component of electric light field produced by high numerical aperture of objective lens. We show that the axial electric field is responsible for lateral components of the scattering and temporal forces, and hence, controls the scattering directions of the Rayleigh particles. These findings provide important information about the dynamic optical trapping of the Rayleigh particles by highly focused ultrashort laser pulses.

EUV soft X-ray characterization of a FEL multilayer optics damaged by multiple shot laser beam

We have investigated the damaging effects of a femtosecond pulsed laser beam with 400 nm wavelength on a Mo/Si EUV multilayer. The exposures have been done in vacuum with multiple pulses (5 pulses/mm 2) of 120 fs varying the laser fluence in the 38–195 mJ/cm 2 range. The analysis of the different irradiated regions has been performed ex-situ by means of different techniques, including specular and diffuse reflectivity, X-ray photoemission spectroscopy (XPS) and total electron yield (TEY) in the EUV and soft X-ray range. Surface images have been acquired by atomic force microscopy (AFM) and scanning electron microscopy (SEM). Results clearly indicate a progressive degradation of the EUV multilayer performances with the increase of the laser fluence. Spectroscopic analysis allowed to correlate the decrease of reflectivity with the degradation of the multilayer stacking, ascribed to Mo–Si intermixing at the Mo/Si interfaces of the first layers, close to the surface of the mirror.

Spatial distribution of carrier-envelope phase for femtosecond pulsed laser beam profile determined by asymmetric spectral interferometry

The spatial distribution of the carrier-envelope phase (CEP) for a femtosecond laser pulse from a regenerative amplifier was measured by a method based on the spectral interferometric technique. Our results show that the spatial distribution of the carrier-envelope phase from an ultrafast regenerative amplified laser is stable from pulse to pulse, but the difference between different locations within the laser profile is significant. In contrast, the CEP spatial distribution for the beam profile from the oscillator is homogenous within the experimental error. We attribute the observed spatial CEP distribution to the discrepancy between the dispersion of group velocity and phase velocity when the laser pulse passes through the dispersive optical elements, which can be corrected by a prism.

Effect of laser polarization direction on high order harmonic generation of oxygen molecule——A simulation via TDDFT

The high order harmonic generation (HHG) of O2 radiated by ultra-strong femto-second pulsed laser beam is simulated by the time dependent density functional theory (TDDFT) method with the general gradient approximation (GGA) of the exchange-correlation energy. The effect of different laser polarization directions on HHG is discussed. The results indicate that the HHG spectrum of O2 has the similar characteristic as the typical atom HHG spectrum. The HHG yields peaks when the molecules are aligned at about 45° from the polarization axis. Good agreements are found with the experiment.

A 04-mm-diameter probe for nonlinear optical imaging

A miniaturized probe that possesses a diameter of 0.4 mm is developed for two-photon-excited fluorescence imaging. The miniaturized probe was manufactured by the collapse of air holes and the formation of a lens on the tip of a double-clad photonic crystal fiber (DCPCF) using electric arc discharging from a conventional fusion splicer. As a result, a femtosecond pulsed laser beam delivered by the DCPCF can be directly focused on a sample for two-photon fluorescence imaging. The numerical aperture of the lensed DCPCF is 0.12. The corresponding focal spot size is 6 microm, which is close to the diffraction limit. This 0.4-mm-diamter probe can provide clear two-photon-excited fluorescence images of 10-microm-diameter fluorescent microspheres.

Femtosecond laser direct writing of metallic microstructures by photoreduction of silver nitrate in a polymer matrix

Continuous silver microstructures were produced by three-dimensional (3-D) direct laser writing using a femtosecond-pulsed laser beam with polyvinylpyrrolidone (PVP) films containing silver ions. The lines drawn by scanning a tightly focused laser beam ranged from 200 nm to 1.7 microm. Using a sample solution of high density of silver nitrate, a continuous silver line with a resistivity of 3.48 x 10(-7) ohms m was produced. Not only 3-D microstructures such as pyramidal models but also hybrid microstructures comprising polymer and silver lines were demonstrated. The 3-D direct laser writing of metallic microstructures has potential for application to 3-D electrical wiring of electronic devices and MEMS devices.

Two-photon-induced three-dimensional optical data storage in CdS quantum-dot doped photopolymer

The authors demonstrate three-dimensional erasable bit optical data storage in a quantum-dot doped photopolymer under two-photon excitation by a near-infrared femtosecond pulsed laser beam. It is shown that the photorefractive polymer consisting of poly(vinyl carbazole), ethyl carbazole, 4-(diethylaminobenzylidene)-malononitrile, and CdS quantum dots exhibits the changes not only in refractive index but also in fluorescence. Such a photosensitivity provides a multimode readout mechanism. In particular, the use of S rich surface quantum dots not only allows the two-photon-induced bit optical data storage with greater contrast but also expands the margin between permanent and erasable recording thresholds.

Deposition of tungsten nanogratings induced by a single femtosecond laser beam

Tungsten nanogratings with sub-100nm linewidths and subwavelength periods are fabricated by laser-induced chemical vapor deposition using a single 400 nm femtosecond pulsed laser beam without any beam shaping. Combining advantages of parallel and direct-write processing, this method can produce various nanograting structures on a wide range of substrates in a single step.