The onset of ultrashort pulse‐induced nanogratings

The fundamental formation process of nanogratings induced by focused ultrashort laser pulses inside the bulk of transparent materials is still object of intense debate. In particular the initial evolutionary steps, including the formation of anisotropic pores, alignment and arrangement in highly periodic grating planes could not been clarified up to now. To this end we have performed a comprehensive investigation of this process by optical retardance measurements, small‐angle X‐ray scattering, and focused ion beam milling in combination with scanning electron microscopy. The results show that the formation of nanogratings starts with isotropic, deterministic voids after the first incident laser pulse which start to elongate perpendicular to the laser scan direction with further illumination and the appearance of cracks along the scan direction. For increasing pulse overlap these cracks as well as randomly aligned voids build the template for the subsequent pore growth perpendicular to the laser polarization. The process of grating formation and subsequent period reduction occurs via increasing number of sheets and mutual realignment forming a more porous glass matrix.

     

Fabrication of multilayer metamaterials by femtosecond laser‐induced forward‐transfer technique

A novel method based on femtosecond laser‐induced forward transfer for high‐throughput and efficient fabrication of periodic multilayer plasmonic metamaterials is demonstrated. With precisely controlling laser raster path applied on sputtered multilayer thin films, the laser‐ablated materials can be transferred to another substrate leaving the fabricated multilayer structure on the original substrate. Subsequently, three‐dimensional metamaterials can be made by multilayer structuring. Moreover, all the experimental results show that to create such multilayer split resonant rings (SRRs) with uniform profile, the laser fluence should be fine controlled under proper conditions. The optical property of fabricated multilayer SRR array is investigated by optical measurements and finite‐difference time‐domain simulations, showing various resonant modes in the middle‐IR region. The calculated induced current distributions exhibit rich resonance properties of the structures as well. This work markedly extends the laser direct writing technique to a wide application in fabricating complicated metamaterials and plasmonic devices efficiently.     

Controllable femtosecond laser‐induced dewetting for plasmonic applications

Dewetting of thin metal films is one of the most widespread method for functional plasmonic nanostructures fabrication. However, simple thermal‐induced dewetting does not allow to control degree of nanostructures order without additional lithographic process steps. Here we propose a novel method for lithography‐free and large‐scale fabrication of plasmonic nanostructures via controllable femtosecond laser‐induced dewetting. The method is based on femtosecond laser surface pattering of a thin film followed by a nanoscale hydrodynamical instability, which is found to be very controllable under specific irradiation conditions. We achieve control over degree of nanostructures order by changing laser irradiation parametrs and film thickness. This allowed us to exploit the method for the broad range of applications: resonant light absorbtion and scattering, sensing, and potential improving of thin‐film solar cells.

     

飞秒激光离焦抽运熔融石英产生超连续白光的实验研究

利用飞秒激光在熔融石英介质中传输产生能量达数毫焦、波长范围覆盖400-900 nm 且光谱分布较为均匀的超连续白光,实验过程中将熔融石英介质离焦放置以避免被击穿. 研究了入射激光能量以及介质离焦距离对超连续白光特性的影响. 结果表明采用高能量的入射激光脉冲离焦抽运介质的方法能够有效避免介质 击穿损伤并提高超连续白光脉冲的能量输出.     

时间整形飞秒激光诱导熔融硅表面纳米周期条纹的电子动力学研究

研究了时间整形飞秒激光在熔融硅表面诱导纳米周期条纹结构的电子动力学过程.通过引入非线性电离机制和表面等离子激元的瞬态作用机理,建立了关于时间整形飞秒激光诱导和调控熔融硅表面纳米周期条纹结构的电子动力学模型,并应用该模型研究获得了纳米条纹周期与时间整形脉冲时间间隔的定量关系.理论研究结果表明,通过调节时间整形脉冲的时间间隔可以实现操控表面等离子激元与激光瞬态干涉过程中的波矢配对,最终可实现对诱导的纳米条纹周期的调控.此模型预测得到的纳米条纹周期与实验结果符合得很好.该研究对于深刻理解整形脉冲链诱导材料表面纳米周期结构的电子动力学操纵机制以及对条纹周期的调控都具有重要的理论价值.     

Time–space transformation of femtosecond free‐electron laser pulses by periodical multilayers

A scattering scheme to probe the time evolution of femtosecond pulses of a soft X‐ray free‐electron laser (FEL) in a multilayer structure is presented. The response of periodic multilayers (MLs) with low and high absorption and various numbers of bi‐layers to a pulse train of Gaussian‐shaped sub‐pulses is calculated. During the passage of the incident pulse the interaction length increases and the scattering profile changes as a function of the spatial position of the pulse within the sample. Owing to stretching of the reflected pulse compared with the incident pulse, the time‐dependent scattering evolution in the ML can be visualized along a spatial coordinate of a position‐sensitive detector. Using a scattering geometry where the mean energy of the incident pulse train is slightly detuned from the energy of maximum reflectivity at the first‐order peak, the response of the ML shows an oscillator behaviour along this spatial coordinate at the detector. For a FEL wavelength of 6.4 nm this effect is promising for MLs with low absorption, such as La/C for example. On the other hand, the oscillations will not be present for MLs with high absorption. Therefore a low‐absorbing ML is a sensitive tool for studying the possible change of sample absorption caused by femtosecond‐pulse interaction with matter.     

Diffraction of X‐ray free‐electron laser femtosecond pulses on single crystals in the Bragg and Laue geometry

A solution of the problem of dynamical diffraction for X‐ray pulses with arbitrary dimensions in the Bragg and Laue cases in a crystal of any thickness and asymmetry coefficient of reflection is presented. Analysis of pulse form and duration transformation in the process of diffraction and propagation in a vacuum is conducted. It is shown that only the symmetrical Bragg case can be used to avoid smearing of reflected pulses.     

飞秒激光烧蚀石英玻璃的实验与理论研究

实验研究了800nm飞秒激光作用下石英玻璃的破坏机理和烧蚀规律，给出了破坏阈值与脉冲宽度的关系.发展了雪崩击穿模型，计算了材料的烧蚀阈值与脉冲宽度的依赖关系，烧蚀深度、烧蚀体积与脉冲能量的依赖关系，研究了导带电子的扩散对材料中激光能量的沉积、分布，以及材料的破坏阈值和烧蚀规律的影响. 关键词： 飞秒激光脉冲 破坏机理 石英玻璃 电子扩散     

Raman spectroscopic studies of pulsed laser‐induced defect evolution in graphene

Raman spectra were obtained for graphene after irradiating the samples by pulsed laser (λ = 248 nm). Changes in the spectra were observed as the pulse laser energy density (PLED) was varied from 0.1 to 0.25 J/cm². Changes in bilayer graphene were accompanied by the appearance of the D peak and the broadening of the G peak. Changes in multilayer graphene are more profound as the Raman spectra changes from a multilayer to bilayer and subsequently to monolayer graphene in response to a slow increase in the PLED. The threshold PLED was found to be dependent on the number of graphene layers. We also irradiate graphene with very high PLED (much above the threshold), and the Raman spectra were found to be significantly changed. The G‐band became broader, and red shifted, while the intensity of the 2D‐band was drastically reduced and an intense defect‐related D peak appeared at about 1350 cm⁻¹. The laser ablation of graphene, both with low‐ and high‐energy intensity, is consistent with the reported theoretical predictions. Copyright © 2013 John Wiley & Sons, Ltd.     

飞秒激光烧蚀硅表面产生微纳结构过程中激光脉冲数目的影响

为了研究飞秒激光脉冲数目与硅表面形貌之间的关系,在相同的SF6气体氛围下,改变照射硅表面的飞秒激光脉冲数,发现在飞秒激光照射下由硅表面形成的微型锥状尖峰的高度与飞秒激光脉冲数呈现一种非线性关系.通过对该关系的研究有利于找出在制造具有较高吸收效率的高微型锥状尖峰的"黑硅"的实验条件,有利于基于"黑硅"材料的光电器件转化效...     

On the role of shot noise in carrier‐envelope phase stabilization

This paper represents a systematic investigation of detection shot noise in carrier‐envelope phase (CEP) stabilization. Numerical simulations are conducted to calculate the influence of shot noise in laser oscillators. These results are compared with experimental results for Ti:sapphire lasers. It is found that shot noise imposes a limitation for obtaining sub‐100 mrad CEP jitters. Careful interferometer design is necessary to push this limit toward 10 mrad. In contrast to oscillator stabilization, shot noise appears to play a much more restrictive role in amplifier stabilization. Using spectral interferometry together with spectral broadening in sapphire, it already appears practically challenging to reach sub‐100 mrad jitters. Adaption of the optical nonlinearity in the broadening step appears key to further improvements of the CEP jitter of amplified systems. We believe that these improvements open a perspective for currently unfeasible applications of CEP stabilized pulses. Moreover, our considerations can be easily adapted to CEP stabilization of other laser types beyond Ti:sapphire.     

K9和熔石英玻璃纳秒基频激光损伤特性的实验对比研究

利用光学元件基频激光损伤测试平台,通过实验测试相同条件下K9和熔石英两类常用 光学元件的初始损伤阈值、损伤增长阈值和损伤增长规律,对比研究了两类光学元件的基频激光损伤特性.结果表明,K9和熔石英光学元件的初始损伤阈值基本相同,损伤面积增长都遵循指数性增长规律,损伤深度成线性增长.但两者损伤增长特性仍有很大的差别,与熔石英相比,K9激光损伤增长阈值较低,并且相同通量下的激光损伤增长更为迅速,通过两类光学材料抗压性能的巨大差异很好地解释了这一现象.该研究结果对国内高功率激光装置的透射光学材料工程应用有非常重要的参考价值.     

Exact solution of the ion‐laser interaction in all regimes

We show that in the trapped ion‐laser interaction all the regimes may be considered analytically. We may solve not only for different laser intensities, but also away from resonance and from the Lamb‐Dicke regime. It is found a dispersive Hamiltonian for the high intensity regime, that, being diagonal, its evolution operator may be easily calculated.     

Three‐dimensional femtosecond laser micromachining of photosensitive glass for biomicrochips

Internal modification of transparent materials such as glass can be carried out using multiphoton absorption induced by a femtosecond (fs) laser. The fs‐laser modification followed by thermal treatment and successive chemical wet etching in a hydrofluoric (HF) acid solution forms three‐dimensional (3D) hollow microstructures embedded in photosensitive glass. This technique is a powerful method for directly fabricating 3D microfluidic structures inside a photosensitive glass microchip. We used fabricated microchips, referred to as a nanoaquarium, for dynamic observations of living microorganisms. In addition, the present technique can also be used to form microoptical components such as micromirrors and microlenses inside the photosensitive glass, since the fabricated structures have optically flat surfaces. The integration of microfluidics and microoptical components in a single glass chip yields biophotonic microchips, in other words, optofluidics, which provide high sensitivity in absorption and fluorescence measurements of small volumes of liquid samples.     

Simultaneous birefringence,small‐ and wide‐angle X‐ray scattering to detect precursors and characterize morphology development during flow‐induced crystallization of polymers

An experimental configuration that combines the powerful capabilities of a short‐term shearing apparatus with simultaneous optical and X‐ray scattering techniques is demonstrated, connecting the earliest events that occur during shear‐induced crystallization of a polymer melt with the subsequent kinetics and morphology development. Oriented precursors are at the heart of the great effects that flow can produce on polymer crystallization (strongly enhanced kinetics and formation of highly oriented crystallites), and their creation is highly dependent on material properties and the level of stress applied. The sensitivity of rheo‐optics enables the detection of these dilute shear‐induced precursors as they form during flow, before X‐ray techniques are able to reveal them. Then, as crystallization occurs from these precursors, X‐ray scattering allows detailed quantification of the characteristics and kinetics of growth of the crystallites nucleated by the flow‐induced precursors. This simultaneous combination of techniques allows unambiguous correlation between the early events that occur during shear and the evolution of crystallization after flow has stopped, eliminating uncertainties that result from the extreme sensitivity of flow‐induced crystallization to small changes in the imposed stress and the material. Experimental data on a bimodal blend of isotactic polypropylenes are presented.     

Measurement of the absolute Raman scattering cross section of the 1584‐cm−1 band of benzenethiol and the surface‐enhanced Raman scattering cross section enhancement factor for femtosecond laser‐nanostructured substrates

The absolute Raman scattering cross section (σ_RS) for the 1584‐cm⁻¹ band of benzenethiol at 897 nm (1.383 eV) has been measured to be 8.9 ± 1.8 × 10⁻³⁰ cm² using a 785‐nm pump laser. A temperature‐controlled, small‐cavity blackbody source was used to calibrate the signal output of the Raman spectrometer. We also measured the absolute surface‐enhanced Raman scattering cross section (σ_SERS) of benzenethiol adsorbed onto a silver‐coated, femtosecond laser‐nanostructured substrate. Using the measured values of 8.9 ± 1.8 × 10⁻³⁰ and 6.6 ± 1.3 × 10⁻²⁴ cm² for σ_RS and σ_SERS respectively, we calculate an average cross‐section enhancement factor (EF) of 0.8 ± 0.3 × 10⁶. Copyright © 2009 John Wiley & Sons, Ltd.     

Micro‐Raman and stratigraphic studies of the paintings on the ‘Cembalo’ model musical instrument (A.D. 1650) and laser‐induced degradation of the detected pigments

Micro‐fragments of the painted part of the ‘Cembalo’ model by Michele Todini (1625–1689) are investigated. The technique used for painting the terracotta base was studied via the stratigraphic analyses. No background layer of inorganic materials, e.g. gypsum, was found. To prevent absorption effects due to the terracotta porosity, a very thin layer of proteinaceous material was probably used. The micro‐Raman analyses have revealed the use of pigments currently used in the post‐Renaissance period (lead white, indigo, yellow of iron hydroxide, gypsum, hematite and carbon black) mixed with a pigment, the Prussian blue, discovered in A.D . 1704. This raises the authenticity problem of the work of art, a problem analysed and discussed in presenting the history of the work of art, and after the pigment study. The presence of degraded lead white is recognized via the laser‐induced degradation of the irradiated material. The possibility of a restoring action of the painted parts, as opposite to the non‐originality of the work, is considered and discussed. Since most part of the investigated pigments shows laser‐induced effects, a careful study of this phenomenon is performed by using the modern counterparts of the ancient pigments. For different laser powers, the temperatures of the investigated zones have been obtained via the detailed balance principle and connected to the laser‐induced degradation effects. Copyright © 2007 John Wiley & Sons, Ltd.     

On the Theory of Hydrogen Atom Ionization by Ultra‐Short Electromagnetic Pulses

An investigation of the probability of hydrogen atom ionization by ultra‐short electromagnetic pulses is carried out in the frame of perturbation theory We consider the case when the electric field strength amplitude E₀ in a pulse by two orders lower than characteristic atomic field strength E_a (E_a ? 5.1 · 10⁹ V/cm). A detailed investigation of the dependence of the probabilities on the pulse duration was performed for Gaussian pulse shapes. In the case where the carrier frequency of the Gaussian pulse is larger than the atomic ionization potential, the probability goes to the standard limit of perturbation per unit time. At the same pulse durations, the probabilities for carrier frequencies less than the ionization potential go to zero. The frequency dependence of the ionization probability becomes equal to the standard threshold dependence with increasing pulse duration time. A comparison between the ionization effects caused by wavelet pulses without carrier frequency and Gaussian pulses with carrier frequency shows that the same ionization probability values are achieved when the pulse carrier frequency is detuned by about 20% from the ionization threshold. (© 2015 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Self‐doping PPV oligomers – electrochemistry and structure of the self‐doped systems

A novel class of self‐doping conjugated oligomers, E,E‐2‐(sulfoalkoxy)‐5‐alkoxy‐1,4‐bis[2‐(2,4,6‐trimethoxyphenyl) ethenyl]benzenes, is presented. The synthesis and spectroscopic characterisation of five such oligomers are described, and an electrochemical analysis using cyclic voltammetry is performed to determine the anodic peak potentials. A structural study is performed on six self‐doping oligomers in which the structures and energies of the possible mono‐molecular forms of the electrically conducting doped material are described and evaluated using Hirshfeld charges and the Quantum Theory of Atoms In Molecules. Copyright © 2009 John Wiley & Sons, Ltd.     

Fabrication of 6,13‐bis(triisopropyl‐silylethynyl)–pentacene thin‐film transistors with the silver ink transfer method using a polymer stamp

We fabricated 6,13‐bis(triisopropylsilylethynyl)–pentacene (TIPS–pentacene) thin film transistors using a direct metal transfer method. Using different metals, such as Au and Ag ink, electrode patterns are formed from the relief region of the polymer mold. TIPS–pentacene TFTs using the Ag ink transfer method show a similar performance to those using the Au metal transfer method. This method has advantages over the Au metal transfer method because it does not require vacuum equipment and a dry etching process. The self‐assembled monolayer (SAM) treated device exhibits a carrier mobility of 9.5 × 10^–2 cm²/V · s, and an on/off ratio of 4.6 × 10⁴. (© 2011 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)