基于菌紫质F态的永久光存储研究

在线偏振飞秒激光激发下, 菌紫质通过双光子光化学反应可以生成具有永久光致各向异性的蓝移产物F₅₄₀态. 基于F₅₄₀态的永久光致各向异性, 通过调控飞秒激光空间光场分布, 可以在菌紫质薄膜中实现永久光信息存储. 本文使用纯相位型空间光调制器调制飞秒激光光场, 在物镜焦平面上生成光学点阵图案, 可以将信息快速记录在菌紫质薄膜中. 同时, 通过改变入射激光偏振方向, 可以实现偏振复用光存储, 这在高密度光存储和数据加密领域具有潜在应用.     

Ultrafast and nanosecond laser-induced desorption of positive ions from lithium fluoride single crystals

We compare desorption of positive ions from lithium fluoride single crystals following pulsed laser excitation using either femtosecond (180 fs, 265 nm) or nanosecond (3 ns, 266 nm) sources. Following optical excitation, desorbed ions are mass analyzed using standard time-of-flight techniques. Several important differences between nanosecond and femtosecond excitation are revealed. Femtosecond excitation produces higher kinetic energy Li⁺ than does nanosecond excitation (10 eV vs. 5 eV) while nanosecond excitation yields significant quantities of impurity ions Na⁺ and K⁺, in addition to efficient Li⁺ emission. The Li⁺ desorption threshold is similar for both laser sources. This similarity is a surprising result, as sub-bandgap nanosecond pulses are only likely to excite defect states efficiently (via linear excitation), while the ultrahigh peak-power femtosecond pulses could in principle induce multiphoton and avalanche excitation. Femtosecond excitation results in much less complicated time-of-flight spectra, as predominantly Li⁺ is detected with some H⁺ also observed. We have measured the Li⁺ yield as a function of time delay between two sub-threshold femtosecond laser pulses. We find that the majority of the Li⁺ yield decays rapidly, largely within the fs pulse duration. However, a weak but measurable decay component of approximately 2 ps is indicated.     

NONLINEAR EXCITED STATE ABSORPTION IN CADMIUM-PORPHYRIN-LIKE

Nonlinear absorption at 532 nm in a cadmium texaphyrin solution has been studied using 8ns and 23ps laser pulses. The experiments show that reverse saturable absorption occurs in the nanosecond case. For picosecond pulses, RSA occurs only at low fluences, and saturable absorption occurs at high fluences. A six-level model is proposed to explain these nonlinear absorption effects. Several photophysical parameters of excited states for cadmium texaphyrin, such as absorption cross-sections at 532nm and lifetime, have been evaluated by fitting theoretical calculations with the experimental results.     

Polarization-sensitive diffractive optical elements fabricated in BR films with femtosecond laser

Multi-photon product (F₅₄₀-state) of bacteriorhodopsin (BR) polymeric films excited by femtosecond laser shows permanently photoinduced birefringence and dichroism. Based on this property, polarization-sensitive diffractive optical elements (PDOEs), e.g., gratings, two-dimensional optical lattice, Bessel zone plate, were firstly fabricated and investigated in BR films by femtosecond laser multi-beam interference with rotationally symmetric pyramid lenses. These fabricated PDOEs are completely stable at room temperature. The dependence of diffraction efficiency on the incident polarization state was measured. The micro-structures of PDOEs were observed under polarization microscope, and the selective readout diffraction patterns from the polarization-multiplexed PDOEs were demonstrated.     

Z-scan studies and optical limiting of nanosecond laser pulses in neutral red dye

The nonlinear optical absorption, refraction and optical limiting behaviour of an organic dye, neutral red, were investigated under excitation with nanosecond laser pulses at 532 nm. The nonlinear optical responses of the material were studied both in solution and solid film, made in methanol and polyvinyl alcohol, respectively, using single-beam Z-scan technique. The open aperture Z-scans of the solution samples displayed a switch over from saturable absorption to enhanced absorption with increase in input intensity. Theoretical fit to the experimental data indicated that the dominant mechanism of nonlinear absorption is two-photon absorption. The closed aperture Z-scans of both the samples denoted positive nonlinearity, which was three orders larger in magnitude in solid film, compared with that in solution. The results of optical limiting experiments revealed that neutral red exhibited strong optical limiting of nanosecond laser pulses with a threshold lower than that of C₆₀ in toluene.     

Studies on third-order nonlinear optical properties and reverse saturable absorption in polythiophene/poly (methylmethacrylate) composites

We report here the studies on third-order nonlinear optical properties of two novel polythiophene composite films investigated using the Z-scan technique. The measurements were carried out using a Q-switched, frequency doubled Nd:YAG laser producing 7 nanosecond laser pulses at 532 nm. Z-scan results reveal that the composite films exhibit self-defocusing nonlinearity. The real and imaginary parts of the third-order nonlinear optical susceptibility were of the order 10⁻¹² esu. The effective excited-state absorption cross section was found to be larger than the ground state absorption cross section, indicating that the operating nonlinear mechanism is reverse saturable absorption (RSA). The polythiophene composite films also exhibit good optical power limiting of the nanosecond laser pulses. The nonlinear optical parameters are found to increase on increasing the strength of the electron-donor group, indicating the dependence of χ ⁽³⁾ on the electron-donor/acceptor units of polythiophenes.     

Nonlinear optical absorption and NIR to blue conversion in highly stable polymeric dye rod

A simple method for preparing transparent crack-free solid polymeric matrices is presented. Different dopants may be hosted in the polymeric matrix. The method is applied to prepare Glycidyl-methacrylate polymeric rods doped with solutions of coumarin 500 laser dye (ethanol and chloroform). The solvent??s effect has appeared as a shift in the absorption and photoluminous spectral bands of the laser dye in the solid polymeric host. The prepared solid samples showed nonlinear optical response on excitation with 532?nm of nanosecond laser pulses using the open aperture z-scan technique. Each sample shows different nonlinear behavior in response to the irradiating laser beam. The theoretical fitting of the experimental data indicates that the dominant mechanism of nonlinear absorption is the two-photon absorption process. Visible amplified spontaneous emission is reported in both polymeric dye rods by NIR pumping. High photostability is reported for the samples.     

Reverse saturable absorption in tetraphenylporphyrins

A decrease of the light transmission with increasing excitation intensity is observed in tetraphenylporphyrin/toluene solutions irradiated with 80 ps pulses at λ=532 nm. The experimental data are compared with simulations using a rate equation model. Excited state absorption cross-sections are evaluated.     

Nanosecond and femtosecond ablation of La0.6Ca0.4CoO3: a comparison between plume dynamics and composition of the films

Thin films of La_0.6Ca_0.4CoO₃ were grown by pulsed laser ablation with nanosecond and femtosecond pulses. The films deposited with femtosecond pulses (248 nm, 500 fs pulse duration) exhibit a higher surface roughness and deficiency in the cobalt content compared to the films deposited with nanosecond pulses (248 nm, 20 ns pulse duration). The origin of these pronounced differences between the films grown by ns and fs ablation has been studied in detail by time-resolved optical emission spectroscopy and imaging. The plumes generated by nanosecond and femtosecond ablation were analyzed in vacuum and in a background pressure of 60 Pa of oxygen. The ns-induced plume in vacuum exhibits a spherical shape, while for femtosecond ablation the plume is more elongated along the expansion direction, but with similar velocities for ns and fs laser ablation. In the case of ablation in the background gas similar velocities of the plume species are observed for fs and ns laser ablation. The different film compositions are therefore not related to different kinetic energies and different distributions of various species in the plasma plume which has been identified as the origin of the deficiency of species for other materials.     

Terahertz radiation by an ultrafast spontaneous polarization modulation of multiferroic BiFeO3 thin films

Terahertz (THz) radiation has been observed from multiferroic BiFeO3 thin films via ultrafast modulation of spontaneous polarization upon carrier excitation with illumination of femtosecond laser pulses. The radiated THz pulses from BiFeO3 thin films were clarified to directly reflect the spontaneous polarization state, giving rise to a memory effect in a unique style and enabling THz radiation even at zero-bias electric field. On the basis of our findings, we demonstrate potential approaches to ferroelectric nonvolatile random access memory with nondestructive readability and ferroelectric domain imaging microscopy using THz radiation as a sensitive probe.     

The nonlinear optical response of a fluorine-containing azoic dye

The nonlinear optical nonlinearities of a fluorine-containing azoic dye in tetrahydrofuran have been investigated by using Z-scan technique with picosecond and nanosecond lasers. The experimental results reveal that the azoic dye has large optical nonlinearity under the excitations of picosecond and nanosecond 532 nm. At the picosecond 532 nm the solution presents negative nonlinear refraction due to the electronic effect, while the larger nonlinear refraction under nanosecond laser excitation is induced by thermal effect. Moreover, the different nonlinear absorption behavior under picosecond and nanosecond excitations is analyzed.     

Spectral dependence of the excitation of the “forbidden” second optical harmonic in an aqueous suspension of purple membranes by femtosecond laser pulses under electronic resonance conditions

The spectral dependence of the efficiency of generation of the forbidden (in the electric-dipole approximation) second harmonic (FSH) and its energy on the energy of the excitation pulses is investigated experimentally in a highly disperse suspension of purple membranes containing bacteriorhodopsin (BR) under excitation by femtosecond laser pulses into the single-photon absorption band of BR. The experimental data for the case of resonance excitation attest to an interference character of the interaction of optical nonlinearities of different orders in the process leading to the formation of the FSH signal. Pis’ma Zh. éksp. Teor. Fiz. 67, No. 4, 251–255 (25 February 1998)     

Reverse saturable absorption and optical limiting in indanthrone dyes

Fluence dependence of transmission in three dyes, viz. indanthrone, dichloroindanthrone and violanthrone, is reported at 532 nm as well as at 1.06 µm. These dyes show optical limiting at both these wavelengths for nanosecond pulses. The limiting is due to the combined effect of reverse saturable absorption from the triplet state and thermal defocussing in the dye solutions.     

Ultrafast spectroscopy of high-lying excited states via eight-wave mixing

We demonstrate the use of eight-wave mixing (8WM) with femtosecond laser pulses for the detection of the high-lying D state of ethylene (C₂H₄) gas. The D state is reached through three-photon absorption of 427 nm light followed by a delayed single-photon probe interaction with the ionization continuum, resulting in an overall 8WM process. This scheme allows the detection of high-lying states with both spatial and temporal resolution before a thermal grating can form. Alternatively, by using a nanosecond delay between pulses, the induced thermal grating may be studied after the population grating has decayed. We verify the precise 8WM nature of this process and show how to use it to study the excited-state dynamics of ethylene and to measure the profile of an ethylene flow.     

Saturable and reverse saturable absorption in aqueous silver nanoparticles at off-resonant wavelength

Silver nano-colloid was prepared by chemical reduction method and its nonlinear absorption properties were investigated by using open aperture z-scan experiment with nanosecond laser pulses operating at 532?nm. Interestingly, a switch over from saturable absorption to reverse saturable absorption was observed when the input intensity is increased from 28.1 to 175.8?MW/cm². The underlying mechanism responsible for the observed switching behaviour is the interplay between ground state plasmon band bleaching and excited state absorption. Theoretical fitting was done by using a model in which nonlinear absorption coefficient as well as saturation intensity are incorporated.     

Single-photon and three-photon absorption induced whispering-gallery mode lasing in ZnO micronails

The ZnO micronails were synthesized by the vapor phase transport method. The heads of the micronails show hexagonal disk structure which is suitable for the whispering-gallery mode lasing microcavity. Under the excitation of a nanosecond pulse at 355 nm, the single-photon absorption induced lasing was stimulated in the micronail with the head diameter of 3.0 μm, the whispering gallery mode and Fabry-Pérot mode lasing were investigated. Under the excitation of femtosecond laser pulses at 804 nm, the second harmonic generation and the three-photon absorption induced photoluminescence were observed from a bulk of micronails, then an individual micronail with the diameter of 9.1 μm was employed to realize the three-photon absorption induced whispering-gallery mode lasing.     

Optical nonlinearities in hyperbranched polyyne studied by?two-photon excited fluorescence and third-harmonic generation spectroscopy

The nonlinear optical properties of a hyperbranched polyyne (hb-Polyyne) have been measured at infrared wavelengths by using femtosecond and nanosecond pulsed excitation. This hyperbranched polyyne exhibited strong and intrinsic (simultaneous) two-photon absorption and upconverted blue fluorescent emission under femtosecond excitation around 800 nm. The hb-Polyyne in chloroform solution is characterized by a large two-photon absorption cross section of 9068 GM (1GM=10⁻⁵⁰ cm⁴ s) and a fluorescence quantum yield of 0.57. On the other hand, by third-harmonic generation (THG) spectroscopy with nanosecond excitation, the measured third-order nonlinear susceptibility χ ⁽³⁾ for solid films of hb-Polyyne ranged from 2.4×10⁻¹¹ to 6.1×10⁻¹¹ esu in the spectral range of 1100–1600 nm, with results comparable to the values exhibited by the well-known conjugated polymer MEH:PPV, but with a much better transparency for visible wavelengths.     

Excited-state absorption in a terpyridyl platinum(II) pentynyl complex

The singlet excited-state lifetime of a terpyridyl platinum(II) pentynyl complex was determined to be 268+/-87 ps by fitting femtosecond transient absorption data, the triplet excited-state lifetime was found to be 62 ns by fitting nanosecond transient absorption decay data, and the triplet quantum yield was measured to be 0.16. A ground-state absorption cross section of 2.5 x 10(-19) cm(2) at 532 nm was deduced from UV-vis absorption data. Excited-state absorption cross sections of 3.5 x 10(-17) cm(2) (singlet) and 4.5 x 10(-17) cm(2) (triplet) were obtained by using a five-level dynamic model to fit open-aperture Z scans at picosecond and nanosecond pulse widths and a variety of pulse energies.     

Nonlinear response and optical limiting in SrBi(2)Ta(2)O(9) thin films

SrBi(2)Ta(2)O(9) (SBT) thin films on quartz substrates were prepared by use of the pulsed-laser deposition technique. The nonlinear refractive indices, n(2) , of the SBT films were measured by use of z-scan techniques with picosecond pulses. Large negative nonlinear refractive indices of 3.84 and 3.58cm(2)/GW were obtained for the wavelengths 532 nm and 1.064mum , respectively. The two-photon absorption coefficient was determined to be 7.3 cm/GW for 532 nm. The limiting behavior of SBT thin film on a quartz substrate was investigated in an f/5 defocusing geometry by use of 38-ps-duration, 532-nm, 1.064mum laser excitation.     

基于细菌视紫红质薄膜的空间光调制器实验研究

阐述了利用细菌视紫红质薄膜（BR薄膜）优良的非线性光学特性作为光寻址的空间光调制器的实验研究.BR有两个重要的光敏中间态（B态和M态），其吸收带（B态吸收峰为570nm，M态吸收峰为412nm）重叠区域较少，利用其正向（B→M）和逆向（M→B）光反应之间转化关系和B态与M态的差异吸收实现了相干光学图像到非相干光学图像的转换实验.采用经基因改性的细菌视紫红质薄膜（BRD96N）材料，使用670nm相干光作为写入光，530nm非相干光作为读出光，得到了分辨率约为200 lines/mm，对比度约为2.1∶1的 关键词： 光寻址空间光调制器 细菌视紫红质薄膜（BR薄膜） 非线性光学特性 相干光与非相干光图像相互转换