Polarization control of multi-photon absorption under intermediate femtosecond laser field

It has been shown that the femtosecond laser polarization modulation is a very simple and well-established method to control the multi-photon absorption process by the light–matter interaction. Previous studies mainly focused on the multiphoton absorption control in the weak field. In this paper, we further explore the polarization control behavior of multiphoton absorption process in the intermediate femtosecond laser field. In the weak femtosecond laser field, the secondorder perturbation theory can well describe the non-resonant two-photon absorption process. However, the higher order nonlinear effect(e.g., four-photon absorption) can occur in the intermediate femtosecond laser field, and thus it is necessary to establish new theoretical model to describe the multi-photon absorption process, which includes the two-photon and four-photon transitions. Here, we construct a fourth-order perturbation theory to study the polarization control behavior of this multi-photon absorption under the intermediate femtosecond laser field excitation, and our theoretical results show that the two-photon and four-photon excitation pathways can induce a coherent interference, while the coherent interference is constructive or destructive that depends on the femtosecond laser center frequency. Moreover, the two-photon and fourphoton transitions have the different polarization control efficiency, and the four-photon absorption can obtain the higher polarization control efficiency. Thus, the polarization control efficiency of the whole excitation process can be increased or decreased by properly designing the femtosecond laser field intensity and laser center frequency. These studies can provide a clear physical picture for understanding and controlling the multi-photon absorption process in the intermediate femtosecond laser field, and also can provide a theoretical guidance for the future experimental realization.     

Up-conversion luminescence tuning in Er~(3+) -doped ceramic glass by femtosecond laser pulse at different laser powers

The up-conversion luminescence tuning of rare-earth ions is an important research topic for understanding luminescence mechanisms and promoting related applications. In this paper, we experimentally study the up-conversion luminescence tuning of Er~(3+)-doped ceramic glass excited by the unshaped, V-shaped and cosine-shaped femtosecond laser field with different laser powers. The results show that green and red up-conversion luminescence can be effectively tuned by varying the power or spectral phase of the femtosecond laser field. We further analyze the up-conversion luminescence tuning mechanism by considering different excitation processes, including single-photon absorption(SPA), two-photon absorption(TPA), excited state absorption(ESA), and energy transfer up-conversion(ETU). The relative weight of TPA in the whole excitation process can increase with the increase of the laser power, thereby enhancing the intensity ratio between green and red luminescence(I_(547)/I_(656)). However, the second ETU(ETU2) process can generate red luminescence and reduce the green and red luminescence intensity ratio I_(547)/I_(656), while the third ESA(ESA3) process can produce green luminescence and enhance its control efficiency. Moreover, the up-conversion luminescence tuning mechanism is further validated by observing the up-conversion luminescence intensity, depending on the laser power and the down-conversion luminescence spectrum under the excitation of 400-nm femtosecond laser pulse. These studies can present a clear physical picture that enables us to understand the up-conversion luminescence tuning mechanism in rare-earth ions, and can also provide an opportunity to tune up-conversion luminescence to promote its related applications.     

Simulating the resonance-mediated (1+2)-three-photon absorption enhancement in Pr3+ ions by a rectangle phase modulation

Enhancing the upconversion luminescence of rare earth ions is crucial for their applications in the laser sources, fiber optic communications, color displays, biolabeling, and biomedical sensors. In this paper, we theoretically study the resonance-mediated (1+2)-three-photon absorption in Pr³⁺ ions by a rectangle phase modulation. The results show that the resonance-mediated (1+2)-three-photon absorption can be effectively enhanced by properly designing the depth and width of the rectangle phase modulation, which can be attributed to the constructive interference between on-resonant and near-resonant three-photon excitation pathways. Further, the enhancement efficiency of resonance-mediated (1+2)-three-photon absorption can be affected by the pulse width (or spectral bandwidth) of femtosecond laser field, final state transition frequency, and absorption bandwidths. This research can provide a clear physical picture for understanding and controlling the multi-photon absorption in rare-earth ions, and also can provide theoretical guidance for improving the up-conversion luminescence.     

Coherent Features of Resonance-Mediated Two-Photon Absorption Enhancement by Varying the Energy Level Structure,Laser Spectrum Bandwidth and Central Frequency

The femtosecond pulse shaping technique has been shown to be an effective method to control the multi-photon absorption by the light-matter interaction. Previous studies mainly focused on the quantum coherent control of the multi-photon absorption by the phase, amplitude and polarization modulation, but the coherent features of the multi-photon absorption depending on the energy level structure, the laser spectrum bandwidth and laser central frequency still lack in-depth systematic research. In this work, we further explore the coherent features of the resonance-mediated two-photon absorption in a rubidium atom by varying the energy level structure, spectrum bandwidth and central frequency of the femtosecond laser field. The theoretical results show that the change of the intermediate state detuning can effectively influence the enhancement of the near-resonant part, which further affects the transform-limited(TL)-normalized final state population maximun. Moreover, as the laser spectrum bandwidth increases, the TL-normalized final state population maximum can be effectively enhanced due to the increase of the enhancement in the near-resonant part, but the TL-normalized final state population maximum is constant by varying the laser central frequency. These studies can provide a clear physical picture for understanding the coherent features of the resonance-mediated two-photon absorption, and can also provide a theoretical guidance for the future applications.     

Optimal spectral phase control of femtosecond laser-induced up-conversion luminescence in Sm3+:NaYF4 glass

The spectral phase of the femtosecond laser field is an important parameter that affects the up-conversion(UC)luminescence efficiency of dopant lanthanide ions.In this work,we report an experi-mental study on controlling the UC lmiiinescence efficiency in Sm^3+:NaYF4 glass by 800-nm femtosec-ond laser pulse shaping using spectral phase modulation.The optimal phase control strategy efficiently enhances or suppresses the UC luminescence intensity.Based on the laser-power dependence of the UC luminescence intensity and its comparison with the luminescence spectrum under direct 266-nm fem-tosecond lciser irradiation,we propose herein an excitation model combining non-resonant two-photon absorption with resonance-media ted three-photon absorption to explain the experimental observations.     

Simulating resonance-mediated two-photon absorption enhancement in rare-earth ions by a rectangle phase modulation

Improving the up-conversion luminescence efficiency of rare-earth ions via the multi-photon absorption process is crucial in several related application areas. In this work, we theoretically propose a feasible scheme to enhance the resonance-mediated two-photon absorption in Er~(3+) ions by shaping the femtosecond laser field with a rectangle phase modulation. Our theoretical results show that the resonance-mediated two-photon absorption can be decomposed into the on-resonant and near-resonant parts, and the on-resonant part mainly comes from the contribution of laser central frequency components, while the near-resonant part mainly results from the excitation of low and high laser frequency components.So, the rectangle phase modulation can induce a constructive interference between the two parts by properly designing the modulation depth and width, and finally realizes the resonance-mediated two-photon absorption enhancement. Moreover, our results also show that the enhancement efficiency of resonance-mediated two-photon absorption depends on the laser pulse width(or laser spectral bandwidth), final state transition frequency, and intermediate and final state absorption bandwidths. The enhancement efficiency modulation can be attributed to the relative weight manipulation of on-resonant and near-resonant two-photon absorption in the whole excitation process. This study presents a clear physical insight for the quantum control of resonance-mediated two-photon absorption in the rare-earth ions, and there will be an important significance for improving the up-conversion luminescence efficiency of rare-earthions.     

Up-conversion luminescence polarization control in Er~(3+)-doped NaYF_4 nanocrystals

We propose a femtosecond laser polarization modulation scheme to control the up-conversion(UC) luminescence in Er~(3+)-doped NaYF_4 nanocrystals dispersed in the silicate glass. We show that the UC luminescence can be suppressed when the laser polarization is changed from linear through elliptical to circular, and the higher repetition rate will yield the lower control efficiency. We theoretically analyze the physical control mechanism of the UC luminescence polarization modulation by considering on- and near-resonant two-photon absorption, energy transfer up-conversion, and excited state absorption, and show that the polarization control mainly comes from the contribution of near-resonant two-photon absorption. Furthermore, we propose a method to improve the polarization control efficiency of UC luminescence in rare-earth ions by applying a two-color femtosecond laser field.     

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.     

Entangled femtosecond free induction signals in a cadmium sulfide crystal at room temperature

Entangled free induction decay (EFID) femtosecond signals are experimentally observed for the first time at a wavelength of 790 nm in a cadmium sulfide (CdS) crystal in the two-photon absorption (TPA) regime upon excitation by two crossed (angle, 60°) laser beams. The sample emitted two EFID signals simultaneously in opposite directions. The signals were diffracted by nonequilibrium electric polarization gratings induced by two laser beams in accordance with the laws of energy and momentum conservation. The possibility of exciting EFID signals in the three-photon absorption regime is discussed.     

Upconversion luminescent characteristics and peak shift of CdSeS nanocrystals under different wavelength laser excitation

Upconversion luminescence was obtained from CdSeS nanocrystals (NCs) under 800 nm femtosecond laser excitation. The structural and optical characteristics of the CdSeS NCs were investigated experimentally by use of UV–visible absorption spectroscopy, transmission electron microscopy, X-ray diffractometry, and time-resolved luminescence dynamics. Peak shift of luminescence in CdSeS NCs can be readily observed under different wavelength femtosecond excitation. The pump power dependence of the luminescence intensity and time-resolved decay revealed that one, two, and three-photon absorption occur. It was found that upconversion luminescence is composed of photoinduced trapping and a band-edge excitonic state, and two types of species are involved in the biexponential luminescence decay kinetics. With increasing Se-doped composition, luminescence lifetimes of CdSeS NCs with similar sizes become shorter. This is not consistent with the changes of undoped CdS NCs and is ascribed to impurity level increased doping in the energy gap, which is favorable for trapping luminescence. A simple energy level of doping NCs is used to interpret upconversion luminescence and the peak shift of steady-state emission.     

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.     

Simultaneous three-photon-excited violet upconversion luminescence of Ce3+:Lu2Si2O7 single crystals by femtosecond laser irradiation

We found that Ce3+:Lu2Si2O7 single crystals could be excited at 800 nm by using a femtosecond Ti:sapphire laser. The emission spectra of Ce3+:Lu2Si2O7 crystals were the same for one-photon excitation at 267 nm as for excitation at 800 nm. The emission intensity of Ce3+:Lu2Si2O7 crystals was found to depend on the cube of the laser power at 800 nm, consistent with simultaneous absorption of three 800 nm photons. The measured value of the three-photon absorption cross section is sigma'3=2.44x10(-77) cm6 s2.     

Three-photon interference spectra in four-level atomic systems

We have considered the interference spectra that occur at the three-photon generated frequency arising from the interaction of three laser fields with a four-level atom, where two of the laser fields are on two-photon resonance with the three levels forming a “λ” scheme while the third laser operates between the second ground and the second excited state of the atom. At low intensities of all three laser fields, the overall intensity of the peak at the three-photon generated frequency, describing the spectrum of an electron in the second excited state, depends on the strength of the combined field of the two laser fields that are on two-photon resonance and it takes negative values. This indicates that light amplification without population inversion is likely to occur at the three-photon generated frequency. The combined field of the three laser fields induces multiphoton excitations near the three-photon generated frequency, whose peaks are characterized by linewidths which are much less than the natural linewidths of the atoms. These excitations describe absorption or stimulating emission processes depending on the values of the detunings of the laser fields. The derived results are graphically presented and discussed. Received: 24 January 2001 / Published online: 8 June 2001     

低强度飞秒激光激发下CdTe和CdTe/CdS核壳量子点的荧光上转换研究

利用400 nm和800 nm不同波长的低强度飞秒激光,对CdTe和CdTe/CdS核壳量子点溶胶进行激发,研究其稳态和时间分辨荧光性质.800 nm飞秒激光激发下,CdTe和CdTe/CdS核壳量子点产生上转换发光现象,上转换荧光峰与400 nm激发下的荧光峰相比蓝移最多达15 nm,而且蓝移值与荧光量子产率有关.变功率激发确认激发光功率与上转换荧光强度间满足二次方关系,时间分辨荧光的研究表明荧光动力学曲线服从双e指数衰减.提出表面态辅助的双光子吸收模型是低激发强度上转换发光的主要机理.CdTe和CdT 关键词： CdTe量子点 CdTe/CdS核壳量子点 时间分辨荧光 上转换荧光     

Efficient multiphoton-absorption-induced luminescence in single-crystalline ZnO at room temperature

At room temperature, multiphoton absorption- (MPA-) induced photoluminescence in ZnO strongly driven by a femtosecond (fs) near-infrared laser is studied. Two-photon absorption and three-photon absorption are proved to be responsible for the intense luminescence, when the wavelength of the fs excitation laser is above and below the half-bandgap of ZnO, respectively. Strong MPA absorption in ZnO is unambiguously evidenced by the interferometric autocorrelation measurements of the luminescence signal.     

Multichannel selective femtosecond coherent control based on symmetry properties

We present and implement a new scheme for extended multichannel selective femtosecond coherent control based on symmetry properties of the excitation channels. Here, an atomic nonresonant two-photon absorption channel is coherently incorporated in a resonance-mediated (2+1) three-photon absorption channel. By proper pulse shaping, utilizing the invariance of the two-photon absorption to specific phase transformations of the pulse, the three-photon absorption is tuned independently over an order-of-magnitude yield range for any possible two-photon absorption yield. Noticeable is a set of "two-photon dark pulses" inducing widely tunable three-photon absorption.     

CS_2分子激发态的紫外多光子电离——双色激光单共振离化的功率密度关系

本文报道气相CS_2紫外双色激光单共振离化的功率密度关系和对高激发态(1~Ⅱg),共振离化特性的研究结果,实验指出通过中间共振态(1~Ⅱ_g)的双光子共振激发三光子离化具有比通过中间共振态((?)A_2)的单光子共振激发三光子离子为高的总离化率,在10~7W/cm~2的功率密度下,观察到饱和效应.实验显示了双色激光单共振离化功率密度关系的研究提供了一种新的光谱学分析方法.这对研究分子高激发态的结构是很重要的.     

Three-photon-induced fluorescence of diphenylhexatriene in solvents and lipid bilayers

We observed the emission of l,6-diphenyl-l,3,5-hexatriene (DPH) when excited with the fundamental output of a fs Ti:sapphire laser at 860 nm. The emission spectra of DPH were identical to that observed for one-photon excitation at 287 nm. The dependence of the DPH emission intensity on laser power was cubic, indicating three-photon excitation of DPH at 860 nm. At a shorter wavelength of 810 nm, the dependence on laser power was quadratic, indicating a two-photon process. At an intermediate wavelength of 830 nm the mode of excitation was a mixture of two- and three-photon excitation. At 830 nm the anisotropy is no longer a molecular parameter, and the mode of excitation and anisotropy of DPH depends on laser power. Frequency-domain anisotropy decays of DPH in triacetin revealed the same rotational correlation times for two- and three-photon excitation. However, the time 0 anisotropy of DPH was larger for three-photon excitation than for two-photon excitation. Steady-state anisotropy data for DPH-labeled membranes revealed the same transition temperature for one- and three-photon excitation. These anisotropy data indicate that membrane heating was not significant with three-photon excitation and that three-photon excitation may thus be of practical usefulness in fluorescence spectroscopy and microscopy of membranes.     

Polarization multiplexed write-once-read-many optical data storage in bacteriorhodopsin films

In polymeric films of bacteriorhodopsin (BR) a photoconversion product, which was named the F620 state, was observed on excitation of the film with 532 nm nanosecond laser pulses. This photoproduct shows a strong nonlinear absorption. Such BR films can be used for write-once-read-many (WORM) optical data storage. We demonstrate that a photoproduct similar or even identical to that obtained with nanosecond pulses is generated on excitation with 532 nm femtosecond pulses. This photoproduct also shows strong anisotropic absorption, which facilitates polarization storage of data. The product is thermally stable and is irretrievable to the initial B state either by photochemical reaction or through a thermal pathway. The experimental results indicate that the product is formed by a two-photon absorption process. Optical WORM storage is demonstrated by use of two polarization states, but more polarization states may be used. The combination of polarization data multiplexing and extremely short recording time in the femtosecond range enables very high data volumes to be stored within a very short time.     

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.