双光子失谐对慢光和光存储影响的实验研究

利用电磁感应透明(EIT)效应在87Rb热原子气室中进行了慢光和光存储的实验研究,在单光子红失谐650 MHz处测量了双光子失谐对光脉冲延迟和光存储的影响.结果表明:在双光子失谐0—0.5 MHz范围内存在显著的光脉冲延迟和光存储恢复信号,其慢光波形与理论计算结果基本相符;而恢复光脉冲信号随着双光子失谐的变化出现形变,这是由于多个EIT子系统之间的干涉引起的.这一研究结果为连续变量光场在热原子系综中的存储提供了实验参考.     

原子系统中远失谐脉冲光束对的群速度操控

基于远失谐的四波混频过程, 在实验上得到了放大的探针光脉冲和产生的共轭光脉冲的同时慢光传输, 并通过改变抽运光和探针光之间的双光子失谐实现了群速度的同时操控. 首先在连续光模式下, 研究了入射探针光和新产生共轭光的增益与单光子失谐之间的变化关系. 随着单光子失谐在一定范围内加大, 探针光和共轭光的增益均表现出先增加后减小的变化趋势. 在具有增益特性的基础上, 分别采用6 μs和365 ns探针光脉冲, 研究了慢光的延迟时间和双光子失谐的关系. 对6 μs的探针光, 得到探针和共轭光脉冲的最大延迟分别为2.1 μs 和1.9 μs, 对应的群速度分别约为0.000119 c和0.000132 c, 相应延迟比分别为0.35和0.32. 对365 ns探针光, 探针和共轭光脉冲的最大延迟分别为756 ns和670 ns, 对应的群速度分别约为0.00033 c和0.00037 c, 相应延迟比提高到2.07和1.83.     

Slow light and saturable absorption

Quantitative analysis of slow light experiments utilising coherent population oscillation (CPO) in a range of saturably absorbing media, including ruby and alexandrite, Er³⁺:Y₂SiO₅, bacteriorhodopsin, semiconductor quantum devices and erbium-doped optical fibres, shows that the observations may be more simply interpreted as saturable absorption phenomena. A basic two-level model of a saturable absorber displays all the effects normally associated with slow light, namely phase shift and modulation gain of the transmitted signal, hole burning in the modulation frequency spectrum and power broadening of the spectral hole, each arising from the finite response time of the non-linear absorption. Only where hole-burning in the optical spectrum is observed (using independent pump and probe beams), or pulse delays exceeding the limits set by saturable absorption are obtained, can reasonable confidence be placed in the observation of slow light in such experiments. Superluminal (“fast light”) phenomena in media with reverse saturable absorption (RSA) may be similarly explained. The article is published in the original.     

两个新合成化合物EPVPC和OPVPC非线性光学特性的理论研究

在杂化密度泛函理论（DFT/B3LYP）的水平上，研究了最新实验室合成的两个化合物分子9-乙烷基-3-{2-[4-2-吡啶-4-乙烯基苯]-乙烯基}-9氢咔唑（EPVPC）和9-十八烷基-3-{2-[4-2-吡啶-4-乙烯基苯]-乙烯基}-9氢咔唑（OPVPC）的非线性光学特性。理论结果与现有的实验测量结果符合得的较好。利用扩展的少态模型方法计算了分子的双光子吸收截面，结果表明三态模型可以很好地描述它们的最大双光子吸收截面。数值模拟显示这两个化合物都具有较大的双光子吸收截面，并且，在低频范围内，OPVPC分子比EPVPC分子显示出较强的双光子吸收特性。     

A variational approach of nonlinear dissipative pulse propagation

A variational technique to deal with nonlinear dissipative pulse propagation is established. By means of a generalization of the Kantorovitch method, suitable for non-conservative systems, we are able to cope with an extended nonlinear Schr?dinger equation (NLSE) which describes pulse propagation under the influence of nonlinear loss and/or gain, in particular, in the presence of two-photon absorption (TPA). Based on the characteristics of the exact solution of the NLSE in the absence of TPA, we investigate the effects of frequency dispersion of the nonlinear susceptibility associated to the two-photon resonance, obtaining the necessary conditions for a solitary wave solution, even in the presence of a self-steepening term. Received: 4 August 1997 / Received in final form: 25 November 1997 / Accepted: 14 January 1998     

Ultra-short optical pulse shaping using semiconductor optical amplifier

Optical ultra-short pulse compression and amplification using semiconductor optical amplifier (SOA) is presented. Using pump-probe pulse configuration, we present an SOA model which includes the nonlinear effects such as, spectral hole burning (SHB), carrier heating (CH), two-photon absorption (TPA) and group velocity dispersion (GVD) taking into account gain spectrum effect. Then by adjusting time delay between the pump pulse and probe pulse we use the model for simultaneous compression and amplification of probe pulse. We also analyze the four wave mixing (FWM) signal during pulse compression process. It is shown that dispersive effect of GVD on output probe pulse becomes more important for larger cavity length and probe-pump pulses relative time delays.     

Optical Properties of a New Two-photon Absorption Dye DEASPI

The two-photon absorption (TPA), TPA-induced frequency up-conversion emission, and two-photon pumped (TPP) frequency up-conversion lasing properties of a new synthesized dye Trans-4-［p-(N,N-diethylamino)styryl］-N-methylpyridinium iodide (DEASPI) were experimentally studied. This new dye has a moderate TPA cross-section of σ2=6.9×10-48 cm4*s/photon at 1064 nm, but exhibits a high lasing efficiency. The overall superradiant lasing conversion efficiency is as high as 10.7% at the pump energy of 2.14 mJ.     

Optical Properties of a New Two-photon Absorption Dye DEASPI

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Single quantum dots for slow and fast light in a planar photonic crystal

We theoretically investigate slow and fast light propagation and pulse velocity control in a nanocavity containing a single quantum dot side-coupled to a planar-photonic-crystal waveguide. We demonstrate that low coupling strength (i.e., the weak coupling regime) between a cavity and a dot, under on-resonance condition, can lead to delays of about +90 ps for a pulse 1/e-width of 280 ps. The group delay dependence on the various coupling parameters suggests achievable delays of +300 ps and consequently very slow light speeds of around 5000 m/s in a 1.5 microm cavity-waveguide section. We also show that under off-resonant condition one can achieve significant pulse advancement of -60 ps.     

Multicontrast nonlinear optical microscopy with a compact and rapid pulse shaper

Homodyne detection can dramatically enhance measurement sensitivity for weak signals. In nonlinear optical microscopy it can make accessible a range of novel, intrinsic, contrast like nonlinear absorption and nonlinear phase contrast. Here a compact and rapid pulse shaper is developed, implemented, and demonstrated for homodyne detection in nonlinear microscopy with high-repetition rate mode-locked femtosecond lasers. With this method we generate two-photon absorption (TPA) and self-phase modulation images of gold nanostars in biological samples. Simultaneous imaging of two-photon luminescence and TPA also enables us to produce two-photon quantum yield images.     

Ultrafast measurement of two-photon absorption by loss modulation

We demonstrate a direct and sensitive technique for measuring two-photon absorption (TPA). An intensity-modulated femtosecond laser beam passes through a sample exhibiting TPA. A TPA signal at twice the modulation frequency is then generated and subsequently measured by a lock-in amplifier. The absolute TPA cross section of Rhodamine 6G at 800nm is found to be (15.3+/-2.0)x10(-50) cm(4) s/photon and agrees well with previously published results obtained with much higher intensity [J.Chem.Phys.112, 9201 (2000)]. Our method may be especially useful in measuring nonlinear absorptions of nonfluorescent materials.     

Two-photon absorption of high-power picosecond pulses in PbWO<Subscript>4</Subscript>, ZnWO<Subscript>4</Subscript>, PbMoO<Subscript>4</Subscript>, and CaMoO<Subscript>4</Subscript> crystals

The nonlinear process of two-photon interband absorption is studied in tungstate and molybdate oxide crystals excited by a sequence of high-power picosecond pulses with a wavelength of 523.5 nm. The transmission of the crystals is measured for the excitation pulse intensity up to 100 GW/cm². The pulse intensity in the crystals initially transparent at a wavelength of 523.5 nm is strongly limited due to two-photon absorption (TPA), and the reciprocal transmission in PbWO₄ and ZnWO₄ crystals reaches 50–60. In all crystals, TPA induces long-lived one-photon absorption, which affects the nonlinear process dynamics and leads to a hysteresis in the dependence of the transmission on the laser excitation intensity. Absorption dichroism manifests itself in a significant difference in the transmission intensities when the principal orthogonal optical axes of the crystals are excited. The TPA coefficients are determined during the excitation of two optical axes of the crystals. TPA coefficients β for the crystals vary over a wide range, namely, from β = 2.4 cm/GW for PbMoO₄ to β = 0.14 cm/GW for CaMoO₄, and the values of β can differ almost threefold when different optical axes of a crystal are excited. Good agreement is achieved between the measured intensities limited by TPA and the estimates calculated from the measured nonlinear coefficients. Stimulated Raman scattering (SRS) upon excitation at a wavelength of 523.5 nm is only detected in two of the four crystals under study. The experimental results make it possible to explain the suppression of SRS by its competition with TPA, and the measured nonlinear coefficients are used to estimate this suppression.     

硒化镉载流子的超快动力学研究

硒化镉是一种可用于X射线全光分幅相机和全光条纹相机的重要探测材料。用基于相位物体的泵浦探测方式,研究了硒化镉在1030nm波长,飞秒脉冲下的载流子超快动力学和非线性光学特性。得到了双光子吸收系数、载流子吸收截面、载流子复合时间等参数。实验表明,硒化镉载流子的动力学和非线性特性是由束缚电子和载流子共同决定的。束缚电子的克尔效应和双光子激发都是瞬态的,而载流子复合持续了较长时间。这些参数和载流子图像的的获得,为X射线超快探测器件的设计和改进提供了参考。     

有机双光子吸收材料的研究进展

本文综述了具有优异双光子吸收/双光子荧光性质的有机功能材料的研究工作和成果。近年来,有机材料凭借其出众的性质、丰富的种类、多重功能性以及快速的非线性光学响应引起国际科学和技术界的极大兴趣。文章介绍了测量材料的非线性光学性质和超快响应的实验方法,它们已被广泛应用于有机材料的研究工作,并且取得了重大的进展。本文描述了对偶极、四极、多枝结构、大环结构以及聚合物等有机材料的非线性光学性质和超快光学响应的研究结果。基于有机材料的迷人性质,具有优异非线性光学性质和超快响应的有机材料将会在很多领域显示出巨大的应用潜力。     

Two-photon echo method to determine the transverse relaxation time of excitonic molecules

A nonlinear optical method to determine the transverse relaxation time of excitonic molecules by means of two-photon echo is proposed. In the case of two-photon transition such as excitonic molecule one needs three pulses to obtain an echo signal. When the wave-vector and frequency of the three successive pulses are denoted by k₁,ω₁, k₂,ω₂ and k₃,ω₃, the two-photon echo can be observed in the direction of 4k₂-2k₁-k₃ with frequency 4ω₂-2ω₁-ω₃. Tuning both ω₁ and ω₂ to be two-photon resonant with excitonic molecule, we can satisfy the phase-matching condition rather easily for appropriate values of ω₃ due to the large dispersion of excitonic polaritons. From the correlation trace of the two-photon echo we can determine directly the transverse relaxation time of excitonic molecules.     

Ultrashort pulse propagation and nonlinear frequency conversion in superconducting and magnetic photonic crystal

We study the propagation and second harmonic generation of ultrashort pulse in nonlinear photonic crystal using a combination of Fourier transform and transfer matrix method. The focus is on the reflected and transmitted output of fundamental pump pulse and second harmonic pulse in frequency and time domains, the temperature dependence of the reflection and transmission spectra where the superconducting transition frequency is close to the magnetic resonance. Interesting features include output pump and second harmonic pulses that can be strongly modulated with the transmitted pulses being delayed by slow light effect.     

飞秒激光脉冲在三能级有机分子介质中传播时的频谱分析

通过采用预估校正的时域有限差分法求解麦克斯韦-布洛赫方程,我们研究了飞秒激光脉冲在三能级有机分子(4,4-二甲氨基二苯乙烯分子)介质中传播时脉冲的频谱演化情况.在单光子共振情况下,即入射脉冲频率等于1、2能级之间的共振频率,对大面积入射脉冲,由于强的二次激发的作用,电场频谱中出现了在ω32附近振荡的频率成分,ω32是2、3能级之间的共振频率,说明对大面积入射脉冲二能级模型已经失效,需要采用多能级模型来描述分子介质.在双光子共振情况下,即入射脉冲频率等于1、3能级之间的共振频率的一半,由于介质中放大的自发辐射和四波混频的作用,部分入射脉冲能量转化为高频和低频电场成分的能量,分子介质表现出了很强的光功率限幅特性.     

Ultrafast femtosecond all-optical modulation through nondegenerate two-photon absorption in silicon-on-insulator waveguides

We present numerical investigations of ultrafast femtosecond (with time duration of 100 fs at 1/e intensity point) all-optical modulation of a pump-probe wave arrangement by using nondegenerate two-photon absorption (TPA), namely cross absorption, inside silicon-on-insulator (SOI) optical waveguides. Our results show that when a pump pulse with femtosecond duration and a continuous probe wave are co-propagating along the SOI, the probe wave can be modulated inversely by the ultrafast pump pulse, whose modulation depth depends strongly on the system parameters such as the waveguide length, the peak power and initial chirp of the pump wave, the group velocity dispersion (GVD), etc.; this means that the modulation depth can be improved by an appropriate increase of the waveguide length, the pump peak, and the initial chirp, in addition, which has a larger value for the probe wavelength in the normal dispersion regime compared with the case of abnormal dispersion when the center wavelength of the pump wave is located at the zero-dispersion wavelength.     

Theory of transient two-photon resonant up-conversion with non-synchronized excitation

The theory of the two-photon resonant up-conversion process (ω_a + ω_a) + ω_c ? ω_d is developed for short pulse excitation. Prominence is given to the case where the pulse at frequency ω_c is not time-synchronized with the pulse ω_a but travels immediately behind it. Not only is the conversion efficiency thereby maximized, but the associated theoretical simplification enables several analytical formulae to be derived which provide new insight into the mechanism of resonant non- linear interactions. In particular, an expression is derived for the maximum useful energy per unit area of the pulse at ω_c. Exceeding this value is of little or no advantage in the non-synchronized case and is positively detrimental when the a- and c-pulses are coincident. The results are supported by computer solutions.     

Generation of ultrafast pulse via combined effects of stimulated Raman scattering and non-degenerate two-photon absorption in silicon nanophotonic chip

A project of ultrafast pulse generation has been presented and demonstrated by utilizing the combined nonlinear effects of stimulated Raman scattering (SRS) and non-degenerate two-photon absorption (TPA) based on silicon nanophotonic chip, in which a continuous wave (CW) and an ultrafast dark pulse are co-propagating in the silicon chip so that the CW will be modulated inversely by the dark pulse during the propagation. As a result, an ultrafast bright pulse is achieved using the technique. Simulation results show that an ultrafast pulse with a pulsewidth (full-width at half-maximum (FWHM)) of about 50 fs is generated at the end of a 5-mm long silicon chip, when the initial conditions, including an input maximum of 0.5 W and FWHM of ∼176 fs for dark pulse, and CW with power of 5 W, are chosen.