强光场下非共振双光子跃迁相干控制

利用飞秒激光脉冲相位整形技术,从理论和实验两方面,对强激光场下分子体系苝溶液中非共振双光子跃迁的相干控制进行了研究。通过对飞秒激光脉冲进行相位扫描和余弦相位调制,发现分子体系中非共振双光子的跃迁几率能够被削弱,但不能完全消除。分子体系中非共振双光子跃迁的相干控制受到激光光场的形状和分子吸收谱谱宽的影响;与原子体系相比,分子体系中非共振双光子跃迁相干控制的调制效率降低。     

Polarization and phase control of two-photon absorption in an isotropic molecular system

<正>We theoretically and experimentally study the polarization and phase control of two-photon absorption in an isotropic molecular system.We theoretically show that the two-photon transition probability decreases when the laser polarization changes from linear through elliptical to circular,and the laser polarization does not affect the control efficiency of two-photon transition probability by shaping the spectral phase.These theoretical results are experimentally confirmed in coumarin 480.Furthermore,we propose that the combination of the laser polarization with the spectral phase modulation can further increase the control efficiency of the two-photon absorption.     

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.     

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.     

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.     

Optimal spectral phase control of femtosecond laser-induced up-conversion luminescence in Sm^3+: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.     

超短脉冲激光在DBASVP分子中传播时的双光子面积演化和光限幅效应

以一维不对称π共轭分子体系（DBASVP分子）为介质,在双光子共振条件下,从双光子面积定理和严格数值求解Maxwell-Bloch方程两方面出发,分别研究超短脉冲激光在该有机分子介质中的传播过程,从而探讨双光子面积的演化规律,并分析双光子面积定理的适用性.提出了一种数值模拟分子介质光限幅特性的理论方法.分子的电子结构和电偶极矩是基于密度泛函理论利用从头计算方法得到的.研究结果表明,基于慢变幅和慢变相近似以及单模场条件下的双光子面积定理不能很好地描述超短脉冲的双光子面积在该分子介质中的演化规律.基于双光子吸收的分子光限幅特性与分子介质的厚度有关. 关键词： 双光子吸收 光限幅效应 双光子面积定理 超短脉冲激光     

Nonlinear spectrum effect on the coherent control of molecular systems

This work demonstrates that the detuning of the fs-laser spectrum from the two-photon absorption band of organic materials can be used to reach further control of the two-photon absorption by pulse spectral phase manipulation. We investigate the coherent control of the two-photon absorption in imidazole-thiophene core compounds presenting distinct two-photon absorption spectra. The coherent control, performed using pulse phase shaping and genetic algorithm, exhibited different growth rates for each sample. Such distinct trends were explained by calculating the two-photon absorption probability considering the intrapulse interference mechanism, taking into account the two-photon absorption spectrum of the samples. Our results indicate that tuning the relative position between the nonlinear absorption and the pulse spectrum can be used as a novel strategy to optimize the two-photon absorption in broadband molecular systems.     

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.     

Temporal coherent control induced by wave packet interferences in one and two photon atomic transitions

The interaction of a sequence of two identical ultrashort laser pulses with an atomic system results in quantum interferences as in Ramsey fringes experiments. These interferences allow achievement of temporal coherent control of the excitation probability. We present the results of a temporal coherent control experiment on two different atomic systems: one-photon absorption in K (4s-4p) and two-photon absorption in Cs (6s-7d). In K, the quantum interferences between the two excitation paths associated with the laser pulses are revealed through rapid oscillations of the excitation probability as a function of the time delay between the two pulses. These oscillations take place at the transition frequency (period T = 2.56 fs). The interferences are modulated by beats (at about 580 fs) resulting from the doublet structure of the excited state (4p (² P _1/2 , ² P _3/2 )). Three complementary interpretations of this experiment are presented: in terms of beats of quantum interferences, of variation in the spectrum intensity, and of wave packet interferences. Whenever the two laser pulses are temporally overlapped, optical interferences are superimposed on to the quantum interferences. The distinction between these two types of interference is clearly revealed in the two-photon excitation scheme performed on Cs (6s-7d (² D _3/2 , ² D _5/2 )) because quantum interferences occur at twice the frequency of the optical interferences. Received: 30 December 1997 / Revised: 28 February 1998 / Accepted: 4 March 1998     

Coherent control calculations for helium atom in short and intensive XUV laser pulses

Coherent control calculations are presented for helium. With the help of a genetic algorithm (GA) phase-modulated extreme ultra violet (XUV) laser pulses were controlled to maximize or minimize the non-resonant two-photon 1s1s 1s3s excitation. Linearly polarized laser pulses were chosen at the frequency of 0.4 a.u. with a duration of about 15 fs and 1014 Wcm-2 peak intensity. We verified the theory that an antisymmetric spectral phase around the two-photon resonance frequency maximizes the transition probability. Dark pulses which do not excite the system at all have however symmetric spectral phases around the two-photon resonance frequency.     

Theoretical analysis on two-photon absorption spectroscopy in a confined four-level atomic system

We investigate theoretically two-photon absorption spectroscopy modified by a control field in a confined Y-type four-level system. Dicke-narrowing effect occurs both in two-photon absorption lines and the dips of transparency against two-photon absorption due to enhanced contribution of slow atoms. We also find that the suppression and the enhancement of two-photon absorption can be modified by changing the strength of the control field and the detuning of three laser fields. This control of two-photon absorption may have some applications in information processing and optical devices.     

双光子吸收的Franz-Keldysh效应

从实验上证实Hg_0.695Cd_0.305Te 光电二极管空间电荷区中存在双光子吸收的Franz-Keldysh效应.利用一个皮秒Nd:YAG激光器抽运的光学参量产生器和差频产生器作为激发光源,测量了入射波长为λ₀=7.92μm的脉冲激光所激发的光响应随入射光强的变化关系.脉冲光响应峰值强度随入射光强的增大呈现二次幂函数增强趋势.采用等效RC电路模型将脉冲光伏信号峰值与入射光强相关联,得到空间电荷区中强电场下单光束 关键词： Franz-Keldysh效应 碲镉汞 双光子吸收 脉冲光伏信号     

Observation of two-photon absorption resonance in spacially separated fields

The paper presents the results obtained in investigating the lineshape of two-photon absorption in the field of two spacially separated standing waves at the 3S–4D transition of Na. Measurements were carried out by using a CW dye laser. This paper was presented, in part, by one of the authors (V.P.Ch.) at the V Vavilov Conference on Nonlinear Optics, Novosibirsk, USSR (June 1977).     

Adaptive pulse compression by two-photon absorption in semiconductors

We investigate the adaptive optimization of broadband laser pulses, using a closed-loop learning algorithm in which the merit function is derived from two-photon absorption in semiconductors. Photoluminescence experiments with CdS thin films and photocurrent measurements of a GaAsP photodiode have been performed. The experimental data demonstrate that reliable and accurate pulse compression to the bandwidth limit can be achieved, unperturbed by nontrivial phase effects. Therefore two-photon absorption proves to be an easy-to-implement alternative to second-harmonic generation for the compression of broadband laser pulses.     

Au纳米颗粒阵列中双光子吸收的饱和过程

采用纳米球蚀刻法制备了Au纳米颗粒阵列.并通过扫描电子显微镜观测了其表面形貌,表明三角形的Au纳米颗粒呈阵列状分布.采用Z扫描方法(800 nm, 50 fs)测量了Au纳米颗粒阵列的三阶非线性光学特性.在较小的激发功率下,结果呈现出双光子吸收效应,随着激发功率不断增加,出现了双光子吸收饱和的过程;非线性折射则呈现出自散焦效应.这种高效率的非线性响应机理使得该种Au纳米颗粒阵列在高速全光开关中有潜在的应用价值. 关键词： 纳米球蚀刻技术 Au纳米颗粒 三阶光学非线性     

Theorie der nichtstationären Anregung von Exziton-Polaritonen durch Zweiphotonenabsorption

Theory of nonstationary Exciton-Polariton Generation by Two-photon Absorption A theory of nonstationary two-photon absorption for nonlinear non-centrosymmetric crystals is presented. The time-dependent radiation flux density of the generated polariton beam is calculated under the condition of an ultrashort laser pulse duration T_L ? ΓT^?1 (ΓT is the exciton line width) and a stationary incoherent test field. The “mechanical” response of the excitons and different group velocities of the polariton and the laser and test fields are taken into account. the spatial dispersion of the exciton motion being neglected. With a rectangular laser pulse shape the analytically nonstationary solutions are discussed for identical and for different group velocities of laser and test fields. Using the conservation laws for energy and quasimomentum we illustrate, by considering the polariton dispersion branches, the various possible cases of two-photon absorption in uniaxial piezocrystals.     

Optical properties of semiconductors under strong pumping in the <Emphasis Type="Italic">M</Emphasis>-band region and two-photon probing of the biexciton state

The behavior of the semiconductor dielectric susceptibility under the action of a strong laser pulse in the range of the luminescent M band and two-photon probe of a biexciton level is investigated. It is shown that the pronounced Autler-Towns effect occurs at the two-photon transition. The position of the absorption peaks is essentially determined by the amplitude and frequency of the pump field.     

基于双光子不对称色锁二阶随机关联的阿秒极化拍研究

基于两双光子过程的相位共轭二阶极化干涉，从理论上研究了四能级系统在阿秒量级的不对称和频极化拍频(FASPB).在抽运光束为窄带情形下，场关联对FASPB信号影响很弱.在宽带情形下，FASPB信号表现出共振-非共振交叉关联，双光子信号展现出混合辐射-物质失谐的THz阻尼振荡，即当激光频率偏离双光子共振跃迁的条件时，信号将呈现阻尼振荡，而且其双光子自相关信号的包络还呈现最大值零延时不对称.还研究了由于两双光子自相关过程零延时的偏差导致的阿秒拍频信号的不对称性，和两个双光子信号的最大值分别向相反的方向偏离零延时点的现象.FASPB作为一种阿秒超快调制过程，从理论上说它可以扩展到任何两偶极禁戒跃迁激发态的能级和系统. 关键词： 阿秒和频 极化拍 四能级 双光子     

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.