An analysis of pulse propagation through a saturable absorber having excited-state absorption

The theoretical study of the propagation of a bell-shaped light pulse through a saturable absorber having excited-state absorption is presented. Assuming that the pulse-width is longer than the first excited-state lifetime of the absorber, a general expression for the steady-state transmission of the absorber is obtained. It is shown that when the excited-state absorption cross-section is larger than the ground-state absorption cross-section (reverse saturable absorber) the absorber acts as a power limiter. An explicit expression for the change of temporal pulse-width in a single transit through the absorber is obtained, which shows that the pulse-width increases due to the presence of excited-state absorption. An analytical expression is presented for the optimum pulse intensity at which the maximum pulse broadening occurs.     

Resonant propagation of femtosecond laser pulse in DBASVP molecule：one-dimensional asymmetric organic molecule

We have investigated the resonant propagation of femtosecond laser pulse in 4-trans-[p-（N, N-Di-n-butylamino）- p-stilbenyl vinyl] pyridine medium with permanent dipole moments. The electronic structures and parameters for the compound have been calculated by using density functional theory. In the optical regime, there is one charge-transfer state, and the molecule can thus be simplified as a two-level system. Both the one- and two-photon transitions occur between the ground and charge-transfer states. The numerical results show that the permanent dipole moments have an obvious effect on the propagation of the ultrashort pulse laser. The ideal self-induced transparency disappears for 2π pulse, and second harmonic spectral components occur significantly due to the two-photon absorption process. For the 6π pulse, continuum frequency generation is produced and a shorter duration pulse in time domain with 465 as is obtained.     

室温条件下掺铒光纤中光脉冲群速可控特性的研究

利用相干布居振荡技术在介质吸收光谱上产生烧孔，孔宽大约为基态粒子数恢复时间的倒数. 由增益理论分析得到不同抽运光功率对介质吸收状态的影响. 在介质的吸收区域，振荡导致光脉冲经历饱和吸收，脉冲传输延迟；在介质的增益区域，振荡又导致光脉冲经历增益饱和，脉冲传输超前. 应用此技术在掺铒光纤中实现了光速人为可控. 在掺铒光纤晶体中观测到了最慢为2.857×10³m/s的光速减慢传输，相应感生群折射率为10.5×10⁴. 根据布居振荡效应及增益理论，由速率方程出发，得到了 关键词： 光谱烧孔 相干布居振荡 饱和吸收 慢光     

Optical limiting with higher fullerenes

Optical limiting has been investigated for higher fullerenes and compared with C₆₀. The transmission through an aperture placed after solutions of C₇₆, C₇₈, and C₈₄ in tetrahydronaphthalene was measured using Q-switched laser pulses with a wavelength of 532 nm and a pulse width of 8 ns FWHM. Unlike C₆₀, the transmission for these higher fullerene solutions decreased linearly with increasing optical pulse energy. We attribute the linearized optical limiting response to self-defocusing of the optical beam and the absence of excited-state absorption. The ground state absorption spectra for the higher fullerenes suggest their use for optical limiting in the near infrared, and the C₈₄-tetrahydronaphthalene solution was found to be an optical limiter at 1.064 m.     

Dye-laser pulse shortening by transient absorption following excited-state intramolecular proton transfer

Molecules undergoing excited-state intramolecular proton transfer often show transient absorption after pulsed optical excitation, due to the tautomeric form in the singlet ground state. This absorption may be used to suppress, after a short time, the laser action of dyes emitting in the transient absorption band. The method is designed for high photochemical stability. Lasing from PBBO, pumped 10 times above threshold by an excimer pumped PTP dye laser, was suppressed after 3.3ns by the addition of 2-(2-hydroxyphenyl)-benzoxazole, which absorbed 30% of the pump energy. At higher concentrations, intense and stable 80ps PBBO laser pulses were obtained. The pulse evolution is simulated by model calculations. A hypothetical super-dye, consisting of chemically linked laser- and absorber-moities, is also discussed. Here Förster energy transfer should result in particularly efficient laser pulse shortening.     

萘酞菁铅化合物的光限幅特性研究

应用调Q倍频ns/ps Nd：YAG脉冲激光,在波长为532nm,脉冲宽度为8ns,重复频率为1Hz的条件下,研究了溶于二甲基亚砜(DMSO)中的萘酞菁铅溶液的反饱和吸收和光限幅特性。实验表明,萘酞菁铅具有良好的光限幅特性,它的有效激发态吸收截面与基态吸收截面的比值约为15．21,大于萘酞菁铜。研究结果表明,萘酞菁铅的光限幅特性优于C60,激发态吸收是其主要的光限幅机理。实验结果证实了重原子效应可以通过增强系际跃迁而使三重态的反饱和吸收增强,从而提高光限幅的能力。     

Excited-state molecular vibration observed for a probe pulse preceding the pump pulse by real-time optical spectroscopy

It is shown experimentally that the absorbance change observed in the "negative" time range, where probe pulse precedes pump pulse in real-time vibrational spectroscopy is induced only by the excited-state wave-packet motion as theoretically expected. Coherent molecular vibration of a polymer in the excited state was observed in the real-time trace without the effect of wave-packet motion in the ground state, which usually makes it difficult to ascribe the signal either to the ground state or to the excited state.     

S1 singlet excited-state absorption of DODCI

1 excited-state absorption cross-section spectrum of DODCI in ethylene glycol is determined in the wavelength range from 500 nm to 750 nm. The S₁ state is populated by amplified femtosecond dye laser pulses (wavelength 592 nm) and the S₁-state absorption and emission behaviour is probed with a femtosecond light continuum. A general analysis procedure is developed to extract absolute excited-state absorption cross-sections from the measured transmissions. For DODCI in ethylene glycol the wavelength regions of saturable absorption (mode-locking application), reverse saturable absorption (optical limiter application), and effective stimulated emission (laser application) are determined. Received: 25 July 1996     

EXCITED-STATE NONLINEAR ABSORPTION AND ITS APPLICATION IN PHOTONIC TECHNOLOGY

The main achievements in our research on the physical phenomena of the excited-state nonlinear absorption in a molecular system and its applications in photonic technology are described. In the first part of this paper, some energy-level models and rate-equations are used to explain various mechanisms of the excited-state nonlinear absorption under differ-ent conditions, such as reverse saturable absorption caused by the triplet and/or the singlet excited-state absorption; saturable absorption due to the first and/or the second singlet excited-state absorption; and the excited-state nonlinear absorption induced by two-photon absorption. The experimental results for metal-organic and C₆₀ materials irradiated by ps and ns laser pulses are consistent with the simulated curves of the transmittance versus flu-ences. In the second part, the applications of excited-state nonlinear absorption in photonic techniques including optical bistability, optical switching, optical limiting, optical modula-tion, optical logic and optical storage are introduced. The working principles of the photonic devices based on the excited-state nonlinear absorption are presented. The experimental characteristic curves are found in good agreement with the theoretical simulations for these devices.     

Nonresonant interaction of femtosecond laser pulse with centrosymmetric molecules

We have derived a system of equations that describes the evolution of the density matrix of a centrosymmetric molecule interacting with a single nonresonant femtosecond laser pulse. The dynamics of the ground electronic state is expressed in terms of the effective Hamiltonian and the coherences between the ground an excited electronic states are functionals of the ground state density matrix. Using the time-dependent perturbation theory, we have calculated the energy deposited in the molecule as a result of rotational stimulated Raman scattering. The effective absorption coefficient is found to be proportional to the fourth power of the pulse amplitude and has a resonance-like dependence with respect to the pulse duration.     

金属卟啉化合物激发态折射与激发态吸收增强瞬态热折射竞争研究

应用激发态吸收增强瞬态热折射理论结合激发态折射理论研究了新型锌卟啉化合物Zn-porphyrin 中激发态吸收增强瞬态热折射与激发态折射间的相互竞争. 样品在不同脉宽激光激发下呈现自聚焦-自散焦间的转化. 当入射激光脉宽为4 ns时,激发态折射占主要地位,样品呈现自聚焦性质;当入射激光脉宽为8ns时,激发态吸收增强瞬态热折射占主要地位,激发态折射占次要地位,样品呈现自散焦性质. 关键词： 金属卟啉化合物 激发态折射 瞬态热折射     

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.     

Dynamics of an extremely short pulse in a Stark medium

Effects of propagation of an extremely short (of one or several oscillation periods) electromagnetic pulse in a medium whose resonance transition is characterized by diagonal as well as nondiagonal matrix elements of the dipole moment operator have been studied numerically. The Maxwell-Bloch system of equations is employed without using the approximation of slowly varying envelopes. An analog of the McCall and Hahn area theorem is discussed as applied to the division of the initial extremely short pulse into subpulses. The solution is obtained in the form of a solitary stable bipolar signal with a nonzero pulse area (nonzero breather).     

超短脉冲激光在有机分子材料中的动力学过程研究

利用从头计算方法，在密度泛函理论上，计算了分子的电子结构和电偶极矩.通过求解麦克斯韦-布洛赫方程，研究了超短脉冲激光与硝基苯胺分子材料的相互作用，着重分析了分子的固有偶极矩对脉冲激光波形、频谱成分以及分子能级占有率产生的影响.研究结果表明，慢变幅近似和旋波近似不能很好地描述超短脉冲在PNA分子介质中传播.分子的固有偶极矩进一步使脉冲传播背离面积定理，引起了脉冲更快地分裂.当脉冲激光在PNA分子介质中以电荷转移态的激发能共振传播时，脉冲激光频谱中明显地出现了二次谐波成分，显示了该分子具有较强的双光子吸收性质. 关键词： 超短脉冲激光 硝基苯胺分子 麦克斯韦-布洛赫方程     

Femtosecond laser pulse train effect on Doppler profile of cesium resonance lines

We present direct observation of the velocity-selective optical pumping of the Cs ground state hyperfine levels induced by the femtosecond (fs) laser oscillator centered at either D2 (6 ²S_1/2↦6 ²P_3/2, 852 nm) or D1 (6 P_1/2, 894 nm) cesium line. We utilized previously developed modified direct frequency comb spectroscopy (DFCS) which uses a fixed frequency comb for the excitation and a weak cw scanning probe laser centered at the ¹³³Cs 6 ²S_1/2↦6 ²P_3/2 transition (D2 line) for ground levels population monitoring. The frequency comb excitation changes the usual Doppler absorption profile into a specific periodic, comblike structure. The mechanism of the velocity selective population transfer between the Cs ground state hyperfine levels induced by fs pulse train excitation is verified in a theoretical treatment of the multilevel atomic system subjected to a pulse train resonant field interaction.     

室温掺铒光纤放大器中实现参量控制无损耗光速减慢传输

本文对掺铒光纤放大器中的光速减慢传输系统进行深入研究,提出一种直接利用掺铒光纤放大器中抽运光 强度和掺铒光纤长度,通过优化控制参量来降低信号光强度损耗系数,从而可以实现无强度损耗光速减慢传输, 研究结果表明:当抽运光功率为3.5 mW时,信号光强度损耗系数近似为零;当抽运光关闭时,掺铒光纤长度为 0.1 m时,信号光强度损耗系数近似为零.     

Novel colliding plasma pulse clipper and optical isolator for high power infra-red lasers

The properties of a high density plasma focus produced inside a ring target with an Nd laser have been investigated. Studies of the axial propagation of a CO₂ laser beam through the plasma focus have shown that the device can be used either as a fast pulse clipper or as an optical isolator for high power infra-red lasers. Self-focussing, strong refraction and defocussing and non-classical absorption of the CO₂ laser beam have all been observed.     

Ultrafast control of coherent population transfer with a train of femtosecond pulse pairs

We investigate the ultrafast control of coherent population transfer in a Λ-type three-level system with a train of pump-Stokes femtosecond pulse pairs, where the pulse sequences can be produced either by optical delay line or by pulse shaping with sinusoidal phase modulation. It is shown that when the pump and Stokes pulses in each pair are applied in the counterintuitive order, similar to that in the stimulated Raman adiabatic passage technique, due to temporal quantum interference (besides optical interference in the case of overlapped subpulses), ultrafast control of coherent population transfer can be achieved by scanning the inter-pair time delay or by changing the sinusoidal phase modulation parameters. This method has potential applications in ultrafast control of chemical reactions and quantum information processing.     

Nonresonant and Resonant Nonlinear Absorption of CdSe-Based Nanoplatelets

We present a comprehensive understanding of the nonlinear absorption characteristics of CdSe-based nanoplatelets(NPLs) synthesized by the solution-phase method and the colloidal atomic layer deposition approach through Z-scan techniques at 532 nm with picosecond pulses. The CdSe NPLs exhibit strong two-photon induced free carrier absorption(effective three-photon absorption) upon the nonresonant excitation, resulting in a remarkable optical limiting behavior with the limiting threshold of approximately 75 GW/cm~2. A nonlinear optical switching from saturable absorption(SA) to reverse saturable absorption(RSA) with increasing the laser intensity is observed when coating CdSe NPLs with a monolayer of CdS shell to realize the resonant absorption. The SA behavior originates from the ground state bleaching and the RSA behavior is attributed to the free carrier absorption.These findings explicitly demonstrate the potential applications of CdSe-based NPLs in nonlinear optoelectronics such as optical limiting devices, optical pulse compressors and optical switching devices.     

基于高聚物光诱导激子漂白的无腔光学双稳态

基于已建立的高聚物光诱导激子漂白动力学理论，模拟计算了一类基态非简并高聚物在光激发和弛豫过程中的瞬态无腔光学双稳态．结果表明，基于高聚物的超快激发和弛豫，可获得瞬态饱和吸收型和增强吸收型无腔光学双稳态，其开关时间均在ps和fs量级．随着入射探测光脉冲相对入射泵浦光脉冲延迟时间的增加，无腔光学双稳态可由饱和吸收型向增强吸收型转变，转变的快慢与高聚物光诱导漂白的弛豫的快慢成正比 关键词：