级联三能级模型下超短脉冲激光与分子相互作用的动力学研究

通过求解麦克斯韦-布洛赫方程，研究了超短脉冲激光和一维对称π共轭分子材料(4,4′-二甲氨基二苯乙烯分子)的相互作用.该分子材料具有较强的非线性光学性质，其分子的电子结构和电偶极矩是在密度泛函理论水平上利用从头计算方法得到的.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该分子介质中的传播.在单光子共振情况下，保持入射脉冲的脉冲宽度不变，当小面积脉冲在该分子介质中传播时，二能级模型可以较好地描述脉冲激光与该分子体系的相互作用过程.但对于大面积脉冲激光，由于较明显地产生了分子的二次激发，此时分子 关键词： 超短脉冲激光 4′-二甲氨基二苯乙烯分子 三能级模型 麦克斯韦-布洛赫方程     

强近共振激光脉冲驱动下二能级系统中试探脉冲的瞬态反应

我们用缀饰模型研究强近共振激光脉冲驱动下二能级系统与弱试探脉冲的相互作用。当试探脉冲的频率ω₂调到共振频率ω₂=ω₁±<Ω₂₁^D>时,试探脉冲呈现吸收或放大效应。还得到非线性混频效应的瞬态过程。共振增强存在于此非线性混频过程中。 关键词：     

激光场作用下钠原子的近共振散射和碰撞感生荧光

一、引 言 关于原子共振和近共振吸收和散射的研究,对于认识等离子体和中性气体的辐射能量转移过程以及原子之间相互作用的特性是非常重要的; 特别是近共振散射能量再分布的研究对于了解星际和星际系介质中辐射能量转移过.程是很关键的.但目前,关于近共振散射再分布函数的直接测量进行得很少.Carlsten等人利用脉冲染料调频激光器,将其频率调到Sr原子4607A0(1p01-1s0)共振线附近,测量了近共振散射光谱的再分布,得到了瑞利散射与△-2(△表示入射激光频率ωl与原子共振频率ω。之差)成比例,得到了感生的共振荧光随△的变化曲线及其随△符号变…     

周期量级超短脉冲激光在有机分子材料中的传播

利用从头计算方法,在密度泛函理论上,计算了硝基苯胺(para-Nitroaniline,pNA)分子的电偶极距.通过严格求解麦克斯韦-布洛赫方程,研究了周期量级超短脉冲激光与硝基苯胺分子材料的相互作用,研究显示当超短脉冲在分子中共振传播时,会出现高频与低频成分,随传播距离的增加.频谱的展宽越来越明显,而分子能级占有率之差在电场为零时,表现出一种台阶的特征;当超短脉冲激光在该分子介质中非共振传播时,脉冲激光频谱中明显地出现了二次谐波成分.     

超短脉冲激光在硝基苯胺分子材料中的非共振传播

通过严格求解麦克斯韦-布洛赫方程,研究了超短脉冲激光与硝基苯胺分子材料的非共振相互作用.研究结果表明,当脉冲激光在该分子介质中以电荷转移态的激发能的二分之一非共振传播时,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.     

稠密V型介质中双色飞秒脉冲及频谱演化的RCEP调制

利用不含慢变振幅近似和旋波近似的全波Maxwell-Bloch方程组的数值解,研究单光子共振和失谐两种条件下,相对载波包络相位(RCEP)对在稠密V型三能级原子介质中传播的双色sech型飞秒超短脉冲及频谱演化的影响.结果表明,RCEP对双色脉冲的传播形式及频谱特性的调制在失谐情况比在单光子共振情况显著,在失谐条件下调节RCEP可获得比单光子共振条件下大得多的频谱展宽,出现了最高频率达到入射脉冲中心频率18倍的超连续谱.     

有机分子第一超极化率色散效应和双光子共振增强理论研究

采用含时Hartree-Fock和多态求和方法计算了半花菁衍生物生色团的第一超极化率色散效应. 采用二能级模型研究了第一超极化率的双光子共振增强特征. 研究发现，第一激发态对半花菁非线性光学性质起决定性作用，随着入射光波长向短波方向移动，二次谐波产生β(-2ω;ω,ω)不断增大并且在950nm附近出现双光子共振效应，理论结果与实验结果较好相符. 此外，共振条件下的二能级模型需要考虑激发态弛豫效应. 研究结果为实验测量和实际应用提供了理论参考. 关键词： 分子非线性光学 超极化率 色散效应 共振增强     

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     

粒子数密度对飞秒Gauss型脉冲传播及光谱特性的影响

利用预估校正-时域有限差分(PC-FDTD)法求解全波Maxwell-Bloch方程,研究介质粒子数密度(N)对飞秒Gauss型激光脉冲在Λ型三能级原子介质中传播及光谱特性的影响.结果表明:小面积2π脉冲在不同N介质中都不发生分裂,脉冲频谱基本没有新的高频成分产生,随N增大中心频率附近光谱强度明显减小.面积4π脉冲,在N较大的稀疏介质及稠密介质中都产生分裂,在稀疏介质中随N增大频谱展宽幅度及高频成分强度增大,但在稠密介质中频谱展宽变小且远小于N较大时的稀疏介质情况.大面积8π脉冲,脉冲分裂情况与4π脉冲情况相似,但随N增大频谱展宽幅度及高频成分强度单调增大,且在稠密介质中的频谱展宽幅度及高频成分强度远大于N较小的稀疏介质情况.     

啁啾系数对飞秒脉冲的分裂及光谱性质的影响

利用预估校正-时域有限差分法求得不含慢变包络近似和旋转波近似的全波Maxwell-Bloch方程的数值解,在Λ型三能级原子介质中研究了啁啾系数C对传播中的飞秒Gauss型脉冲分裂情况及光谱性质的影响.结果表明:面积小于等于3π的啁啾脉冲在介质中不出现分裂,但脉冲啁啾会引起脉冲频谱的震荡;对于4π面积啁啾脉冲,啁啾系数C较小时脉冲在介质中发生分裂,C较大的脉冲不再产生分裂,即分裂的子脉冲数量减少;随着C增大,脉冲中心频率附近频谱震荡愈加剧烈,高频成分的范围及强度明显减小;对于大面积8π脉冲,脉冲分裂情况与4π情况相似,但随C增大,脉冲高频成分的范围和强度没有明显变化,而高频成分中的峰值分布却显著不同.     

SPECTRUM OF A FEW-CYCLE LASER PULSE PROPAGATING IN A TWO-LEVEL ATOM MEDIUM

The spectrum evolution of a few-cycle optical pulse in a resonant two-level atom medium is studied theoretically by using the full Maxwell--Bloch equations. On the propagating pulse, significantly much faster oscillation components separated with the main pulse appear due to strong self-phase modulation and pulse reshaping. In this case, ideal self-induced transparency cannot occur for a 2π pulse. The spectrum of the 4π pulse shows an evident oscillatory feature because of the continuum interference of the separate pulses. For larger pulse areas, continuum generation from near ultraviolet to infrared occurs.     

Generation of an acoustic supercontinuum under conditions of the hypersound intrapulse scattering mode

The nonlinear generation of an acoustic supercontinuum in a solid doped with impurity paramagnetic ions is studied theoretically. It is shown that generation can be the most efficient at two certain carrier frequencies of input pulses lying above the resonance spin-phonon absorption line and determined by the time and spatial dispersions, respectively. The generated supercontinuum lies well below the resonance absorption line. Generation of the supercontinuum in the single-frequency regime is accompanied by a shift of the input pulse spectrum mainly to the red. In the two-frequency regime, cross scattering is possible when a higher-frequency pulse is scattered by the powerful supercontinuum generated by a pulse with a different, lower carrier frequency. As a result, the spectrum of the high-frequency pulse experiences a strong modulation and broadening both to the red and blue. The efficiency of supercontinuum generation both in the single-frequency and two-frequency regimes can be on the order of 1%.     

Resonant transparency regimes under conditions of long/short-wave coupling

Nonlinear two-component electromagnetic pulse propagation through a resonant axially symmetric anisotropic medium having a permanent dipole moment is analyzed under conditions of strong coupling between the ordinary (short-wavelength) and extraordinary (long-wavelength) pulse components. It is shown that a pulse can propagate through the medium in regimes different from self-induced transparency if its ordinary component is detuned off resonance. In particular, a pulse propagating in the regime of self-induced super-transparency substantially changes quantum-level populations, but its group velocity remains almost equal to the linear velocity. If a pulse propagates in the extraordinary transparency regime and the carrier-frequency detuning from resonance is small, then its group velocity is substantially lower, while the level populations remain virtually invariant. Regimes of propagation through weakly excited media under quasi-resonance conditions are also identified.     

Small-area ultrashort pulse propagation through a three-level medium

Propagation of an ultrashort, small-area (circularly polarized) pulse through a gas medium of three-level atoms near one-photon resonance is studied. The expression for the propagating pulse shape is obtained within the rotating wave and dipole approximations. Results are compared, both analytically and numerically, with those for two-level model. Sinusoidal and Gaussian shapes of input pulses are compared, and a high sensitivity of modulation of the light pulse for envelope to its input shape is revealed.     

The electromagnetic Brillouin precursor in one-dimensional photonic crystals

We have calculated the electromagnetic Brillouin precursor that arises in a one-dimensional photonic crystal that consists of two homogeneous slabs which each have a single electron resonance. This forerunner is compared with the Brillouin precursor that arises in a homogeneous double-electron resonance medium. In both types of medium, the precursor consists of the components of the applied pulse that have their frequencies below the lowest of the two electron resonances. In the inhomogeneous medium however, the slab contrast starts affecting the precursor field after a certain rise time of the precursor: its spectrum starts to peak at the geometric scattering resonances of the medium whereas minima appear at the Bragg-scattering frequencies.     

Emission of radiation by a resonance medium excited with a variable superluminal velocity

Specific properties of the radiation emitted by a spatially modulated resonance medium excited by an ultrashort light pulse propagating through the medium at a variable superluminal velocity are analyzed. In so doing, frequencies different from that of the resonance transition of the medium may appear in the emission spectrum. It is demonstrated that, in contrast to an earlier studied case of medium excitation at constant velocity, variation of the excitation velocity leads to generation of a spectral continuum, the boundaries of which are determined by the range of variation of the medium-excitation velocity.     

Interference model of femtosecond laser pulse conical emission in dispersive medium

A simple interference model is proposed for conical emission frequency-angular spectrum formation during the filamentation of femtosecond laser pulse in a nonlinear dispersive medium. The model allows to obtain analytical expressions for frequency-angular distributions of the supercontinuum spectral components of pulses at different wavelengths in media with arbitrary material dispersion law. The model reproduces the supercontinuum frequency-angular spectrum transformation for the case of laser pulse splitting into several subpulses and for multiple refocusing of the light field in filament. Frequency-angular spectra analytically calculated from the proposed interference model are in good agreement with the results of numerical simulations performed for the filamentation of femtosecond laser pulses in fused silica.     

Comparison of effects of relative carry-envelope phase on two-color few cycle pulses propagating in dense and dilute lambda-type mediums

In this paper we compared effects of relative carry-envelope phase (RCEP) of two-color few cycle pulses on propagation behavior and spectral property under the single-photon resonant condition in the dense and dilute lambda-type three-level atomic mediums. It is found that, in the dense medium, with propagation distance increasing, the compound pulse of the two-color few cycle pulses will split into two or three sub-pulses with different amplitudes and shapes, or does not split, and this is completely determined by value size of RCEP; with value of RCEP decreasing, range and strength of the spectrum (particularly the higher spectral components) increase obviously, the highest frequency is about eight times of the resonance frequency. In the corresponding dilute medium, effect of RCEP on propagating behavior and spectral property is much different from that in the dense medium; specially with value of RCEP decreasing, spectral strength increasing is evident but spectral range not, the highest frequency of the spectrum is only about two times of the resonance frequency.