Coherent control of non-resonant two-photon transition in molecular system

In this paper,we study theoretically and experimentally the coherent control of non-resonant two-photon transition in a molecular system (Perylene dissolved in chloroform solution) by shaping the femtosecond pulses with simple phase patterns (cosinusoidal and π phase step-function shape).The control efficiency of the two-photon transition probability is correlated with both the laser field and the molecular absorption bandwidth.Our results demonstrate that,the two-photon transition probability in a molecular system can be reduced but not completely eliminated by manipulating the laser field,and the control efficiency is minimal when the molecular absorption bandwidth is larger than twice the laser spectral bandwidth.     

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。     

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.     

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.     

Quantum control of two-photon photochromism in the solid phase

Phase and polarization control of photochromism in the solid phase is experimentally demonstrated. Photochromism initiated by a two-photon absorption of femtosecond laser pulses in a three-dimensional solid-phase polymer sample of spiropyran is controlled by varying the polarization state and the chirp of laser pulses.     

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.     

Doppler-free two-photon spectroscopy

We describe atomic transitions where two or more photons are simultaneously absorbed by an atom or a molecule (without any intermediate resonant level). We show theoretically and experimentally the possibilities of these transitions for numerous high-resolution spectroscopic studies. The principle of the method is discussed: the Doppler broadening is suppressed in two-photon transitions if the atoms are irradiated by two laser beams travelling in opposite directions, because the Doppler shift in one wave cancels that in the other. A generalization is made for multiphotonic transitions. Calculations of the multiphotonic transition probability are summarized and their hypotheses specified: one deals with line shape and orders of magnitude in practical conditions. The problem of light shifts is also discussed. A typical experimental set-up with a cw dye laser is described in detail. Typical recordings of two-photon transitions are given; they show line widths smaller than 4 MHz (on a Doppler width of 2000 MHz). Other experiments show the possibility of increasing the transition probability by using two lasers with slightly different wave lengths. One experiment with a three-photon Doppler-free transition is also described. In conclusion, we make a brief comparison with the saturated absorption technique.     

Highly selective population of two excited states [2mm]in nonresonant two-photon absorption

A nonresonant two-photon absorption process can be manipulated by tailoring the ultra-short laser pulse. In this paper, we theoretically demonstrate a highly selective population of two excited states in the nonresonant two-photon absorption process by rationally designing a spectral phase distribution. Our results show that one excited state is maximally populated while the other state population is widely tunable from zero to the maximum value. We believe that the theoretical results may play an important role in the selective population of a more complex nonlinear process comprising nonresonant two-photon absorption, such as resonance-mediated (2+1)-three-photon absorption and (2+1)-resonant multiphoton ionization.     

Two photon absorption and coherent control with broadband down-converted light

We experimentally demonstrate two-photon absorption with broadband down-converted light (squeezed vacuum). Although incoherent and exhibiting the statistics of a thermal noise, broadband down-converted light can induce two-photon absorption with the same sharp temporal behavior as femtosecond pulses, while exhibiting the high spectral resolution of the narrow band pump laser. Using pulse-shaping methods, we coherently control two-photon absorption in rubidium, demonstrating spectral and temporal resolutions that are 3-5 orders of magnitude below the actual bandwidth and temporal duration of the light itself. Such properties can be exploited in various applications such as spread-spectrum optical communications, tomography, and nonlinear microscopy.     

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.     

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.     

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.     

Quantum coherent control of two-photon transitions by square phase-modulation

A femtosecond laser pulse can be tailored to control the two-photon transitions using the ultra-fast pulse-shaping technique. This paper theoretically and experimentally demonstrates that two-photon transitions in molecular system with broad absorption line can be effectively controlled by square phase-modulation in frequency domain, and the influence of all parameters characterizing the square phase-modulation on two-photon transitions is systemically investigated and discussed. The obtained results have potential application in nonlinear spectroscopy and molecular physics.     

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     

Experimental investigation of a bistable system in the presence of noise and delay

We experimentally analyze the behavior of a non-Markovian bistable system with noise, using a vertical cavity surface emitting laser with time-delayed optoelectronic feedback. The effects of the delayed feedback are observed in the probability distribution of the residence times of the two orthogonal polarization states, and in the polarization-resolved power spectrum. They agree well with recent theoretical predictions based on a two-state model with transition rates depending on an earlier state of the system. We also observe experimentally and explain theoretically that the residence time probability distribution deviates from exponential decay for residence times close to (and smaller than) the delay time.     

Dispersion effects in a highly birefringent fiber laser sensor with fiber Bragg grating reflectors

The effects of dispersion in the highly birefringent fiber Bragg grating reflectors of a polarimetric elliptical-core fiber laser sensor are experimentally and theoretically investigated. The laser sensor is designed to measure fluid pressure. It is experimentally and theoretically shown that the wavelength-dependent phase shifts in the gratings can be employed to remove the near degeneracy of the polarization mode beat frequencies of a given order, which substantially improves the resolution of the sensor. A resolution of a few parts in 10(6) of the free spectral range of the laser is demonstrated.     

Development of two-color laser system for high-resolution polarization spectroscopy measurements of atomic hydrogen

We have developed a high-spectral-resolution laser system for two-photon pump, polarization spectroscopy probe (TPP-PSP) measurements of atomic hydrogen in flames. In the TPP-PSP technique, a 243-nm laser beam excites the two-photon 1S-2S transition, and excited n=2 atoms are then detected by polarization spectroscopy of the n=2 to n=3 transition using 656-nm laser radiation. The single-frequency-mode 243 and 656-nm beams are produced using injection-seeded optical parametric generators coupled with pulsed dye amplifiers. The use of single-mode lasers allows accurate measurement of signal line shapes and intensities even with significant pulse-to-pulse fluctuations in pulse energies. Use of single-mode lasers and introduction of a scheme to select nearly constant laser energies enable repeatable extraction of important spectral features in atomic hydrogen transitions.     

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.     

Theoretical Investigation of Coherent Enhancement for Resonant Two-Photon Transitions

We theoretically investigate the coherent enhancement of resonant two-photon transitions （TPT） in a three-level atomic system. The TPT can be coherently enhanced by modulating spectral amplitude due to eliminating the destructive interference, though partial laser energy losses. Maximal enhancement of TPT can be achieved by modulating spectral phase due to establishing completely constructive interference. Our research provides a theoretical basis for experimental investigation and appears to have potential application on coherent control in the complicated quantum system.