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.     

High-Resolution Selective Excitation of Resonance-Enhanced Multiphoton-Ionization Photoelectron Spectroscopy by Shaping Femtosecond Laser Pulses

Femtosecond laser-induced resonance-enhanced multiphoton-ionization photoelectron spectroscopy （REMPI-PS） is faced with two drawbacks of low spectral resolution and poor selective excitation due to the broad spectral bandwidth. We propose a scheme to obtain a high-resolution selective excitation of （2＋1） REMPI-PS by com- bining 7r and cosinusoidal phase modulation. Our theoretical results indicate that the （2＋1） REMPI-PS signals related to neighboring excited states can be differentiated from their indistinguishable photoelectron spectra by the 7r phase modulation, and then their selective excitation can be realized by supplementally adding the cosi- nusoidal phase modulation. Furthermore, the physical mechanism of the high-resolution selective excitation of （2＋1） REMPI-PS is explained by considering the two-photon power spectrum.     

Achievement of Narrow-Band CARS Signal by Manipulating Broad-band Laser Spectrum

We theoretically demonstrate the achievement of narrow-band coherent anti-Stokes Raman scattering （CARS） signal by manipulating broad-band probe spectrum. The narrowing of the CARS signal depends on the spectrum bandwidth of the probe beam, and thus high-resolution CARS signal for a complicated quantum system can be obtained by the simple spectrum manipulation. Furthermore, the energy-level diagram for the complicated quantum system can also be labelled by measuring the CARS signal at a given frequency.     

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.     

Two-color laser wavelength effect on intense terahertz generation in air

Near-IR femtosecond lasers have been proposed to produce high-field terahertz radiation in the air via the laser-plasma interaction, but the physical mechanism still needs to be further explored. In this work, we theoretically investigate the effect of the two-color laser wavelength on the terahertz generation in the air based on a transient photocurrent model.We show that the long wavelength laser excitation can greatly enhance the terahertz amplitude for a given total laser intensity. Furthermore, we utilize a local current model to illustrate the enhancement mechanism. Our analysis shows that the terahertz amplitude is determined by the superposition of contributions from individual ionization events, and for the long wavelength laser excitation, the electron production concentrates in a few ionization events and acquires the larger drift velocities, which results in the stronger terahertz radiation generation. These results will be very helpful for understanding the terahertz generation process and optimizing the terahertz output.     

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.     

超快电子衍射技术及其应用

时间和空间上实时观测原子运动对于自然科学研究有着非常重大的意义, 而超快电子衍射(UED)技术同时具备飞秒激光脉冲的高时间分辨特性和电子衍射技术的高空间特性, 可以为实时观测原子级分辨尺度物质的结构变化提供一种有效工具. 本文综述了超快电子衍射技术的发展历史、实验方法以及相关应用, 并且展望了超快电子衍射技术未来的发展.     

飞秒激光脉冲整形技术及其应用

通过频域上控制飞秒激光脉冲幅度、相位和偏振在时域上可以获得几乎任意形状的飞秒激光脉冲,这种飞秒激光脉冲整形技术可为研究光与原子分子非线性相互作用提供一种全新实验技术手段.本文介绍飞秒激光脉冲整形发展历史、技术方法、控制方式及其相关应用,并展望飞秒激光脉冲整形技术未来的发展方向.     

二溴甲烷相干反斯托克斯拉曼光谱（CARS）的选择激发

相干反斯托克斯拉曼光谱（CARS）由于信号强度符合无损伤探测等特点，已经日益在生物显微成像、燃烧诊断等领域得到广泛应用。而影响CARS进一步应用的障碍在于非共振信号以及所要激发振动模式周围的能级的干扰。因此要实现对某一振动能级精确激发，或提高拉曼光谱的分辨率，对振动模式的选择激发是非常必要的。