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首页> 外文期刊>Chemphyschem: A European journal of chemical physics and physical chemistry >Systematic Control of Nonlinear Optical Processes Using Optimally Shaped Femtosecond Pulses
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Systematic Control of Nonlinear Optical Processes Using Optimally Shaped Femtosecond Pulses

机译:使用最佳成形飞秒脉冲的非线性光学过程的系统控制

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摘要

This article reviews experimental efforts to control multiphoton transitions using shaped femtosecond laser pulses,and it lays out the systematic study being followed by us for elucidating the effect of phase on nonlinear optical laser-molecule interactions.Starting with a brief review of nonlinear optics and how nonlinear optical processes depend on the electric field inducing them,a number of conclusions can be drawn directly from analytical solutions of the equations.From a Taylor expansion of the phase in the frequency domain,we learn that nonlinear optical processes are affected only by the second- and higher-order terms.This simple result has significant implications on how pulse-shaping experiments are to be designed.If the phase is allowed to vary arbitrarily as a continuous function,then an infinite redundancy that arises from the addition of a linear phase function across the spectrum with arbitrary offset and slope could prevent us from carrying out a closed-loop optimization experiment.The early results illustrate how the outcome of a nonlinear optical transition depends on the cooperative action of all frequencies in the bandwidth of a laser pulse.Maximum constructive or destructive interference can be achieved by programming the phase using only two phase values,0 and pi.This assertion has been confirmed experimentally,where binary phase shaping (BPS) was shown to outperform other alternative functions,sometimes by at least on order of magnitude,in controlling multiphoton processes.Here we discuss the solution of a number of nonlinear problems that range from narrowing the second harmonic spectrum of a laser pulse to optimizing the competition between two- and three-photon transitions.This Review explores some present and future applications of pulse shaping and coherent control.
机译:本文回顾了使用成形飞秒激光脉冲控制多光子跃迁的实验工作,并提出了系统的研究方法,以阐明相位对非线性光学激光-分子相互作用的影响。首先简要回顾一下非线性光学及其原理非线性光学过程取决于感应电场,可以从这些方程的解析解直接得出许多结论。从频域中相位的泰勒展开式中,我们了解到非线性光学过程仅受第二次光学过程的影响。 -和高阶项。这个简单的结果对如何设计脉冲整形实验有重大影响。如果允许相位作为连续函数任意变化,则由于添加线性相位会产生无限冗余具有任意偏移和斜率的频谱上的函数可能会阻止我们进行闭环优化在实验中,早期的结果说明了非线性光学跃迁的结果如何取决于激光脉冲带宽内所有频率的协同作用。通过仅使用两个相位值对相位进行编程就可以实现最大的相长或相消干涉,0在实验上已经证实了这一主张,其中在控制多光子过程中,二进制相位整形(BPS)的性能优于其他替代功能,有时至少在数量级上。在这里,我们讨论许多非线性问题的解决方案范围从缩小激光脉冲的二次谐波频谱到优化两光子跃迁和三光子跃迁之间的竞争。本文探讨了脉冲整形和相干控制的一些当前和未来应用。

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