Nonperturbative response functions: A tool for the interpretation of four-wave-mixing signals beyond third order.
Nonperturbative response functions: A tool for the interpretation of four-wave-mixing signals beyond third order.
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DOI：
10.1063/1.5004763
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发表时间：
2017-12
期刊：
影响因子：
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通讯作者：
Lipeng Chen;Elisa Palacino-González;M. Gelin;W. Domcke
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文献类型：
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作者：
Lipeng Chen;Elisa Palacino-González;M. Gelin;W. Domcke
考虑一个耦合到振动自由度的电子二能级系统，在短而强的非重叠激光脉冲驱动下，我们引入了非微扰响应函数的概念。这些响应函数表示在有效的电子跃迁偶极矩，这取决于场物质耦合的强度和脉冲持续时间。结果表明，非线性偏振表示四波混频信号可以优雅地表示在这些非微扰响应函数的所有订单的场-物质耦合。非微扰响应函数将常见的三阶响应函数的解释能力推广到强激光脉冲的四波混频实验。
Considering an electronic two-level system coupled to vibrational degrees of freedom and driven by short and intense non-overlapping laser pulses, we introduce the concept of nonperturbative response functions. These response functions are expressed in terms of effective electronic transition dipole moments which depend on the strength of the field-matter coupling and on the pulse durations. It is shown that the nonlinear polarization representing four-wave-mixing signals can elegantly be expressed in terms of these nonperturbative response functions to all orders in the field-matter coupling. The nonperturbative response functions generalize the interpretative power of the familiar third-order response functions to four-wave-mixing experiments with intense laser pulses.