Institut Fresnel, CNRS, Aix-Marseille Université, Ecole Centrale Marseille, Campus de St Jérôme, 13013 Marseille, France.
Phys Rev Lett. 2010 Sep 17;105(12):123903. doi: 10.1103/PhysRevLett.105.123903.
Polarization-resolved coherent anti-Stokes Raman scattering (CARS) is usually applied to measure the depolarization ratio in solutions or evidence orientation effects in anisotropic media. We present an extensive approach based on multiple-field polarization-resolved CARS, in order to unravel the complexity of vibrational resonances up to the fourth-order symmetry, at the microscopic scale in nonisotropic media. The CARS polarized signals measured under a continuous variation of the incident pump and/or Stokes excitation beams are analyzed using a full tensorial picture both in the nonresonant and resonant regimes. This method evidences the strong influence of vibrational symmetries on polarized CARS, and more specifically the occurrence of Kleinman symmetry deviations at the vicinity of the Raman lines frequencies. This technique, illustrated on a cubic symmetry crystal, is general and can be applied to other medium symmetries.
偏振解析相干反斯托克斯拉曼散射（CARS）通常用于测量溶液中的退偏比或各向异性介质中的取向效应。我们提出了一种基于多场偏振解析 CARS 的广泛方法，以便在各向异性介质中微观尺度上揭示高达四阶对称的振动共振的复杂性。在连续变化的入射泵浦和/或斯托克斯激发光束下测量的 CARS 偏振信号，在非共振和共振两种情况下，使用全张量图进行分析。该方法证明了振动对称性对偏振 CARS 的强烈影响，特别是在拉曼线频率附近 Kleinman 对称性偏差的发生。该技术在立方对称晶体上进行了说明，具有通用性，可应用于其他介质对称性。
