It has long been known that nonlinear refraction in solvents can depend on pulse width, and this along with experimental uncertainties has led to orders-of-magnitude disagreements in nonlinear refractive coefficients reported in the literature. To resolve this issue, we perform beam-deflection (BD) measurements of the rigorously defined nonlinear impulse response function for 24 commonly used solvents selected from various classes of molecules. Using this polarization-resolved BD, the bound-electronic and the three major nuclear contributions are separately measured by determining the magnitudes, symmetry, and temporal dynamics of each mechanism. This allows us to construct the response functions that we use to accurately establish self-consistent references for predicting and interpreting the outcomes of other experiments performed on these materials over the temporal range from 10 fs to 1 ns. The results also provide insight into relating solvent nonlinearities with their molecular structures and exploring the effects of the Lorentz–Lorenz local field. We find that nonconjugated molecules with small polarizability anisotropy exhibit negligible reorientational response, and hence the nonlinear refraction is almost independent of pulse width. Knowledge of the response functions also allows engineering the transient nonlinear refractive properties of solutions of organic dyes, for example, materials with effectively zero nonlinear refraction.

中文翻译：

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溶剂的非线性光学响应的​​时间和偏振依赖性

早就知道溶剂中的非线性折射可能取决于脉冲宽度，而这与实验的不确定性一起导致了文献中报道的非线性折射系数的数量级分歧。为解决此问题，我们对选自各种分子类别的24种常用溶剂执行了严格定义的非线性脉冲响应函数的光束偏转（BD）测量。使用这种偏振分辨的BD，可以通过确定每种机制的幅度，对称性和时间动态来分别测量束缚电子和三个主要核贡献。这使我们能够构建响应函数，以便准确地建立自洽参考，以预测和解释在10 fs至1 ns的时间范围内对这些材料进行的其他实验的结果。结果还提供了将溶剂非线性与分子结构相关联的见解，并探索了洛伦兹-洛伦茨局部场的影响。我们发现极化率各向异性小的非共轭分子表现出可忽略的重定向响应，因此非线性折射几乎与脉冲宽度无关。了解响应函数还可以设计有机染料溶液（例如，具有有效零非线性折射的材料）的瞬态非线性折射特性。结果还提供了将溶剂非线性与分子结构相关联的见解，并探索了洛伦兹-洛伦茨局部场的影响。我们发现极化率各向异性小的非共轭分子表现出可忽略的重定向响应，因此非线性折射几乎与脉冲宽度无关。了解响应函数还可以设计有机染料溶液（例如，具有有效零非线性折射的材料）的瞬态非线性折射特性。结果还提供了将溶剂非线性与分子结构相关联的见解，并探索了洛伦兹-洛伦茨局部场的影响。我们发现极化率各向异性小的非共轭分子表现出可忽略的重定向响应，因此非线性折射几乎与脉冲宽度无关。了解响应函数还可以设计有机染料溶液（例如，具有有效零非线性折射的材料）的瞬态非线性折射特性。因此，非线性折射几乎与脉冲宽度无关。了解响应函数还可以设计有机染料溶液（例如，具有有效零非线性折射的材料）的瞬态非线性折射特性。因此，非线性折射几乎与脉冲宽度无关。了解响应函数还可以设计有机染料溶液（例如，具有有效零非线性折射的材料）的瞬态非线性折射特性。