论文标题
分子的两光子吸收通过分子键入光子对：光子数字相关性和光谱相关的作用
Two-photon absorption of time-frequency-entangled photon pairs by molecules: the roles of photon-number correlations and spectral correlations
论文作者
论文摘要
虽然已经预测，分子与分离的时间频率输入的光子对（EPP）的两光子吸收（TPA）和其他形式的非线性相互作用可以显示出多种引人入胜的效果，但它们在实用的量子范围内分子光谱中的潜在使用需要仔细检查。本文介绍了通过光子数相关性和光谱相关性的量子增强TPA的详细理论研究，包括对分散体的有害影响的描述。尽管自发参数降低转换产生的EPP中的这种相关性可以显着提高TPA速率在极低的光学通量的状态下，我们发现，对于溶液中的典型分子，这种状态对应于TPA事件速率低，以至于在实践中无法观察到。我们的结果支持EPP光谱在原子或其他窄线宽度系统中的有用性，同时质疑这种方法对包括溶液中分子在内的宽带系统的疗效。
While two-photon absorption (TPA) and other forms of nonlinear interactions of molecules with isolated time-frequency-entangled photon pairs (EPP) have been predicted to display a variety of fascinating effects, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This paper presents a detailed theoretical study of quantum-enhanced TPA by both photon-number correlations and spectral correlations, including an account of the deleterious effects of dispersion. While such correlations in EPP created by spontaneous parametric down conversion can increase the TPA rate significantly in the regime of extremely low optical flux, we find that for typical molecules in solution this regime corresponds to such low TPA event rates as to be unobservable in practice. Our results support the usefulness of EPP spectroscopy in atomic or other narrow-linewidth systems, while questioning the efficacy of such approaches for broadband systems including molecules in solution.
