Temperature-Controlled Entangled-Photon Absorption Spectroscopy
Temperature-Controlled Entangled-Photon Absorption Spectroscopy
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DOI：
10.1103/physrevlett.123.023601
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发表时间：
2019-07-09
影响因子：
8.6
通讯作者：
U'Ren, Alfred B.
中科院分区：
文献类型：
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作者：
Leon-Montiel, Roberto de J.;Svozilik, Jiri;U'Ren, Alfred B.
纠缠双光子吸收光谱（TPA）已被广泛认为是揭示复杂分子系统结构相关信息的有力工具。然而，到目前为止，这种技术的实验实现仍然难以捉摸，主要是因为两个主要的困难：第一，需要用具有不同时间相关性的双光子状态进行多次实验，这意味着实验者必须拥有数十个，如果不是数百个，纠缠光子源;第二，需要有吸收介质的最低中间能级的先验知识。在这项工作中，我们提出了一个简单的实验方案，成功地克服了这两个限制。通过利用温度控制的纠缠光子源，它允许调谐吸收光子的中心频率，我们表明，TPA信号，作为产生成对光子的非线性晶体的温度的函数测量，以及它们之间的可控延迟，携带关于吸收介质的电子能级结构的所有信息，这可以通过简单的傅里叶变换来揭示。
Entangled two-photon absorption spectroscopy (TPA) has been widely recognized as a powerful tool for revealing relevant information about the structure of complex molecular systems. However, to date, the experimental implementation of this technique has remained elusive, mainly because of two major difficulties: first, the need to perform multiple experiments with two-photon states bearing different temporal correlations, which translates into the necessity to have at the experimenter's disposal tens, if not hundreds, of sources of entangled photons; second, the need to have a priori knowledge of the absorbing medium's lowest-lying intermediate energy level. In this work, we put forward a simple experimental scheme that successfully overcomes these two limitations. By making use of a temperature-controlled entangled-photon source, which allows the tuning of the central frequencies of the absorbed photons, we show that the TPA signal, measured as a function of the temperature of the nonlinear crystal that generates the paired photons, and a controllable delay between them, carries all information about the electronic level structure of the absorbing medium, which can be revealed by a simple Fourier transformation.