Colors of entangled two-photon absorption
Colors of entangled two-photon absorption
复制标题
纠缠双光子吸收的颜色
DOI：
10.1073/pnas.2307719120
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发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Goodson, Theodore
中科院分区：
文献类型：
--
作者：
Varnavski, Oleg;Giri, Sajal Kumar;Chiang, Tse-Min;Zeman, Charles J.;Schatz, George C.;Goodson, Theodore
纠缠光子的多光子吸收提供了获取有关化学和生物过程的独特信息的方法。使用纠缠光子进行测量可以在非常低的光照水平下以高选择性感测生物特征，以防止光损伤。在本文中，我们提出了分子系统中纠缠双光子吸收（ETPA）过程的激发波长依赖性的理论和实验研究，这提供了关于纠缠如何影响分子光谱的见解。我们证明，ETPA 激发光谱可能不同于经典 TPA 以及双倍频率光子的单光子共振吸收 (OPA) 的激发光谱。这些结果是通过假设 ETPA 横截面由双光子激发态辐射线宽而不是电子-声子相互作用控制来建模的，这导致激发光谱与观察到的结果相匹配。此外，我们发现具有最高 TPA 和 ETPA 强度的双光子允许态具有较高的电子纠缠，其中 ETPA 特别有利于具有最长辐射寿命的态。这些结果为基于量子光的光谱学和显微镜的发展提供了概念，这将导致 ETPA 传感器和低强度检测方案的效率更高。
Multiphoton absorption of entangled photons offers ways for obtaining unique information about chemical and biological processes. Measurements with entangled photons may enable sensing biological signatures with high selectivity and at very low light levels to protect against photodamage. In this paper, we present a theoretical and experimental study of the excitation wavelength dependence of the entangled two-photon absorption (ETPA) process in a molecular system, which provides insights into how entanglement affects molecular spectra. We demonstrate that the ETPA excitation spectrum can be different from that of classical TPA as well as that for one-photon resonant absorption (OPA) with photons of doubled frequency. These results are modeled by assuming the ETPA cross-section is governed by a two-photon excited state radiative linewidth rather than by electron-phonon interactions, and this leads to excitation spectra that match the observed results. Further, we find that the two-photon-allowed states with highest TPA and ETPA intensities have high electronic entanglements, with ETPA especially favoring states with the longest radiative lifetimes. These results provide concepts for the development of quantum light–based spectroscopy and microscopy that will lead to much higher efficiency of ETPA sensors and low-intensity detection schemes.
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