Entangled Photon Spectroscopy
Entangled Photon Spectroscopy
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纠缠光子光谱
DOI：
10.1021/acs.accounts.1c00687
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发表时间：
2022
影响因子：
18.3
通讯作者：
Goodson, Theodore
中科院分区：
文献类型：
--
作者：
Eshun, Audrey;Varnavski, Oleg;Villabona-Monsalve, Juan P.;Burdick, Ryan K.;Goodson, Theodore
概述对量子相关现象的兴趣增强为化学家提供了突破化学过程检测和分析极限的新机会。正如一些人所说的第二次量子革命，现在是将之前量子现象研究中学到的规则应用于对化学家来说很重要的新方法和技术的时候了。虽然最近人们对量子信息科学（QIS）产生了极大的兴趣，但了解光的非经典态如何与物质相互作用的探索已经持续了二十多年。我们大约在这个时候开始进入这个领域，使用材料来产生非经典的光态。在这里，多光子吸收的过程导致光的光子数压缩状态，其中光子统计数据是亚泊松的。除了对产生光的压缩态有极大的兴趣外，人们对光的纠缠态的形成也很感兴趣。虽然大部分工作仍在基础物理学方面，但关于如何将量子纠缠应用于光谱学、成像和传感，有许多新途径。这些机会可能会对化学界的广泛应用产生巨大影响。在本报告中，我们讨论了纠缠（或量子）光在光谱学中的使用以及在显微镜和干涉测量中的应用。详细讨论了使用量子光的潜在好处。从我们组的 Dong-Ik Lee 博士在卟啉树枝状聚合物系统中进行的首次实验，到对黄素蛋白等生物系统的纠缠两个光子吸收截面的测量，纠缠光在光谱学中的有用性已经得到说明。这些早期测量为对纠缠光和纠缠光子吸收截面的独特特性进行更先进的测量开辟了道路，这为操纵分子中的激发态提供了新的控制旋钮。荧光诱导的纠缠过程的第一个报告是在有机发色团中测量了纠缠光子截面。这些结果后来对纠缠双光子显微镜等应用产生了广泛影响。通过我们对量子纠缠光子激发显微镜的设计、构建和实现，在107光子/秒的前所未有的低激发强度下实现了重要的成像能力，这比经典双光子图像的激发水平低6个数量级。新的报告还说明了非经典光在拉曼成像中的优势。从更精确测量的角度来看，在量子干涉测量中使用纠缠光子可能为化学研究提供新的机会。利用红欧曼德尔（HOM）干涉仪中纠缠光子的相关性，进行了分子光谱学和量子干涉测量相结合的实验。最初的实验表明，HOM 信号对放置在干涉仪一个臂中的共振有机样品的存在很敏感。此外，还获得了诸如移相时间之类的参数，为未来更先进的现象学提供了机会。
ConspectusThe enhanced interest in quantum-related phenomena has provided new opportunities for chemists to push the limits of detection and analysis of chemical processes. As some have called this the second quantum revolution, a time has come to apply the rules learned from previous research in quantum phenomena toward new methods and technologies important to chemists. While there has been great interest recently in quantum information science (QIS), the quest to understand how nonclassical states of light interact with matter has been ongoing for more than two decades. Our entry into this field started around this time with the use of materials to produce nonclassical states of light. Here, the process of multiphoton absorption led to photon-number squeezed states of light, where the photon statistics are sub-Poissonian. In addition to the great interest in generating squeezed states of light, there was also interest in the formation of entangled states of light. While much of the effort is still in foundational physics, there are numerous new avenues as to how quantum entanglement can be applied to spectroscopy, imaging, and sensing. These opportunities could have a large impact on the chemical community for a broad spectrum of applications.In this Account, we discuss the use of entangled (or quantum) light for spectroscopy as well as applications in microscopy and interferometry. The potential benefits of the use of quantum light are discussed in detail. From the first experiments in porphyrin dendrimer systems by Dr. Dong-Ik Lee in our group to the measurements of the entangled two photon absorption cross sections of biological systems such as flavoproteins, the usefulness of entangled light for spectroscopy has been illustrated. These early measurements led the way to more advanced measurements of the unique characteristics of both entangled light and the entangled photon absorption cross-section, which provides new control knobs for manipulating excited states in molecules.The first reports of fluorescence-induced entangled processes were in organic chromophores where the entangled photon cross-section was measured. These results would later have widespread impact in applications such as entangled two-photon microscopy. From our design, construction and implementation of a quantum entangled photon excited microscope, important imaging capabilities were achieved at an unprecedented low excitation intensity of 107photons/s, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. New reports have also illustrated an advantage of nonclassical light in Raman imaging as well.From a standpoint of more precise measurements, the use of entangled photons in quantum interferometry may offer new opportunities for chemistry research. Experiments that combine molecular spectroscopy and quantum interferometry, by utilizing the correlations of entangled photons in a Hong–Ou–Mandel (HOM) interferometer, have been carried out. The initial experiment showed that the HOM signal is sensitive to the presence of a resonant organic sample placed in one arm of the interferometer. In addition, parameters such as the dephasing time have been obtained with the opportunity for even more advanced phenomenology in the future.