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Journal of Applied Optics

Measurement method of correlated properties of broad spectral sources based on two-photon absorption

Wei Liu, 西安应用光学研究所，陕西西安 710065, HOU Libing, Yingchun Wu, Zhanming Li, SUN Qiyao, LI Shan, ZHANG Weiguo, DUAN Wenbo

Published Jan 1, 2024• 0 citations

Abstract

以“鬼成像”为代表的关联成像具有新颖的物理现象和潜在的应用价值，已经吸引了众多学者的研究兴趣，其中光源关联特性的测量显得格外重要。然而，热光光源（太阳光、钨丝灯光）的相干时间太短，以至于无法采用现有探测器直接测量，阻碍了被动关联成像技术的发展。对此，基于虚能级极短寿命的超快时间分辨能力的双光子吸收过程，提出使用光子计数型光电倍增管探测器，采用迈克尔逊干涉仪对谱宽为150 nm的超连续激光的关联特性进行测量，测得的相干时间为60 fs、峰背比为2.6∶1，与理论预测一致，此外，与自发辐射光源（峰背比4∶1）和脉冲光（峰背比8∶1）的二阶关联函数相比，超连续激光的关联函数的峰背比展示出了不同的结果（峰背比2.6∶1），基于双光子吸收过程测量光源关联特性的方法给识别不同种类的光源提供了一种新的途径。该方法的实验装置更加简单紧凑，为直接使用太阳光进行“鬼成像”提供了一种新思路。

DOI: 10.5768/jao202445.0601007

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以“鬼成像”为代表的关联成像具有新颖的物理现象和潜在的应用价值，已经吸引了众多学者的研究兴趣，其中光源关联特性的测量显得格外重要。然而，热光光源（太阳光、钨丝灯光）的相干时间太短，以至于无法采用现有探测器直接测量，阻碍了被动关联成像技术的发展。对此，基于虚能级极短寿命的超快时间分辨能力的双光子吸收过程，提出使用光子计数型光电倍增管探测器，采用迈克尔逊干涉仪对谱宽为150 nm的超连续激光的关联特性进行测量，测得的相干时间为60 fs、峰背比为2.6∶1，与理论预测一致，此外，与自发辐射光源（峰背比4∶1）和脉冲光（峰背比8∶1）的二阶关联函数相比，超连续激光的关联函数的峰背比展示出了不同的结果（峰背比2.6∶1），基于双光子吸收过程测量光源关联特性的方法给识别不同种类的光源提供了一种新的途径。该方法的实验装置更加简单紧凑，为直接使用太阳光进行“鬼成像”提供了一种新思路。

Entangled photon pairs have been used for molecular spectroscopy in the form of entangled two-photon absorption and in quantum interferometry for precise measurements of light source properties and time delays. We present an experiment that combines molecular spectroscopy and quantum interferometry by utilizing the correlations of entangled photons in a Hong-Ou-Mandel (HOM) interferometer to study molecular properties. We find that the HOM signal is sensitive to the presence of a resonant organic sample placed in one arm of the interferometer, and the resulting signal contains information pertaining to the light-matter interaction. We can extract the dephasing time of the coherent response induced by the excitation on a femtosecond time scale. A dephasing time of 102 fs is obtained, which is relatively short compared to times found with similar methods and considering line width broadening and the instrument entanglement time As the measurement is done with coincidence counts as opposed to simply intensity, it is unaffected by even-order dispersion effects, and because interactions with the molecular state affect the photon correlation, the observed measurement contains only these effects and no other classical losses. The experiments are accompanied by theory that predicts the observed temporal shift and captures the entangled photon joint spectral amplitude and the molecule's transmission in the coincidence counting rate. Thus, we present a proof-of-concept experimental method based of entangled photon interferometry that can be used to characterize optical properties in organic molecules and can in the future be expanded on for more complex spectroscopic studies of nonlinear optical properties.

Broadband photon-pairs from a parametric down-conversion (PDC) source are essential for quantum optics experiments in the context of spectroscopy, quantum optical coherence tomography and entangled two-photon absorption [1]–[2]. Entangled two-photon absorption benefits from the ultra-short correlation time of a highly time-frequency entangled photon-pair which increases the absorption cross-section while in spectroscopy, broad spectral coverage in the mid-infrared allows one to enter the regime of life science applications.

光谱测量与成像技术的进步，已成为生命科学与材料科学研究中的关键表征手段。然而，在针对光学响应微弱的样品（如低维材料、活体细胞等）进行实际观测时，高功率激发光往往引入显著经典噪声，并造成不可忽视的光致损伤，从而限制了光学测量的信噪比与应用范围。在此背景下，具备特殊量子统计特性的非经典光源（如纠缠光与压缩光）为实现超越经典极限的信噪比提升提供了极具潜力的解决方案。本文聚焦于量子增强光谱与成像领域，系统梳理了基于纠缠光与压缩光两类重要量子光源的最新研究进展。纠缠光凭借光子间的量子关联特性，在关联成像、非探测光子成像及超快干涉测量等应用中展现出卓越的抗噪声能力；而压缩光则通过压缩光场噪声，在位移传感、等离激元探测及非线性显微成像等方面显著提升了探测灵敏度与信噪比。本文进一步系统阐述了量子光源在提高信噪比、降低光致损伤、提升时间分辨率以及增强非线性转换效率等方面的独特优势，并分析了当前制约量子成像技术实用化的关键挑战，包括光源亮度低，系统损耗大等问题。最后，对该领域未来的发展方向进行了展望。

The calibration method based on correlated photons can realize absolute calibration without standard transfer. The solar spectral irradiance meter using this calibration method needs a correlated photon source with a broad spectrum to achieve absolute calibration in the solar reflection band. In the early stage, non-collinear phase matching combined with multiple crystals was generally adopted to achieve wide spectral coverage. In this paper, a continuous wide spectral correlated photon source is obtained using pumping a BBO crystal by a 532nm laser and continuous angle tuning collinear phase matching. The collinear phase matching positions at different wavelengths are determined by the rotation crystal which shrinks the relevant photon rings into circular spots. The spectral range and correlation of the broad spectral correlated photon source are verified by the correlated photon ring image and the coincidence counting of four pairs of correlated photons of 800nm/1580nm, 840nm/1450nm, 900 nm/ 1300nm, and 950nm/1200nm.