Manipulating Two-Photon Absorption of Molecules through Efficient Optimization of Entangled Light

Sajal Kumar Giri, George C. Schatz
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Abstract

We report how the unique temporal and spectral features of pulsed entangled photons from a parametric downconversion source can be utilized for manipulating electronic excitations through the optimization of their spectral phase. A new comprehensive optimization protocol based on Bayesian optimization has been developed in this work to selectively excite electronic states accessible by two-photon absorption. Using our optimization method, the entangled two-photon absorption probability for a thiophene dendrimer can be enhanced by up to a factor of 20 while classical light turns out to be nonoptimizable. Moreover, the optimization involving photon entanglement enables selective excitation that would not be possible otherwise. In addition to optimization, we have explored entangled two-photon absorption in the small entanglement time limit showing that entangled light can excite molecular electronic states that are vanishingly small for classical light. We demonstrate these opportunities with an application to a thiophene dendrimer.
通过有效优化纠缠光操纵分子的双光子吸收
我们报告了如何利用参数下转换源产生的脉冲纠缠光子的独特时间和光谱特征,通过优化其光谱相位来操纵电子激发。这项研究开发了一种基于贝叶斯优化法的新的综合优化方案,以选择性地激发双光子吸收所能达到的电子状态。利用我们的优化方法,噻吩树枝状聚合物的纠缠双光子吸收概率最多可提高 20 倍,而经典光原来是不可优化的。此外,涉及光子纠缠的优化还能实现选择性激发,而这在其他情况下是不可能实现的。除了优化之外,我们还探索了小纠缠时间极限下的纠缠双光子吸收,结果表明纠缠光可以激发分子电子态,而这对于经典光来说是微乎其微的。我们将这些机会应用于噻吩树枝状聚合物。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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