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Photonics for Quantum (PfQ)

Two-photon excitation with classical and entangled light

Oleg P. Varnavski, Juan P. Villabona-Monsalve, Audrey V. Eshun, Carolyn E. Gunthardt, Theodore G. Goodson III

Published Jul 9, 2021• 0 citations
Publisher
DOI
10.1117/12.2600805

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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.
Quantum entanglement has been shown to imply correlations stronger than those allowed by classical models. The possibility of performing tasks that are classically impossible has made quantum entanglement a powerful resource for the development of novel methods and applications in various fields of research such as quantum computing, quantum cryptography, and quantum metrology. There is a great need for the development of next generation instrumentation and technologies utilizing entangled quantum light. Among the many applications of nonclassical states of light, nonlinear microscopy has the potential to make an impact in broad areas of science from physics to biology. Here, the microscopic image created by the fluorescence selectively excited by the process of the entangled two-photon absorption is reported. Entangled two-photon microscopy offers nonlinear imaging capabilities at an unprecedented low excitation intensity 10 7, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. The nonmonotonic dependence of the image on the femtosecond delay between the components of the entangled photon pair is demonstrated. This delay dependence is a result of specific quantum interference effects associated with the entanglement and this is not observable with classical excitation light. In combination with novel spectroscopic capabilities provided by a nonclassical light excitation, this is of critical importance for sensing and biological applications.