Generation of pseudo-sunlight via quantum entangled photons and the interaction with molecules

Light incident upon molecules trigger fundamental processes in diverse systems present in nature. However, under natural conditions, such as sunlight illumination, it is impossible to assign known times for photon arrival owing to continuous pumping, and therefore, the photo-induced processes cannot be easily investigated. In this work, we theoretically demonstrate that characteristics of sunlight photons such as photon number statistics and spectral distribution can be emulated through quantum entangled photon pair generated with the parametric down-conversion (PDC). We show that the average photon number of the sunlight in a specific frequency spectrum, e.g., the visible light, can be reconstructed by adjusting the PDC crystal length and pump frequency, and thereby molecular dynamics induced by the pseudo-sunlight can be investigated. The entanglement time, which is the hallmark of quantum entangled photons, can serve as a control knob to resolve the photon arrival times, enabling investigations on real-time dynamics triggered by the pseudo-sunlight photons.