Wavepacket control and simulation protocol for entangled two-photon-absorption of molecules

Abstract: Quantum light spectroscopy, providing novel molecular information non-accessible by classical light, necessitates new computational tools when applied for complex molecular systems. We introduce two computational protocols for the molecular nuclear wave packet dynamics interacting with an entangled photon pair to produce the entangled two-photon absorption signal. The first involves summing over transition pathways in a temporal grid defined by two light-matter interaction times accompanied by the field correlation functions of quantum light. The signal is obtained by averaging over the two-time distribution characteristic of the entangled photon state. The other protocol involves a Schmidt decomposition of the entangled light and requires summing over the Schmidt modes. We demonstrate how photon entanglement can be used to control and manipulate the two-photon excited nuclear wave packets in a displaced harmonic oscillator model.