Multichromatic Quantum Superpositions in Entangled Two-Photon Absorption Spectroscopy

Abstract: Quantum information science is driving progress in a vast number of scientific and technological areas that cover molecular spectroscopy and matter-light interactions in general. In these fields, the ability to generate quantum mechanically-entangled photons is opening avenues to explore the interaction of molecules with quantum light. This work considers an alternative way of correlating photons by including energy superpositions. We study how the multichromatic quantum superposition, or color superposition of photon-pair states, influences the optical properties of organic chromophores. This work uses electronic structure calculations based on time-dependent density functional theory, and a simple modification of the standard entangled two-photon absorption theory. Our calculations show that it is possible to substantially modify the optical absorption cross section of molecules, where constructive and destructive interferences are computed. The quantum interference effects are more pronounced than the constructive ones. These quantum effects, or related ones, could be observed in quantum spectroscopic experiments where qudit photon states are generated.