Coherent quantum control of dark excitons in hybrid metal organic chalchogenolates

Abstract

Artificial atom-like systems are a promising candidate for next generation quantum processing. Among them, dark excitons exhibit one of the longest lifetimes at high temperatures. Here, we demonstrate coherent control of dark excitonic states in metal-organic chalcogenolates (MOChas) by using an ultrafast pulse shaper at room temperature. These dark exciton states are optically accessed via two-photon absorption and directly read out with a four-wave mixing process. The system is described by a non-perturbative, two-photon Hamiltonian based on well-known atomic physics and applied to a three level system comprised of two dark excitons. Empirical and theoretical state specific optical access is shown via a simple optical pulse shape. The developed Hamiltonian-based description is a first step towards a quantum processing platform using three-level systems and two photon transitions, one example being dark excitons in the MOCha silver benzeneselenolate (mithrene). Simple conditions for gate operations are laid out and described.