Ultrafast Optical Control of Polariton Energy in an Organic Semiconductor Microcavity

Abstract The manipulation of exciton-polaritons and their condensates is of great interest due to their applications in polariton simulators and high-speed, all-optical logic devices. Until now, methods of trapping and manipulating such condensates are not dynamically reconfigurable or resulted in an undesirable reduction in the exciton-photon coupling strength. Here, a new strategy for the ultrafast control of polariton resonances via transient modification of an optical cavity mode is presented. Multilayer organic semiconductor microcavities that contain two absorbers are constructed: one strongly-coupled to the cavity photon mode and one that is out-of-resonance. By selectively exciting the out-of-resonance absorber using ultrashort laser pulses, the cavity refractive index is modulated, and fully-reversible blueshifts of the lower polariton branch by up to 8 meV in sub-ps timescales with no corresponding reduction in the exciton-photon coupling strength are generated. This work demonstrates the ability to manipulate polariton energy landscapes over ultrafast timescales with important applications in emerging computing technologies.