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Cavity quantum electrodynamics has been studied as a potential approach tomodify free charge carrier generation in donor-acceptor heterojunctions becauseof the delocalization and controllable energy level properties of hybridizedlight-matter states known as polaritons. However, in many experimental systems,cavity coupling decreases charge separation. Here, we theoretically study thequantum dynamics of a coherent and dissipative donor-acceptor cavity system, toinvestigate the dynamical mechanism and further discover the conditions underwhich polaritons may enhance free charge carrier generation. We use openquantum system methods based on single-pulse pumping to find that polaritonshave the potential to connect excitonic states and charge separated states,further enhancing free charge generation on an ultrafast timescale of severalhundred femtoseconds. The mechanism involves that polaritons with proper energylevels allow the exciton to overcome the high Coulomb barrier induced byelectron-hole attraction. Moreover, we propose that a second-hybridizationbetween a polariton state and dark states with similar energy enables theformation of the hybrid charge separated states that are optically active.These two mechanisms lead to a maximum of 50% enhancement of free chargecarrier generation on a short timescale. However, our simulation reveals thaton the longer timescale of picoseconds, internal conversion and cavity lossdominate and suppress free charge carrier generation, reproducing theexperimental results. Thus, our work shows that polaritons can affect thecharge separation mechanism and promote free charge carrier generationefficiency, but predominantly on a short timescale after photoexcitation.

Polariton Enhanced Free Charge Carrier Generation in Donor-Acceptor Cavity Systems by a Second-Hybridization Mechanism