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

• URL: http://arxiv.org/abs/2210.01278v1
• Date: Mon, 3 Oct 2022 23:58:20 GMT
• Title: Polariton Enhanced Free Charge Carrier Generation in Donor-Acceptor Cavity Systems by a Second-Hybridization Mechanism
• Authors: Weijun Wu, Andrew E. Sifain, Courtney A. Delpo, and Gregory D. Scholes
• Abstract summary: We study the quantum dynamics of a coherent donor-acceptor cavity system. We find that polaritons have the potential to connect excitonic states and charge separated states. Our work shows that polaritons can affect the charge separation mechanism and promote free charge carrier generation efficiency.
• Score: 0.0
• License: http://creativecommons.org/licenses/by-nc-sa/4.0/
• Abstract: Cavity quantum electrodynamics has been studied as a potential approach to modify free charge carrier generation in donor-acceptor heterojunctions because of the delocalization and controllable energy level properties of hybridized light-matter states known as polaritons. However, in many experimental systems, cavity coupling decreases charge separation. Here, we theoretically study the quantum dynamics of a coherent and dissipative donor-acceptor cavity system, to investigate the dynamical mechanism and further discover the conditions under which polaritons may enhance free charge carrier generation. We use open quantum system methods based on single-pulse pumping to find that polaritons have the potential to connect excitonic states and charge separated states, further enhancing free charge generation on an ultrafast timescale of several hundred femtoseconds. The mechanism involves that polaritons with proper energy levels allow the exciton to overcome the high Coulomb barrier induced by electron-hole attraction. Moreover, we propose that a second-hybridization between a polariton state and dark states with similar energy enables the formation of the hybrid charge separated states that are optically active. These two mechanisms lead to a maximum of 50% enhancement of free charge carrier generation on a short timescale. However, our simulation reveals that on the longer timescale of picoseconds, internal conversion and cavity loss dominate and suppress free charge carrier generation, reproducing the experimental results. Thus, our work shows that polaritons can affect the charge separation mechanism and promote free charge carrier generation efficiency, but predominantly on a short timescale after photoexcitation.

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