Solid-State Lithium-Ion Batteries as a Method for Doping Halide Perovskites with an In Situ Optical Readout of Dopant Concentration

[Image: see text] Controlled doping of halide perovskites is a longstanding challenge for efficient optoelectronic applications. Here, a solid-state lithium-ion battery (LIB) inspired device is used as a method of extrinsically doping a halide perovskite in a controlled and measurable fashion. The Burstein–Moss band gap shift induced by the electronic doping is measured using in situ optical spectroscopy to monitor the fraction of injected charges that successfully n-type dope the perovskite. By comparing the optical and electrochemical readouts of the charge density, we demonstrate a 96% doping efficiency during the insertion process. Subsequent charge removal steps demonstrate only a partial “undoping” of the perovskite, providing insights into the capacity degradation pathways in perovskite LIB electrodes.