Publication date: 15th December 2025
Organic–inorganic lead-halide perovskites now underpin record-breaking single-junction solar-cell efficiencies (>26 %) and highly tuneable light-emitting diodes (LEDs). Yet both technologies still suffer performance losses linked to trap-mediated recombination and field-dependent carrier imbalances. Crucially, these loss pathways emerge only under true operating conditions, where built-in and applied electric fields, charge-transport layers, space-charge accumulation, and ion migration reshape the local potential landscape in ways different from the neat films.
In this talk, I will outline our progress toward producing operando, molecular-scale “movies” of the electronic dynamics that govern perovskite devices. I will begin by showing how nanosecond transient-absorption spectroscopy allows us to track the real-time behaviour of free charge carriers; by analysing subtle features in the resulting spectra we can map the internal electric field and pinpoint where carriers become either trapped or accelerated within the device stack.
I will then describe how these measurements are complemented by ultrafast mid-infrared pump–probe, or “optical-control,” spectroscopy, which selectively excites and monitors bound excitonic and polaronic states—early-stage species that often lead to non-radiative losses in perovskite photovoltaic and light-emitting structures. Both action spectroscopy with photocurrent and photovoltage detection will be presented.
Taken together, the two spectroscopic approaches provide a unified view of both free and bound charge populations under realistic operating conditions. Finally, I will show how coupling these experimental insights to drift-diffusion modelling closes the loop between microscopic dynamics and macroscopic performance, yielding concrete design rules for faster, more efficient optoelectronic devices.
