Mobility-lifetime relation links photodegradation in spin-coated and gravure-printed organic solar cells

Abstract

The degradation mechanisms of organic solar cells (OSCs) have been studied primarily in spin-coated, laboratory-scale devices, whereas scalable processing modifies the device architecture, active-layer morphology, and underlying charge-transport and recombination properties. Whether these changes also alter how solar cells degrade remains unclear. Here, we compare spin-coated and fully roll-to-roll-compatible gravure-printed PM6:Y12 solar cells during $\sim$1000 h of continuous illumination. Despite distinct initial properties and degradation signatures, the loss of power-conversion efficiency systematically follows the mobility-lifetime product $μτ$. Remarkably, ageing of the printed devices increases the recombination lifetime while strongly reducing charge-carrier mobility, showing that a longer lifetime alone does not imply improved device performance. The mobility reduction is accompanied by decreased PM6 lamellar order, whereas the additional open-circuit voltage loss originates predominantly from increased non-radiative recombination. Dark recovery further reveals a metastable contribution specific to the printed architecture. These results identify the mobility-lifetime product as a unifying physical descriptor for photodegradation, linking ageing-induced microscopic changes to macroscopic performance loss across spin-coated and scalable printed OSCs.