Abstract
PL-based external radiative efficiency (ERE) and implied open-circuit
voltage (iV OC) metrics were introduced for thin-film
solar absorbers to better understand the voltage deficit and diagnose
losses in solar cells. Traditionally, elevated ERE and iV
OC measurements are associated with diminished
recombination within the solar device, a rationale heavily reliant on
the assumption of a uniform bandgap and high carrier mobilities in the
absorber. In this study, we investigate the possible reasons of elevated
iV OC in realistic CdSeTe absorbers with a graded Se
profile. By employing light-induced transient grating measurements, we
reveal that hole mobility significantly decreases—by more than an
order of magnitude—with increasing Se content. Using detailed
numerical models of iV OC, we examine how the bandgap
nonuniformity and the reduced hole mobility within graded CdSeTe
absorbers influence iV OC measurements. We show that
high iV OC may result from inflated quasi-Fermi-level
splitting in the front region of a CdSeTe absorber with slow hole
transport. Based on our results, we conclude that the iV
OC metric (or ERE metric) for graded CdSeTe devices may
be misleading, is not suitable for quantitative assessments, and should
not be used as a sole metric of absorber quality. We discuss possible
ways to extract useful information from the iV OC–V
OC gap by supplementing the front-side illumination
measurements with back-side illumination measurements.