In this work, the smallest and analogous organic spacers
“ethylammonium”
(EA) and “ethylenediammonium” (EDA) are incorporated
in MAPbI3 to form RP-EA and DJ-EDA perovskites (n = 1–4), respectively, in order to compare their
structural, morphological, optical, and optoelectronic properties,
which revealed significantly different characteristics of both perovskite
phases. Effective high frequency dielectric constants (εeff) of RP-EA and DJ-EDA are correlated with their optical
properties, which show that the large difference between the εeff’s of DJ-EDA (9.62; n = 1 to 7.58; n = 4) and MAPbI3 (6.5) is responsible for sharp
exciton absorbance peaks in DJ-EDA perovskites. Compared to RP-EA,
the DJ-EDA perovskites showed improved stability and a higher photoresponsivity
of ∼1.00 mA/W (n = 4) and retained 97.67%
(n = 2) of the initial photocurrent after 50 cycles
of transient photocurrent under 1 sun illumination (100 mW/cm2) performed under ambient atmosphere conditions owing to their
van der Waals gap free structure. On the other hand, RP-EA perovskites
possess relatively fast response times which are attributed to better
band alignment and in-plane morphology. Our results provide fundamental
insights about the structural and photophysical properties of the
smallest carbon chain organic spacer-based RP and DJ perovskites,
and these findings are crucial in order to find a suitable replacement
of bulk perovskites for commercial PV applications.