The considerable potential of perovskite-inspired Cu2AgBiI6 (CABI) photovoltaics under both solar and artificial lighting has been recently highlighted. However, to realistically ensure the suitability of CABI-based indoor photovoltaics (IPVs) to...
The perovskite‐inspired Cu2AgBiI6 (CABI) material has been gaining increasing momentum as photovoltaic (PV) absorber due to its low toxicity, intrinsic air stability, direct bandgap, and a high absorption coefficient in the range of 105 cm−1. However, the power conversion efficiency (PCE) of existing CABI‐based PVs is still seriously constrained by the presence of both intrinsic and surface defects. Herein, antimony (III) (Sb3+) is introduced into the octahedral lattice sites of the CABI structure, leading to CABI‐Sb with larger crystalline domains than CABI. The alloying of Sb3+ with bismuth (III) (Bi3+) induces changes in the local structural symmetry that dramatically increase the formation energy of intrinsic defects. Light‐intensity dependence and electron impedance spectroscopic studies show reduced trap‐assisted recombination in the CABI‐Sb PV devices. CABI‐Sb solar cells feature a nearly 40% PCE enhancement (from 1.31% to 1.82%) with respect to the CABI devices mainly due to improvement in short‐circuit current density. This work will promote future compositional design studies to enhance the intrinsic defect tolerance of next‐generation wide‐bandgap absorbers for high‐performance and stable PVs.
Perovskite-inspired Cu2AgBiI6 (CABI) absorber has recently gained increased popularity due to its low toxicity, intrinsic air stability, and wide bandgap ≈ 2 eV, which makes it ideal for indoor photovoltaics (IPVs). However, the considerable presence of both intrinsic and surface defects is responsible of the still modest indoor power conversion efficiency (PCE(i)) of CABI- based IPVs, with the short-circuit current density (JSC) being nearly half of the theoretical limit. Herein, we introduce antimony (III) (Sb3+) into the octahedral lattice sites of CABI structure, leading to CABI-Sb with substantially larger crystalline domains than CABI. The alloying of Sb3+ with bismuth (III) (Bi3+) induces changes in the local structural symmetry, in turn causing a remarkably increased formation energy of intrinsic defects. This accounts for the overall reduced defect density in CABI-Sb. CABI-Sb IPVs feature an outstanding PCE(i) of nearly 10% (9.53%) at 1000 lux, which represents an almost double PCE(i) compared to that of CABI devices (5.52%) mainly due to an improvement in JSC. This work will promote future compositional design studies to reduce the intrinsic defect tolerance of next-generation wide- bandgap absorbers for high-performance and stable IPVs.
The stability of
perovskite solar cells (PSCs) is greatly affected
by the interface between the perovskite active layer and the hole
transport material (HTM). The rational design of HTMs with effective
anchoring to the perovskite surface is an emerging elegant strategy
to promote compact and ordered interfaces that lead to highly efficient
and stable PSCs. Herein, we propose two fluorene-based HTM molecular
architectures (SCF1 and SCF2) derived from
the popular yet expensive Spiro-OMeTAD. Their employment as dopant-free
HTMs in standard triple-cation CsFAMA PSCs leads to superior device
stability, with a T
80 lifetime well above
1 year (431 days). Our combined theoretical and experimental study
of the CsFAMA|HTM interface reveals that the improved adhesion of
the SCF-HTMs to the perovskite layer is the key to minimize
the non-radiative recombination, reduce the hole trap density, and
enhance the long-term stability of the corresponding devices. The
simplified structures of SCF1 and SCF2,
obtained by removing the orthogonal fragment of the Spiro-OMeTAD scaffold,
show a lower molecular distortion than Spiro-OMeTAD, thus promoting
a favorable electronic interaction between the SCF-HTMs
and the perovskite. This study provides useful design criteria for
achieving highly stable PSCs including dopant-free HTMs with optimized
adhesion to the perovskite surface.
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