Mixed-halide
CsPbI
2
Br perovskite is promising for efficient
and thermally stable all-inorganic solar cells; however, the use of
conventional antisolvent methods and additives-based hole-transporting
layers (HTLs) currently hampers progress. Here, we have employed hot-air-assisted
perovskite deposition in ambient condition to obtain high-quality
photoactive CsPbI
2
Br perovskite films and have extended
stable device operation using metal cation doping and dopant-free
hole-transporting materials. Density functional theory calculations
are used to study the structural and optoelectronic properties of
the CsPbI
2
Br perovskite when it is doped with metal cations
Eu
2+
and In
3+
. We experimentally incorporated
Eu
2+
and In
3+
metal ions into CsPbI
2
Br films and applied dopant-free copper(I) thiocyanate (CuSCN) and
poly(3-hexylthiophene) (P3HT)-based materials as low-cost hole transporting
layers, leading to record-high power conversion efficiencies of 15.27%
and 15.69%, respectively, and a retention of >95% of the initial
efficiency
over 1600 h at 85 °C thermal stress.
Earth-abundant
quaternary chalcogenides are promising candidate
materials for thin-film solar cells. Here we have synthesized Cu2NiSnS4 nanocrystals and thin films in a novel zincblende
type cubic phase using a facile hot-injection method. The structural,
electronic, and optical properties are studied using various experimental
techniques, and the results are further corroborated within first-principles
density functional theory based calculations. The estimated direct
band gap ∼ 1.57 eV and high optical absorption coefficient
∼ 106 cm–1 indicate potential
application in a low-cost thin-film solar cell. Further, the alignments
for both conduction and valence bands are directly measured through
cyclic voltametry. The 1.47 eV electrochemical gap and very small
conduction band offset of −0.12 eV measured at the CNTS/CdS
heterojunction are encouraging factors for the device. These results
enable us to model carrier transport across the heterostructure interface.
Finally, we have fabricated a CNTS solar cell device for the first
time, with high open circuit voltage and fill factor. The results
presented here should attract further studies.
Semiconductors based on bismuth halides have gained attention for a wide range of electronic applications, including photovoltaics, light-emitting diodes, and radiation detectors. Their appeal is due to their low toxicity, high environmental stability under ambient conditions, and easy processability by a wide range of scalable methods. The performance of Bi-based semiconductors is dictated by electron–phonon interactions, which limit carrier mobilities and can also influence optoelectronic performance, for example, by giving rise to a large Stokes shift for photoluminescence, unavoidable energy loss channels, or shallow optical absorption onsets. In this Perspective, we discuss the recent understanding of how polarons and self-trapped excitons/carriers form in Bi-based semiconductors (particularly for the case of Cs2AgBiBr6), their impact on the optoelectronic properties of the materials, and the consequences on device performance. Finally, we discuss the opportunities that control of electron–phonon coupling enables, including stable solid-state white lighting, and the possibilities of exploiting the strong coupling found in bipolarons for quantum technologies.
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