Atomic-Scale Imaging and Nano-Scale Mapping of Cubic α‑CsPbI3 Perovskite Nanocrystals for Inverted Perovskite Solar Cells

Colloidal synthesized cubic α-CsPbI3 perovskite nanocrystals having a smaller lattice constant (a = 6.2315 Å) compared to the standard structure, and nanoscale mapping of their surfaces are reported to achieve superior photovoltaic performance under 45–55% humidity conditions. Atomic scale transmiss...

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Veröffentlicht in:ACS applied materials & interfaces 2022-02, Vol.14 (7), p.9711-9723
Hauptverfasser: Mahato, Somnath, Ghorai, Arup, Mondal, Ajoy, Srivastava, Sanjeev Kumar, Modak, Mantu, Das, Shreyasi, Ray, Samit K
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Sprache:eng
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Zusammenfassung:Colloidal synthesized cubic α-CsPbI3 perovskite nanocrystals having a smaller lattice constant (a = 6.2315 Å) compared to the standard structure, and nanoscale mapping of their surfaces are reported to achieve superior photovoltaic performance under 45–55% humidity conditions. Atomic scale transmission electron microscopic images have been utilized to probe the precise arrangement of Cs, Pb, and I atoms in a unit cell of α-CsPbI3 NCs, which is well supported by the VESTA structure. Theoretical calculation using density functional theory of our experimental structure reveals the realization of direct band to band transition with a lower band gap, a higher absorption coefficient, and stronger covalent bonding between the Pb and I atoms in the [PbI6]4– octahedral, as compared to reported standard structure. Nanoscale surface mapping using Kelvin probe force microscopy yielding contact potential difference (CPD) and conductive atomic force microscopy for current mapping have been employed on α-CsPbI3 NCs films deposited on different DMSO doped PEDOT:PSS layers. The difference of CPD value under dark and light illumination suggests that the hole injection strongly depends on the interfaces with PEDOT:PSS layer. The carrier transport through grain interiors and grain boundaries in α-CsPbI3 probed by the single-point c-AFM measurements reveal the excellent photosensitivity under the light conditions. Finally, inverted perovskite solar cells, employing α-CsPbI3 NCs film as an absorber layer and PEDOT:PSS layer as a hole transport layer, have been optimized to achieve the highest power conversion efficiency of 10.6%, showing their potential for future earth abundant, low cost, and air stable inverted perovskite photovoltaic devices.
ISSN:1944-8244
1944-8252
DOI:10.1021/acsami.1c20794