Synthesis Recipe

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Table 1. Device architecture and photovoltaic parameters of double perovskite-based solar cells.

Double perovskites Device configuration Perovskite deposition method Voc [V] Jsc [mA cm2] FF PCE [%] Reference

Cs2AgBiBr6 ITO/SnO2/ Cs2AgBiBr6/ One-step spin-coating and 1.04 1.78 0.78 1.44 [74]
P3HT/Au low-pressure-assisted method
Cs2AgBiBr6 ITO/SnO2/ Cs2AgBiBr6/Au One-step spin-coating and 0.95 1.5 0.6 0.86 [74]
low-pressure-assisted method
Cs2AgBiBr6 ITO/Cu-NiO/Cs2AgBiBr6/C60/ One-step spin coating with antisolvent 1.01 3.19 0.69 2.23 [96]
BCP/Ag
Cs2AgBiBr6 FTO/cl-TiO2/mp-TiO2/ One-step spin coating 0.98 3.93 0.63 2.43 [66]
Cs2AgBiBr6/Spiro-OMeTAD/Au
Cs2AgBiBr6 ITO/cl-TiO2/Cs2AgBiBr6/ One-step spin coating 1.06 1.55 0.74 1.22 [75]
Spiro-OMeTAD/Au
Cs2AgBiBr6 FTO/cl-TiO2/mp-TiO2/ One-step spin coating with antisolvent 1.02 1.84 0.67 1.26 [76]
Cs2AgBiBr6/PTAA/Au
Cs2AgBiBr6 FTO/cl-TiO2/mp-TiO2/ One-step spin coating with antisolvent 0.64 2.45 0.57 0.9 [76]
Cs2AgBiBr6/Spiro-OMeTAD/Au
Cs2AgBiBr6 FTO/cl-TiO2/mp-TiO2/ One-step spin coating with antisolvent 0.71 1.67 0.57 0.68 [76]
Cs2AgBiBr6/PCPDTBT/Au
Cs2AgBiBr6 FTO/cl-TiO2/Cs2AgBiBr6/ Sequential vapor deposition 1.12 1.79 NA 1.37 [113]
P3HT/Au
Cs2NaBiI6 FTO/cl-TiO2/mp-TiO2/ One-step spin coating 0.47 1.99 0.44 0.42 [78]
Cs2NaBiI6/Spiro-OMeTAD/Au
Vacancy-ordered double perovskite
Cs2TiBr6 FTO/TiO2/Cs2TiBr6/P3HT/Au Two-step vapor deposition 0.89 4.03 0.63 2.26 [79]
Cs2TiBr6 FTO/TiO2/C60/Cs2TiBr6/ Two-step vapor deposition 1.02 5.69 0.56 3.28 [79]
P3HT/Au
Cs2SnI6 FTO/cl-ZnO/mp-ZnO/Cs2SnI6/ One-step spin coating 0.52 3.2 0.51 0.86 [82]
P3HT/Ag
Cs2SnI6 FTO/cl-TiO2/Cs2SnI6/P3HT/Ag Two-step sequential vapor deposition 0.51 5.41 0.35 0.96 [80]
Cs2SnI6 FTO/cl-TiO2/Cs2SnI6/P3HT/Ag Chemical bath deposition 0.25 7.41 0.24 0.47 [81]
Cs2SnI6xBrx FTO/cl-TiO2/Sn-TiO2/ Two-step solution synthesis 0.56 6.22 0.57 2.03 [83]
Cs2SnI6xBrx/Cs2SnI6 HTM/
LPAH/FTO

optical absorption.[94] Bandgap engineering was adopted by Du respectively.[95] The simulation indicated that bandgap transition
et al. to adjust the electronic band structure.[62] The Bi in the was attributed to the metal-to-metal charge transition. The crys-
B-site was substituted with Sb or In with a maximum amount tallized single crystal from concentrated acid solution showed no
before phase segregation. Cs2Ag(Bi1xMx)Br6 (M ¼ In, Sb) PL peaks, which was ascribed to the symmetry-forbidden transi-
showed a phase stability with the In3þ content up to 75% or tion. Despite the long carrier lifetime (microseconds) and narrow
the Sb3þ content up to 37.5%. The bandgap was broadened with bandgap, the incorporation of Tl still hindered this material from
the incorporation of In3þ and narrowed with the incorporation of practical use due to its high toxicity of Tl. Alternative metal ion
Sb3þ. The atomic substitution enabled the bandgap modulation substitution has been demonstrated for the synthesized
of 0.41 eV. From the DFT calculations, the shift of bandgap was Cs2AgInxBi1–xCl6, which shows direct bandgap and improved
ascribed to the electronic structure of Sb for Sb-substituted sam- PLQE.[94] Details of such material will be addressed in
ples. For the In-substituted samples, the In 5s states and the Section 3.1.2.
reduced chemical bonds of Bi atoms demonstrated the opposite Due to the tunable bandgap, long carrier lifetime, and light
effect on bandgap shift. Upon In substitution, the band transi- effective masses, Cs2AgBiX6 (X ¼ Br, Cl) double perovskites have
tion of Cs2Ag(Bi1xInx)Br6 remained in the indirect nature. been regarded as potential candidates for Pb-free PSCs.[66] Greul
Moreover, a weak and shifted PL intensity suggested the exis- et al. first demonstrated the fabrication of Cs2BiAgBr6 thin film
tence of defects. It is noted that as-synthesized materials deliv- by the one-step solution process and further integrated it into
ered a decent stability up to 60 days in the ambient environment. PSCs. As shown in Figure 5a, the spin-coated Cs2AgBiBr6 was
Due to the wide bandgap of Cs2AgBiBr6 (>2 eV), Slavney et al. annealed at a temperature of above 250  C to obtain pure double
synthesized Cs2AgTlX6 (X ¼ Br and Cl) members with a bandgap perovskite phase. The as-fabricated thin film was integrated in
of 1.96 and 0.95 eV for Cs2AgTlCl6 and Cs2AgTlBr6, PSCs composed of fluorine-doped tin oxide (FTO)/compact layer

Sol. RRL 2020, 4, 1900306 1900306 (12 of 32) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

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