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Composition-dependent band structure parameters and band-gap bowing effect in a caesium lead mixed halide system: a cyclic voltammetry investigation. | LitMetric

Cyclic voltammetry techniques have been employed to study the effect of halide substitution on the band edge parameters and band gap bowing effect in the case of CsPbX [X = I, Br, Cl] perovskite nanocrystals (PNCs). A series of compositions, CsPbI, CsPb(I-Br), CsPbBr, CsPb(Br-Cl) and CsPbCl, have been prepared by a hot injection method. From powder XRD and HR-TEM analysis, the formation of a highly crystalline, cubic phase of the perovskite having size in the range from 7-20 nm has been confirmed. Sharp peaks in the photoluminescence spectra suggest the formation of quantum dots with narrow-size distribution. The composition-dependent optical band gap (opgap) for CsPbX displays a systematic shift towards shorter wavelengths from I to Br to Cl substitutions. The cyclic voltammetry investigation on the dispersion of PNCs in nonaqueous solvents yielded prominent cathodic and anodic peaks. These are correlated to conduction (e) and valence band edge (h) positions, respectively. The h has been decreased substantially with I to Br to Cl in CsPbX. Meanwhile, e shows a marginal increase. The values derived from CV data demonstrated an excellent match with UVPS results, reported for a similar system. From these results, the quasi-particle gap (qpgap) and exciton binding energy have been estimated for all the compositions. The negative band gap bowing effect noted in these PNCs is attributed to the size quantization effect. The band-edge parameters reported in this work will be valuable in matching these heterojunctions with suitable electron/hole transport materials for optimum device-performance.

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http://dx.doi.org/10.1039/d3cp05956aDOI Listing

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