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. 2023 Aug 3;13(33):23348-23358.
doi: 10.1039/d3ra04085b. eCollection 2023 Jul 26.

[(CH3)2NH2]2PdBr4, a layered hybrid halide perovskite semiconductor with improved optical and electrical properties

Kawther Trabelsi  1 , Nidhal Drissi  2 , Fadhel Hajlaoui  3 , Mustapha Zighrioui  4 , Abdallah Rhaiem  1 , Nathalie Audebrand  5 , Thierry Roisnel  5 , Karoui Karim  1   4
Affiliations

[(CH3)2NH2]2PdBr4, a layered hybrid halide perovskite semiconductor with improved optical and electrical properties

Kawther Trabelsi et al. RSC Adv. .

Abstract

Inspired by the success of three-dimensional hybrid perovskites (CH3NH3)PbX3 (X = Cl, Br, I), two-dimensional (2D) organic-inorganic hybrid metal halides have drawn immense attention due to their highly tunable physical properties. Moreover, although 3D hybrid perovskite materials have been reported, the development of new organic-inorganic hybrid semiconductors is still an area in urgent need of investigation. Here, we used the dimethylammonium cation to construct a palladium-based halide perovskite material [(CH3)2NH2]2PdBr4 with a 2D layered structure. This layered perovskite undergoes one endothermic peak at 415 K corresponding to melting of the organic molecule. The thermal stability of the compound is up to about 500 K. The activation energy and conduction mechanisms are discussed, and the optical study shows a gap energy equal to 2.5 eV. The electrical AC conductivity is in the order of 10-4 Ω-1 cm-1, which confirms the semiconductor character of this material and indicates its importance in the optoelectronic domain.

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Conflict of interest statement

There are no conflicts to declare.

Figures

Fig. 1
Fig. 1. The structural assembly process of compound [(CH3)2NH2]2PdBr4: (a) view of the [(CH3)2NH2]2PdBr4 single crystal showing a lamellar nature; (b) the asymmetric unit of [(CH3)2NH2]2PdBr4; (c) packing diagram of [(CH3)2NH2]2PdBr4 along the b-direction; (d) packing structure of the compound along the c-axis; (e) extended network structure connected by corner-shared octahedra (view of 2D [PdBr4]2− reticulated framework). Hydrogen bonds are shown with red dashed lines. Symmetry codes: (i) −x + 3/2, −y + 3/2, −z + 1.
Fig. 2
Fig. 2. (a) Variation of the absorbance wavelength, (b) plot of (αhν)2vs. hν, (c) plot of ln(α) vs. hν for [(CH3)2NH2]2PdBr4.
Fig. 3
Fig. 3. DTA and TGA curves for the [(CH3)2NH2]2PdBr4 crystal during the heating run.
Fig. 4
Fig. 4. DSC results as a function of temperature, obtained by heating and cooling the [(CH3)2NH2]2PdBr4 compound at a rate of 5 K min−1.
Fig. 5
Fig. 5. Raman spectra of [(CH3)2NH2]2PdBr4 at various temperatures.
Fig. 6
Fig. 6. The position of PdBr42− vibration modes before and after the melting temperature of [(CH3)2NH2]2PdBr4.
Fig. 7
Fig. 7. (a) Nyquist plots and equivalent circuit model of [(CH3)2NH2]2PdBr4. (b) Variation of the imaginary part and (c) real part of impedance as a function of frequency, and (d) the plot of ln(σg) versus 1000/T.
Fig. 8
Fig. 8. (a) Angular frequency dependence of the imaginary part of the electric modulus at several temperatures for the [(CH3)2NH2]2PdBr4 compound, (b) using the tangent method of M′; (inset, c) the plot of ln(ωgmax) versus 1000/T.
Fig. 9
Fig. 9. (a) Plots of the imaginary modulus M′′ vs. real modulus M′. (b) Frequency dependence of relaxation peaks, M′′ and −Z′′, for [(CH3)2NH2]2PdBr4.
Fig. 10
Fig. 10. Frequency dependence of the capacitance (a) and AC conductivity (b) at various temperatures for the [(CH3)2NH2]2PdBr4 compound. (inset, c) The variation of universal exponent s as a function of temperature.
Fig. 11
Fig. 11. Fitting of AC conductivity at different frequencies using the NSPT model.
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