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Scanning Photocurrent Microscopy in Single Crystal Multidimensional Hybrid Lead Bromide Perovskites

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Abstract

We investigated solution-grown single crystals of multidimensional 2D–3D hybrid lead bromide perovskites using spatially resolved photocurrent and photoluminescence. Scanning photocurrent microscopy (SPCM) measurements where the electrodes consisted of a dip probe contact and a back contact. The crystals revealed significant differences between 3D and multidimensional 2D–3D perovskites under biased detection, not only in terms of photocarrier decay length values but also in the spatial dynamics across the crystal. In general, the photocurrent maps indicate that the closer the border proximity, the shorter the effective decay length, thus suggesting a determinant role of the border recombination centers in monocrystalline samples. In this case, multidimensional 2D–3D perovskites exhibited a simple fitting model consisting of a single exponential, while 3D perovskites demonstrated two distinct charge carrier migration dynamics within the crystal: fast and slow. Although the first one matches that of the 2D–3D perovskite, the long decay of the 3D sample exhibits a value two orders of magnitude larger. This difference could be attributed to the presence of interlayer screening and a larger exciton binding energy of the multidimensional 2D–3D perovskites with respect to their 3D counterparts.

How to cite

Initials first
E. Segura-Sanchis, R. García-Aboal, R. Fenollosa, F. Ramiro-Manzano and P. Atienzar. Scanning Photocurrent Microscopy in Single Crystal Multidimensional Hybrid Lead Bromide Perovskites. Nanomaterials 13, 2570 (2023). DOI: 10.3390/nano13182570.
Family name first
Segura-Sanchis, E., García-Aboal, R., Fenollosa, R., Ramiro-Manzano, F., & Atienzar, P. (2023). Scanning photocurrent microscopy in single crystal multidimensional hybrid lead bromide perovskites. Nanomaterials, 13, 2570. https://doi.org/10.3390/nano13182570

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This open-access article is distributed under the Creative Commons Attribution 4.0 licence; the journal version is the authoritative record. Official MDPI article record · CC BY 4.0 licence · MDPI rights and permissions.

Figures

Figure 1. Schematic representation of the electric contact on the microcrystalline samples, showing the irradiation objective at the bottom part controlled with a piezoelectric stage.
Figure 1. Schematic representation of the electric contact on the microcrystalline samples, showing the irradiation objective at the bottom part controlled with a piezoelectric stage.

Source: E. Segura-Sanchis et al., Nanomaterials 13, 2570 (2023), CC BY 4.0.

Figure 2. X-ray diffraction patterns for 3D and 2D–3D perovskite samples, including the low-angle inset.
Figure 2. X-ray diffraction patterns for 3D (A) and 2D–3D perovskite (B). The inset shows a magnification of the low-angles region characteristic of the layered phase. Red peaks correspond to the 3D phase and blue peaks to the 2D phase (PbBr4)2−.

Source: E. Segura-Sanchis et al., Nanomaterials 13, 2570 (2023), CC BY 4.0.

Figure 3. FESEM images of crystalline 3D and 2D–3D perovskites.
Figure 3. FESEM image of crystalline 3D (A) and 2D–3D perovskite (B).

Source: E. Segura-Sanchis et al., Nanomaterials 13, 2570 (2023), CC BY 4.0.

Figure 4. Photoluminescence, diffuse-reflectance and transmittance spectra of 3D and 2D–3D perovskites.
Figure 4. (A) Photoluminescence emission spectra of polycrystalline 3D (a) and 2D–3D (b) samples. (B) Diffuse-reflectance UV–Vis absorption spectra of (a) 3D and (b) mixed 2D–3D perovskite; the inset magnifies the absorption edge. (C) Photoluminescence emission of single crystals measured with SPCM. (D) Transmittance spectra of (a) 3D and (b) mixed 2D–3D single crystals.

Source: E. Segura-Sanchis et al., Nanomaterials 13, 2570 (2023), CC BY 4.0.

Figure 5. Scanning photocurrent microscopy images and profile analysis of 2D–3D and 3D perovskite samples.
Figure 5. Scanning photocurrent microscopy images and profile analysis. (a) PL and (b) ISC images of a multidimensional 2D–3D sample. (c) PL and (d) ISC images of a 3D sample. (e,f) Edge extraction and (g,h) photocurrent sections of the 2D–3D and 3D samples, respectively. (i) Effective-like photocurrent length extracted from the dashed lines (e−1) of (g,h).

Source: E. Segura-Sanchis et al., Nanomaterials 13, 2570 (2023), CC BY 4.0.

Figure 6. Model fits to experimental photocurrent profiles for 2D–3D and 3D perovskite samples.
Figure 6. Model fit to experimental photocurrent profiles. (a,b) Experimental (red) and fitted (black) profiles for the 2D–3D sample corresponding to a short and a long distance to the collection tip electrode. Dashed sections indicate experimental points disregarded for fitting. (c,d) The same for the 3D sample.

Source: E. Segura-Sanchis et al., Nanomaterials 13, 2570 (2023), CC BY 4.0.

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