Publication date: 11th March 2026
Surface and interface-related defects are widely recognized as one of the main factors hindering efficient charge transport and long-term operational stability in metal halide perovskite single crystals. In this work, we address these challenges through a simple yet effective 2D/3D interface engineering approach, where MAPbBr3 single crystals are passivated using an ultrathin layer of phenethylammonium lead bromide (PEA2PbBr4). Structural characterization confirms that the intrinsic crystal structure and bulk stoichiometry of MAPbBr3 remain unaffected after passivation, while the surface exhibits a uniform, slightly roughened morphology without cracks or phase segregation, indicative of a 2D perovskite overlayer. Energy-dispersive X-ray spectroscopy (EDS) reveals a pronounced presence of carbon element accompanied by reduced Pb and Br contributions, consistent with an organic compound-based surface layer. Raman spectroscopy further confirms successful 2D passivation through the emergence of pronounced aromatic vibrational modes of the phenethylammonium cation, including C–C/C=C stretches (~1400–1600 cm⁻¹, phenyl ring), CH₂ twist/wag (~1255 cm⁻¹), phenyl-ring breathing (~1000 cm⁻¹), and aromatic C–H bending/CH₃ wag (~910–970 cm⁻¹). Optical measurements show enhanced steady-state photoluminescence intensity and a reduced fast decay component in time-resolved photoluminescence (TRPL) for the 2D-passivated MAPbBr3, indicating suppressed non-radiative recombination and prolonged carrier lifetimes.
Electrical measurements further highlight the positive impact of the 2D passivation layer on interfacial charge transport. Current-voltage and capacitance-voltage analysis reveal more efficient charge extraction and a reduced tendency for charge accumulation at the interface in the 2D/3D heterostructure. Electrochemical impedance spectroscopy shows decreased charge transfer and recombination resistances, along with suppressed ionic migration, with clear trends under varying temperature, applied bias, and illumination conditions following 2D passivation. These results indicate improved interfacial electronic quality and more stable ion-electron interactions in the passivated system. Taken together, these findings establish PEA2PbBr4 surface passivation as a robust strategy for simultaneously enhancing optical response and electrical transport in MAPbBr3 single crystals, underscoring the promise of 2D/3D perovskite heterostructures for reliable, high-performance photovoltaic and other optoelectronic applications.
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