Hybrid organic-inorganic halide perovskites, such as methylammonium lead iodide (CH3NH3PbI3) have emerged as potential hot-carrier (HC) solar cell materials. Recently, 2D/Layered perovskites with alternating organic and inorganic atomic layers have gained significant attention owing to enhanced ambient stability, high luminescence quantum yield, ultrafast spin relaxation via exchange interaction and strong excitonic effects. Although carrier-phonon interactions in 3D analogs of hybrid perovskites are widely investigated, the differences between electron and hole scattering processes are still poorly understood for the layered perovskites. We have shown that extreme ultraviolet (XUV) spectroscopy in the 40 to 80 eV energy range measures Iodine 4d → 5p transitions and provides separate signals for valence band and conduction band dynamics. We use this technique to measure the carrier cooling rate in prototypical single-layer perovskite systems, (PEA)2PbI4 (PEA = phenethylammonium) and (NBA)2PbI4 (NBA = n-butylammonium) after visible light excitation. The tabletop instrument uses high-harmonic generation to produce 15 femtosecond XUV probe pulses, enabling us to observe both carrier cooling and carrier specific dynamics on the femtosecond to picosecond time scales.

Understanding carrier specific dynamics in 2D layered lead halide perovskites by femtosecond tabletop extreme ultraviolet spectroscopy

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.