Real-time Characterization of Organizational Dynamics and Optical Properties of Ultrathin MAPbI₃ Films Deposited on Graphene via Molecular Beam Epitaxy under UHV Conditions
Christian Perest SONNY TSOTEZEM a, Aimeric OUVRARD a, Anouchah MOMENI a b, Abdelkarim OUERGHI c, Elena Magdalena STAICU CASAGRANDE a, Yimin GUAN a, Laurent GUILLEMOT a, Hocine KHEMLICHE a
a ISMO, Université Paris-Saclay, CNRS, 91405, Orsay, France
b CY Cergy Paris Université, 95000 Cergy, France
c C2N, Université Paris-Saclay, CNRS, 91405, Orsay, France
NIPHO25
Proceedings of International Conference on Perovskite Thin Film Photovoltaics and Perovskite Photonics and Optoelectronics (NIPHO25)
Cagliari, Italy, 2025 June 9th - 10th
Organizers: Giulia Grancini, Daniela Marongiu and Aldo Di Carlo
Oral, Christian Perest SONNY TSOTEZEM, presentation 030
Publication date: 24th April 2025

The production of halide perovskite layers under ultra-high vacuum (UHV) conditions, with real-time monitoring of their growth dynamics, is a promising way for addressing their longstanding instability issue. It is indeed expected that pristine layers, with high purity and near perfect crystalline order, represent an ideal playground for understanding the relative importance of intrinsic and extrinsic instabilities. For the vacuum deposition MAPbI3, the volatility of methylammonium iodide (MAI) represents a significant challenge in achieving the right stoichiometry. In our study, we emphasized the crucial role of lead iodide (PbI₂) flux in the process. Using molecular beam epitaxy (MBE), we achieved the controlled growth of MAPbI3 films on a graphene/SiC(0001) substrate; the growing layer is characterized in real time by correlating the optical properties and the growth dynamics.

To achieve the best control of the growth process, the growing layer is characterized in real-time by GIFAD (Grazing Incidence Fast Atom Diffraction), QMS (Quadrupole Mass Spectrometry), and SDRS (Surface Differential Reflectance Spectroscopy). In particular, GIFAD, a non-destructive technique provides fine information on the organization dynamics and can monitor the growth of the most fragile materials for hours without any damage [1]. SDRS yields information on the optical properties, which can then be correlated to the changes of the growing layer provided by GIFAD. GIFAD data reveal a layer-by-layer growth mode without evidence of crystallization in the early stage. SDRS measurements show the evolution of the optical features as a function of film thcikness. Notably, threee primary electronic transitions chracteristic of MAPbI3 are observed at approximately 375 nm, 480nm, and 760 nm.

[1] A. Momeni et al., J. Phys. Chem. Lett. 9, 908, 2018

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