Gatto Lorenzo, Poli Isabella, Meggiolaro Daniele, Grandi Federico, Folpini Giulia, Treglia Antonella, Cinquanta Eugenio, Petrozza Annamaria, De Angelis Filippo, Vozzi Caterina
Istituto di Fotonica e Nanotecnologie-CNR (CNR-IFN), Milano 20133, Italy.
Center for Sustainable Future Technologies@Polito, Istituto Italiano di Tecnologia, via Livorno 60, Torino 10144, Italy.
ACS Energy Lett. 2025 Feb 25;10(3):1382-1388. doi: 10.1021/acsenergylett.4c02558. eCollection 2025 Mar 14.
Tin halide perovskites are promising materials to replace lead-based materials for perovskite optoelectronics, yet their performance is limited by their high self-p-doping. To quantify the impact of p-doping on carrier dynamics, we combine terahertz spectroscopy and density functional theory calculations to investigate the coupling of charge carriers to the lattice in prototypical tin-based perovskites. Doping is shown to influence the charge-phonon interactions significantly. We identify the formation of polarons at doping densities below 10 cm, while a Drude-like response is found for photogenerated carriers at higher charge density, confirming that for highly p-doped systems, the terahertz response is dominated by quasi-free charge carriers. Our study suggests that charge-phonon coupling could serve as a proxy for the self-p-doping level, offering additional insights into fundamental charge-transport properties of tin halide perovskites and their potential optimization for photovoltaic applications.
卤化锡钙钛矿是有望替代用于钙钛矿光电器件的铅基材料的材料,但其性能受到高自p型掺杂的限制。为了量化p型掺杂对载流子动力学的影响,我们结合太赫兹光谱和密度泛函理论计算,研究典型锡基钙钛矿中电荷载流子与晶格的耦合。结果表明,掺杂会显著影响电荷-声子相互作用。我们发现在掺杂密度低于10 cm时会形成极化子,而在较高电荷密度下光生载流子呈现出类似德鲁德的响应,这证实了对于高p型掺杂体系,太赫兹响应主要由准自由电荷载流子主导。我们的研究表明,电荷-声子耦合可以作为自p型掺杂水平的一个指标,为卤化锡钙钛矿的基本电荷传输特性及其在光伏应用中的潜在优化提供更多见解。