Carrier relaxation and exciton dynamics in chemical-vapor-deposited two-dimensional hybrid halide perovskites†

IF 5.7 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Dallar Babaian, Daniel Hill, Ping Yu and Suchismita Guha
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Abstract

Chemical vapor deposition (CVD), without the use of any solvents, is a viable option for the growth of high-quality two-dimensional (2D) Ruddlesden–Popper-type hybrid halide perovskite films. Insights into carrier relaxation and exciton dynamics are crucial for the application of such 2D perovskite films in optoelectronics. By employing broadband transient absorption (TA) spectroscopy and time-resolved photoluminescence, we compare the carrier relaxation and exciton dynamics in two prototypical 2D lead-iodide perovskite systems with butylammonium (BA) and phenylethylammonium (PEA) cations grown by CVD. Along with neat 2D perovskite films, heterojunctions with tin oxide layers were also investigated. The TA peaks show differences in the lifetime and evolution between the two perovskite films and their heterojunction counterparts, providing valuable insights into the structural disparities between these perovskites and the underlying factors governing excitonic dynamics. The TA peak at 530 nm decays faster in PEA2PbI4 compared with BA2PbI4 highlighting the role of the organic cation and the polaronic nature of this peak. Fast carrier cooling times of 150 fs, signaling the absence of any phonon bottleneck effect, are observed. The decay dynamics of the band-edge bleach reveal a strong contribution from the Auger recombination process at early times, when the system is far from equilibrium.

Abstract Image

化学气相沉积二维杂化卤化物钙钛矿中的载流子弛豫和激子动力学
化学气相沉积(CVD),不使用任何溶剂,是高质量的二维(2D) ruddlesden - popper型杂化卤化物钙钛矿薄膜生长的可行选择。深入了解载流子弛豫和激子动力学对于这种二维钙钛矿薄膜在光电子学中的应用至关重要。利用宽带瞬态吸收(TA)光谱和时间分辨光致发光技术,我们比较了CVD生长的两种典型2D碘化铅钙钛矿体系中丁铵(BA)和苯乙铵(PEA)阳离子的载流子弛豫和激子动力学。除了整洁的二维钙钛矿薄膜外,还研究了与氧化锡层的异质结。TA峰显示了两种钙钛矿薄膜及其异质结薄膜之间的寿命和进化差异,为这些钙钛矿之间的结构差异和控制激子动力学的潜在因素提供了有价值的见解。与BA2PbI4相比,PEA2PbI4在530 nm处的TA峰衰减更快,这突出了有机阳离子的作用和该峰的极化性质。观察到150 fs的快速载流子冷却时间,表明没有任何声子瓶颈效应。带边漂白剂的衰变动力学表明,在系统远离平衡状态的早期,俄歇复合过程对漂白剂的衰变有很大贡献。
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来源期刊
Journal of Materials Chemistry C
Journal of Materials Chemistry C MATERIALS SCIENCE, MULTIDISCIPLINARY-PHYSICS, APPLIED
CiteScore
10.80
自引率
6.20%
发文量
1468
期刊介绍: The Journal of Materials Chemistry is divided into three distinct sections, A, B, and C, each catering to specific applications of the materials under study: Journal of Materials Chemistry A focuses primarily on materials intended for applications in energy and sustainability. Journal of Materials Chemistry B specializes in materials designed for applications in biology and medicine. Journal of Materials Chemistry C is dedicated to materials suitable for applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry C are listed below. This list is neither exhaustive nor exclusive. Bioelectronics Conductors Detectors Dielectrics Displays Ferroelectrics Lasers LEDs Lighting Liquid crystals Memory Metamaterials Multiferroics Photonics Photovoltaics Semiconductors Sensors Single molecule conductors Spintronics Superconductors Thermoelectrics Topological insulators Transistors
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