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Revealing Ultrafast Charge-Carrier Thermalization in Tin-Iodide Perovskites through Novel Pump–Push–Probe Terahertz Spectroscopy
ACS Photonics ( IF 6.5 ) Pub Date : 2021-08-08 , DOI: 10.1021/acsphotonics.1c00763 Aleksander M Ulatowski 1 , Michael D Farrar 1 , Henry J Snaith 1 , Michael B Johnston 1 , Laura M Herz 1
ACS Photonics ( IF 6.5 ) Pub Date : 2021-08-08 , DOI: 10.1021/acsphotonics.1c00763 Aleksander M Ulatowski 1 , Michael D Farrar 1 , Henry J Snaith 1 , Michael B Johnston 1 , Laura M Herz 1
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Tin-iodide perovskites are an important group of semiconductors for photovoltaic applications, promising higher intrinsic charge-carrier mobilities and lower toxicity than their lead-based counterparts. Controllable tin vacancy formation and the ensuing hole doping provide interesting opportunities to investigate dynamic intraband transitions of charge carriers in these materials. Here, we present for the first time an experimental implementation of a novel Optical-Pump–IR-Push–THz-Probe spectroscopic technique and demonstrate its suitability to investigate the intraband relaxation dynamics of charge carriers brought into nonequilibrium by an infrared “push” pulse. We observe a push-induced decrease of terahertz conductivity for both chemically- and photodoped FA0.83Cs0.17SnI3 thin films and show that these effects derive from stimulated THz emission. We use this technique to reveal that newly photogenerated charge carriers relax within the bands of FA0.83Cs0.17SnI3 on a subpicosecond time scale when a large, already fully thermalized (cold) population of charge-carriers is present. Such rapid dissipation of the initial charge-carrier energy suggests that the propensity of tin halide perovskites toward unintentional self-doping resulting from tin vacancy formation makes these materials less suited to implementation in hot-carrier solar cells than their lead-based counterparts.
中文翻译：
通过新型泵-推-探针太赫兹光谱揭示碘化锡钙钛矿中的超快载流子热化
碘化锡钙钛矿是一组重要的用于光伏应用的半导体，与铅基对应物相比，具有更高的内在电荷载流子迁移率和更低的毒性。可控的锡空位形成和随之而来的空穴掺杂为研究这些材料中电荷载流子的动态带内跃迁提供了有趣的机会。在这里，我们首次展示了一种新型光泵-IR-Push-THz-Probe 光谱技术的实验实现，并证明其适用于研究通过红外“推动”脉冲进入非平衡状态的电荷载流子的带内弛豫动力学. 我们观察到化学掺杂和光掺杂 FA 0.83 Cs 0.17 SnI的太赫兹电导率的推动性降低3薄膜并表明这些效应源自受激太赫兹发射。我们使用这种技术来揭示当存在大量已经完全热化（冷）的载流子时，新的光生载流子在 FA 0.83 Cs 0.17 SnI 3的带内在亚皮秒时间尺度内弛豫。初始电荷载流子能量的这种快速消散表明，卤化锡钙钛矿倾向于由锡空位形成导致的无意自掺杂，使得这些材料比铅基材料更不适合在热载流子太阳能电池中实施。
更新日期：2021-08-19
中文翻译：
通过新型泵-推-探针太赫兹光谱揭示碘化锡钙钛矿中的超快载流子热化
碘化锡钙钛矿是一组重要的用于光伏应用的半导体，与铅基对应物相比，具有更高的内在电荷载流子迁移率和更低的毒性。可控的锡空位形成和随之而来的空穴掺杂为研究这些材料中电荷载流子的动态带内跃迁提供了有趣的机会。在这里，我们首次展示了一种新型光泵-IR-Push-THz-Probe 光谱技术的实验实现，并证明其适用于研究通过红外“推动”脉冲进入非平衡状态的电荷载流子的带内弛豫动力学. 我们观察到化学掺杂和光掺杂 FA 0.83 Cs 0.17 SnI的太赫兹电导率的推动性降低3薄膜并表明这些效应源自受激太赫兹发射。我们使用这种技术来揭示当存在大量已经完全热化（冷）的载流子时，新的光生载流子在 FA 0.83 Cs 0.17 SnI 3的带内在亚皮秒时间尺度内弛豫。初始电荷载流子能量的这种快速消散表明，卤化锡钙钛矿倾向于由锡空位形成导致的无意自掺杂，使得这些材料比铅基材料更不适合在热载流子太阳能电池中实施。
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