Department of Chemistry, Purdue University, West Lafayette, IN 47907, USA.
National Renewable Energy Laboratory, 15013 Denver West Parkway, Golden, CO 80401, USA.
Science. 2017 Apr 7;356(6333):59-62. doi: 10.1126/science.aam7744.
The Shockley-Queisser limit for solar cell efficiency can be overcome if hot carriers can be harvested before they thermalize. Recently, carrier cooling time up to 100 picoseconds was observed in hybrid perovskites, but it is unclear whether these long-lived hot carriers can migrate long distance for efficient collection. We report direct visualization of hot-carrier migration in methylammonium lead iodide (CHNHPbI) thin films by ultrafast transient absorption microscopy, demonstrating three distinct transport regimes. Quasiballistic transport was observed to correlate with excess kinetic energy, resulting in up to 230 nanometers transport distance that could overcome grain boundaries. The nonequilibrium transport persisted over tens of picoseconds and ~600 nanometers before reaching the diffusive transport limit. These results suggest potential applications of hot-carrier devices based on hybrid perovskites.
如果可以在热载流子热化之前收集它们,那么太阳能电池效率的 Shockley-Queisser 限制就可以被突破。最近,在杂化钙钛矿中观察到载流子冷却时间长达 100 皮秒,但尚不清楚这些长寿命的热载流子是否可以长距离迁移以进行有效的收集。我们通过超快瞬态吸收显微镜报告了在碘化甲基铵(CHNHPbI)薄膜中热载流子迁移的直接可视化,证明了三种不同的输运机制。准弹道输运与过剩动能相关,从而实现了高达 230 纳米的传输距离,可以克服晶粒边界。在达到扩散输运极限之前,非平衡输运持续了数十个皮秒和~600 纳米。这些结果表明基于杂化钙钛矿的热载流子器件具有潜在的应用前景。