Zeiske Stefan, Sandberg Oskar J, Zarrabi Nasim, Wolff Christian M, Raoufi Meysam, Peña-Camargo Francisco, Gutierrez-Partida Emilio, Meredith Paul, Stolterfoht Martin, Armin Ardalan
Sustainable Advanced Materials (Sêr-SAM), Department of Physics, Swansea University, Singleton Park, Swansea SA2 8PP, United Kingdom.
EPFL STI IEM PV-LAB, Rue de la Maladière 71b, CH-2002 Neuchâtel 2, Switzerland.
J Phys Chem Lett. 2022 Aug 11;13(31):7280-7285. doi: 10.1021/acs.jpclett.2c01652. Epub 2022 Aug 2.
In crystalline and amorphous semiconductors, the temperature-dependent Urbach energy can be determined from the inverse slope of the logarithm of the absorption spectrum and reflects the static and dynamic energetic disorder. Using recent advances in the sensitivity of photocurrent spectroscopy methods, we elucidate the temperature-dependent Urbach energy in lead halide perovskites containing different numbers of cation components. We find Urbach energies at room temperature to be 13.0 ± 1.0, 13.2 ± 1.0, and 13.5 ± 1.0 meV for single, double, and triple cation perovskite. Static, temperature-independent contributions to the Urbach energy are found to be as low as 5.1 ± 0.5, 4.7 ± 0.3, and 3.3 ± 0.9 meV for the same systems. Our results suggest that, at a low temperature, the dominant static disorder in perovskites is derived from zero-point phonon energy rather than structural disorder. This is unusual for solution-processed semiconductors but broadens the potential application of perovskites further to quantum electronics and devices.
在晶体和非晶半导体中,温度依赖的乌尔巴赫能量可以从吸收光谱对数的反斜率确定,并反映静态和动态能量无序。利用光电流光谱方法灵敏度的最新进展,我们阐明了含不同数量阳离子组分的卤化铅钙钛矿中温度依赖的乌尔巴赫能量。我们发现,对于单阳离子、双阳离子和三阳离子钙钛矿,室温下的乌尔巴赫能量分别为13.0±1.0、13.2±1.0和13.5±1.0毫电子伏特。对于相同体系,发现乌尔巴赫能量中与温度无关的静态贡献低至5.1±0.5、4.7±0.3和3.3±0.9毫电子伏特。我们的结果表明,在低温下,钙钛矿中主要的静态无序源自零点声子能量而非结构无序。这对于溶液处理的半导体来说是不寻常的,但进一步拓宽了钙钛矿在量子电子学和器件方面的潜在应用。