Kuruppu Udara M, Rahman Mohammad A, Gangishetty Mahesh K
Department of Chemistry, Mississippi State University, Mississippi State, Mississippi 39762, United States.
Department of Physics and Astronomy, Mississippi State University, Mississippi State, Mississippi 39762, United States.
ACS Nano. 2024 Jan 16;18(2):1647-1657. doi: 10.1021/acsnano.3c09824. Epub 2024 Jan 3.
Lead-free low-dimensional copper-based metal halides are promising luminescent materials for broadband LEDs owing to their broad self-trapped exciton (STE) emission. However, recently, in 1D CsCuI, a discrepancy between their electroluminescence (EL) and photoluminescence (PL) has been observed. As a result, the overall output color from LEDs is significantly different than the anticipated emission. To unveil the origin of this discrepancy, here, we provide comprehensive analyses and show that the shift in the EL is caused neither by any structural/optical interactions between CsCuI and electron transport layers (ETL) nor by the degradation of 1D CsCuI. Instead, it depends on the carrier imbalance on CsCuI, mainly due to the difference in the electron mobility of the ETLs and the electron density on the CsCuI layer. By varying the ETLs, different colored 1D CsCuI LEDs with peaks at 556, 590, and 647 nm are fabricated, and a maximum luminance of over 2000 cd/m is achieved for a 556 nm LED. Further, by limiting the electron mobility and injection to 1D CsCuI using an insulating LiF layer at the CsCuI/ETL interface, more red-shifted LEDs are achieved confirming the critical role of electron density on the EL characteristics of 1D CsCuI.
无铅低维铜基金属卤化物因其宽泛的自陷激子(STE)发射而成为宽带发光二极管(LED)颇具前景的发光材料。然而,最近在一维CsCuI中,观察到了其电致发光(EL)和光致发光(PL)之间的差异。结果,LED的整体输出颜色与预期发射有显著不同。为了揭示这种差异的根源,在此我们进行了全面分析并表明,EL的偏移既不是由CsCuI与电子传输层(ETL)之间的任何结构/光学相互作用引起的,也不是由一维CsCuI的降解引起的。相反,它取决于CsCuI上的载流子失衡,主要是由于ETL的电子迁移率与CsCuI层上的电子密度不同。通过改变ETL,制备出了峰值分别位于556、590和647 nm的不同颜色的一维CsCuI LED,并且556 nm的LED实现了超过2000 cd/m²的最大亮度。此外,通过在CsCuI/ETL界面使用绝缘LiF层来限制电子向一维CsCuI的迁移率和注入,实现了更多红移的LED,证实了电子密度对一维CsCuI的EL特性的关键作用。