Tabassum Madeeha, Zia Qasim, Ye Huanqing, Neal William George, Aslam Sameen, Zhang Jinshuai, Su Lei
Key Laboratory of Advanced Materials and Nanotechnology, School of Engineering and Materials Science, Queen Mary, University of London, London E14NS, U.K.
NanoVision Centre for Structural and Chemical Analysis, School of Engineering and Materials Science, Queen Mary, University of London, London E14NS, U.K.
ACS Appl Electron Mater. 2024 Jan 4;6(1):550-558. doi: 10.1021/acsaelm.3c01542. eCollection 2024 Jan 23.
The past decade has seen a rapid development in metal halide perovskite nanocrystals (NCs), which has been witnessed by their potential applications in nanotechnology. The inimitable chemical nature behind their unique photoluminescence characteristics has attracted a growing body of researchers. However, the low intrinsic stability and surface defects of perovskite NCs have hampered their widespread applications. Therefore, numerous techniques such as doping and encapsulation (polymer matrices, silica coating, salt matrix, etc.) have been examined for the surface modification of perovskite NCs and to increase their efficiency and stability. In this study, we demonstrated the self-passivation method for surface defects by introducing potassium (K) or rubidium (Rb) during the colloidal fabrication of NCs, resulting in the much-improved crystallinity, photoluminescence, and improved radiative efficiency. In addition, K-doped NCs showed a long-term colloidal stability of more than 1 month, which indicates the strong bonding between the NCs and the smaller-sized potassium cations (K). We observed the enhancement of the radiative lifetime that can also be explained by the prevention of "Frenkel defects" when K stays at the interstitial site of the nanocrystal structure. Furthermore, our current findings signify the importance of surface modification techniques using alkali metal ions to reduce the surface traps of perovskite nanocrystals (PeNCs). Comparable developments could be applied to polycrystalline perovskite thin films to reduce the interface trap densities. The findings of this study have several important implications for future light-emitting applications.
在过去十年中,金属卤化物钙钛矿纳米晶体(NCs)发展迅速,其在纳米技术中的潜在应用就是明证。其独特光致发光特性背后独特的化学性质吸引了越来越多的研究人员。然而,钙钛矿纳米晶体固有的低稳定性和表面缺陷阻碍了它们的广泛应用。因此,人们研究了许多技术,如掺杂和封装(聚合物基质、二氧化硅涂层、盐基质等),用于钙钛矿纳米晶体的表面改性,以提高其效率和稳定性。在本研究中,我们展示了一种自钝化表面缺陷的方法,即在纳米晶体的胶体制备过程中引入钾(K)或铷(Rb),从而显著提高了结晶度、光致发光和辐射效率。此外,K掺杂的纳米晶体表现出超过1个月的长期胶体稳定性,这表明纳米晶体与较小尺寸的钾阳离子(K)之间有很强的键合。我们观察到辐射寿命的延长,这也可以通过K位于纳米晶体结构的间隙位置时防止“弗伦克尔缺陷”来解释。此外,我们目前的研究结果表明了使用碱金属离子进行表面改性技术对减少钙钛矿纳米晶体(PeNCs)表面陷阱的重要性。类似的进展可应用于多晶钙钛矿薄膜,以降低界面陷阱密度。本研究结果对未来的发光应用具有几个重要意义。