Lin Na, Xiao Li, Wu Yishi, Wu Yi-Fan, Li Zi-Xian, Yan Tian-Yu, Chen Zhi-Wei, Yue Cheng-Yang, Yan Dongpeng, Lei Xiao-Wu
Research institute of Optoelectronic Functional Materials, School of Chemistry, Chemical Engineering and Materials, Jining University, Qufu, Shandong, 273155, P. R. China.
School of Chemistry and Chemical Engineering, Qufu Normal University, Qufu, Shandong, 273165, P. R. China.
Adv Mater. 2025 Aug 14:e01560. doi: 10.1002/adma.202501560.
Excitation- and temperature-dependent multicolor luminescent materials are valuable in advanced optoelectronic devices while they haven't been realized in 2D metal halides owing to the restrictions of Kasha's rule. Herein, we reported a novel 2D lead-free halide of (AMP)CuBr (AMP = N-aminomorpholine) through structural engineering, in which the [CuBr] layer is composed of corner- and edge-shared [CuBr] tetrahedron. The non-centrosymmetric structure enables (AMP)CuBr to exhibit an impressive second-harmonic generation signal of ≈0.8 times that of KHPO (KDP). Remarkably, (AMP)CuBr possesses two independent self-trapped exciton-emitting states under different excitation energies, which display multicolor luminescence outputs from blue, white, to orange with near-unity photoluminescence quantum yields (PLQYs). Additionally, the luminescence can be regulated in a wide temperature range of 300-400 K due to reversible energy transfer between two emitting bands, acting as a luminescence ratio thermometer with a ultrahigh relative thermal sensitivity of 56.755% K. High PLQY and large Stokes shift further endow (AMP)CuBr strong radioluminescence with an ultrahigh light yield of 92,400 photons·MeV, low detection limit of 121 nGy·s and a short afterglow of 0.41 ms. The abundant photophysical properties highlight the multiple optoelectronic applications of 2D cuprous halide in white light-emitting, laser technology, flexible temperature sensors, and X-ray imaging.
激发和温度依赖的多色发光材料在先进光电器件中具有重要价值,但由于卡莎规则的限制,二维金属卤化物尚未实现这一特性。在此,我们通过结构工程报道了一种新型的二维无铅卤化物(AMP)CuBr(AMP = N-氨基吗啉),其中[CuBr]层由角共享和边共享的[CuBr]四面体组成。非中心对称结构使(AMP)CuBr表现出令人印象深刻的二次谐波产生信号,约为KHPO(KDP)的0.8倍。值得注意的是,(AMP)CuBr在不同激发能量下具有两个独立的自陷激子发射态,呈现出从蓝色、白色到橙色的多色发光输出,光致发光量子产率(PLQY)接近100%。此外,由于两个发射带之间的可逆能量转移,发光可以在300-400 K的宽温度范围内调节,作为一种发光比率温度计,具有56.755% K的超高相对热灵敏度。高PLQY和大斯托克斯位移进一步赋予(AMP)CuBr强的辐射发光,具有92400光子·MeV的超高光产率、121 nGy·s的低检测限和0.41 ms的短余辉。丰富的光物理性质突出了二维卤化亚铜在白光发射、激光技术、柔性温度传感器和X射线成像等多种光电器件中的应用潜力。