TY - JOUR
T1 - Computation-assisted design of stable quasi-2D organic sulfate perovskite NIR light-emitting diodes
AU - Jana, Atanu
AU - Sree, Vijaya Gopalan
AU - Ba, Qiankai
AU - Lee, Chi Ho
AU - Das, Deblina
AU - Meena, Abhishek
AU - Mal, Sourav
AU - Lee, Sang Uck
AU - Cho, Sangeun
N1 - Publisher Copyright:
© 2025 The Author(s).
PY - 2025/11/19
Y1 - 2025/11/19
N2 - Quasi-two-dimensional (2D) perovskite light-emitting diodes (PeLEDs) exhibit high red-emission efficiency but poor stability due to defect-mediated recombination and ion migration in hybrid perovskite nanocrystals (NCs). Here, we present a solvent-free mechanochemical synthesis of red-emitting quasi-2D (OA)2(MA)2Pb2I8(PbSO4) NCs using dioctylammonium sulfate (DOS), guided by first-principles calculations. The DOS ligand promotes PbSO4 layer formation, which passivates defects, suppresses ion migration, and enhances humidity resistance. Unlike iodide-based octylammonium iodide (OAI) devices that degrade rapidly and emit only at 763 nm, DOS-stabilized PeLEDs show dual emission at 651 and 763 nm, indicating improved phase stability. The devices achieve a peak luminance of 7,039 cd/cm2 and an external quantum efficiency of 9.76%, retaining over 60% of initial EQE after 100 days, markedly outperforming conventional OAI-MAPbI3 PeLEDs (<20%). These results demonstrate that sulfate passivation provides a simple and scalable route to robust, durable red-emitting quasi-2D PeLEDs, offering a promising strategy for high-performance optoelectronic devices.
AB - Quasi-two-dimensional (2D) perovskite light-emitting diodes (PeLEDs) exhibit high red-emission efficiency but poor stability due to defect-mediated recombination and ion migration in hybrid perovskite nanocrystals (NCs). Here, we present a solvent-free mechanochemical synthesis of red-emitting quasi-2D (OA)2(MA)2Pb2I8(PbSO4) NCs using dioctylammonium sulfate (DOS), guided by first-principles calculations. The DOS ligand promotes PbSO4 layer formation, which passivates defects, suppresses ion migration, and enhances humidity resistance. Unlike iodide-based octylammonium iodide (OAI) devices that degrade rapidly and emit only at 763 nm, DOS-stabilized PeLEDs show dual emission at 651 and 763 nm, indicating improved phase stability. The devices achieve a peak luminance of 7,039 cd/cm2 and an external quantum efficiency of 9.76%, retaining over 60% of initial EQE after 100 days, markedly outperforming conventional OAI-MAPbI3 PeLEDs (<20%). These results demonstrate that sulfate passivation provides a simple and scalable route to robust, durable red-emitting quasi-2D PeLEDs, offering a promising strategy for high-performance optoelectronic devices.
KW - defect passivation
KW - density functional theory
KW - ion migration
KW - organic-inorganic hybrid perovskite
KW - quasi-2D red light-emitting perovskite
KW - red light-emitting diodes
KW - solid-state synthesis
KW - sulfate ion passivation
UR - https://www.scopus.com/pages/publications/105022104215
U2 - 10.1016/j.xcrp.2025.102907
DO - 10.1016/j.xcrp.2025.102907
M3 - Article
AN - SCOPUS:105022104215
SN - 2666-3864
VL - 6
JO - Cell Reports Physical Science
JF - Cell Reports Physical Science
IS - 11
M1 - 102907
ER -