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Two-dimensional (2D) layered hybrid perovskites provide an ideal platform forstudying the properties of excitons. Here, we report on a strongtriplet-exciton and longitudinal-optical (LO) phonon coupling in 2D(C6H5CH2CH2NH3, PEA)2PbBr4 perovskites. The triplet excitons exhibit strongphotoluminescence (PL) in thick perovskite microflakes, and the PL is notdetectable for monolayer microflakes. The coupling strength of the tripletexciton-LO phonon is approximately two to three times greater than that of thesinglet exciton-LO phonon with a LO phonon energy of about 21 meV. Thisdifference might due to the different locations of singlet excitons located inthe well and triplet excitons located in the barrier in the 2D layeredperovskite. Revealing the strong coupling of triplet exciton-LO phonon providesa fundamental understanding of many-body interaction in hybrid perovskites,which is useful to develop and optimize the optoelectronic devices based on 2Dperovskites in the future.

Strong Triplet-Exciton-LO-Phonon Coupling in Two-Dimensional Layered Organic-Inorganic Hybrid Perovskite Single Crystal Microflakes