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Lanthanide metal–organic frameworks are of great interest in the development of photoluminescence (PL) materials owing to their structural tunability and intrinsic features of lanthanide elements. However, there exists some limitations arising from poor matching with metal ions, thereby exhibiting a weak ligand‐to‐metal energy transfer (LMET) process. Here we demonstrate a pressure‐treated strategy for achieving high PL performance in green‐emitting Tb(BTC)(H2O)6. The PL quantum yield of pressure‐treated sample increased from 50.6 % to 90.4 %. We found that the enhanced hydrogen bonds locked the conjugated configuration formed by two planes of carboxyl group and benzene ring, enabling the promoted intersystem crossing to effectively drive LMET. Moreover, the optimized singlet and triplet states also validated the facilitated LMET process. This work opens the opportunity of structure optimization to improve PL performance in MOFs by pressure‐treated engineering. [ABSTRACT FROM AUTHOR]

Lanthanide metal–organic frameworks are of great interest in the development of photoluminescence (PL) materials owing to their structural tunability and intrinsic features of lanthanide elements. However, there exists some limitations arising from poor matching with metal ions, thereby exhibiting a weak ligand‐to‐metal energy transfer (LMET) process. Here we demonstrate a pressure‐treated strategy for achieving high PL performance in green‐emitting Tb(BTC)(H2O)6. The PL quantum yield of pressure‐treated sample increased from 50.6 % to 90.4 %. We found that the enhanced hydrogen bonds locked the conjugated configuration formed by two planes of carboxyl group and benzene ring, enabling the promoted intersystem crossing to effectively drive LMET. Moreover, the optimized singlet and triplet states also validated the facilitated LMET process. This work opens the opportunity of structure optimization to improve PL performance in MOFs by pressure‐treated engineering. [ABSTRACT FROM AUTHOR]