Jikun Yang, Meng-Jie Zhu, Hua-Yang Ru, Bo-han Yao, Meng‐En Sun, Manman He, Yani Yang, Qiu-Yang Wan, Qi Li, Meng Zhou, Gaosong Chen, Yuchen Wu, Lei Jiang, Shuang-quan ZANG
High-pressure reversibility is a predominant challenge restricting the practical application of hydrostatic pressure in high-pressure synthesis. Herein, we have successfully preserved the high-pressure metastable phase of an atomically precise chiral silver nanocluster {[ Ag 8 H( D / L -dtp) 6 (PPh 3 ) 2 ](CF 3 COO); ( D / L -Ag 8 )} with a high quantum yield (QY) under ambient conditions based on pressure-enhanced argentophilic interactions. D / L -dtp and PPh 3 represent ( D / L )- o, o ′-di[2-isopropyl-5-methylcyclohex-1-yl]dithiophosphoric acid and triphenylphosphine ligands, respectively. Initially, D / L -Ag 8 exhibits low-quality red circularly polarized luminescence (CPL). Under compression, D / L -Ag 8 presents a substantially enhanced piezoluminescence. At 2.3 GPa, the QY of D / L -Ag 8 is boosted from an initial 2.4% to a maximum of 70.5%. Notably, the pressure-amplified QY (21.5%) of D / L -Ag 8 is preserved even after the pressure is released. The single-crystal X-ray diffraction results reveal that the D / L -Ag 8 kernel comprises a seven-nucleus silver polyhedron ( Ag 7 ) and an independent silver atom (Ag8). High-pressure structural characterization and theoretical calculations demonstrate that pressure induces the contraction of interatomic distances, triggering additional argentophilic interactions between Ag 7 and Ag8. In situ high-pressure femtosecond transient absorption combined with Raman spectra further confirms that pressure-enhanced argentophilic interactions significantly suppress nonradiative energy dissipation caused by the disordered vibration of Ag atoms through strengthening the structural rigidity of the D / L -Ag 8 core. This is responsible for the enhancement of piezoluminescence and the pressure-trapped efficient QY of D / L -Ag 8 . Our work opens a novel avenue for preparing high-performance chiral materials via high pressure without changing the chemical composition.