Molecular emitters that combine circularly polarized luminescence (CPL) and high radiative rate constants of the triplet exciton decay are highly attractive for electroluminescent devices (OLEDs) or next-generation photonic applications, such as spintronics, quantum computing, cryptography, or sensors. However, the design of such emitters is a major challenge because the criteria for enhancing these two properties are mutually exclusive. In this contribution, we show that enantiomerically pure {Cu(Cbz^R)[(S/R)-BINAP]} [R = H (1), 3,6-tBu (2)] are efficient thermally activated delayed fluorescence (TADF) emitters with high radiative rate constants of k_TADF up to 3.1 × 10⁵ s^-1 from ^1/3LLCT states according to our temperature-dependent time-resolved luminescence studies. The efficiency of the TADF process and emission wavelengths are highly sensitive to environmental hydrogen bonding of the ligands, which can be disrupted by grinding of the crystalline materials. The origin of this pronounced mechano-stimulus photophysical behavior is a thermal equilibrium between the ^1/3LLCT states and a ³LC state of the BINAP ligand, which depends on the relative energetic order of the excited states and is prone to inter-ligand C-H···π interactions. The copper(I) complexes are also efficient CPL emitters displaying exceptional dissymmetry values g_lum of up to ±0.6 × 10^-2 in THF solution and ±2.1 × 10^-2 in the solid state. Importantly for application in electroluminescence devices, the C-H···π interactions can also be disrupted by employing sterically bulky matrices. Accordingly, we have investigated various matrix materials for successful implementation of the chiral copper(I) TADF emitters in proof-of-concept CP-OLEDs.

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