or noble transition metals, pure organic systems with RTP have received considerable achievements recently. [3] Generally, the lifetime and quantum efficiency are difficult to exceed 10 ms and 20% for pure organic materials because their intersystem crossing (ISC) is inherently inefficient and the active triplet state is readily exhausted through nonradiative relaxation. [4] To address this issue, most efforts have been focused on designing organic RTP molecules with ultralong lifetime and/or higher quantum efficiency. [5] For instance, phosphorescence with lifetime long as 2.81 s and efficiency high to 76% has been recently obtained from a phosphor monomer by polymerization and complexation synergistic enhancement. [5a] In addition, the modulation of phosphorescence color of RTP materials has also attracted enormous attention very recently. [6] A series of host-guest phosphors with color variation from cyan (502 nm) to orange-red (608 nm) have been achieved by modulating different chromophore guests. [6a] Notably, compared with the multicolor phosphorescence realized by multiple components, single-component phosphors with tunable RTP colors are extremely attractive because of their potential superiorities in simple fabrication and device stability for practical applications. [7] However, it is well known that the observed emission is generally determined by the lowest excited state according to Kasha's rule, thus it is extremely difficult to achieve multicolor RTP from single-component materials. Actually, only scattered examples were reported on multicolor single-component RTP, in which feasible strategies were tried including construction of chromophores in isolated or aggregated states, multichromophore crosslinked copolymerization, and cluster-induced emission (CIE). [8] A single-component RTP material with dynamic color tuning from violet to green, for instance, was first reported by mixing molecular phosphorescence and H-aggregation phosphorescence. [8a] Analogous colortunable RTP from blue to yellow was achieved through incorporating two organic phosphorescence emitting centers into one polymer. [8e] Nonetheless, the color switching is relatively limited or saltatory in most reported single-component multicolor RTP (Table S1, Supporting Information), it remains highly Tunable full-color room temperature phosphorescence (RTP) is charming due to its potentials in multiple anticounterfeitings, all-color displays, and multichannel biomarkers. However, it is a huge challenge to achieve excitationdependent continuously adjustable full-color RTP from a single-component compound. Herein, two Zn(II)-based organic coordination polymers are reported, which are the first examples characterized by blue, cyan, green, yellow, orange, and red continuously tunable phosphorescence with decent quantum efficiencies in response to variation of excitation energy at ambient conditions. The unique photoluminescence behavior is induced by the selective formation and decay of multiple triplet excited states, i.e., ligand...

More and more attention has been paid to the important roles of external fields in controlled radical polymerization (CRP). However, their essential roles have not been studied thoroughly yet, which hinders the in‐depth understanding of the mechanism and kinetics. Herein, a strategy combining quantum chemical calculations (QCC) and kinetic modeling was adopted to identify the essential roles of light and ultrasonication in the dual‐stimuli regulated bulk atom transfer radical polymerization (ATRP). At the molecular level, the impact of light on Cu‐catalyzed ATRP was investigated. The CuIIBr/Me6TREN has high absorbance at an experimental wavelength of 365 nm (main excitation S0 → D7 accounts for 84.93%). Electron transfer reactions involving Me6TREN are more favorable paths for photochemical reactions, and the mechanism of the copper activation/deactivation pathway is inner sphere electron transfer. At the micro‐scale, a kinetic model based on the method of moment was established with a “series” encounter pair model to consider the influence of ultrasound on diffusional limitation. Simulation results show that the changes of the reaction rate coefficients ka, kda, and kt at high conversion reflect the degree of diffusional limitation by ultrasound. The multiscale modeling strategy applied in this study identifies the essential roles of photo and ultrasonication in dual‐stimuli regulated model systems, which can be extended to other external‐field regulated CRP to improve the mechanistic understanding.