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摘要
0D organic-inorganic antimony halides have attracted increasing attention due to the non-toxicity, high stability, and superior photoluminescence quantum yield (PLQY). Here, a series of hybrid antimony chlorides with the same organic cation ethyltriphenylphosphonium (Ph3EtP+), including non-emissive (Ph3EtP)2Sb2Cl8 and nine (Ph3EtP)2SbCl5-based emissive compounds, are synthesized and characterized. These emissive compounds are namely, the guest-free (Ph3EtP)2SbCl5 and (Ph3EtP)2SbCl5 center dot guest (guest = glycol, acetic acid, methanol, ethanol, n-propanol, i-propanol, acetone, and acetonitrile). The solvent used can alter the coordination mode of Sb because the solvation effect affects the reactivity of the anions ([SbCl4]- and Cl-), leading to the formation of either A2Sb2Cl8 or A2SbCl5. The solvents can be even incorporated into the crystal structure, where stronger interaction with [SbCl5]2- leads to higher temperature of the escape of the solvent. The guest molecules could increase the structural rigidity of [SbCl5]2- via hydrogen bonding and dipole-dipole interactions, which tends to reduce the room-temperature photoluminescence (PL) Stokes shift and temperature-dependent PL shift by decreasing the [SbCl5]2- deformability, along with enhanced PLQY from 81% in guest-free to near-unity in (Ph3EtP)2SbCl5 center dot glycol. This work shows that targeted synthesis and diversified choices of solvents provide an efficient tool to generate steady variations in hybrid emissive materials for optoelectronics. @@@ Here, a family of hybrid antimony chlorides with the same organic cation is prepared. Solvation effect is used to demonstrate the difference between formation mechanisms of A2Sb2Cl8 and A2SbCl5. Eight solvents can be even incorporated to form A2SbCl5 center dot guest, exhibiting tunable optical properties, where stronger interaction between host and guest leads to reduced Stokes shift. image
