Multicolour single-mode polarized microlasers with visible to near-infrared output have very important applications in photonic integration and multimodal biochemical sensing/imaging but are very difficult to realize. Here, we demonstrate a single crystal with multiple segments based on the host-guest metal-organic framework ZJU-68 hierarchically hybridized with different dye molecules generating controllable single-mode green, red, and near-infrared lasing, with the lasing mode mechanism revealed by computational simulation. The segmented and oriented assembly of different dye molecules within the ZJU-68 microcrystal causes it to act as a shortened resonator, enabling us to achieve dynamically controllable multicolour single-mode lasing with a low three-colour-lasing threshold of ~1.72 mJ/cm² (approximately seven times lower than that of state-of-the-art designed heterostructure alloys, as reported by Fan F et al. (Nat. Nanotechnol. 10:796–803, 2015) considering the single pulse energy density) and degree of polarization >99.9%. Furthermore, the resulting three-colour single-mode lasing possesses the largest wavelength coverage of ~186 nm (ranging from ~534 to ~720 nm) ever reported. These findings may open a new route to the exploitation of multicolour single-mode micro/nanolasers constructed by MOF engineering for photonic and biochemical applications.

具有可见光到近红外输出的多色单模偏振微型激光器在光子集成和多模态生化传感/成像方面具有非常重要的应用，但实现起来非常困难。在这里，我们展示了基于主客体金属有机框架ZJU-68的多片段单晶与不同染料分子分层杂化，产生可控的单模绿光、红光和近红外激光，并揭示了激光模式机制通过计算模拟。ZJU-68 微晶内不同染料分子的分段和定向组装使其充当缩短的谐振器，使我们能够实现动态可控的多色单模激光，三色激光阈值约为 1.72 mJ/cm ²（根据 Fan F 等人的报告（Nat. Nanotechnol. 10:796–803, 2015）考虑到单脉冲能量密度，比最先进设计的异质结构合金低约七倍）和程度偏振度>99.9%。此外，由此产生的三色单模激光具有有史以来报道的最大波长覆盖范围~186 nm（范围从~534到~720 nm）。这些发现可能为开发由 MOF 工程构建的多色单模微/纳米激光器用于光子和生化应用开辟一条新途径。