Although high-entropy materials are excellent candidates for a range of functional materials, their formation traditionally requires high-temperature synthetic procedures of over 1,000 °C and complex processing techniques such as hot rolling^1,2,3,4,5. One route to address the extreme synthetic requirements for high-entropy materials should involve the design of crystal structures with ionic bonding networks and low cohesive energies. Here we develop room-temperature-solution (20 °C) and low-temperature-solution (80 °C) synthesis procedures for a new class of metal halide perovskite high-entropy semiconductor (HES) single crystals. Due to the soft, ionic lattice nature of metal halide perovskites, these HES single crystals are designed on the cubic Cs₂MCl₆ (M=Zr⁴⁺, Sn⁴⁺, Te⁴⁺, Hf⁴⁺, Re⁴⁺, Os⁴⁺, Ir⁴⁺ or Pt⁴⁺) vacancy-ordered double-perovskite structure from the self-assembly of stabilized complexes in multi-element inks, namely free Cs⁺ cations and five or six different isolated [MCl₆]^2– anionic octahedral molecules well-mixed in strong hydrochloric acid. The resulting single-phase single crystals span two HES families of five and six elements occupying the M-site as a random alloy in near-equimolar ratios, with the overall Cs₂MCl₆ crystal structure and stoichiometry maintained. The incorporation of various [MCl₆]^2– octahedral molecular orbitals disordered across high-entropy five- and six-element Cs₂MCl₆ single crystals produces complex vibrational and electronic structures with energy transfer interactions between the confined exciton states of the five or six different isolated octahedral molecules.

尽管高熵材料是一系列功能材料的优秀候选者，但其形成传统上需要超过 1,000 °C 的高温合成程序和复杂的加工技术，例如热轧^1,2,3,4,5。解决高熵材料极端合成要求的一种途径应涉及设计具有离子键网络和低内聚能的晶体结构。在这里，我们开发了新型金属卤化物钙钛矿高熵半导体（HES）单晶的室温溶液（20°C）和低温溶液（80°C）合成程序。由于金属卤化物钙钛矿的软离子晶格性质，这些 HES 单晶设计在立方 Cs ₂ MCl ₆ (M=Zr ⁴⁺ , Sn ⁴⁺ , Te ⁴⁺ , Hf ⁴⁺ , Re ⁴⁺ , Os ⁴⁺、Ir ⁴⁺或 Pt ⁴⁺ ) 空位有序双钙钛矿结构，来自多元素油墨中稳定配合物的自组装，即游离 Cs ⁺阳离子和五种或六种不同的孤立的 [MCl ₆ ] ^2–阴离子八面体分子在强盐酸中充分混合。所得单相单晶跨越两个由五种和六种元素组成的 HES 族，以接近等摩尔比的形式占据 M 位点，并保持整体 Cs 2 MCl 6_晶体结构_和化学计量。在高熵五元和六元 Cs ₂ MCl ₆单晶中掺入各种无序的 [MCl ₆ ] ^2–八面体分子轨道，产生复杂的振动和电子结构，并在五元或六元的受限激子态之间产生能量转移相互作用。不同的孤立八面体分子。