AI 中文总结
本研究针对卤化物钙钛矿机械化学研磨的核心问题，提出利用机械能作为合成变量调控相选择、实现亚稳态可编程的思路，为该领域从经验性方法转向预测性科学奠定基础。
AI 中文摘要
机械化学研磨被视为一种可规模化、无溶剂的方法，可制备溶液加工无法得到的卤化物钙钛矿。不过，其更深层的潜力在于，机械力有望成为合成控制的新维度，将研磨从经验性方法转变为预测性科学。卤化物钙钛矿是实现这一目标的理想平台：其软晶格和低形成能使其对机械激活具有固有响应性。要实现这一点，需要明确研磨实际生成了什么以及如何生成：研磨得到的相能否真正被捕获在非平衡态，还是仅为获取平衡相的便捷途径，以及其原子级作用路径是什么？这些问题大多基于假设，而用于解决其他材料类问题的原位和计算工具已存在。缩小这一差距将解锁两项设计能力：将机械能用作调节相选择的合成变量，以及使亚稳态可编程，从而生成无法通过溶液途径获得的捕获相、特定中间体和组成。最后，两项测试可验证这种控制是否具有实际意义：研磨过程中调控的状态必须能在工作器件中保留，且该方法必须在整个器件生命周期中真正更环保，而非仅无溶剂。
英文摘要
Mechanochemical milling is regarded as a scalable, solvent-free method that makes halide perovskites that solution processing cannot. Its deeper promise, though, is that mechanical force could become a new axis of synthetic control to turn milling from an empirical method into a predictive science. Halide perovskites are the ideal platform to establish this: their soft lattices and low formation energies make them intrinsically responsive to mechanical activation. Realising this requires settling what milling actually makes, and how: can a milled phase genuinely be trapped outside equilibrium, or is it just a convenient way to the equilibrium phase, and by what atomistic pathway does it work? These questions are mostly answered by assumption, while the in-situ and computational tools that resolved them for other material classes already exist. Closing this gap will unlock two design capabilities: mechanical energy used as a synthetic variable to tune phase selection, and metastability made programmable, producing trapped phases, specific intermediates, and compositions that have no possible solution route. Finally, two tests decide whether that control reaches practice: the state engineered during milling must survive into a working device, and the method must prove genuinely greener across the full device life cycle, rather than just solvent-free.
Comments23 pages, 3 figures
