脉冲串激发揭示混合卤化物钙钛矿中的时间-剂量互易性失效
Pulse-Burst Excitation Reveals Time-Dose Reciprocity Breakdown in Mixed-Halide Perovskites
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中文总结 AI 辅助
该研究通过脉冲串激发实验，发现混合卤化物钙钛矿在光诱导卤化物偏析与再混合中违反时间-剂量互易性，提出光子时序作为新的材料状态控制参数，为光学存储和神经形态光子学提供新框架。
中文摘要 AI 辅助
时间-剂量互易性通常与Bunsen-Roscoe定律相关，该定律指出光敏系统的响应仅取决于总曝光剂量，而与该能量在时间上的传递方式无关。混合卤化物钙钛矿中的光敏过程，如光诱导卤化物偏析，通常表现出阈值样行为，这种行为可能违反该原理，并使得通过光子时序实现材料状态控制成为可能。我们使用脉冲串激发对此进行测试，该方法引入了超越传统参数（如脉冲通量、重复频率和平均功率）的额外时间控制维度。通过将相同的光子剂量在微秒至毫秒时间尺度上重新分配，我们创造了不同的非平衡激发条件，并表明混合卤化物钙钛矿可以演化到不同的亚稳态，从而揭示了卤化物偏析和再混合联合过程中时间-剂量互易性的失效。这一额外的时间自由度不仅能够实现材料状态的控制，还为解开光诱导卤化物再分布背后相互竞争的过程提供了新的实验框架。我们的发现确立了光子时序作为钙钛矿光化学的控制参数，并为光学存储和神经形态光子应用开辟了额外机会。
英文摘要
Time-dose reciprocity, commonly associated with the Bunsen-Roscoe law, states that the response of a photosensitive system depends only on the total exposure dose, regardless of how that energy is delivered over time. Light-sensitive processes in mixed-halide perovskites, such as photoinduced halide segregation, often exhibit threshold-like behavior that may violate this principle and enable material-state control by photon timing. We test this using pulse-burst excitation, which introduces an additional temporal control dimension beyond conventional parameters such as pulse fluence, repetition rate, and average power. By redistributing the same photon dose over microsecond-to-millisecond timescales, we create distinct nonequilibrium excitation conditions and show that mixed-halide perovskites can evolve into different metastable states, revealing a breakdown of time-dose reciprocity in the combined processes of halide segregation and remixing. This additional temporal degree of freedom not only enables control of the material state but also provides a new experimental framework for disentangling the competing processes underlying photoinduced halide redistribution. Our findings establish photon timing as a control parameter for perovskite photochemistry and open additional opportunities for optical memory and neuromorphic photonic applications.
发表机构
- Lund University（隆德大学）
- Technical University of Dresden（德累斯顿工业大学）
- Leibniz Institute for Solid State and Materials Research Dresden（德累斯顿莱布尼茨固体与材料研究所）
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