Accurately probing the interatomic potential (IP) in crystals is essential for understanding the dynamic mechanisms in phase transitions and chemical reactions. Here, by interrogating laser-induced coherent phonon dynamics, we propose a new kind of optical microscopy for determining effective interatomic potentials beyond the harmonic and adiabatic approximation. This technique is tested against available experimental and first-principles data, by which the interatomic potential of graphene and a few other materials are successfully reconstructed in a large configuration space and beyond the ground state. A significant nonadiabatic effect emerges in nonlinear phonon dynamics and the IP reconstruction, which corrects the anharmonic part of IP much stronger (up to 50%) than the harmonic part. The nonadiabaticity-modulated potentials can lead to ∼10% correction on thermal expansion coefficients and ∼0.3 eV on phase transition barriers. This work offers a new strategy for probing complex interactions in quantum materials and exemplifies the universality of nonadiabaticity, which deserves a full consideration for precisely determining physical properties of quantum many-body systems.

准确探测晶体中的原子间势 (IP) 对于理解相变和化学反应的动态机制至关重要。在这里，通过询问激光诱导的相干声子动力学，我们提出了一种新的光学显微镜，用于确定谐波和绝热近似之外的有效原子间势。该技术针对可用的实验数据和第一性原理数据进行了测试，通过这些数据，石墨烯和其他一些材料的原子间势在一个大的配置空间和基态之外被成功地重建。在非线性声子动力学和 IP 重建中出现了显着的非绝热效应，它对 IP 的非谐波部分的校正比谐波部分强得多（高达 50%）。非绝热调制电位可导致热膨胀系数校正约 10%，相变势垒校正约 0.3 eV。这项工作为探索量子材料中的复杂相互作用提供了一种新策略，并体现了非绝热性的普遍性，在精确确定量子多体系统的物理性质时值得充分考虑。