Linearized augmented planewaves combined with local-orbitals (LAPW + lo) are arguably the most precise basis set to represent Kohn–Sham states. When employed within real-time time-dependent density functional theory (RT-TDDFT), they promise ultimate precision achievable for exploring the evolution of electronic excitations. In this work, we present an implementation of RT-TDDFT in the full-potential LAPW + lo code exciting. We benchmark our results against those obtained by linear-response TDDFT with exciting and by RT-TDDFT calculations with the Octopus code, finding a satisfactory level of agreement. To illustrate possible applications of our implementation, we have chosen three examples: the dynamic behavior of excitations in MoS₂ induced by a laser pulse, the third harmonic generation in silicon, and a pump–probe experiment in diamond. Besides, we provide further benchmark results.

线性增强平面波结合局部轨道 (LAPW + lo) 可以说是表示 Kohn-Sham 状态的最精确的基组。当在实时瞬态密度泛函理论 (RT-TDDFT) 中使用时，它们有望实现探索电子激发演化的终极精度。在这项工作中，我们在全潜力 LAPW + lo 代码中展示了 RT-TDDFT 的实现，令人兴奋。我们将我们的结果与通过令人兴奋的线性响应 TDDFT和使用 Octopus 代码的 RT-TDDFT 计算获得的结果进行对比，找到了令人满意的一致性。为了说明我们实现的可能应用，我们选择了三个例子：MoS ₂中激发的动态行为由激光脉冲、硅中的三次谐波产生和金刚石中的泵浦探测实验引起。此外，我们提供了进一步的基准测试结果。