Nonlinear phononics provides a route to control crystal structures through light-induced phonon excitation. In this study, we apply nonlinear phononics to an iron-based superconductor, LaFeAsO, with the aim of tuning its crystal structure toward the ideal one to enhance superconductivity. We simulate light-induced phonon dynamics on the anharmonic lattice potential determined by first-principles calculations. We find that the anion height $h$, a key structural parameter in iron-based superconductors, approaches its ideal value when an appropriate infrared-active phonon mode is selectively excited. This result suggests the possibility of controlling crystal structures and enhancing superconductivity in iron-based superconductors based on the concept of nonlinear phononics.

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• Anharmonic lattice dynamics
• Lattice dynamics
• Optical & microwave phenomena
• Optical phonons
• Phonons
• Superconductors
• Density functional theory
• First-principles calculations