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We investigate the ultrafast structural dynamics of LaAlO3 thin films driven by short mid-infrared laser pulses at 20 THz. Time-resolved X-ray diffraction reveals an immediate lattice expansion and an acoustic breathing mode of the film. First-principles theory and a spring-mass model identify the direct coupling between coherently driven infrared-active phonons and strain as the underlying mechanism. Time-resolved optical birefringence measurements confirm that the amplitude of this acoustic mode scales linearly with the pump fluence, which agrees with the theory. Furthermore, time-resolved X-ray diffuse scattering indicates that THz excitation enhances crystallinity by inducing a non-thermal increase in structural symmetry originating from preexisting defects. These findings highlight the potential of a multimodal approach-combining time-resolved X-ray and optical measurements and first-principles theory-to elucidate and control structural dynamics in nanoscale materials.

In magnetic topological insulators, spontaneous time-reversal symmetry breaking by intrinsic magnetic order can open an energy gap in the topological surface spectrum. In the resulting state, exotic properties like axion electrodynamics, the quantum anomalous Hall effect, and other topological magnetoelectric responses are expected to emerge. A detailed understanding of the magnetic order and its coupling to the topological surface states is essential to harness and tune these properties. Here, we leverage near-resonant electric quadrupole optical second harmonic generation to probe magnetic fluctuations in the candidate axion insulator EuSn$_2$(As,P)$_2$ across its antiferromagnetic phase boundary. We observe a pronounced dimensional crossover in the quantum decoherence induced by magnetic fluctuations, where two-dimensional in-plane ferromagnetic correlations at high temperatures give way to three-dimensional long-range order at the N\'eel temperature. We also observe the breaking of rotational symmetry within the long-range-ordered antiferromagnetic state and map out the resulting spatial domain structure. More generally, we demonstrate the unique capabilities of nonlinear optical spectroscopy to study quantum coherence and fluctuations in magnetic quantum materials.