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We have carried out Raman spectroscopy experiments to investigate two-magnonexcitations in epitaxial thin films of the quasi-two-dimensionalantiferromagnetic Mott insulator Sr$_2$IrO$_4$ under in-plane misfit strain.With in-plane biaxial compression, the energy of the two-magnon peak increases,and the peak remains observable over a wider temperature range above the N\'eeltemperature, indicating strain-induced enhancement of the superexchangeinteractions between $\it{J}_{eff}$ = 1/2 pseudospins. From density functionaltheory calculations, we have found an increase of the nearest-neighbor hoppingparameter and exchange interaction with increasing biaxial compressive strain,in agreement with the experimental observations. Our experimental andtheoretical results provide perspectives for systematic, theory-guided straincontrol of the primary exchange interactions in 5$\it{d}$ transition metaloxides.

Compressive-strain induced enhancement of exchange interactions and short-range magnetic order in Sr$_2$IrO$_4$ investigated by Raman spectroscopy