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The similarities to cuprates make iridates an interesting potential platformfor investigating superconductivity. Equally attractive are their puzzlingcomplex intrinsic interactions. Here, we report an ultrafast opticalspectroscopy investigation of a coherent phonon mode in Sr3Ir2O7, a bilayerRuddlesden-Popper perovskite iridate. An anomaly in the A1g optical phonon({\nu} = 4.4 THz) is unambiguously observed below the N\'eel temperature (TN),which we attribute to pseudospin-lattice coupling (PLC). Significantly, we findthat PLC is the dominant interaction at low temperature, and we directlymeasure the PLC coefficient to be {\lambda} = 150 +/- 20 cm-1, which is twoorders of magnitude higher than that in manganites (< 2.4 cm-1) and comparableto that in CuO (50 cm-1, the strongest PLC or spin-lattice coupling (SLC)previously known). Moreover, we find that the strong PLC induces an anisotropicnegative thermal expansion. Our findings highlight the key role of PLC iniridates and uncovers another intriguing similarity to cuprates.

Strong Pseudospin-Lattice Coupling in Sr3Ir2O7: Coherent Phonon Anomaly and Negative Thermal Expansion