Observation of cooperative strong coupling between optical phonon and crystal-field excitations in a pseudo Jahn-Teller system
Cooperative interactions between localized electronic excitations and crystal lattice are central to the emergence of complex structural phases in materials. However, the scaling relations governing these collective behaviors remain largely unexplored. Here, using magneto-Raman spectroscopy, we report the direct observation of the strongly coupled optical phonon and non-degenerate crystal-field excitations (CFEs) in ErFeO3. By independently tuning the effective population of Jahn-Teller-active erbium ions through temperature and chemical dilution with Jahn-Teller-inactive yttrium ions, we identify the coupling strength varies linearly with the square root of electronic excitations population. Notably, Y-doping reveals the hybridization gap reduces significantly faster than predicted by density scaling alone, indicating phonon coherence is essential for establishing this cooperative interaction. Our findings highlight the role of optical phonons in mediating short-range interactions that drive cooperative Jahn-Teller effect, evidencing the pathway for tailoring electronic and vibrational properties of Jahn-Teller materials through population control.