Coherent control of rare earth 4f shell wavefunctions in the quantum spin liquid Tb2Ti2O7

The resonant excitation of electronic transitions with coherent laser sources creates quantum coherent superpositions of the involved electronic states. Most time-resolved studies have focused on gases or isolated subsystems embedded in insulating solids, aiming for applications in quantum information. Here, we focus on the coherent control of orbital wavefunctions in the correlated quantum material Tb2Ti2O7, which forms an interacting spin liquid ground state. We show that resonant excitation with a strong THz pulse creates a coherent superposition of the lowest energy Tb 4f states. The coherence manifests itself as a macroscopic oscillating magnetic dipole, which is detected by ultrafast resonant x-ray diffraction. We envision the coherent control of orbital wavefunctions demonstrated here to become a new tool for the ultrafast manipulation and investigation of quantum materials. Recent years have seen significant progress in the coherent control of collective excitations such as magnons and phonons in quantum materials using ultrafast laser pulses. Here the authors report evidence of coherent excitation of orbitals in a rare earth pyrochlore spin liquid material Tb2Ti2O7 by THz pulses.