Femtosecond Polarization Switching of [CrCo] Dinuclear Complex Crystals.
2020
: Capability to control macroscopic molecular properties with external stimuli offers the possibility to exploit molecules as switching devices of various types. However, application of such molecular-level switching schemes has been often limited by its speed and thus efficiency. Here, we demonstrate the ultrafast, photoinduced polarization switching in the crystal of the [CrCo] dinuclear complex by ultrafast pump-probe spectroscopy in the visible and mid-infrared regions. Our data clearly show that the photoinduced polarization switching is an ultrafast process with a time constant of 280 fs, demonstrating itself as the fastest polarization switching material realized using the metastable state. Moreover, the pump-probe data in the visible region reveal pronounced appearance of coherent nuclear wavepacket motion with a frequency as low as 22 cm-1, which we attribute to a lattice vibrational mode. The pronounced non-Condon effect for its resonance Raman enhancement implies that this mode couples the relevant electronic states, thereby facilitating the ultrafast polarization switching.
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