Quantum beats of vibrational modes in both the low and high wavenumber regions studied by fs-CARS

We have studied the quantum beats of vibrational modes in different phase samples by employing femtosecond time-resolved coherent anti-Stokes Raman scattering (fs-CARS) technique. The temporal chirped white-light continuum (WLC) is used for the Stokes pulse, we have achieved the selective excitation of vibrational modes in both the low and high wavenumber regions without complicated laser system, and observed quantum coherence between vibrational modes. This work is of special significance to enhance our understanding of quantum coherence and develop the applications of quantum technologies.

► We studied quantum beats of vibrational modes in different phase samples by fs-CARS. ► We achieve the selective excitation of low and high wavenumber vibrational modes. ► Well-defined quantum beat signals are observed as we expect. ► No complicated laser system is required for the wavelength tuning of Stokes pulse.