Ultrafast Generation of Coherent Phonons in Two-Dimensional Bismuthene.

Coherent phonons generated through regulation of lattice oscillation via ultrafast laser pulses or X-rays have been desired in various fields, including optoelectronics, thermal and quantum information, and communications. Phonon coherence of two-dimensional (2D) materials is particularly attractive as it enables controllable information transmission but is challenging as the weak interplanar coupling makes phonon excitation extremely difficult. Herein we managed to generate size-dependent phonon coherence from bulk Bi to few-layer bismuthene by an ultrafast femtosecond laser pulse and made a systematic comparison thorough a combination of computation, transient absorption, and reflectance spectroscopic methods. The results witnessed the A 1g phonon excitation in all of the three Bi materials with distinct thicknesses, and the quantum size effect of 2D materials caused phonon confinement and eventual bond softening manifested as a red-shifted vibration frequency and shortened decoherence time compared with those of their bulk counterpart. This study offers new perspectives for tailoring coherent phonons in 2D materials for quantum science and technology including quantum communication, computing, and design of novel quantum devices, etc.