Spectral Shaping of an Optical Frequency Comb to Control Atomic Dynamics

In advanced spectroscopy, the classical symmetric optical frequency comb is limited in temporal flexibility and selection freedom, which constrains the efficiency and stability of quantum manipulation. To overcome this limitation, we propose a method to realize precise energy-level manipulation using a femtosecond non-temporally symmetric optical frequency comb in the semiclassical three-level system. Numerical calculations show that the fall time of the pulse is the key parameter to realize the precise manipulation, and a shorter fall time contributes to the efficient accumulation of population. By optimizing the pulse parameters, 99.15% accumulation of population in the target state can be successfully achieved and stably maintained using an asymmetric slowly turned-on and rapidly turned-off (STRT) pulse train. Our demonstration of the non-temporally symmetric optical frequency comb provides a promising approach to efficient quantum-state preparation using spectral modulation.