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Photonics

Spectral Shaping of an Optical Frequency Comb to Control Atomic Dynamics

Yichi Zhang, Zhenqi Bai, Hongyan Fan, X. Y. Wang

Published Oct 14, 2025• 1 citation

Abstract

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.

DOI: 10.3390/photonics12101015

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Abstract A single femtosecond optical frequency comb is implemented to induce two‐photon transitions between molecular vibrational levels to form ultracold molecules. The phase across an individual pulse in the pulse train is sinusoidally modulated with a carefully chosen modulation amplitude and frequency. Piecewise population transfer is fulfilled to the final state by each pulse in the applied pulse train providing a controlled population accumulation in the final, ultracold state. The dynamics of rovibrational cooling is discussed on an example of the KRb molecule. © 2010 Wiley Periodicals, Inc. Int J Quantum Chem, 2010