We propose and experimentally demonstrate a method for detection of light scalar Dark Matter (DM), through probing temporal oscillations of fundamental constants in an atomic optical transition. Utilizing the quantum information notion of Dynamic Decoupling (DD) in a table-top setting, we are able to obtain model-independent bounds on variations of $alpha$ and $m_e$ at frequencies up to the MHz scale. We interpret our results to constrain the parameter space of light scalar DM field models. We consider the generic case, where the couplings of the DM field to the photon and to the electron are independent, as well as the case of a relaxion DM model, including the scenario of a DM boson star centered around Earth. Given the particular nature of DD, allowing to directly observe the oscillatory behaviour of coherent DM, and considering future experimental improvements, we conclude that our proposed method could be complimentary to, and possibly competitive with, gravitational probes of light scalar DM.
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