We conduct frequency comparisons between a state-of-the-art strontium optical lattice clock, a cryogenic crystalline silicon cavity, and a hydrogen maser to set new bounds on the coupling of ultralight dark matter to Standard Model particles and fields in the mass range of $10^{-16}$ $-$ $10^{-21}$ eV. The key advantage of this two-part ratio comparison is the differential sensitivities to time variation of both the fine-structure constant and the electron mass, achieving a substantially improved limit on the moduli of ultralight dark matter, particularly at higher masses than typical atomic spectroscopic results. Furthermore, we demonstrate an extension of the search range to even higher masses by use of dynamical decoupling techniques. These results highlight the importance of using the best performing atomic clocks for fundamental physics applications as all-optical timescales are increasingly integrated with, and will eventually supplant, existing microwave timescales.
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