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We conduct frequency comparisons between a state-of-the-art strontium opticallattice clock, a cryogenic crystalline silicon cavity, and a hydrogen maser toset new bounds on the coupling of ultralight dark matter to Standard Modelparticles and fields in the mass range of $10^{-16}$ $-$ $10^{-21}$ eV. The keyadvantage of this two-part ratio comparison is the differential sensitivitiesto time variation of both the fine-structure constant and the electron mass,achieving a substantially improved limit on the moduli of ultralight darkmatter, particularly at higher masses than typical atomic spectroscopicresults. Furthermore, we demonstrate an extension of the search range to evenhigher masses by use of dynamical decoupling techniques. These resultshighlight the importance of using the best performing atomic clocks forfundamental physics applications as all-optical timescales are increasinglyintegrated with, and will eventually supplant, existing microwave timescales.

Precision Metrology Meets Cosmology: Improved Constraints on Ultralight Dark Matter from Atom-Cavity Frequency Comparisons