We report new limits on ultralight scalar dark matter (DM) with dilaton-like couplings to photons that can induce oscillations in the fine-structure constant α. Atomic dysprosium exhibits an electronic structure with two nearly degenerate levels whose energy splitting is sensitive to changes in α. Spectroscopy data for two isotopes of dysprosium over a two-year span is analyzed for coherent oscillations with angular frequencies below 1 rad s −1 . No signal consistent with a DM coupling is identified, leading to new constraints on dilaton-like photon couplings over a wide mass range. Under the assumption that the scalar field comprises all of the DM, our limits on the coupling exceed those from equivalence-principle tests by up to 4 orders of magnitude for masses below 3 · 10 −18 eV. Excess oscillatory power, inconsistent with fine-structure variation, is detected in a control channel, and is likely due to a systematic effect. Our atomic spectroscopy limits on DM are the first of their kind, and leave substantial room for improvement with state-of-the-art atomic clocks.Dark matter (DM) makes up the majority of matter density in our Universe. Its ubiquitous abundance can be measured through its gravitational influence, but little is known about the microphysical properties of the DM particle(s), such as the mass, spin, and any nongravitational interactions. If the DM is bosonic rather than fermionic, it can have a sub-eV mass and such high occupation numbers that it acts more like a classical wavewith frequency equal to its mass-than a particle. Light bosonic dark matter has a natural production mechanism, namely early-universe misalignment of the field relative to the minimum of its potential [1][2][3]. Several motivated candidates in this category exist in the literature, most notably the QCD axion [4-6] and other axion-like particles, which, as parity-odd pseudo-Nambu-Goldstone bosons (PNGBs) of compact symmetry groups, primarily have derivative interactions with matter [7]. Light, parity-even bosons may also arise as PNGBs of noncompact groups such as those of scale, conformal, or shift symmetries, the most famous examples of which are dilatons [8][9][10]. Small explicit breakings of these symmetries may induce nonderivative operators for the scalar fields, such as mass terms and higher-dimensional operators coupling them to matter.We focus on ultralight scalar fields φ with couplings to the (square of the) electromagnetic field tensor F µν :where κ ≡ √ 4πG N , G N is Newton's constant, and e ≈ 0.303 is the electromagnetic gauge coupling (we use units in which = c = 1). The interaction is normalized such that d e = 1 yields an attractive force of gravitational strength between electromagnetic energy densities at distances smaller than the inverse mass (r m and naturalness considerations together suggest a minimum mass-squared for φ. However, given the existing hierarchy problems of the Standard Model, we remain agnostic to this issue and consider the full m φ -d e parameter space (see Ref.[13] for more discuss...