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Axion-like particles (ALPs) arise from well-motivated extensions to the Standard Model and could account for dark matter. ALP dark matter would manifest as a field oscillating at an (as of yet) unknown frequency. The frequency depends linearly on the ALP mass and plausibly ranges from 10⁻²²to 10 eV/c². This motivates broadband search approaches. We report on a direct search for ALP dark matter with an interferometer composed of two atomic K-Rb-³He comagnetometers, one situated in Mainz, Germany, and the other in Kraków, Poland. We leverage the anticipated spatio-temporal coherence properties of the ALP field and probe all ALP-gradient-spin interactions covering a mass range of nine orders of magnitude. No significant evidence of an ALP signal is found. We thus place new upper limits on the ALP-neutron, ALP-proton and ALP-electron couplings reaching belowg_aNN < 10⁻⁹ GeV⁻¹,g_aPP < 10⁻⁷ GeV⁻¹andg_aee < 10⁻⁶ GeV⁻¹, respectively. These limits improve upon previous laboratory constraints for neutron and proton couplings by up to three orders of magnitude. 

We propose and demonstrate a general method to calibrate the frequency-dependent response of selfcompensating noble-gas–alkali-metal comagnetometers to arbitrary spin perturbations. This includes magnetic and nonmagnetic perturbations such as rotations and exotic spin interactions. The method is based on a fit of the magnetic field response to an analytical model. The frequency-dependent response of the comagnetometer to arbitrary spin perturbations can be inferred using the fit parameters. We demonstrate the effectiveness of this method by comparing the inferred rotation response to an experimental measurement of the rotation response. Our results show that experiments relying on zero-frequency calibration of the comagnetometer response can over- or underestimate the comagnetometer sensitivity by orders of magnitude over a wide frequency range. Moreover, this discrepancy accumulates over time as operational parameters tend to drift during comagnetometer operation. The demonstrated calibration protocol enables accurate prediction and control of comagnetometer sensitivity to, for example, ultralight bosonic dark-matter fields coupling to electron or nuclear spins, as well as accurate monitoring and control of the relevant system parameters.