We report on a search for a new, short-range, spin-dependent interaction using a modified version of the experimental apparatus used to measure the permanent neutron electric dipole moment at the Paul Scherrer Institute. This interaction, which could be mediated by axion-like particles, concerned the unpolarized nucleons (protons and neutrons) near the material surfaces of the apparatus and polarized ultracold neutrons stored in vacuum. The dominant systematic uncertainty resulting from magnetic-field gradients was controlled to an unprecedented level of approximately 4 pT/cm using an array of optically-pumped cesium vapor magnetometers and magnetic-field maps independently recorded using a dedicated measurement device. No signature of a theoretically predicted new interaction was found, and we set a new limit on the product of the scalar and the pseudoscalar couplings $g_sg_p\lambda^2 < 8.3 \times 10^{-28}\,\text{m}^2$ (95% C.L.) in a range of $5\,\mu\text{m} < \lambda < 25\,\text{mm}$ for the monopole-dipole interaction. This new result confirms and improves our previous limit by a factor of 2.7 and provides the current tightest limit obtained with free neutrons.
