Agreement between theoretical calculations of atomic structure and spectroscopic measurements is used to constrain possible contribution of exotic spin-dependent interactions between electrons to the energy differences between states in helium-4. In particular, constraints on dipole-dipole interactions associated with the exchange of pseudoscalar bosons (such as axions or axion-like particles, ALPs) with masses 10 −2 eV m 10 4 eV are improved by a factor of ∼ 100. The first atomic-scale constraints on several exotic velocity-dependent dipole-dipole interactions are established as well. The most commonly employed framework for the purpose of comparing different experimental searches for exotic spin-dependent interactions is that introduced in Ref.[1] to describe long-range spin-dependent potentials associated with the axion and extended in Ref.[2] to encompass long-range potentials associated with any generic spin-0 or spin-1 boson. The spin-dependent potentials enumerated in Ref. [2] are characterized by dimensionless coupling constants that specify the strength of the interaction between various particles and a characteristic range λ for the interaction associated with the reduced Compton wavelength of the new boson of mass m 0 , λ = /(m 0 c), where is the reduced Planck constant and c is the speed of light. Depending on the nature of the new interaction, different particles will have different coupling constants. In the present work, we study dipole-dipole interactions between electrons at the atomic scale through investigation of the electronic structure of helium-4.Laboratory searches for exotic spin-dependent interactions mediated by new bosons are sensitive and broadly inclusive probes for global symmetries broken at high energy scales [1,2]. For example, the fundamental proper- * Electronic address: filip.ficek@student.uj.edu.pl ties of axions and the axion-like-particles (ALPs) mentioned above [1][2][3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19] are characterized by a symmetry breaking scale f a and an interaction scale Λ. These scales determine, for example, the mass of the ALPand the interaction of an ALP with a Standard Model fermion X is proportional to m X c 2 /f a where m X is the fermion mass. In particular, this work improves laboratory constraints on exotic spin-spin forces between electrons mediated by bosons in the mass range between 10 −2 eV and 10 4 eV by two orders of magnitude. Our research is complementary to experiments searching for an axion/ALP coupling to photons, such as the Axion Dark Matter eXperiment (ADMX) [26], the CERN Axion Solar Telescope (CAST) [27], and light-shining-throughwall experiments such as the Any Light Particle Search (ALPS) [28], since He spectroscopy probes the electron-ALP interaction as opposed to the photon-ALP interaction and is sensitive to a mass range beyond that probed by experiments such as ADMX, CAST, and ALPS. Although star cooling rates constrain certain broad classes of ALPs [29,30], there are a number of loopholes in the astrophysica...