Recent progress with the thermally-driven spin-state crossover in LaCoO 3 has made it increasingly apparent that the nominally non-magnetic low spin ground state of this material actually hosts novel defect-based magnetism. This is investigated here via a small-angle neutron scattering (SANS) study of LaCoO 3-δ crystals. The results provide: (i) the surprising finding that the spin-state crossover is clearly reflected in SANS via quasielastic/inelastic scattering from paramagnetic spin fluctuations/excitations, and (ii) evidence for the formation, likely around oxygen defects, of local entities known as magnetic excitons. The latter generate distinct magnetic scattering below 60 K, providing valuable quantitative information on exciton densities and interactions. Potential relevance to the unexpected ferromagnetism recently discovered in epitaxial LaCoO 3 films is discussed.PACS Nos: 75.47.Lx, 75.30.Wx, Corresponding author: CL (leighton@umn.edu) 2 Magnetism in LaCoO 3 has attracted attention and controversy for almost 50 years, largely due to the only marginal dominance of the crystal field splitting of t 2g and e g states over the Hund exchange energy [1,2]. A low spin (LS, t 2g 6 e g 0 , S = 0) configuration is thus observed in the ground state, but is stable only to ∼30 K, at which point excited spin-states are gradually populated [1][2][3][4][5][6][7][8][9][10][11][12]. These excited states can be simplistically described as intermediate spin ( Despite these challenges, substantial recent progress has been achieved. This encompasses:(i) Increased recognition that characterization of excited states as atomic-like "IS" or "HS" is likely misleading due to significant spin-orbit coupling [15] and ; (ii) A suite of experiments using electron spin resonance [6,11], X-ray absorption spectroscopy/magnetic circular dichroism [7], and inelastic neutron spectroscopy (INS) [8,9], that consistently identify a zero-field-split triplet as the first excited state; (iii) Direct measurement of both a 0.6 meV excitation associated with this triplet [8,9] and a g-factor of 3-3.5 [6,11]; and (iv) Consistent interpretation of these results in terms of a spin-orbit triplet excited state [6,8,9,11,15]. While the understanding of the spin-state problem in LaCoO 3 thus remains incomplete, it is nevertheless advancing. [27]. Noteworthy in comparison to conventional magnetic polarons is that these excitons / spin-state polarons form as the host lattice crosses over to an S = 0 ground state; they can thus exist in a non-magnetic (as opposed to para-or antiferro-magnetic) matrix.Here, a study of the magnetism of LaCoO 3 crystals using small-angle neutron scattering (SANS) is reported. The magnetic SANS is found to have two contributions: A low scattering wavevector (q) part with strong q dependence that turns on below 60 K, and a higher q part with 4 negligible q dependence that increases gradually on warming above 30 K. The latter is shown to be due to the spin-state crossover, which SANS is demonstrated to be sensitive to via the qua...