Magnetization measurements of a truly axial symmetry Mn12-tBuAc molecular nanomagnet with a spin ground state of S = 10 show resonance tunneling. This compound has the same magnetic anisotropy as Mn12-Ac but the molecules are better isolated and the crystals have less disorder and a higher symmetry. Hysteresis loop measurements at several temperatures reveal a well-resolved step fine-structure which is due to level crossings of excited states. All step positions can be modeled by a simple spin Hamiltonian. The crossover between thermally assisted and pure quantum tunneling can be investigated with unprecedented detail.PACS numbers: 75.50. Xx, 75.60.Jk, 75.75.+a, 75.45.+j Mn 12 -Ac for short, was the first single-molecule magnet (SMM), exhibiting slow magnetization relaxation of its S = 10 spin ground state which is split by axial zero-field splitting [1]. It was also the first system to show thermally assisted tunneling of magnetization [2,3,4]. During the last several years, many more SMMs have been discovered and they are now among the most promising candidates for observing the limits between classical and quantum physics since they have a well defined structure, spin ground state and magnetic anisotropy [5,6,7,9].Nevertheless, Mn 12 -Ac is still the most widely studied SMM [10,11,12,13,14,15,16,17,18,19,20,21,22]. While a rough understanding of the quantum phenomena in Mn 12 -Ac was clear from the early studies, a detailed understanding has not yet emerged. For example, current theoretical models assume the presence of quadratic and quartic transverse crystal-field interactions in the spin Hamiltonian, where the former has been ascribed to solvent disorder [21]. However, these interactions, which contain only even powers of the raising and lowering operators, do not provide an explanation for the observation of odd tunneling steps in the hysteresis loops. It has been proposed that easy-axis tilting might give the missing odd transverse interactions [18]. Although such solvent disorder induced tilts exist, the tilt values are still unclear [24]. Hyperfine, dipolar, and Dzyaloshinsky-Moriya interactions were also proposed to be responsible for odd transverse terms [10,13].Other theoretical and experimental studies concern the crossover between thermally assisted and pure quantum tunneling [11,12,13,14,15,22,23]. The crossover can occur in a narrow temperature interval with the field at which the system crosses the anisotropy barrier shifting abruptly with temperature, or the crossover can occur in a broad interval of temperature with this field changing smoothly [15,22,23]. The first studies were published on Mn 12 -Ac [11,12,13] We show that this compound has the same magnetic anisotropy as Mn 12 Ac but the molecules are better isolated and the crystals contain less disorder and a higher symmetry. Hysteresis loop measurements at several temperatures reveal a fine structure of steps which is due to the dominating energy level crossings. All step positions can be modeled by a simple spin Hamiltonian. The cr...