A transverse magnetic field is used to scan the diagonal and off-diagonal susceptibility of the uniaxial quantum magnet, LiHo 0:045 Y 0:955 F 4 . Clusters of strongly coupled spins act as the primary source for the response functions, which result from a field-induced quantum projection of the system into a classically forbidden (meaning non-Ising) regime. Calculations based on spin pairs reproduce only some features of the data and fail to predict the measured off-diagonal response, providing evidence of a multispin collective state. DOI: 10.1103/PhysRevLett.99.057203 PACS numbers: 75.45.+j, 75.50.Dd, 75.50.Lk, 76.30.Kg A basic feature of quantum mechanics is the superposition of states and the projection of these superpositions into observable quantities. From the Stern-Gerlach experiment of 1922, where quantum projection was first demonstrated with angular momentum states in silver atoms [1], to spin echoes in nuclear magnetic resonance [2], where a series of radio frequency pulses induce the precession of nuclear spins projected into classically inaccessible states, strict experimental protocols have been derived for quantum manipulation at the atomic level. For quantum information purposes, it would be advantageous to extend these techniques to coherent clusters of atoms and to explore such effects in solids. In this Letter, we pioneer measurements of the off-diagonal susceptibility to observe quantum mixing effects in a uniaxial magnetic salt, where we are able to rotate clusters of spins into a classically forbidden (meaning non-Ising) state, transverse to the spin axis. The spins can be manipulated by a combination of ac and dc magnetic fields, detected by a multiaxis susceptometer, and parsed for their quantum-mechanical (xy) or classical (polarized along z, the Ising axis) nature by sweeping transverse magnetic field or temperature, respectively. Our technique takes full advantage of the tensor nature of the magnetic susceptibility, revealing the fundamental role played by the off-diagonal terms [3] in the Hamiltonian.Comparison of the results with calculations including only single ions and pairs of ions shows that the off-diagonal response is not only large, but that it also displays the characteristics of a quantum spin liquid [3].The results of the technique depend crucially on two properties of our system: (i) the ability to introduce quantum mechanics via a controllable, external tuning parameter, and (ii) the predilection of disorder to form spin clusters that may occur rarely but can dominate the physics. In particular, the random distribution of magnetic Ho ions in the diluted, spin-1=2 Ising system LiHo 0:045 Y 0:955 F 4 gives rise to regions where the local density of Ho is comparable to that of the pure compound, and hence are locally ferromagnetic or antiferromagnetic depending on the displacement between nearest neighbors. The Ising spins are constrained to point up or down along the crystallographic c axis, and can be controllably mixed with the application of a magnetic field H t tr...