An important challenge in magnetism is the unambiguous identification of a quantum spin liquid 1,2 , of potential importance for quantum computing. In such a material, the magnetic spins should be fluctuating in the quantum regime, instead of frozen in a classical long-range-ordered state. While this requirement dictates systems 3,4 wherein classical order is suppressed by a frustrating lattice 5 , an ideal system would allow tuning of quantum fluctuations by an external parameter. Conventional three-dimensional antiferromagnets can be tuned through a quantum critical point-a region of highly fluctuating spins-by an applied magnetic field. Such systems suffer from a weak specific-heat peak at the quantum critical point, with little entropy available for quantum fluctuations 6 . Here we study a different type of antiferromagnet, comprised of weakly coupled antiferromagnetic spin-1/2 chains as realized in the molecular salt K 2 PbCu(NO 2 ) 6 . Across the temperature-magnetic field boundary between three-dimensional order and the paramagnetic phase, the specific heat exhibits a large peak whose magnitude approaches a value suggestive of the spinon Sommerfeld coefficient of isolated quantum spin chains. These results demonstrate an alternative approach for producing quantum matter via a magnetic-field-induced shift of entropy from one-dimensional short-range order to a three-dimensional quantum critical point.Previous work on field-tuning of quantum fluctuations has focused on the transverse-field Ising model where the magnetic field (H) couples to a sector of the Hamiltonian not directly modifying the order parameter. While this paradigm has been explored in the three-dimensional (3D) dipolar ferromagnet LiHoF 4 (refs 7,8 ), and the 1D system CoNb 2 O 6 (ref. ), the need for a unique Ising-axis normal restricts the number of potential quantum-spin-liquid host materials. For the much broader class of 3D antiferromagnets (AFs), H can indeed tune the Néel temperature (T N ) into the quantum regime. Within the ordered state, however, on increasing H from zero one first encounters a spin-flop transition (for finite spin anisotropy), followed by a gradual reorientation of those spins (Fig. 1a). Hence, in destroying Néel order, H decreases the transverse components of the staggered moment to a value that is vanishingly small near the transition to the field-polarized state, leaving little entropy to be lost near T = 0, and thus low spectral weight available for quantum entanglement 6 . Here we demonstrate a different approach to tuning through a quantum critical point (QCP). The quasi-1D spin-1/2 AF K 2 PbCu(NO 2 ) 6 orders classically at 0.68 K (ref.
10; Fig. 1b). At lower temperatures within the Néel state, applied H values less than the intra-chain mean field cause little change in the specific heat C(T, H). At the phase boundary, however, a large amount of entropy is released, leading to a peak in C/T (Fig. 1c), the value of which (~ 2 J mol -1 K -2 at the lowest temperatures studied) is suggestive of the spinon ...