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In this work, a systematic study of Cu(NO 3 ) 2 ·2.5 H 2 O (copper nitrate hemipentahydrate, CN), an alternating Heisenberg antiferromagnetic chain model material, is performed with multi-technique approach including thermal tensor network (TTN) simulations, first-principles calculations, as well as magnetization measurements. Employing a cutting-edge TTN method developed in the present work, we verify the couplings  J  = 5.13 K,  α  = 0.23(1) and Landé factors  g  ∥ = 2.31,  g  ⊥  = 2.14 in CN, with which the magnetothermal properties have been fitted strikingly well. Based on first-principles calculations, we reveal explicitly the spin chain scenario in CN by displaying the calculated electron density distributions, from which the distinct superexchange paths are visualized. On top of that, we investigated the magnetocaloric effect (MCE) in CN by calculating its isentropes and magnetic Grüneisen parameter. Prominent quantum criticality-enhanced MCE was uncovered near both critical fields of intermediate strengths as 2.87 and 4.08 T, respectively. We propose that CN is potentially a very promising quantum critical coolant.

Criticality-Enhanced Magnetocaloric Effect in Quantum Spin Chain Material Copper Nitrate