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The nature of the enigmatic pseudogap region of the phase diagram is the most important and intriguing unsolved puzzle in the field of high transition-temperature (Tc) superconductivity. This region, the temperature range above Tc and below a charact eristic temperature T*, is characterized by highly anomalous magnetic, charge transport, thermodynamic and optical properties. Associated with the pseudogap puzzle are open questions pertaining to the number of distinct phases and the presence of a quantum-critical point underneath the superconducting dome. Here we use polarized neutron diffraction to demonstrate for the model superconductor HgBa2CuO4+d (Hg1201) that T* marks the onset of an unusual magnetic order, and hence a novel state of matter with broken time-reversal symmetry. Together with prior results for YBa2Cu3O6+d (YBCO), this observation constitutes an essential and decisive demonstration of the universal existence of such a state. The new findings appear to rule out a large class of theories that regard T* as a crossover temperature rather than a phase transition temperature. Instead, they are consistent with a variant of previously proposed charge-current-loop order that involves apical oxygen orbitals, and with the notion that many of the unusual properties arise from the presence of a quantum-critical point.
The compound HgBa$_2$CuO$_{4+Delta}$ (Hg1201) exhibits a simple tetragonal crystal structure and the highest superconducting transition temperature (T$_c$) among all single Cu-O layer cuprates, with T$_c$ = 97 K (onset) at optimal doping. Due to a la ck of sizable single crystals, experimental work on this very attractive system has been significantly limited. Thanks to a recent breakthrough in crystal growth, such crystals have now become available. Here, we demonstrate that it is possible to identify suitable heat treatment conditions to systematically and uniformly tune the hole concentration of Hg1201 crystals over a wide range, from very underdoped (T$_c$ = 47 K, hole concentration p ~ 0.08) to overdoped (T$_c$ = 64 K, p ~ 0.22). We then present quantitative magnetic susceptibility and DC charge transport results that reveal the very high-quality nature of the studied crystals. Using XPS on cleaved samples, we furthermore demonstrate that it is possible to obtain large surfaces of good quality. These characterization measurements demonstrate that Hg1201 should be viewed as a model high-temperature superconductor, and they provide the foundation for extensive future experimental work.
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