Crystalline materials that include 4f- and 5f-electron elements frequently exhibit a variety of intriguing phenomena including spin and charge orderings, spin and valence fluctuations, heavy fermion behavior, breakdown of Fermi liquid behavior, and unconventional superconductivity. [5, 6, 7, 8, 9, 10, 11, 12, 13] Amongst such materials, the Kondo lattice system URu2Si2 stands out as being particularly unusual. [14, 15, 16] While at high temperature it exhibits behavior that is typical for an f-electron lattice immersed in a sea of conduction electrons, at T0 = 17:5 K there is a second order phase transition that is followed by unconventional superconductivity near Tc 1:5 K. [15] Despite three decades of work, the order parameter for the transition at T0 remains unknown and hence, it has been named "hidden order". There have been a multitude of experimental attempts to unravel hidden order, mainly through tuning of the electronic state via pressure, applied magnetic field, and chemical substitution. [17, 18] While these strategies reveal interesting phase diagrams, a longstanding challenge is that any such approach explores the phase space along an unknown vector: i.e., many different factors are affected. To address this issue, we developed a new organizational map for the U-based ThCr2Si2-type compounds that are related to URu2Si2 and thus guided, we explored a new chemical tuning axis: Si -> P. Our studies were enabled by the development of a new molten metal crystal growth method for URu2Si2 which produces high quality single crystals and allows us to introduce high vapor pressure elements, such as phosphorous. [19, 20] Si -> P tuning reveals that while the high temperature Kondo lattice behavior is robust, the low temperature phenomena are remarkably sensitive to electronic tuning. [21, 22] In the URu2Si2-xPx phase diagram we find that while hidden order is monotonically suppressed and destroyed for x < 0.035, the superconducting strength evolves non-monotonically with a maximum near x = 0.01 and that superconductivity is destroyed near x = 0.028. For 0.03 < x < 0.26 there is a region with Kondo coherence but no ordered state. Antiferromagnetism abruptly appears for x = 0.26. This phase diagram differs significantly from those produced by most other tuning strategies in URu2Si2, including applied pressure, and isoelectronic chemical substitution (i.e. Ru -> Fe and Os), where hidden order and magnetism share a common phase boundary. [2, 23, 24] We discuss implications for understanding hidden order, its relationship to magnetism, and prospects for uncovering novel sibling electronic states.
