Our research program encompasses a methodical search for new materials in single-crystal form, and a systematic effort to elucidate the underlying physics of these materials.

Materials Discovery and Synthesis: Wesearch for new, interesting quantum materials and sythesize them in single-crystal form using flux andfloating-zone techniques (see Section Facilities).

We have worked on the following groups of materials: Iridates, Ruthenates, Rhodates and 4d- and 5d-electron-based chalcogenides (see Section Quantum Materials).

Materials Characterization: We utilize a wide suiteof tools for experimental studies of structural, transport, magnetic, thermal and dielectric properties as functions of chemical composition, temperature, magnetic field,pressure and electrical current. Measurements are often carried out at extreme conditions, i.e., ultralow temperatures, high magnetic fields and high pressures (see Section Facilities)

A Common Feature Shared byAll Materials We Are Interested:Quantum states of these materialsare primarilydictated by a combined effect of both spin-orbitandCoulomb interactions andfeaturea high susceptibility to external stimuli, such as magnetic field B, electrical field E, pressure P, light hv or electrical current I.These external stimuli readily couple to the lattice and are control "knobs" we utilize to discover andstudy exotic states, as schematically shown below.

Highlights of Our Recently Published Work

I. Control of Quantum States

A. Electric-current control

  • ,Yu Zhang, Yifei Ni, Hengdi Zhao, Sami Hakani, Feng Ye, Lance DeLong, Itamar Kimchiand Gang Cao,Nature611,467–472 (2022)

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Current-controlled chiral orbital currents in a colossal magnetoresistance material

  • , Gang Cao,Journal of Physics: Condensed Matter,2020.
  • , Hengdi Zhao, Bing Hu, Feng Ye, Christina Hoffmann, Itamar Kimchiand Gang Cao;Phys. Rev. B100, 241104(R)(2019)

Highlights:The Temperature-Current-Density Phase Diagram for 3% Mn dope Ca2RuO4illustrates that the applied current drives the system from the native AFM state (purple) through the critical regime near 0.15 A/cm2(gray) to the current-induced, nonequilibrium orbital state (blue).

  • , G. Cao, J. Terzic, H. D. Zhao, H. Zheng, Peter Riseborough, L. E. DeLong, Phys. Rev. Lett.120, 017201 (2018);Editors'Suggestion

Highlights:Diagrams for Sr2IrO4illustrate that the current-induced lattice expansion(a)causes the unusual I-V curves and(b)increases Ir-O-Ir bond angle(red) and decreases magnetic canting (black arrows) with increasing current I. The reduced lattice distortions lead to enhanced electron mobility.

Diagrams for Sr2IrO4 illustrate that the current-induced lattice expansion (a) causes the unusual I-V curves and (b) increases Ir-O-Ir bond angle  (red) and decreases magnetic canting (black arrows) with increasing current I. The reduced lattice distortions lead to enhanced electron mobility.

B. Pressure control

Schematic of pressure control

  • "Observation of a pressure-induced transition from interlayer ferromagnetism to intralayer antiferromagnetism in Sr4Ru3O10",H . Zheng,W.H. Song, J. Terzic, H. D. Zhao, Y. Zhang, Y. F. Ni, L. E. DeLong, P. Schlottmann and G. Cao,Phys. Rev. B98,064418(2018);DOI: 10.1103/PhysRevB.98.064418;Editors'Suggestion

Highlights: Temperature-Pressure Phase Diagram for Sr4Ru3O10 indicates that application of modest pressure readily drives the ground state from ferromagnetism to antiferromagnetism.

Temperature-Pressure Phase Diagram indicates that application of modest pressure drives the ground state from ferromagnetism to anti ferromagnetism.

  • "Persistent Insulating State at Megabar Pressures in Strongly Spin-Orbit-Coupled Sr2IrO4", Chunhua Chen,Yonghui Zhou,Xuliang Chen, Tao Han,Chao An, Ying Zhou, Yifang Yuan,Bowen Zhang,Shuyang Wang, Ranran Zhang,Lili Zhang, Changjing Zhang, Zhaorong Yang, Lance E. DeLongandGangCao,Phys. Rev. B101, 144102 (2020);DOI:10.1103/PhysRevB.101.144102

Highlights:The temperature dependence of the basal-plane resistance R of Sr2IrO4 over pressures ranging from0.6 GPa to185 GPa. Note thatSr2IrO4unexpectedlyremains insulating up to185 GPaand R shows a tendency of saturation at P > 124 GPa. Inset:A snapshot of the diamond anvil cell at 27 GPa.

II. Key Issues Review on Iridates

  • , Gang Cao and Pedro Schlottmann, Reports on Progress in Physics 81 042502(2018)

Highlights: Schematics of spin-orbit-driven electronicbandsfor Iridates:(a)The traditionally anticipated broad t2gband for 5d-electrons;(b)Thesplitting ofthet2gband into Jeff=1/2 and Jeff=3/2 bands due to strong spin-orbit interactions;(c)Ir4+(5d5) ions provide five 5d-electrons, four of them fill the lower Jeff= 3/2 bands, and one electron partially fills the Jeff= 1/2 band where the Fermi level EFresides; and(d)For Ir5+(5d4) ions, four 5d-electrons fill the Jeff=3/2 bands, leading to a singlet Jeff= 0 state for the strong spin-orbit interactionlimit.

 (a) The traditionally anticipated broad t2g band for 5d-electrons; (b) The splitting of the t2g band into Jeff=1/2 and Jeff=3/2 bands due to SOI; (c) Ir4+(5d5) ions provide five 5d-electrons, four of them fill the lower Jeff = 3/2 bands, and one electron partially fills the Jeff = 1/2 band where the Fermi level EF resides; and (d) For Ir5+(5d4) ions, four 5d-electrons fill the Jeff=3/2 bands, leading to a singlet Jeff = 0 state for the strong SOI limit.

With a few exceptions, almost alliridatesare magnetically insulating andhighly sensitive to even slight chemical doping. However,the insulating state can persist up tomegabar pressures. The lattice symmetry and dynamics play a unique, crucial role in determing the ground states of spin-orbit coupled matter, whichoffers a perspective for understandingthe discrepancies between recent theoretical proposals andexperimental results in iridates, including the absence ofsuperconductivity in Sr2IrO4.

III. Quantum Liquid in an Unfrustrated Lattice

  • , G. Cao, H. D. Zhao, H. Zheng, Y. F. Ni, Christopher. A. Pocs, Y. Zhang, Feng, Ye,Christina Hoffmann, Xiaoping Wang,Minhyea Lee, Michael Hermele and Itamar Kimchi, npj Quantum Mater. 5, 26 (2020)
  • ,Y. Shen, J. Sears, G. Fabbris, A. Weichselbaum, W. Yin, H. Zhao, D. G. Mazzone, H. Miao, M. H. Upton, D. Casa, R. S. Acevedo-Esteves, C. Nelson, A. M. Barbour, C. Mazzoli, G. Cao, and M. P. M. Dean,Phys. Rev. Lett.129, 207201(2022)

Highlights: New Type of Quantum Liquid in a Un-frustrated Lattice Ba4Ir3O10: Trimer units (ovals on top) recombine into c-axis 1D zigzag chains (solid lines) that couple via the remaining trimer-midpoint spins (dashed lines). The average frustration parameter is greater than 2000.

Schematic of quantum liquid