We report the successful synthesis of single crystals of the layered iridate (Na1−xLix)2IrO3, 0 ≤ x ≤ 0.9, and a thorough study of its structural, magnetic, thermal, and transport properties. This compound allows a controlled interpolation between Na2IrO3 and Li2IrO3, while maintaining the quantum magnetism of the honeycomb Ir4+ planes. The measured phase diagram demonstrates a suppression of the Néel temperature TN at an intermediate x, indicating that the magnetic orders in Na2IrO3 and Li2IrO3 are distinct. X-ray data show that for x ≈ 0.7, when TN is suppressed the most, the honeycomb structure is least distorted, leading to the speculation that at this intermediate doping of the material is closest to the spin liquid that has been sought after in Na2IrO3 and Li2IrO3. By analyzing our magnetic data with a single-ion theoretical model we also show that the trigonal splitting on the Ir4+ ions changes sign from Na2IrO3 to Li2IrO3.

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Published in Physical Review B, v. 88, issue 22, 220414, p. 1-4.

©2013 American Physical Society

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This work was supported by the National Science Foundation under Grants No. DMR-0856234, No. EPS-0814194, No. DMR-1265162, and No. DMR-1056536 (R.K.K. and M.T.).

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See Supplemental Material at http://link.aps.org/supplemental/ 10.1103/PhysRevB.88.220414 for methods of crystal growth, additional measurements and details of theoretical calculations.

NaLiIrO_supp.pdf (1540 kB)
Supplemental Material