Pressure tuning of competing interactions on a honeycomb lattice

Piyush Sakrikar, Bin Shen, Eduardo H.T. Poldi, Faranak Bahrami, Xiaodong Hu, Eric M. Kenney, Qiaochu Wang, Kyle W. Fruhling, Chennan Wang, Ritu Gupta, Rustem Khasanov, Hubertus Luetkens, Stuart A. Calder, Adam A. Aczel, Gilberto Fabbris, Russell J. Hemley, Kemp W. Plumb, Ying Ran, Philipp Gegenwart, Alexander A. TsirlinDaniel Haskel, Michael J. Graf, Fazel Tafti

Research output: Contribution to journalArticlepeer-review

Abstract

Exchange interactions are mediated via orbital overlaps across chemical bonds. Thus, modifying the bond angles by physical pressure or strain can tune the relative strength of competing interactions. Here we present a remarkable case of such tuning between the Heisenberg (J) and Kitaev (K) exchange, which respectively establish magnetically ordered and spin liquid phases on a honeycomb lattice. We observe a rapid suppression of the Néel temperature (TN) with pressure in Ag3LiRh2O6, a spin-1/2 honeycomb lattice with both J and K couplings. Using a combined analysis of x-ray data and first-principles calculations, we find that pressure modifies the bond angles in a way that increases the ∣K/J∣ ratio and thereby suppresses TN. Consistent with this picture, we observe a spontaneous onset of muon spin relaxation (μSR) oscillations below TN at low pressure, whereas in the high pressure phase, oscillations appear only when T < TN/2. Unlike other candidate Kitaev materials, Ag3LiRh2O6is tuned toward a quantum critical point by pressure while avoiding a structural dimerization in the relevant pressure range.

Original languageEnglish
Article number4712
JournalNature Communications
Volume16
Issue number1
DOIs
StatePublished - Dec 2025

Funding

The authors thank L. Hozoi for fruitful discussions. The work at Boston College was funded by the US Department of Energy, Office of Basic Energy Sciences, Division of Physical Behavior of Materials under award number DE-SC0023124. The work in Augsburg was funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)\u2014TRR 360-492547816. Bin Shen acknowledges the financial support of the Alexander von Humboldt Foundation. K.W.P. and Q.W. were supported by the US Department of Energy, Office of Basic Energy Sciences, under Grant No. DE-SC0021223. This work is based in part on experiments performed at the Swiss Muon Source S\u03BCS, Paul Scherrer Institute, Villigen, Switzerland. Neutron scattering experiments were carried out at the High Flux Isotope Reactor and Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Y.R. and X.H. acknowledge support from the National Science Foundation under Grant No. DMR-1712128. E.P. and R.J.H. acknowledge support from DOE-SC (DE-SC0020340), DOE-NNSA (DE-NA0003975), and NSF (DMR-2118020 and DMR-2119308). Operations of HPCAT (Sector 16, APS, ANL) are supported by DOE-NNSA\u2019s Office of Experimental Sciences. Work at the Advanced Photon Source was supported by the US Department of Energy Office of Science, Office of Basic Energy Sciences, under Award No. DE-AC02-06CH11357.

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