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Pressure tuning of competing interactions on a honeycomb lattice

Journal Article · · Nature Communications
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  1. Boston College, Chestnut Hill, MA (United States)
  2. University of Augsburg (Germany)
  3. University of Illinois, Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
  4. Boston College, Chestnut Hill, MA (United States); High Energy Accelerator Research Organization (KEK), Ibaraki (Japan)
  5. Brown University, Providence, RI (United States)
  6. PSI Center for Neutron and Muon Sciences CNM, Villigen PSI (Switzerland)
  7. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  8. Argonne National Laboratory (ANL), Argonne, IL (United States)
  9. University of Illinois, Chicago, IL (United States)
+ Show Author Affiliations
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, Ag3LiRh2O6 is tuned toward a quantum critical point by pressure while avoiding a structural dimerization in the relevant pressure range.
Research Organization:
Boston College, Chestnut Hill, MA (United States); Chicago Office, Argonne, IL (United States); University of Illinois, Chicago, IL (United States)
Sponsoring Organization:
Deutsche Forschungsgemeinschaft; National Science Foundation; National Science Foundation (NSF); USDOE; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357; NA0003975; NA0004153; SC0020340; SC0021223; SC0023124
OSTI ID:
2567618
Alternate ID(s):
OSTI ID: 2568316
OSTI ID: 2568088
OSTI ID: 3018294
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 16; ISSN 2041-1723
Country of Publication:
United States
Language:
English

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Related Subjects

36 MATERIALS SCIENCE
74 ATOMIC AND MOLECULAR PHYSICS
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
Magnetic properties and materials
Pressure
Kitaev
spin liquid.