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Tunable Quantum Magnetism
in Frustrated Yb-Based van
der Waals Materials
Jiayi Li (329430)
Arun Ramanathan (9992643)
Thom J. Snoeren (14552217)
Willa Mihalyi-Koch (14351710)
Jamie Cleron (12361018)
Anna Champ (12530937)
Hemamala I. Karunadasa (1415041)
Mykhaylo Ozerov (5810771)
Daniel R. Gamelin (1286040)
Allen Scheie (10903972)
Xavier Roy (1395136)
Biophysics
Physical Sciences not elsewhere classified
Medicine
Evolutionary Biology
Environmental Sciences not elsewhere classified
Chemical Sciences not elsewhere classified
Ecology
Hematology
state kramers doublet
tunable quantum magnetism
systematic anion substitution
range correlation regimes
direct chemical handle
magnetic quantum criticality
powerful design principle
eff </ sub
quantum fluctuations
range order
magnetic order
ligand substitution
chemical modifications
>< sub
xy </
j </
f </
type lattice
systematically tune
suppressed long
replacing chalcogenide
photoluminescence reveal
notoriously difficult
infrared magnetospectroscopy
halide ligands
frustrated yb
diffuse reflectance
close proximity
), provides
The border between magnetic order and a quantum disordered
ground
state is notoriously difficult to reach by design. Here we show that
systematic anion substitution in a family of rare-earth van der Waals
(vdW) magnets, YbChX (Ch = S, Se; X = Br, I), provides a direct chemical
handle on this boundary. By replacing chalcogenide and halide ligands
on the FeOCl-type lattice, we systematically tune the crystal electric
field hierarchy, the degree of <i>XY</i> anisotropy, and
the strength of quantum fluctuations in the ground-state Kramers doublet,
affecting the exchange interactions without changing the distorted
triangular lattice topology. The result is a series of <i>J</i><sub>eff</sub> = 1/2 magnets with large frustration factors (<i>f</i> = 9–76), extended short-range correlation regimes,
and suppressed long-range order, placing the entire family in close
proximity to magnetic quantum criticality. Far-infrared magnetospectroscopy,
diffuse reflectance, and photoluminescence reveal that the same ligand
substitution that reshapes the magnetic landscape simultaneously tunes
f–f optical transitions, opening a route to access potential
spin–photon coupling through chemical modifications. These
results establish anion substitution as a powerful design principle
for chemically navigating frustrated quantum magnets toward exotic
ground states in the vdW family.
2026-10-01T00:00:00Z
Text
Journal contribution
10.1021/jacs.6c12112.s001
https://figshare.com/articles/journal_contribution/Tunable_Quantum_Magnetism_in_Frustrated_Yb-Based_van_der_Waals_Materials/34042337
CC BY-NC 4.0