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Kinetic Magnetism in Triangular Moiré Materials
Kinetic Magnetism in Triangular Moiré Materials
Moiré heterostructures of two-dimensional materials provide We study two R-type MoSe2/WS2 heterostructures encapsulated in
a platform for the investigation of the physics of strongly corre- h-BN. The lattice mismatch and twist angle between the TMD monolay-
lated electrons. In contrast to well-studied quantum materials, ers create a moiré superlattice with a lattice constant of about 7.5 nm.
these moiré materials provide a very high degree of tunability of The minima of the resulting electronic potential for the conduction
the parameters relevant for controlling correlations, such as carrier band are located at high-symmetry points at which the metal atoms in
density and the ratio of interaction energy to hopping strength. the two layers are aligned (MM sites). The electrons that are injected
Moreover, unlike cold-atom quantum simulators, the physics and occupy the triangular lattice of MM sites as shown in Fig. 1a. In sample I,
functionality of moiré materials can be varied using readily accessible the charge density and the electric field in the heterostructure can be
external electric and magnetic fields, creating a platform in which tuned independently using top and bottom graphene gates, whereas
different many-body phases compete. Since the first realization of sample II is only single-gated.
a moiré material, a wealth of correlation physics ranging from cor-
related Mott–Wigner states to the quantum anomalous Hall effect to
superconductivity has been observed both in magic-angle-twisted Doping-dependent spectrum of MoSe2/WS2
bilayer graphene and in bilayers of transition metal dichalcoge- The reflection spectrum as a function of electron density in Fig. 1b
nides (TMDs)11–21. Except for orbital magnetism in twisted bilayer shows several resonances close to the energy of the optical transitions
graphene15,22 as well as early spin susceptibility and scanning probe in monolayer MoSe2, consistent with previous reports32,33. Intensity
measurements in TMD bilayers17,23–26, quantum magnetism in moiré maxima and cusps in the resonance energies appear at equally spaced
materials has until recently remained experimentally unexplored. gate voltages (see Extended Data Fig. 2 for extended range). These volt-
Theoretical works have investigated the magnetic properties of the ages correspond to commensurate filling of the moiré superlattice with
correlated Mott state in a moiré lattice with one electron per lat- one or two electrons per site (ν = 1 and 2, respectively), at which incom-
tice site27,28 and focused on the possibility of realizing quantum spin pressible states are formed. We focus here on the resonance at 1.58 eV,
liquids29–31. which can be identified as an attractive polaron resonance associated
Here we investigate the magnetic properties of electrons in MoSe2/ with collective excitation of bound electron–exciton pairs (trions)
WS2 heterobilayers using low-temperature confocal microscopy. We located at the moiré potential minima9,10,34. As shown in Fig. 1c, the
focus on magnetization as a function of temperature T and out-of-plane area, or equivalently the oscillator strength, of the attractive polaron
magnetic field Bz at dopings around one electron per moiré lattice resonance increases linearly as a function of electron density up to
site (ν = 1). For ν > 1, our experiments show that the itinerant electrons filling factor ν = 1 and subsequently decreases again linearly between
exhibit a positive Curie–Weiss constant θCW. The linear increase in spin ν = 1 and 2.
susceptibility as a function of the density of doubly occupied sites at This behaviour is consistent with the presence of an isolated Hub-
T ≈ 140 mK is indicative of kinetic ferromagnetic correlations linked bard band in which all electrons occupy the same lattice sites, forming
to the Nagaoka mechanism1,2. doubly occupied sites (doublons) for ν > 1 and empty sites (holons) for
1
Institute for Quantum Electronics, ETH Zürich, Zürich, Switzerland. 2Departament de Física Quàntica i Astrofísica, Facultat de Física, Universitat de Barcelona, Barcelona, Spain. 3Institut de
Ciències del Cosmos, Universitat de Barcelona, Barcelona, Spain. 4Department of Physics and Astronomy, University of Tennessee, Knoxville, TN, USA. 5Min H. Kao Department of Electrical
Engineering and Computer Science, University of Tennessee, Knoxville, TN, USA. 6Research Center for Electronic and Optical Materials, National Institute for Materials Science, Tsukuba, Japan.
7
Research Center for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan. 8Institute for Theoretical Physics, ETH Zürich, Zürich, Switzerland. 9These authors
contributed equally: L. Ciorciaro, T. Smoleński, I. Morera. ✉e-mail: imamoglu@phys.ethz.ch
Q= 0 1
1 2
1.66
AP area
1.64
0
0 1 2
1.62 Filling factor Q
Energy (eV)
d V+
V−
1.60 2
ΔR/R0
x2
1.58 1
0 2 4 6 8 1.60 1.65
Gate voltage (V) Energy (eV)
Fig. 1 | Optical response of the moiré bilayer. a, Moiré potential in the polaron (AP) resonance as function filling factor at B z = 0. The linear increase
conduction band. Electrons occupy the potential minima at the MM sites. and decrease confirm that electrons occupy a single minimum in the moiré unit
b, Gate-voltage-dependent normalized reflectance spectrum ΔR/R0 = cell, forming an isolated Hubbard band. d, Polarization-resolved reflection
(R − R0)/R0, where R is the reflection spectrum of MoSe2/WS2 and R0 is the spectrum at ν = 1, B z = 1 T and T = 4.2 K. The attractive polaron resonance at
background spectrum (see section ‘Background subtraction’). The gate 1.58 eV is sensitive to spin polarization of the electrons through its degree of
voltage tunes the doping of the heterostructure. At integer fillings, intensity circular polarization. The data in this figure were measured on sample II.
maxima and cusps in the resonance energies appear. c, Area of the attractive
T · dUAP/dBz (K T–1)
0.5
0.3 2
0
UAP
–0.5
–0.3 1
–10 0 10
–1.0
–300 –200 –100 0 100 200 300 1.0 1.5
Bz (mT) Filling factor Q
c d
Q = 1.0
Q = 1.3 100
0.5
(dUAP/dB)–1 (T)
TCW (mK)
–100
0
0 0.5 1.0 1.0 1.5
Temperature (K) Filling factor Q
Fig. 2 | Signatures of kinetic magnetism in single-frequency measurements diverges faster than 1/T for 1 < ν < 1.5. c, Inverse susceptibility as a function of
on sample I at low temperatures. a, Degree of polarization ρAP of the attractive temperature with linear fits yielding the Curie–Weiss constant θCW. d, Fitted
polaron resonance as a function of magnetic field B z . Inset, linear fit around Curie–Weiss constant as a function of ν. Vertical error bars correspond to
B z = 0 yielding the susceptibility. b, Doping dependence of the slope dρAP/dB z the standard error of the fit (b–d) and horizontal error bars (c) indicate the
around B z = 0 and at different temperatures T, each multiplied by T. A sharp uncertainty in the temperature measurement (see sections ‘Temperature
increase in spin susceptibility is observed beyond ν = 1, and the susceptibility calibration’ and ‘Curie–Weiss fit’).
paramagnetic behaviour for ν ≤ 1, ferromagnetic interactions for for a triangular lattice36. By contrast, the ferromagnetic correlations
1 < ν < 3/2 and anti-ferromagnetic interactions for ν > 3/2. We focus disappear for ν ≥ 3/2 in our experiments.
here on the origin of the ferromagnetic correlations. On the basis of these considerations and the fact that strong Coulomb
In general, exchange interactions are expected to play a key part in interactions put the moiré structure in the strongly correlated regime of
determining the magnetic order of the system. For a moiré structure extended Hubbard model physics, we attribute the observed magnetic
with a lattice constant of 7.5 nm, the on-site repulsion is large, leading interactions to the Nagaoka mechanism: in a Hubbard band close to
to small super-exchange interactions Jsup. By contrast, strong Coulomb half filling (ν = 1), mobile charge carriers can reduce their kinetic energy
interactions together with finite overlap of localized Wannier orbitals by inducing magnetic order even in the limit of vanishing exchange
could ensure that the strength of direct exchange Jdir exceeds that of Jsup interactions1,2,37. The linear increase in the Curie–Weiss constant at small
(ref. 28). Using first-principles calculations, we estimate Jdir = − 0.61 meV doublon doping experimentally agrees with the theoretical prediction
(see section ‘Model parameters’). The magnetic properties at ν = 1, for of this model5. Each injected doublon creates a small ferromagnetic
which the electrons form an incompressible Mott insulator and are region (magnetic polaron) that results in a linear dependence of fer-
localized on moiré lattice sites, should be exclusively determined by romagnetic interactions with doping. The dip in the susceptibility and
exchange interactions. Surprisingly, we do not find a significant devia- Curie–Weiss constant at ν = 4/3 (Fig. 2b,d, dashed line) further corrobo-
tion from paramagnetic behaviour at ν = 1 (Fig. 2b,d). This suggests rates the kinetic nature of the magnetic interactions: at commensurate
that predictions based on density functional theory calculations do fractional fillings, the electrons form incompressible Mott–Wigner
not fully capture the physics of our system and exchange interactions states18,25,32, suppressing the contribution of kinetic energy.
do not play a notable part in determining the magnetic properties We note that the disappearance of ferromagnetic correlations at
of electrons. A possible explanation for this is that the electrons are ν = 3/2 could be associated with the emergence of a spatially ordered
more strongly localized than predicted by theory because of a deeper structure with a larger period, such as a stripe phase or paired electron
moiré potential. crystal. However, treatment of the behaviour at this large doublon
Although we cannot rule out a contribution from exchange interac- density is beyond the scope of our work.
tions, the asymmetric behaviour for ν = 1 ± δ cannot be accounted for
by a purely exchange-based mechanism, as it would give rise to similar
magnetic interactions for doublon and holon doping. Moreover, a Theoretical model and numerical analysis
Stoner instability or flat band ferromagnetism would probably lead In a single-band Fermi–Hubbard model on a triangular lattice in the
to signatures peaking at the van Hove singularity located at ν = 3/2 strongly interacting regime, the ferromagnetic interactions for
t t+A Conclusion
We demonstrated that the spin susceptibility of electrons in moiré
materials can be accurately determined through polarization-resolved
attractive polaron oscillator strength measurements at pW power
levels. We have used this method to study the filling-factor-dependent
b c spin susceptibility and found a sudden appearance of ferromagnetic
1.0
correlations for ν > 1. Our experimental findings, supported by ten-
Ms(Q)
F(Q)
0 0
0 30 our observation of a paramagnetic response at ν = 1 suggests that
1.0 0 20 30
direct exchange and super-exchange interactions are weak and the
0.8 1.0 1.2 1.4 0 0.2 0.4
spin physics is dominated by effective kinetic interactions. The strong
Filling factor Q gPBB/t
asymmetry between ν < 1 and ν > 1 indicates the presence of a large
Coulomb-assisted hopping of doublons. Moreover, long-range Cou-
Fig. 3 | Theoretical analysis of kinetic magnetism strength. a, Hopping lomb interactions and disorder renormalize the effective hopping for
processes for holons and doublons. The presence of long-range interactions holons and doublons, which in turn ensures that magnetic order in
introduces an assisted hopping A that modifies the doublon hopping strength. deep moiré potentials exhibiting topologically trivial bands may be
b, Simulated spin susceptibility as a function of filling factor for assisted observed for only very low temperatures below 100 mK.
hopping A = 10t and temperature kBT = A, but in the absence of nearest-neighbour During the preparation of this paper, we became aware of several
Coulomb interaction (V = 0), disorder (Δ = 0) and exchange interactions parallel works exploring different aspects of magnetism in bilayer
( Jdir = 0 = Jsup). The assisted hopping leads to an asymmetry between doublons
MoTe2 moiré structures38–40.
and holons. The normalization is chosen such that the value 1 corresponds to a
paramagnetic response. c, Simulated degree of spin polarization as a function
of the magnetic field at ν = 0.89 and T = 0. Both disorder with distribution
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ferromagnetic correlations. Error bars correspond to the standard deviation Any methods, additional references, Nature Portfolio reporting summa-
from multiple disorder realizations. ries, source data, extended data, supplementary information, acknowl-
edgements, peer review information; details of author contributions
and competing interests; and statements of data and code availability
doublon doping induced by the kinetic mechanism are accompanied are available at https://doi.org/10.1038/s41586-023-06633-0.
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Extended Data Fig. 2 | Optical response of the moiré bilayer in an extended voltage range. Normalized reflectance spectrum measured as a function of the
applied gate voltage on sample I in an extended voltage range.
Extended Data Fig. 3 | High-temperature measurements of electron spin slope dρAP/dB z measured at two different powers, plotted as function of
polarization on sample II. a, Inverse slope dρAP/dB z measured at ν = 0.75 as temperature and filling factor. The power dependence changes with both
function of temperature for different excitation powers. For each power, the temperature and filling factor and is most prominent at small ν and low
data are precisely reproduced by the Curie–Weiss formula with the Curie– temperatures. The grey dashed lines mark contours of fixed susceptibility
Weiss constant getting sizably lower for larger powers due to light-induced ratios (as indicated). d, Degree of polarization measured at fixed magnetic
electron spin depolarization. b, Fitted CurieWeiss constant as function of field of B z = 9 T with different excitation powers and base temperature of the
electron filling factor for three different excitation powers. For ν < 1, the dilution refrigerator. Even at high magnetic field, an excitation power of 19 nW
light-induced spin depolarization leads to apparent negative Curie–Weiss is sufficient at mK temperatures to strongly depolarize the spins and reduce ρAP
constants. Error bars correspond to the standard error of the fit. c, Ratio of the from 1.0 to 0.7.
Article
Extended Data Fig. 6 | Measurement of the optical spin-pumping effect. the vertical axis, indicating that the magnetization is slightly affected by the
a, Reflection of a laser (11.7 pW) resonant with the attractive polaron as function laser polarization. b, Same data as in a but with the σ+ points mirrored on the
of magnetic field measured in both circular polarizations, normalized to lie in horizontal axis. The loop formed by the two curves indicates a small optical
the range [ − 1, 1]. The crossing of the two curves occurs at a negative value on spin-pumping effect.
Extended Data Fig. 7 | Detailed low-temperature magnetization curves for
different electron densities. Degree of polarization ρAP measured as a
function of the magnetic field for several filling factors of the moiré lattice.
Article
Extended Data Fig. 8 | Curie–Weiss temperature determined using a the minimum temperature shifts the curve vertically without affecting it
different temperature calibration. Curie–Weiss constant as function of qualitatively. Error bars correspond to the standard error of the fit.
filling factor for different Tmin used in the temperature calibration. Changing
Extended Data Fig. 9 | Exciton energy in MoSe2 monolayer as a function of
temperature. The energy of exciton optical transition measured at charge-
neutrality for MoSe2 monolayer at different temperatures. The solid line marks
the quadratic fit to the data EX(T) = E0 − γT2 with E0 = 1.6352 eV and γ = 1.57 μeV/K 2.
Article