Atomic-level defects in van der Waals (vdW) materials
are essential
building blocks for quantum technologies and quantum sensing applications.
The layered magnetic semiconductor CrSBr is an outstanding candidate
for exploring optically active defects because of a direct gap, in
addition to a rich magnetic phase diagram, including a recently hypothesized
defect-induced magnetic order at low temperature. Here, we show optically
active defects in CrSBr that are probes of the local magnetic environment.
We observe a spectrally narrow (1 meV) defect emission in CrSBr that
is correlated with both the bulk magnetic order and an additional
low-temperature, defect-induced magnetic order. We elucidate the origin
of this magnetic order in the context of local and nonlocal exchange
coupling effects. Our work establishes vdW magnets like CrSBr as an
exceptional platform to optically study defects that are correlated
with the magnetic lattice. We anticipate that controlled defect creation
allows for tailor-made complex magnetic textures and phases with direct
optical access.
Correlated
quantum phenomena in one-dimensional (1D)
systems that
exhibit competing electronic and magnetic order are of strong interest
for the study of fundamental interactions and excitations, such as
Tomonaga–Luttinger liquids and topological orders and defects
with properties completely different from the quasiparticles expected
in their higher-dimensional counterparts. However, clean 1D electronic
systems are difficult to realize experimentally, particularly for
magnetically ordered systems. Here, we show that the van der Waals
layered magnetic semiconductor CrSBr behaves like a quasi-1D material
embedded in a magnetically ordered environment. The strong 1D electronic
character originates from the Cr–S chains and the combination
of weak interlayer hybridization and anisotropy in effective mass
and dielectric screening, with an effective electron mass ratio of m
X
e/m
Y
e ∼ 50. This extreme
anisotropy experimentally manifests in strong electron–phonon
and exciton–phonon interactions, a Peierls-like structural
instability, and a Fano resonance from a van Hove singularity of similar
strength to that of metallic carbon nanotubes. Moreover, because of
the reduced dimensionality and interlayer coupling, CrSBr hosts spectrally
narrow (1 meV) excitons of high binding energy and oscillator
strength that inherit the 1D character. Overall, CrSBr is best understood
as a stack of weakly hybridized monolayers and appears to be an experimentally
attractive candidate for the study of exotic exciton and 1D-correlated
many-body physics in the presence of magnetic order.
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