Nathan Wilson

Probing the Influence of Dielectric Environment on Excitons in Monolayer WSe2: Insight from High Magnetic Fields

Excitons in atomically thin semiconductors necessarily lie close to a surface, and therefore their properties are expected to be strongly influenced by the surrounding dielectric environment. However, systematic studies exploring this role are challenging, in part because the most readily accessible exciton parameter-the excitons optical transition energy-is largely unaffected by the surrounding medium. Here we show that the role of the dielectric environment is revealed through its systematic influence on the size of the exciton, which can be directly measured via the diamagnetic shift of the exciton transition in high magnetic fields. Using exfoliated WSe2 monolayers affixed to single-mode optical fibers, we tune the surrounding dielectric environment by encapsulating the flakes with different materials and perform polarized low-temperature magneto-absorption studies to 65 T. The systematic increase of the excitons size with dielectric screening, and concurrent reduction in binding energy (also inferred from these measurements), is quantitatively compared with leading theoretical models. These results demonstrate how exciton properties can be tuned in future 2D optoelectronic devices.

Giant tunneling magnetoresistance in spin-filter van der Waals heterostructures

An intrinsic magnetic tunnel junction An electrical current running through two stacked magnetic layers is larger if their magnetizations point in the same direction than if they point in opposite directions. These so-called magnetic tunnel junctions, used in electronics, must be carefully engineered. Two groups now show that high magnetoresistance intrinsically occurs in samples of the layered material CrI3 sandwiched between graphite contacts. By varying the number of layers in the samples, Klein et al. and Song et al. found that the electrical current running perpendicular to the layers was largest in high magnetic fields and smallest near zero field. This observation is consistent with adjacent layers naturally having opposite magnetizations, which align parallel to each other in high magnetic fields. Science, this issue p. 1218, p. 1214 The atomic layers of the material CrI3 act as spin filters in graphite/CrI3/graphite junctions. Magnetic multilayer devices that exploit magnetoresistance are the backbone of magnetic sensing and data storage technologies. Here, we report multiple-spin-filter magnetic tunnel junctions (sf-MTJs) based on van der Waals (vdW) heterostructures in which atomically thin chromium triiodide (CrI3) acts as a spin-filter tunnel barrier sandwiched between graphene contacts. We demonstrate tunneling magnetoresistance that is drastically enhanced with increasing CrI3 layer thickness, reaching a record 19,000% for magnetic multilayer structures using four-layer sf-MTJs at low temperatures. Using magnetic circular dichroism measurements, we attribute these effects to the intrinsic layer-by-layer antiferromagnetic ordering of the atomically thin CrI3. Our work reveals the possibility to push magnetic information storage to the atomically thin limit and highlights CrI3 as a superlative magnetic tunnel barrier for vdW heterostructure spintronic devices.

Electrical control of 2D magnetism in bilayer CrI 3

Controlling magnetism via electric fields addresses fundamental questions of magnetic phenomena and phase transitions1–3, and enables the development of electrically coupled spintronic devices, such as voltage-controlled magnetic memories with low operation energy4–6. Previous studies on dilute magnetic semiconductors such as (Ga,Mn)As and (In,Mn)Sb have demonstrated large modulations of the Curie temperatures and coercive fields by altering the magnetic anisotropy and exchange interaction2,4,7–9. Owing to their unique magnetic properties10–14, the recently reported two-dimensional magnets provide a new system for studying these features15–19. For instance, a bilayer of chromium triiodide (CrI3) behaves as a layered antiferromagnet with a magnetic field-driven metamagnetic transition15,16. Here, we demonstrate electrostatic gate control of magnetism in CrI3 bilayers, probed by magneto-optical Kerr effect (MOKE) microscopy. At fixed magnetic fields near the metamagnetic transition, we realize voltage-controlled switching between antiferromagnetic and ferromagnetic states. At zero magnetic field, we demonstrate a time-reversal pair of layered antiferromagnetic states that exhibit spin-layer locking, leading to a linear dependence of their MOKE signals on gate voltage with opposite slopes. Our results allow for the exploration of new magnetoelectric phenomena and van der Waals spintronics based on 2D materials.Electrical control of magnetism in a bilayer of CrI3 enables the realization of an electrically driven magnetic phase transition and the observation of the magneto-optical Kerr effect in 2D magnets.

Interlayer valley excitons in heterobilayers of transition metal dichalcogenides

Stacking different two-dimensional crystals into van der Waals heterostructures provides an exciting approach to designing quantum materials that can harness and extend the already fascinating properties of the constituents. Heterobilayers of transition metal dichalcogenides are particularly attractive for low-dimensional semiconductor optics because they host interlayer excitons—with electrons and holes localized in different layers—which inherit valley-contrasting physics from the monolayers and thereby possess various novel and appealing properties compared to other solid-state nanostructures. This Review presents the contemporary experimental and theoretical understanding of these interlayer excitons. We discuss their unique optical properties arising from the underlying valley physics, the strong many-body interactions and electrical control resulting from the electric dipole moment, and the unique effects of a moiré superlattice on the interlayer exciton potential landscape and optical properties.This Review discusses the contemporary experimental and theoretical understanding of interlayer excitons in heterobilayers of transition metal dichalcogenides.

Valley Manipulation by Optically Tuning the Magnetic Proximity Effect in WSe2/CrI3 Heterostructures

Monolayer valley semiconductors, such as tungsten diselenide (WSe2), possess valley pseudospin degrees of freedom that are optically addressable but degenerate in energy. Lifting the energy degeneracy by breaking time-reversal symmetry is vital for valley manipulation. This has been realized by directly applying magnetic fields or via pseudomagnetic fields generated by intense circularly polarized optical pulses. However, sweeping large magnetic fields is impractical for devices, and the pseudomagnetic fields are only effective in the presence of ultrafast laser pulses. The recent rise of two-dimensional (2D) magnets unlocks new approaches to controlling valley physics via van der Waals heterostructure engineering. Here, we demonstrate the wide continuous tuning of the valley polarization and valley Zeeman splitting with small changes in the laser-excitation power in heterostructures formed by monolayer WSe2 and 2D magnetic chromium triiodide (CrI3). The valley manipulation is realized via the optical control of the CrI3 magnetization, which tunes the magnetic exchange field over a range of 20 T. Our results reveal a convenient new path toward the optical control of valley pseudospins and van der Waals magnetic heterostructures.