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Register a new userDefect healing and charge transfer mediated valley polarization in MoS$_2$/MoSe$_2$/MoS$_2$ trilayer van der Waals heterostructures
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Paulina Plochocka Dr
Publication date
2017
fields
Physics
and research's language is
English
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Monolayer transition metal dichalcogenides (TMDC) grown by chemical vapor deposition (CVD) are plagued by a significantly lower optical quality compared to exfoliated TMDC. In this work we show that the optical quality of CVD-grown MoSe$_2$ is completely recovered if the material is sandwiched in MoS$_2$/MoSe$_2$/MoS$_2$ trilayer van der Waals heterostructures. We show by means of density-functional theory that this remarkable and unexpected result is due to defect healing: S atoms of the more reactive MoS$_2$ layers are donated to heal Se vacancy defects in the middle MoSe$_2$ layer. In addition, the trilayer structure exhibits a considerable charge-transfer mediated valley polarization of MoSe$_2$ without the need for resonant excitation. Our fabrication approach, relying solely on simple flake transfer technique, paves the way for the scalable production of large-area TMDC materials with excellent optical quality.
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In this letter we present photoluminescence measurements with different excitation energies on single-layer MoS$_2$ and MoSe$_2$ in order to examine the resonance behavior of the conservation of circular polarization in these transition metal dichalcogenides. We find that the circular polarization of the emitted light is conserved to 100% in MoS$_2$ and 84% / 79% (A/A$^-$ peaks) in MoSe$_2$ close to resonance. The values for MoSe$_2$ surpass any previously reported value. However, in contrast to previous predictions, the degree of circular polarization decreases clearly at energies less than the two-phonon longitudinal acoustic phonon energy above the resonance. Our findings indicate that at least two competing processes underly the depolarization of the emission in single-layer transition metal dichalcogenides.
The optics of dangling-bond-free van der Waals heterostructures containing transition metal dichalcogenides are dominated by excitons. A crucial property of a confined exciton is the quantum confined Stark effect (QCSE). Here, such a heterostructure is used to probe the QCSE by applying a uniform vertical electric field across a molybdenum disulfide (MoS$_2$) monolayer. The photoluminescence emission energies of the neutral and charged excitons shift quadratically with the applied electric field provided the electron density remains constant, demonstrating that the exciton can be polarized. Stark shifts corresponding to about half the homogeneous linewidth were achieved. Neutral and charged exciton polarizabilities of $(7.8~pm~1.0)times 10^{-10}~tr{D~m~V}^{-1}$ and $(6.4~pm~0.9)times 10^{-10}~tr{D~m~V}^{-1}$ at relatively low electron density ($8 times 10^{11}~tr{cm}^{-2}$) have been extracted, respectively. These values are one order of magnitude lower than the previously reported values, but in line with theoretical calculations. The methodology presented here is versatile and can be applied to other semiconducting layered materials as well.
Degenerate extrema in the energy dispersion of charge carriers in solids, also referred to as valleys, can be regarded as a binary quantum degree of freedom, which can potentially be used to implement valleytronic concepts in van der Waals heterostructures based on transition metal dichalcogenides. Using magneto-photoluminescence spectroscopy, we achieve a deeper insight into the valley polarization and depolarization mechanisms of interlayer excitons formed across a MoS$_2$/MoSe$_2$/MoS$_2$ heterostructure. We account for the non-trivial behavior of the valley polarization as a function of the magnetic field by considering the interplay between exchange interaction and phonon mediated intervalley scattering in a system consisting of Zeeman-split energy levels. Our results represent a crucial step towards the understanding of the properties of interlayer excitons, with strong implications for the implementation of atomically thin valleytronic devices.
Semiconducting ferromagnet-nonmagnet interfaces in van der Waals heterostructures present a unique opportunity to investigate magnetic proximity interactions dependent upon a multitude of phenomena including valley and layer pseudospins, moire periodicity, or exceptionally strong Coulomb binding. Here, we report a charge-state dependency of the magnetic proximity effects between MoSe$_2$ and CrBr$_3$ in photoluminescence, whereby the valley polarization of the MoSe$_2$ trion state conforms closely to the local CrBr$_3$ magnetization, while the neutral exciton state remains insensitive to the ferromagnet. We attribute this to spin-dependent interlayer charge transfer occurring on timescales between the exciton and trion radiative lifetimes. Going further, we uncover by both the magneto-optical Kerr effect and photoluminescence a domain-like spatial topography of contrasting valley polarization, which we infer to be labyrinthine or otherwise highly intricate, with features smaller than 400 nm corresponding to our optical resolution. Our findings offer a unique insight into the interplay between short-lived valley excitons and spin-dependent interlayer tunnelling, while also highlighting MoSe$_2$ as a promising candidate to optically interface with exotic spin textures in van der Waals structures.
The optical and electronic properties of 2D semiconductors are intrinsically linked via the strong interactions between optically excited bound species and free carriers. Here we use near-field scanning microwave microscopy (SMM) to image spatial variations in photoconductivity in MoS$_2$--WS$_2$ lateral multijunction heterostructures using photon energy-resolved narrowband illumination. We find that the onset of photoconductivity in individual domains corresponds to the optical absorption onset, confirming that the tightly bound excitons in transition metal dichalcogenides can nonetheless dissociate into free carriers. These photogenerated carriers are most likely n-type and are seen to persist for up to days, and informed by finite element modeling we reveal that they can increase the carrier density by up to 200 times. This persistent photoconductivity appears to be dominated by contributions from the multilayer MoS$_2$ domains, and we attribute the flake-wide response in part to charge transfer across the heterointerface. Spatial correlation of our SMM imaging with photoluminescence (PL) mapping confirms the strong link between PL peak emission photon energy, PL intensity, and the local accumulated charge. This work reveals the spatially and temporally complex optoelectronic response of these systems and cautions that properties measured during or after illumination may not reflect the true dark state of these materials but rather a metastable charged state.
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