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Register a new userLocalized Excitons in Defective Monolayer Germanium Selenide
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Arielle Cohen
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Germanium Selenide (GeSe) is a van der Waals-bonded layered material with promising optoelectronic properties, which has been experimentally synthesized for 2D semiconductor applications. In the monolayer, due to reduced dimensionality and, thus, screening environment, perturbations such as the presence of defects have a significant impact on its properties. We apply density functional theory and many-body perturbation theory to understand the electronic and optical properties of GeSe containing a single selenium vacancy in the $-2$ charge state. We predict that the vacancy results in mid-gap trap states that strongly localize the electron and hole density and lead to sharp, low-energy optical absorption peaks below the predicted pristine optical gap. Analysis of the exciton wavefunction reveals that the 2D Wannier-Mott exciton of the pristine monolayer is highly localized around the defect, reducing its Bohr radius by a factor of four and producing a dipole moment along the out-of-plane axis due to the defect-induced symmetry breaking. Overall, these results suggest that the vacancy is a strong perturbation to the system, demonstrating the importance of considering defects in the context of material design.
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Covalent amorphous semiconductors, such as amorphous silicon (a-Si) and germanium (a-Ge), are commonly believed to have localized electronic states at the top of the valence band and the bottom of the conduction band. Electrical conductivity is thought to be by the hopping mechanism through localized states. The carrier mobility of these materials is usually very low, in the order of ~10^-3 - 10^-2 cm^2/(Vs) at room temperature. In this study, we present the Hall effect characterization of a-Ge prepared by self-ion implantation of Ge ions. The a-Ge prepared by this method is highly homogenous and has a mass density within 98.5% of the crystalline Ge. The material exhibits an exceptionally high electrical conductivity and carrier mobility (~100 cm^2/(Vs)) for an amorphous semiconductor. The temperature-dependent resistivity of the material is very-well defined with two distinctive regions, extrinsic and intrinsic conductivity, as in crystalline Ge. These results are direct evidence for a largely-preserved band structure and non-localized states of the valence band in a-Ge, as proposed by Tauc et al. from optical characterization alone. This finding is not only significant for the understanding of electrical conductivity in covalent disordered semiconductors, but the exceptionally high mobility we have observed in amorphous Ge opens up device applications not previously considered for amorphous semiconductors.
The strong Coulomb forces in monolayer transition metal dichalcogenides ensure that optical excitation of band electrons gives rise to Wannier-Mott excitonic states, each of which can be conceptualized as a composite of a Gaussian wavepacket corresponding to center-of-mass motion and an orbital state corresponding to the motion of the electron and hole about the center-of-mass. Here, we show that at low temperature in monolayer MoS2, given quasi-localized excitons and consequently a significant inter-exciton spacing, the excitons undergo dipole-dipole interaction and annihilate one another in a manner analogous to Auger recombination. To construct our model, we assume that each exciton is localized in a region whose length is on the same scale as the excitonic diameter, thus causing the exciton to behave in a fermionic manner, while the distance between neighboring excitons is much larger than the exciton diameter. We construct the orbital ladder operators for each exciton and apply Fermis Golden Rule to derive the overall recombination rate as a function of exciton density.
Monolayer van der Waals (vdW) magnets provide an exciting opportunity for exploring two-dimensional (2D) magnetism for scientific and technological advances, but the intrinsic ferromagnetism has only been observed at low temperatures. Here, we report the observation of room temperature ferromagnetism in manganese selenide (MnSe$_x$) films grown by molecular beam epitaxy (MBE). Magnetic and structural characterization provides strong evidence that in the monolayer limit, the ferromagnetism originates from a vdW manganese diselenide (MnSe$_2$) monolayer, while for thicker films it could originate from a combination of vdW MnSe$_2$ and/or interfacial magnetism of $alpha$-MnSe(111). Magnetization measurements of monolayer MnSe$_x$ films on GaSe and SnSe$_2$ epilayers show ferromagnetic ordering with large saturation magnetization of ~ 4 Bohr magnetons per Mn, which is consistent with density functional theory calculations predicting ferromagnetism in monolayer 1T-MnSe$_2$. Growing MnSe$_x$ films on GaSe up to high thickness (~ 40 nm) produces $alpha$-MnSe(111), and an enhanced magnetic moment (~ 2x) compared to the monolayer MnSe$_x$ samples. Detailed structural characterization by scanning transmission electron microscopy (STEM), scanning tunneling microscopy (STM), and reflection high energy electron diffraction (RHEED) reveal an abrupt and clean interface between GaSe(0001) and $alpha$-MnSe(111). In particular, the structure measured by STEM is consistent with the presence of a MnSe$_2$ monolayer at the interface. These results hold promise for potential applications in energy efficient information storage and processing.
Just as photons are the quanta of light, plasmons are the quanta of orchestrated charge-density oscillations in conducting media. Plasmon phenomena in normal metals, superconductors and doped semiconductors are often driven by long-wavelength Coulomb interactions. However, in crystals whose Fermi surface is comprised of disconnected pockets in the Brillouin zone, collective electron excitations can also attain a shortwave component when electrons transition between these pockets. Here, we show that the band structure of monolayer transition-metal dichalcogenides gives rise to an intriguing mechanism through which shortwave plasmons are paired up with excitons. The coupling elucidates the origin for the optical side band that is observed repeatedly in monolayers of WSe$_2$ and WS$_2$ but not understood. The theory makes it clear why exciton-plasmon coupling has the right conditions to manifest itself distinctly only in the optical spectra of electron-doped tungsten-based monolayers.
When electron-hole pairs are excited in a semiconductor, it is a priori not clear if they form a fermionic plasma of unbound particles or a bosonic exciton gas. Usually, the exciton phase is associated with low temperatures. In atomically thin transition metal dichalcogenide semiconductors, excitons are particularly important even at room temperature due to strong Coulomb interaction and a large exciton density of states. Using state-of-the-art many-body theory including dynamical screening, we show that the exciton-to-plasma ratio can be efficiently tuned by dielectric substrate screening as well as charge carrier doping. Moreover, we predict a Mott transition from the exciton-dominated regime to a fully ionized electron-hole plasma at excitation densities between $3times10^{12}$ cm$^{-2}$ and $1times10^{13}$ cm$^{-2}$ depending on temperature, carrier doping and dielectric environment. We propose the observation of these effects by studying excitonic satellites in photoemission spectroscopy and scanning tunneling microscopy.
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