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Register a new userExciton propagation and halo formation in two-dimensional materials
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The interplay of optics, dynamics and transport is crucial for the design of novel optoelectronic devices, such as photodetectors and solar cells. In this context, transition metal dichalcogenides (TMDs) have received much attention. Here, strongly bound excitons dominate optical excitation, carrier dynamics and diffusion processes. While the first two have been intensively studied, there is a lack of fundamental understanding of non-equilibrium phenomena associated with exciton transport that is of central importance e.g. for high efficiency light harvesting. In this work, we provide microscopic insights into the interplay of exciton propagation and many-particle interactions in TMDs. Based on a fully quantum mechanical approach and in excellent agreement with photoluminescence measurements, we show that Auger recombination and emission of hot phonons act as a heating mechanism giving rise to strong spatial gradients in excitonic temperature. The resulting thermal drift leads to an unconventional exciton diffusion characterized by spatial exciton halos.
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Noncentrosymmetric nature of single-layer transition metal dichalcogenides manifest itself in the finite piezoelectricity and valley-Zeeman coupling. We microscopically model nonlinear exciton transport in nano-bubble of single-layers of transition metal dichalcogenide. Thanks to the giant piezoelectric effect, we obtain an enormous internal electric field, $E_{rm piezo}sim 10^7$V/m, resulting in a built-in dipole moment of excitons. We demonstrate that the piezo-induced dipole-dipole interaction provides a novel channel for the nonlinear exciton transport distinct from the conventional isotropic funneling of excitons and leading to the formation of hexagon-shaped exciton droplet on top of a circularly symmetric nano-bubble. The effect is tunable via the bubble size dependence of the piezo-electric field $E_{rm piezo} sim h^2_{rm max}/R^3$ with $h_{rm max}$ and $R$ being the bubble height and radius, respectively.
Exciton problem is solved in the two-dimensional Dirac model with allowance for strong electron-hole attraction. The exciton binding energy is assumed smaller than but comparable to the band gap. The exciton wavefunction is found in the momentum space as a superposition of all four two-particle states including electron and hole states with both positive and negative energies. The matrix element of exciton generation is shown to depend on the additional components of the exciton wavefunction. Both the Coulomb and the Rytova-Keldysh potentials are considered. The dependence of the binding energy on the coupling constant is analyzed for the ground and first excited exciton states. The binding energy and the oscillator strength are studied as functions of the environmental-dependent dielectric constant for real transition metal dichalcogenide monolayers. We demonstrate that the multicomponent nature of the exciton wavefunction is crucial for description of resonant optical properties of two-dimensional Dirac systems.
Spatially resolved EELS has been performed at diffuse interfaces between MoS$_2$ and MoSe$_2$ single layers. With a monochromated electron source (20 meV) we have successfully probed excitons near the interface by obtaining the low loss spectra at the nanometer scale. The exciton maps clearly show variations even with a 10 nm separation between measurements; consequently the optical bandgap can be measured with nanometer-scale resolution, which is 50 times smaller than the wavelength of the emitted photons. By performing core-loss EELS at the same regions, we observe that variations in the excitonic signature follow the chemical composition. The exciton peaks are observed to be broader at interfaces and heterogeneous regions, possibly due to interface roughness and alloying effects. Moreover, we do not observe shifts of the exciton peak across the interface, possibly because the interface width is not much larger than the exciton Bohr radius.
We study exciton radiative decay in a two-dimensional material, taking into account large thermal population in the non-radiative states, from which excitons are scattered into the radiative states by acoustic phonons. We find an analytical solution of the kinetic equation for the non-equilibrium distribution function of excitons in the radiative states. Our estimates for bright excitons in transition metal dichalcogenides indicate a strong depletion of radiative state population due to insufficient exciton-phonon scattering rate at low temperatures.
Low-dimensional materials differ from their bulk counterpart in many respects. In particular, the screening of the Coulomb interaction is strongly reduced, which can have important consequences such as the significant increase of exciton binding energies. In bulk materials the binding energy is used as an indicator in optical spectra to distinguish different kinds of excitons, but this is not possible in low-dimensional materials, where the binding energy is large and comparable in size for excitons of very different localization. Here we demonstrate that the exciton band structure, which can be accessed experimentally, instead provides a powerful way to identify the exciton character. By comparing the ab initio solution of the many-body Bethe-Salpeter equation for graphane and single-layer hexagonal BN, we draw a general picture of the exciton dispersion in two-dimensional materials, highlighting the different role played by the exchange electron-hole interaction and by the electronic band structure. Our interpretation is substantiated by a prediction for phosphorene.
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