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Register a new userExciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors
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Two-dimensional group-VI transition metal dichalcogenide semiconductors, such as MoS2, WSe2 and others, exhibit strong light-matter coupling and possess direct band gaps in the infrared and visible spectral regimes, making them potentially interesting candidates for various applications in optics and optoelectronics. Here, we review their optical and optoelectronic properties with emphasis on exciton physics and devices. As excitons are tightly bound in these materials and dominate the optical response even at room-temperature, their properties are examined in depth in the first part of this article. We discuss the remarkably versatile excitonic landscape, including bright, dark, localized and interlayer excitons. In the second part, we provide an overview on the progress in optoelectronic device applications, such as electrically driven light emitters, photovoltaic solar cells, photodetectors and opto-valleytronic devices, again bearing in mind the prominent role of excitonic effects. We conclude with a brief discussion on challenges that remain to be addressed to exploit the full potential of transition metal dichalcogenide semiconductors in possible exciton-based applications.
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We study theoretically the Coulomb interaction between excitons in transition metal dichalcogenide (TMD) monolayers. We calculate direct and exchange interaction for both ground and excited states of excitons. The screening of the Coulomb interaction, specific to monolayer structures, leads to the unique behavior of the exciton-exciton scattering for excited states, characterized by the non-monotonic dependence of the interaction as function of the transferred momentum. We find that the nontrivial screening enables the description of TMD exciton interaction strength by approximate formula which includes exciton binding parameters. The influence of screening and dielectric environment on the exciton-exciton interaction was studied, showing qualitatively different behavior for ground state and excited states of excitons. Furthermore, we consider exciton-electron interaction, which for the excited states is governed by the dominant attractive contribution of the exchange component, which increases with the excitation number. The results provide a quantitative description of the exciton-exciton and exciton-electron scattering in transition metal dichalcogenides, and are of interest for the design of perspective nonlinear optical devices based on TMD monolayers.
Strain in two-dimensional (2D) transition metal dichalcogenide (TMD) has led to localized states with exciting optical properties, in particular in view of designing one photon sources. The naturally formed of the MoS2 monolayer deposed on hBN substrate leads to a reduction of the bandgap in the strained region creating a nanobubble. The photogenerated particles are thus confined in the strain-induced potential. Using numerical diagonalization, we simulate the spectra of the confined exciton states, their oscillator strengths and radiative lifetimes. We show that a single state of the confined exciton is optically active, which suggests that the MoS2/hBN nanobubble is a good candidate for the realisation of single-photon sources. Furthermore, the exciton binding energy, oscillator strength and radiative lifetime are enhanced due to the confinement effect.
Strong many-body interactions in two-dimensional (2D) semiconductors give rise to efficient exciton-exciton annihilation (EEA). This process is expected to result in the generation of unbound high energy carriers. Here, we report an unconventional photoresponse of van der Waals heterostructure devices resulting from efficient EEA. Our heterostructures, which consist of monolayer transition metal dichalcogenide (TMD), hexagonal boron nitride (hBN), and few-layer graphene, exhibit photocurrent when photoexcited carriers possess sufficient energy to overcome the high energy barrier of hBN. Interestingly, we find that the device exhibits moderate photocurrent quantum efficiency even when the semiconducting TMD layer is excited at its ground exciton resonance despite the high exciton binding energy and large transport barrier. Using ab initio calculations, we show that EEA yields highly energetic electrons and holes with unevenly distributed energies depending on the scattering condition. Our findings highlight the dominant role of EEA in determining the photoresponse of 2D semiconductor optoelectronic devices.
The direct gap interband transitions in transition metal dichalcogenides monolayers are governed by chiral optical selection rules. Determined by laser helicity, optical transitions in either the $K^+$ or $K^-$ valley in momentum space are induced. Linearly polarized laser excitation prepares a coherent superposition of valley states. Here we demonstrate the control of the exciton valley coherence in monolayer WSe2 by tuning the applied magnetic field perpendicular to the monolayer plane. We show rotation of this coherent superposition of valley states by angles as large as 30 degrees in applied fields up to 9 T. This exciton valley coherence control on ps time scale could be an important step towards complete control of qubits based on the valley degree of freedom.
Auger-like exciton-exciton annihilation (EEA) is considered the key fundamental limitation to quantum yield in devices based on excitons in two-dimensional (2d) materials. Since it is challenging to experimentally disentangle EEA from competing processes, guidance of a quantitative theory is highly desirable. The very nature of EEA requires a material-realistic description that is not available to date. We present a many-body theory of EEA based on first-principle band structures and Coulomb interaction matrix elements that goes beyond an effective bosonic picture. Applying our theory to monolayer MoS$_2$ encapsulated in hexagonal BN, we obtain an EEA coefficient in the order of $10^{-3}$ cm$^{2}$s$^{-1}$ at room temperature, suggesting that exciton annihilation is often dominated by other processes, such as defect-assisted scattering. Our studies open a perspective to quantify the efficiency of intrinsic EEA processes in various 2d materials in the focus of modern materials research.
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