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Register a new userHarnessing Exciton-Exciton Annihilation in Two-Dimensional Semiconductors
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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.
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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.
We investigate the excitonic dynamics in MoSe2 monolayer and bulk samples by femtosecond transient absorption microscopy. Excitons are resonantly injected by a 750-nm and 100-fs laser pulse, and are detected by a probe pulse tuned in the range of 790 - 820 nm. We observe a strong density-dependent initial decay of the exciton population in monolayers, which can be well described by the exciton-exciton annihilation. Such a feature is not observed in the bulk under comparable conditions. We also observe the saturated absorption induced by exciton phase-space filling in both monolayers and the bulk, which indicates their potential applications as saturable absorbers.
The elementary optical excitations of a two-dimensional electron or hole system have been identified as exciton-Fermi-polarons. Nevertheless, the connection between the bound state of an exciton and an electron, termed trion, and exciton-polarons is subject of ongoing debate. Here, we use an analogy to the Tavis-Cummings model of quantum optics to show that an exciton-polaron can be understood as a hybrid quasiparticle -- a coherent superposition of a bare exciton in an unperturbed Fermi sea and a bright collective excitation of many trions. The analogy is valid to the extent that the Chevy Ansatz provides a good description of dynamical screening of excitons and provided the Fermi energy is much smaller than the trion binding energy. We anticipate our results to bring new insight that could help to explain the striking differences between absorption and emission spectra of two-dimensional semiconductors.
The exceptionally strong Coulomb interaction in semiconducting transition-metal dichalcogenides (TMDs) gives rise to a rich exciton landscape consisting of bright and dark exciton states. At elevated densities, excitons can interact through exciton-exciton annihilation (EEA), an Auger-like recombination process limiting the efficiency of optoelectronic applications. Although EEA is a well-known and particularly important process in atomically thin semiconductors determining exciton lifetimes and affecting transport at elevated densities, its microscopic origin has remained elusive. In this joint theory-experiment study combining microscopic and material-specific theory with time- and temperature-resolved photoluminescence measurements, we demonstrate the key role of dark intervalley states that are found to dominate the EEA rate in monolayer WSe$_2$. We reveal an intriguing, characteristic temperature dependence of Auger scattering in this class of materials with an excellent agreement between theory and experiment. Our study provides microscopic insights into the efficiency of technologically relevant Auger scattering channels within the remarkable exciton landscape of atomically thin semiconductors.
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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