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Two-dimensional plasmonic polarons in n-doped monolayer MoS2

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 Added by Fabio Caruso
 Publication date 2021
  fields Physics
and research's language is English




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We report experimental and theoretical evidence of strong electron-plasmon interaction in n-doped single-layer MoS2. Angle-resolved photoemission spectroscopy (ARPES) measurements reveal the emergence of distinctive signatures of polaronic coupling in the electron spectral function. Calculations based on many-body perturbation theory illustrate that electronic coupling to two-dimensional (2D) carrier plasmons provides an exhaustive explanation of the experimental spectral features and their energies. These results constitute compelling evidence of the formation of plasmon-induced polaronic quasiparticles, suggesting that highly-doped transition-metal dichalcogenides may provide a new platform to explore strong-coupling phenomena between electrons and plasmons in 2D.



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We demonstrate that the temperature and doping dependencies of the photoluminescence (PL) spectra of a doped MoS2 monolayer have several peculiar characteristics defined by trion radiative decay. While only zero-momentum exciton states are coupled to light, radiative recombination of non-zero momentum trions is also allowed. This leads to an asymmetric broadening of the trion spectral peak and redshift of the emitted light with increasing temperature. The lowest energy trion state is dark, which is manifested by the sharply non-monotonic temperature dependence of the PL intensity. Our calculations combine the Dirac model for the single-particle states, the parameters for which are obtained from the first principle calculations, and the direct solution of the three-particle problem within the Tamm-Dancoff approximation. The numerical results are well captured by a simple model that yields analytical expressions for the temperature dependencies of the PL spectra.
Heterointerfaces in complex oxide systems open new arenas in which to test models of strongly correlated material, explore the role of dimensionality in metal-insulator-transitions (MITs) and small polaron formation. Close to the quantum critical point Mott MITs depend on band filling controlled by random disordered substitutional doping. Delta-doped Mott insulators are potentially free of random disorder and introduce a new arena in which to explore the effect of electron correlations and dimensionality. Epitaxial films of the prototypical Mott insulator GdTiO3 are delta-doped by substituting a single (GdO)+1 plane with a monolayer of charge neutral SrO to produce a two-dimensional system with high planar doping density. Unlike metallic SrTiO3 quantum wells in GdTiO3 the single SrO delta-doped layer exhibits thermally activated DC and optical conductivity that agree in a quantitative manner with predictions of small polaron transport but with an extremely high two-dimensional density of polarons, ~ 7E14 cm-2
Single crystals of electron-doped SrMnO3 with a cubic perovskite structure have been systematically investigated as the most canonical (orbital-degenerate) double-exchange system, whose ground states have been still theoretically controversial. With only 1-2% electron doping by Ce substitution for Sr, a G-type antiferromagnetic metal with a tiny spin canting in a cubic lattice shows up as the ground state, where the Jahn-Teller polarons with heavy mass are likely to form. Further electron doping above 4%, however, replaces this isotropic metal with an insulator with tetragonal lattice distortion, accompanied by a quasi-one-dimensional 3z^2-r^2 orbital ordering with the C-type antiferromagnetism. The self-organization of such dilute polarons may reflect the critical role of the cooperative Jahn-Teller effect that is most effective in the originally cubic system.
Two-dimensional semiconductors such as MoS2 are an emerging material family with wide-ranging potential applications in electronics, optoelectronics and energy harvesting. Large-area growth methods are needed to open the way to the applications. While significant progress to this goal was made, control over lattice orientation during growth still remains a challenge. This is needed in order to minimize or even avoid the formation of grain boundaries which can be detrimental to electrical, optical and mechanical properties of MoS2 and other 2D semiconductors. Here, we report on the uniform growth of high-quality centimeter-scale continuous monolayer MoS2 with control over lattice orientation. Using transmission electron microscopy we show that the monolayer film is composed of coalescing single islands that share a predominant lattice orientation due to an epitaxial growth mechanism. Raman and photoluminescence spectra confirm the high quality of the grown material. Optical absorbance spectra acquired over large areas show new features in the high-energy part of the spectrum, indicating that MoS2 could also be interesting for harvesting this region of the solar spectrum and fabrication of UV-sensitive photodetectors. Even though the interaction between the growth substrate and MoS2 is strong enough to induce lattice alignment, we can easily transfer the grown material and fabricate field-effect transistors on SiO2 substrates showing mobility superior to the exfoliated material.
Monolayer transition metal dichalcogenide semiconductors, with versatile experimentally accessible exciton species, offer an interesting platform for investigating the interaction between excitons and a Fermi sea of charges. Using hexagonal boron nitride encapsulated monolayer MoSe2, we study the impact of charge density tuning on the ground and excited Rydberg states in the atomic layer. Consistent excitonpolaron behavior is revealed in both photoluminescence and reflection spectra of the A exciton 1s (A:1s) Rydberg state, in contrast to previous studies. The A:2s Rydberg state provides an opportunity to understand such interactions with greatly reduced exciton binding energy. We found that the impact of the Fermi sea becomes much more dramatic. With a photoluminescence upconversion technique, we further verify the 2s polaron-like behavior for the repulsive branch of B:2s exciton whose energy is well above the bare bandgap. Our studies show that the polaron-like interaction features are quite generic and highly robust, offering key insights into the dressed manybody state in a Fermi sea.
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