Publication date: Jun 02, 2023
Nonlinear interactions between excitons strongly coupled to light are key for accessing quantum many-body phenomena in polariton systems. Atomically-thin two-dimensional semiconductors provide an attractive platform for strong light-matter coupling owing to many controllable excitonic degrees of freedom. Among these, the recently emerged exciton hybridization opens access to unexplored excitonic species, with a promise of enhanced interactions. Here, we employ hybridized interlayer excitons (hIX) in bilayer MoS₂ to achieve highly nonlinear excitonic and polaritonic effects. Such interlayer excitons possess an out-of-plane electric dipole as well as an unusually large oscillator strength allowing observation of dipolar polaritons (dipolaritons) in bilayers in optical microcavities. Compared to excitons and polaritons in MoS₂ monolayers, both hIX and dipolaritons exhibit approximately 8 times higher nonlinearity, which is further strongly enhanced when hIX and intralayer excitons, sharing the same valence band, are excited simultaneously. This provides access to an unusual nonlinear regime which we describe theoretically as a mixed effect of Pauli exclusion and exciton-exciton interactions enabled through charge tunnelling. The presented insight into many-body interactions provides new tools for accessing few-polariton quantum correlations.
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Fig1c.xlsx
MD5md5:f697e7d053c347b60dddc024a040ebfc
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46.1 KiB | RC spectrum of encapsulated MoS2 bilayer at low temperature |
Fig1e.xlsx
MD5md5:a481b8d0a82732dab5086f9bc7edd50d
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34.2 KiB | RC spectra of excitons in BL MoS2 detected in two circular polarizations in an out-of-plane magnetic field of 8 T at T = 4 K |
Fig2b.xlsx
MD5md5:b0363ef881c0ae356e45773564e03c64
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1.0 MiB | Low temperature (4K) RC spectra measured as a function of the cavity-exciton detuning (∆ = Ecav−Eexc) for cavity scans across XA energy |
Fig2c.xlsx
MD5md5:da00f05b37173655326c9fbe720a8690
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763.0 KiB | Low temperature (4K) RC spectra measured as a function of the cavity-exciton detuning (∆ = Ecav−Eexc) for cavity scans across hIX energy |
Fig2d.xlsx
MD5md5:4523da44ad629f3ea23aee0d5c19bcc7
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43.2 KiB | Waterfall plot of RC spectra measured for the cavity-exciton detunings in the vicinity of the anticrossing between hIX and the cavity mode. |
Fig2e.xlsx
MD5md5:3c485ebf3b449e63ec283fa22d94620a
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17.4 KiB | Dipolariton dispersion measured with circularly polarized detection for 8 T magnetic field |
Fig2f.xlsx
MD5md5:26c086427fde3cef1e13cd0d804f8f45
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16.4 KiB | RC spectra at 8 T at the hIX-cavity anticrossing measured with circularly polarized detection |
Fig3a.xlsx
MD5md5:58c0f6086565d532071d4c96079b1f26
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17.8 KiB | RC spectra measured with the NB (FWHM=28 nm) excitation for the XA at different fluences |
Fig3b.xlsx
MD5md5:f4ae7e01d8b99f6686ad795e1fa15d6f
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18.7 KiB | RC spectra measured with the NB (FWHM=28 nm) excitation for the hIX at different fluences |
Fig3c.xlsx
MD5md5:b6caa65cf5b16ead31ba852a45746e4d
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30.5 KiB | RC spectra measured with the BB (FWHM=50 nm) excitation at different fluences |
Fig3d.xlsx
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16.1 KiB | The energy shift ∆E (top) and normalized integrated intensity (bottom) as a function of the exciton density for the hIX (first worksheet) and XA (second worksheet) |
Fig4a.xlsx
MD5md5:15d4077ddb8db5082bca832fc2b8dd89
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48.9 KiB | Reflectance contrast dispersion spectra of the MoS2 bilayer placed in a monolithic cavity. The low fluence case (0.6 µJ cm−2) |
Fig4b.xlsx
MD5md5:dda0cafb7da057c32e5ae6808a465e02
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48.4 KiB | Reflectance contrast dispersion spectra of the MoS2 bilayer placed in a monolithic cavity. The high fluence case (58.5 µJ cm−2 ) |
Fig4c.xlsx
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17.3 KiB | RC spectra measured at the anticrossing as a function of the laser fluence |
Fig4de.xlsx
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10.4 KiB | Measured UPB , LPB peak energies and normalised Rabi splitting as a function of the laser fluence and the corresponding polariton density. Rabi splittings are normalised by the Rabi splitting obtained at the lowest fluence. |
2023.88 (version v1) [This version] | Jun 02, 2023 | DOI10.24435/materialscloud:xm-bm |