Charalambos Louca^1*, Armando Genco^2*, Salvatore Chiavazzo³, Thomas P. Lyons^1,4, Sam Randerson¹, Chiara Trovatello², Peter Claronino^1,5, Rahul Jayaprakash¹, Xuerong Hu¹, James Howarth^6,7, Kenji Watanabe⁸, Takashi Taniguchi⁹, Stefano Dal Conte², Roman Gorbachev^6,7, David G. Lidzey¹, Giulio Cerullo², Oleksandr Kyriienko³, Alexander I. Tartakovskii^1*

1 Department of Physics and Astronomy, The University of Sheffield, Sheffield S3 7RH, UK

2 Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci, 32, Milano, 20133, Italy

3 Department of Physics, University of Exeter, Stocker Road, Exeter, EX4 4PY, UK

4 RIKEN Center for Emergent Matter Science, Wako, Saitama, 351-0198, Japan

5 Department of Physics and Mathematics, University of Hull, Rober Blackburn, Hull HU6 7RX, UK

6 National Graphene Institute, University of Manchester, Manchester, UK

7 Department of Physics and Astronomy, University of Manchester, Manchester, UK

8 Research Center for Electronic and Optical Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan

9 Research Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan

* Corresponding authors emails: charalambos.louca@polimi.it, armando.genco@polimi.it, a.tartakovskii@sheffield.ac.uk

DOI10.24435/materialscloud:xm-bm [version v1]

Publication date: Jun 02, 2023

How to cite this record

Charalambos Louca, Armando Genco, Salvatore Chiavazzo, Thomas P. Lyons, Sam Randerson, Chiara Trovatello, Peter Claronino, Rahul Jayaprakash, Xuerong Hu, James Howarth, Kenji Watanabe, Takashi Taniguchi, Stefano Dal Conte, Roman Gorbachev, David G. Lidzey, Giulio Cerullo, Oleksandr Kyriienko, Alexander I. Tartakovskii, Interspecies exciton interactions lead to enhanced nonlinearity of dipolar excitons and polaritons in MoS₂ bilayers, Materials Cloud Archive 2023.88 (2023), https://doi.org/10.24435/materialscloud:xm-bm

Description

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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Files

File name	Size	Description
Fig1c.xlsx MD5md5:f697e7d053c347b60dddc024a040ebfc	46.1 KiB	RC spectrum of encapsulated MoS2 bilayer at low temperature
Fig1e.xlsx MD5md5:a481b8d0a82732dab5086f9bc7edd50d	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	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	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	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	17.4 KiB	Dipolariton dispersion measured with circularly polarized detection for 8 T magnetic field
Fig2f.xlsx MD5md5:26c086427fde3cef1e13cd0d804f8f45	16.4 KiB	RC spectra at 8 T at the hIX-cavity anticrossing measured with circularly polarized detection
Fig3a.xlsx MD5md5:58c0f6086565d532071d4c96079b1f26	17.8 KiB	RC spectra measured with the NB (FWHM=28 nm) excitation for the XA at different fluences
Fig3b.xlsx MD5md5:f4ae7e01d8b99f6686ad795e1fa15d6f	18.7 KiB	RC spectra measured with the NB (FWHM=28 nm) excitation for the hIX at different fluences
Fig3c.xlsx MD5md5:b6caa65cf5b16ead31ba852a45746e4d	30.5 KiB	RC spectra measured with the BB (FWHM=50 nm) excitation at different fluences
Fig3d.xlsx MD5md5:d79c78f5d8b19840e63145eafbb32c02	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	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	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 MD5md5:c47bd4f049fad001ea9d005e4849f224	17.3 KiB	RC spectra measured at the anticrossing as a function of the laser fluence
Fig4de.xlsx MD5md5:bfd97b8b88b4e315d887b64f18a7742f	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.

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Keywords

2D materials Experimental Exciton-polaritons H2020 RCUK Marie Curie Fellowship