journal article·2023-01-01Open access

Signatures of dark excitons in exciton–polariton optics of transition metal dichalcogenides

Beatriz Ferreira, Roberto Rosati, Jamie M Fitzgerald, Ermin Malic

2D Materials· Volume 10· Issue 1

Abstract

Abstract Integrating 2D materials into high-quality optical microcavities opens the door to fascinating many-particle phenomena including the formation of exciton–polaritons. These are hybrid quasi-particles inheriting properties of both the constituent photons and excitons. In this work, we investigate the so-far overlooked impact of dark excitons on the momentum-resolved absorption spectra of hBN-encapsulated WSe2 and MoSe2 monolayers in the strong-coupling regime. In particular, thanks to the efficient phonon-mediated scattering of polaritons into energetically lower dark exciton states, the absorption of the lower polariton branch in WSe2 is much higher than in MoSe2. It shows unique step-like increases in the momentum-resolved profile indicating opening of specific scattering channels. We study how different externally accessible quantities, such as temperature or mirror reflectance, change the optical response of polaritons. Our study contributes to an improved microscopic understanding of exciton–polaritons and their interaction with phonons, potentially suggesting experiments that could determine the energy of dark exciton states via momentum-resolved polariton absorption.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Strong Light-Matter Interactions · Perovskite Materials and Applications · 2D Materials and Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (42)

Show source-provided references
1. Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors10.1038/s41699-018-0074-2 ↗
2. Mapping of the dark exciton landscape in transition metal dichalcogenides10.1103/PhysRevB.98.020301 ↗
3. Tightly bound excitons in monolayer WSe210.1103/PhysRevLett.113.026803 ↗
4. Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor10.1038/nmat4061 ↗
5. Colloquium: excitons in atomically thin transition metal dichalcogenides10.1103/RevModPhys.90.021001 ↗
6. Optical absorption by indirect excitons in a transition metal dichalcogenide/hexagonal boron nitride heterostructure10.1088/1361-648X/aabe53 ↗
7. Exciton optics, dynamics, and transport in atomically thin semiconductors10.1063/5.0107665 ↗
8. Strong light–matter coupling in two-dimensional atomic crystals10.1038/nphoton.2014.304 ↗
9. Exciton–polaritons in Van der Waals heterostructures embedded in tunable microcavities10.1038/ncomms9579 ↗
10. Two-dimensional semiconductors in the regime of strong light-matter coupling10.1038/s41467-018-04866-6 ↗
11. Theory of the contribution of excitons to the complex dielectric constant of crystals10.1103/PhysRev.112.1555 ↗
12. Exciton-polariton Bose-Einstein condensation10.1103/RevModPhys.82.1489 ↗
13. Dark excitons in transition metal dichalcogenides10.1103/PhysRevMaterials.2.014002 ↗
14. Experimental evidence for dark excitons in monolayer WSe210.1103/PhysRevLett.115.257403 ↗
15. Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides10.1038/ncomms13279 ↗
16. Phonon-assisted photoluminescence from indirect excitons in monolayers of transition-metal dichalcogenides10.1021/acs.nanolett.0c00633 ↗
17. Dark exciton anti-funneling in atomically thin semiconductors10.1038/s41467-021-27425-y ↗
18. Microscopic modeling of exciton-polariton diffusion coefficients in atomically thin semiconductors10.1103/PhysRevMaterials.6.034008 ↗
19. Kavokin · 2017 · vol 21
20. Input and output in damped quantum systems: quantum stochastic differential equations and the master equation10.1103/PhysRevA.31.3761 ↗
21. Dark and bright exciton formation, thermalization and photoluminescence in monolayer transition metal dichalcogenides10.1088/2053-1583/aabea3 ↗
22. Tunable phases of moiré excitons in van der Waals heterostructures10.1021/acs.nanolett.0c03019 ↗
23. Haus · 1984 · p 402
24. Haug · 2009
25. Analytical approach to excitonic properties of MoS210.1103/PhysRevB.89.125309 ↗
26. k ⋅ p theory for two-dimensional transition metal dichalcogenide semiconductors10.1088/2053-1583/2/2/022001 ↗
27. Finite-momentum exciton landscape in mono- and bilayer transition metal dichalcogenides10.1088/2053-1583/ab0e1d ↗
28. Proposal for dark exciton based chemical sensors10.1038/ncomms14776 ↗
29. Dark exciton-exciton annihilation in monolayer WSe210.1103/PhysRevB.104.L241406 ↗
30. Momentum-resolved observation of exciton formation dynamics in monolayer WS210.1021/acs.nanolett.1c01839 ↗
31. Exciton relaxation cascade in two-dimensional transition metal dichalcogenides10.1038/s41598-018-25906-7 ↗
32. Twist angle tuning of moiré exciton polaritons in van der Waals heterostructures10.1021/acs.nanolett.2c01175 ↗
33. Phonon signatures in spectra of exciton polaritons in transition metal dichalcogenides10.1103/PhysRevB.104.L241301 ↗
34. Quantum theory of phonon-assisted exciton formation and luminescence in semiconductor quantum wells10.1103/PhysRevB.62.2706 ↗
35. Rossi · 2011
36. Adler · 1960
37. Periodic models for thin optimal absorbers of electromagnetic radiation10.1103/PhysRevB.55.R16072 ↗
38. Total absorption by degenerate critical coupling10.1063/1.4885517 ↗
39. Bulk exciton polaritons in GaAs microcavities10.1103/PhysRevB.52.1800 ↗
40. Microcavity exciton-polariton splitting in the linear regime10.1103/PhysRevB.51.14437 ↗
41. Intrinsic transport properties of electrons and holes in monolayer transition-metal dichalcogenides10.1103/PhysRevB.90.045422 ↗
42. Intrinsic lifetime of higher excitonic states in tungsten diselenide monolayers10.1039/C9NR04211C ↗