Laterally extended states of interlayer excitons in reconstructed MoSe2/WSe2 heterostructures
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Abstract
Abstract Heterostructures made from 2D transition-metal dichalcogenides are known as ideal platforms to explore excitonic phenomena ranging from correlated moiré excitons to degenerate interlayer exciton ensembles. So far, it is assumed that the atomic reconstruction appearing in some of the heterostructures gives rise to a dominating localization of the exciton states. We demonstrate that the center-of-mass wavefunction of the excitonic states in reconstructed MoSe2/WSe2 heterostructures can extend well beyond the moiré periodicity of the investigated heterostructures. The results are based on real-space calculations yielding a lateral potential map for interlayer excitons within the strain-relaxed heterostructures with weak random disorder, as expected for realistic samples, and the corresponding real-space center-of-mass excitonic wavefunctions. We combine the theoretical results with cryogenic photoluminescence experiments, which support the computed level structure and relaxation characteristics of the interlayer excitons.
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Research context
OpenAlex topics: 2D Materials and Applications · Perovskite Materials and Applications · Chalcogenide Semiconductor Thin Films
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References (57)
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1. Novoselov, K. S., Mishchenko, A., Carvalho, A. & Castro Neto, A. H. 2D materials and van der Waals heterostructures. Science 353, aac9439 (2016).10.1126/science.aac9439 ↗
2. Ajayan, P., Kim, P. & Banerjee, K. Two-dimensional van der Waals materials. Phys. Today 69, 38–44 (2016).10.1063/PT.3.3297 ↗
3. Manzeli, S., Ovchinnikov, D., Pasquier, D., Yazyev, O. V. & Kis, A. 2D transition metal dichalcogenides. Nat. Rev. Mater. 2, 1–15 (2017).10.1038/natrevmats.2017.33 ↗
4. Wang, G. et al. Colloquium: excitons in atomically thin transition metal dichalcogenides. Rev. Mod. Phys. 90, 021001 (2018).10.1103/RevModPhys.90.021001 ↗
5. Kormányos, A. et al. k.p theory for two-dimensional transition metal dichalcogenide semiconductors. 2D Mater. 2, 022001 (2015).10.1088/2053-1583/2/2/022001 ↗
6. Xiao, D., Liu, G.-B., Feng, W., Xu, X. & Yao, W. Coupled spin and valley physics in monolayers of MoS2 and other group-VI dichalcogenides. Phys. Rev. Lett. 108, 196802 (2012).10.1103/PhysRevLett.108.196802 ↗
7. Brotons-Gisbert, M., Gerardot, B. D., Holleitner, A. W. & Wurstbauer, U. Interlayer and Moiré excitons in atomically thin double layers: From individual quantum emitters to degenerate ensembles. MRS Bull. 49, 914–931 (2024).10.1557/s43577-024-00772-z ↗
8. Rivera, P. et al. Observation of long-lived interlayer excitons in monolayer MoSe2-WSe2 heterostructures. Nat. Commun. 6, 6242 (2015).10.1038/ncomms7242 ↗
9. Miller, B. et al. Long-Lived Direct and Indirect Interlayer Excitons in van der Waals Heterostructures. Nano Lett. 17, 5229–5237 (2017).10.1021/acs.nanolett.7b01304 ↗
10. Hong, X. et al. Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures. Nat. Nanotechnol. 9, 682–686 (2014).10.1038/nnano.2014.167 ↗
11. Wilson, N. R. et al. Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures. Sci. Adv. 3, e1601832 (2017).10.1126/sciadv.1601832 ↗
12. Nayak, P. K. et al. Probing evolution of twist-angle-dependent interlayer excitons in MoSe2/WSe2 van der Waals Heterostructures. ACS Nano 11, 4041–4050 (2017).10.1021/acsnano.7b00640 ↗
13. Jauregui, L. A. et al. Electrical control of interlayer exciton dynamics in atomically thin heterostructures. Science 366, 870–875 (2019).10.1126/science.aaw4194 ↗
14. Cao, Y. et al. Unconventional superconductivity in magic-angle graphene superlattices. Nature 556, 43–50 (2018).10.1038/nature26160 ↗
15. Jung, J., Raoux, A., Qiao, Z. & MacDonald, A. H. Ab initio theory of moiré superlattice bands in layered two-dimensional materials. Phys. Rev. B 89, 205414 (2014).10.1103/PhysRevB.89.205414 ↗
16. Weston, A. et al. Atomic reconstruction in twisted bilayers of transition metal dichalcogenides. Nat. Nanotechnol. 15, 592–597 (2020).10.1038/s41565-020-0682-9 ↗
17. Rosenberger, M. R. et al. Twist angle-dependent atomic reconstruction and moiré patterns in transition metal dichalcogenide heterostructures. ACS Nano. 14, 4550–4558 (2020).10.1021/acsnano.0c00088 ↗
18. Zhang, C. et al. Interlayer couplings, Moiré patterns, and 2D electronic superlattices in MoS2/WSe2 hetero-bilayers. Sci. Adv. 3, e1601459 (2017).10.1126/sciadv.1601459 ↗
19. Jin, C. et al. Observation of moiré excitons in WSe2/WS2 heterostructure superlattices. Nature 567, 76–80 (2019).10.1038/s41586-019-0976-y ↗
20. Zhao, S. et al. Excitons in mesoscopically reconstructed moiré heterostructures. Nat. Nanotechnol. 18, 572–579 (2023).10.1038/s41565-023-01356-9 ↗
21. Fogler, M. M., Butov, L. V. & Novoselov, K. S. High-temperature superfluidity with indirect excitons in van der Waals heterostructures. Nat. Commun. 5, 4555 (2014).10.1038/ncomms5555 ↗
22. Alexeev, E. M. et al. Resonantly hybridized excitons in moiré superlattices in van der Waals heterostructures. Nature 567, 81–86 (2019).10.1038/s41586-019-0986-9 ↗
23. Steinhoff, A. et al. Exciton-exciton interactions in Van der Waals heterobilayers. Phys. Rev. X 14, 031025 (2024).
24. Brotons-Gisbert, M. et al. Moiré-trapped interlayer trions in a charge-tunable WSe2/MoSe2 heterobilayer. Phys. Rev. X 11, 031033 (2021).
25. Lagoin, C. & Dubin, F. Key role of the moiré potential for the quasicondensation of interlayer excitons in van der Waals heterostructures. Phys. Rev. B 103, L041406 (2021).10.1103/PhysRevB.103.L041406 ↗
26. Rossi, A. et al. Anomalous interlayer exciton diffusion in WS2/WSe2 Moiré Heterostructure. ACS Nano. 18, 18202–18210 (2024).10.1021/acsnano.4c00015 ↗
27. Nielsen, C. E. M., da Cruz, M., Torche, A. & Bester, G. Accurate force-field methodology capturing atomic reconstructions in transition metal dichalcogenide moiré system. Phys. Rev. B 108, 045402 (2023).10.1103/PhysRevB.108.045402 ↗
28. Seyler, K. L. et al. Signatures of moiré-trapped valley excitons in MoSe2/WSe2 heterobilayers. Nature 567, 66–70 (2019).10.1038/s41586-019-0957-1 ↗
29. Zhang, L. et al. Twist-angle dependence of moiré excitons in WS2/MoSe2 heterobilayers. Nat. Commun. 11, 5888 (2020).10.1038/s41467-020-19466-6 ↗
30. Sigl, L. et al. Signatures of a degenerate many-body state of interlayer excitons in a van der Waals heterostack. Phys. Rev. Res. 2, 042044 (2020).10.1103/PhysRevResearch.2.042044 ↗
31. Troue, M. et al. Extended spatial coherence of interlayer excitons in MoSe2/WSe2 heterobilayers. Phys. Rev. Lett. 131, 036902 (2023).10.1103/PhysRevLett.131.036902 ↗
32. Richter, M. Theory of interlayer exciton dynamics in two-dimensional transition metal dichalcogenide heterolayers under the influence of strain reconstruction and disorder. Phys. Rev. B 109, 125308 (2024).10.1103/PhysRevB.109.125308 ↗
33. Enaldiev, V., Zólyomi, V., Yelgel, C., Magorrian, S. & Fal’ko, V. Stacking domains and dislocation networks in marginally twisted bilayers of transition metal dichalcogenides. Phys. Rev. Lett. 124, 206101 (2020).10.1103/PhysRevLett.124.206101 ↗
34. Singh, R. et al. Localization dynamics of excitons in disordered semiconductor quantum wells. Phys. Rev. B 95, 235307 (2017).10.1103/PhysRevB.95.235307 ↗
35. Richter, M., Singh, R., Siemens, M. & Cundiff, S. T. Deconvolution of optical multidimensional coherent spectra. Sci. Adv. 4, eaar7697 (2018).10.1126/sciadv.aar7697 ↗
36. Khatibi, Z. et al. Impact of strain on the excitonic linewidth in transition metal dichalcogenides. 2D Mater. 6, 015015 (2018).10.1088/2053-1583/aae953 ↗
37. Wu, F., Lovorn, T. & MacDonald, A. H. Theory of optical absorption by interlayer excitons in transition metal dichalcogenide heterobilayers. Phys. Rev. B 97, 035306 (2018).10.1103/PhysRevB.97.035306 ↗
38. Tran, K. et al. Evidence for moiré excitons in van der Waals heterostructures. Nature 567, 71–75 (2019).10.1038/s41586-019-0975-z ↗
39. Ruiz-Tijerina, D. A., Soltero, I. & Mireles, F. Theory of moiré localized excitons in transition metal dichalcogenide heterobilayers. Phys. Rev. B 102, 195403 (2020).10.1103/PhysRevB.102.195403 ↗
40. Fallahazad, B. et al. Shubnikov–de Haas oscillations of high-mobility holes in monolayer and bilayer WSe2: Landau level degeneracy, effective mass, and negative compressibility. Phys. Rev. Lett. 116, 086601 (2016).10.1103/PhysRevLett.116.086601 ↗
41. Mostaani, E. et al. Diffusion quantum Monte Carlo study of excitonic complexes in two-dimensional transition-metal dichalcogenides. Phys. Rev. B 96, 075431 (2017).10.1103/PhysRevB.96.075431 ↗
42. Jin, Z., Li, X., Mullen, J. T. & Kim, K. W. Intrinsic transport properties of electrons and holes in monolayer transition-metal dichalcogenides. Phys. Rev. B 90, 045422 (2014).10.1103/PhysRevB.90.045422 ↗
43. Shree, S. et al. Observation of exciton-phonon coupling in MoSe2 monolayers. Phys. Rev. B 98, 035302 (2018).10.1103/PhysRevB.98.035302 ↗
44. Zimmermann, R., Runge, E. & Savona, V. in Quantum Coherence Correlation and Decoherence in Semiconductor Nanostructures Ch. 4 (ed. Takagahara, T.) 89–165 (Academic Press, San Diego, 2003).10.1016/B978-012682225-0/50005-5 ↗
45. Hermann, K. Periodic overlayers and moiré patterns: theoretical studies of geometric properties. J. Phys.: Condens. Matter 24, 314210 (2012).
46. Fang, H. et al. Localization and interaction of interlayer excitons in MoSe2/WSe2 heterobilayers. Nat. Commun. 14, 6910 (2023).10.1038/s41467-023-42710-8 ↗
47. Urbach, F. The long-wavelength edge of photographic sensitivity and of the electronic absorption of solids. Phys. Rev. 92, 1324–1324 (1953).10.1103/PhysRev.92.1324 ↗
48. Piccardo, M. et al. Localization landscape theory of disorder in semiconductors. II. Urbach tails of disordered quantum well layers. Phys. Rev. B 95, 144205 (2017).10.1103/PhysRevB.95.144205 ↗
49. Katzer, M. et al. Exciton-phonon scattering: competition between the bosonic and fermionic nature of bound electron-hole pairs. Phys. Rev. B 108, L121102 (2023).10.1103/PhysRevB.108.L121102 ↗
50. Sigl, L. et al. Optical dipole orientation of interlayer excitons in MoSe2/WSe2 heterostacks. Phys. Rev. B 105, 035417 (2022).10.1103/PhysRevB.105.035417 ↗
51. Sun, Z. et al. Excitonic transport driven by repulsive dipolar interaction in a van der Waals heterostructure. Nat. Photonics 16, 79–85 (2022).10.1038/s41566-021-00908-6 ↗
52. Malic, E., Perea-Causin, R., Rosati, R., Erkensten, D. & Brem, S. Exciton transport in atomically thin semiconductors. Nat. Commun. 14, 3430 (2023).10.1038/s41467-023-38556-9 ↗
53. Wietek, E. et al. Nonlinear and negative effective diffusivity of interlayer excitons in Moir\’e-Free heterobilayers. Phys. Rev. Lett. 132, 016202 (2024).10.1103/PhysRevLett.132.016202 ↗
54. Fowler-Gerace, L. H., Zhou, Z., Szwed, E. A., Choksy, D. J. & Butov, L. V. Transport and localization of indirect excitons in a van der Waals heterostructure. Nat. Photonics 18, 823–828 (2024).10.1038/s41566-024-01435-w ↗
55. Balay, S., Gropp, W. D., McInnes, L. C. & Smith, B. F. in Modern Software Tools in Scientific Computing (eds Arge, E., Bruaset, A. M. & Langtangen, H. P.) 163–202 (Birkhäuser Press, 1997).10.1007/978-1-4612-1986-6_8 ↗
56. Balay, S. et al. PETSc Web page. https://petsc.org/ (2023).
57. Balay, S. et al. PETSc/TAO users manual. Tech. Rep. ANL-21/39 - Revision 3.19, Argonne National Laboratory (2023).