Intercell moiré exciton complexes in electron lattices

Xi Wang; Xiaowei Zhang; Jiayi Zhu; Heonjoon Park; Yingqi Wang; Chong Wang; William G. Holtzmann; Takashi Taniguchi; Kenji Watanabe; Jiaqiang Yan; Daniel R. Gamelin; Wang Yao; Di Xiao; Ting Cao; Xiaodong Xu

doi:10.1038/s41563-023-01496-2

Intercell moiré exciton complexes in electron lattices

Xi Wang, Xiaowei Zhang, Jiayi Zhu, Heonjoon Park, Yingqi Wang, Chong Wang, William G. Holtzmann, Takashi Taniguchi, Kenji Watanabe, Jiaqiang Yan, Daniel R. Gamelin, Wang Yao, Di Xiao, Ting Cao, Xiaodong Xu

Correlated Electron Materials

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20 Scopus citations

Abstract

Excitons, Coulomb-bound electron–hole pairs, play a crucial role in both optical excitation and correlated phenomena in solids. When excitons interact with other quasiparticles, few- and many-body excited states can appear. Here we report an interaction between exciton and charges enabled by unusual quantum confinement in two-dimensional moiré superlattices, which results in many-body ground states composed of moiré excitons and correlated electron lattices. In an H-stacked (60^o-twisted) WS₂/WSe₂ heterobilayer, we found an interlayer moiré exciton whose hole is surrounded by its partner electron’s wavefunction distributed among three adjacent moiré traps. This three-dimensional excitonic structure enables large in-plane electrical quadrupole moments in addition to the vertical dipole. Upon doping, the quadrupole facilitates the binding of interlayer moiré excitons to the charges in neighbouring moiré cells, forming intercell charged exciton complexes. Our work provides a framework for understanding and engineering emergent exciton many-body states in correlated moiré charge orders.

Original language	English
Pages (from-to)	599-604
Number of pages	6
Journal	Nature Materials
Volume	22
Issue number	5
DOIs	https://doi.org/10.1038/s41563-023-01496-2
State	Published - May 2023

Funding

Research on the exciton many-body ground states is mainly supported by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) under award DE-SC0018171. Measurements on the R-stacked moir\u00E9 superlattice are supported as part of Programmable Quantum Materials, an Energy Frontier Research Center funded by the US DOE BES, under award DE-SC0019443. The first-principles calculation is mainly supported by NSF MRSEC DMR-1719797. Computational resources were provided by HYAK at the University of Washington. The theoretical analysis and modelling effort is supported by DOE DE-SC0012509. Device fabrication is partially supported by the Army Research Office (ARO) Multidisciplinary University Research Initiative (MURI) programme (grant number W911NF-18-1-0431). The AFM-related measurements were performed using instrumentation supported by the US National Science Foundation through the UW Molecular Engineering Materials Center (MEM-C), a Materials Research Science and Engineering Center (DMR-1719797). W.Y. acknowledges support by the University Grants Committee/Research Grant Council of Hong Kong SAR (AoE/P-701/20, HKU SRFS2122-7S05) and the Tencent Foundation. Bulk WSe2 crystal growth and characterization by J.Y. is supported by the US DOE BES, Materials Sciences and Engineering Division. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan (grant number JPMXP0112101001) and JSPS KAKENHI (grant numbers 19H05790, 20H00354 and 21H05233). T.C. acknowledges support from the Micron Foundation. X.X. acknowledges support from the State of Washington-funded Clean Energy Institute and from the Boeing Distinguished Professorship in Physics. W.G.H. was supported by the NSF Graduate Research Fellowship Program under grant number DGE-1762114. Research on the exciton many-body ground states is mainly supported by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) under award DE-SC0018171. Measurements on the R-stacked moir\u00E9 superlattice are supported as part of Programmable Quantum Materials, an Energy Frontier Research Center funded by the US DOE BES, under award DE-SC0019443. The first-principles calculation is mainly supported by NSF MRSEC DMR-1719797. Computational resources were provided by HYAK at the University of Washington. The theoretical analysis and modelling effort is supported by DOE DE-SC0012509. Device fabrication is partially supported by the Army Research Office (ARO) Multidisciplinary University Research Initiative (MURI) programme (grant number W911NF-18-1-0431). The AFM-related measurements were performed using instrumentation supported by the US National Science Foundation through the UW Molecular Engineering Materials Center (MEM-C), a Materials Research Science and Engineering Center (DMR-1719797). W.Y. acknowledges support by the University Grants Committee/Research Grant Council of Hong Kong SAR (AoE/P-701/20, HKU SRFS2122-7S05) and the Tencent Foundation. Bulk WSe crystal growth and characterization by J.Y. is supported by the US DOE BES, Materials Sciences and Engineering Division. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan (grant number JPMXP0112101001) and JSPS KAKENHI (grant numbers 19H05790, 20H00354 and 21H05233). T.C. acknowledges support from the Micron Foundation. X.X. acknowledges support from the State of Washington-funded Clean Energy Institute and from the Boeing Distinguished Professorship in Physics. W.G.H. was supported by the NSF Graduate Research Fellowship Program under grant number DGE-1762114. 2

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title = "Intercell moir{\'e} exciton complexes in electron lattices",

abstract = "Excitons, Coulomb-bound electron–hole pairs, play a crucial role in both optical excitation and correlated phenomena in solids. When excitons interact with other quasiparticles, few- and many-body excited states can appear. Here we report an interaction between exciton and charges enabled by unusual quantum confinement in two-dimensional moir{\'e} superlattices, which results in many-body ground states composed of moir{\'e} excitons and correlated electron lattices. In an H-stacked (60o-twisted) WS2/WSe2 heterobilayer, we found an interlayer moir{\'e} exciton whose hole is surrounded by its partner electron{\textquoteright}s wavefunction distributed among three adjacent moir{\'e} traps. This three-dimensional excitonic structure enables large in-plane electrical quadrupole moments in addition to the vertical dipole. Upon doping, the quadrupole facilitates the binding of interlayer moir{\'e} excitons to the charges in neighbouring moir{\'e} cells, forming intercell charged exciton complexes. Our work provides a framework for understanding and engineering emergent exciton many-body states in correlated moir{\'e} charge orders.",

author = "Xi Wang and Xiaowei Zhang and Jiayi Zhu and Heonjoon Park and Yingqi Wang and Chong Wang and Holtzmann, {William G.} and Takashi Taniguchi and Kenji Watanabe and Jiaqiang Yan and Gamelin, {Daniel R.} and Wang Yao and Di Xiao and Ting Cao and Xiaodong Xu",

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AU - Wang, Xi

AU - Zhang, Xiaowei

AU - Zhu, Jiayi

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AU - Wang, Yingqi

AU - Wang, Chong

AU - Holtzmann, William G.

AU - Taniguchi, Takashi

AU - Watanabe, Kenji

AU - Yan, Jiaqiang

AU - Gamelin, Daniel R.

AU - Yao, Wang

AU - Xiao, Di

AU - Cao, Ting

AU - Xu, Xiaodong

PY - 2023/5

Y1 - 2023/5

N2 - Excitons, Coulomb-bound electron–hole pairs, play a crucial role in both optical excitation and correlated phenomena in solids. When excitons interact with other quasiparticles, few- and many-body excited states can appear. Here we report an interaction between exciton and charges enabled by unusual quantum confinement in two-dimensional moiré superlattices, which results in many-body ground states composed of moiré excitons and correlated electron lattices. In an H-stacked (60o-twisted) WS2/WSe2 heterobilayer, we found an interlayer moiré exciton whose hole is surrounded by its partner electron’s wavefunction distributed among three adjacent moiré traps. This three-dimensional excitonic structure enables large in-plane electrical quadrupole moments in addition to the vertical dipole. Upon doping, the quadrupole facilitates the binding of interlayer moiré excitons to the charges in neighbouring moiré cells, forming intercell charged exciton complexes. Our work provides a framework for understanding and engineering emergent exciton many-body states in correlated moiré charge orders.

AB - Excitons, Coulomb-bound electron–hole pairs, play a crucial role in both optical excitation and correlated phenomena in solids. When excitons interact with other quasiparticles, few- and many-body excited states can appear. Here we report an interaction between exciton and charges enabled by unusual quantum confinement in two-dimensional moiré superlattices, which results in many-body ground states composed of moiré excitons and correlated electron lattices. In an H-stacked (60o-twisted) WS2/WSe2 heterobilayer, we found an interlayer moiré exciton whose hole is surrounded by its partner electron’s wavefunction distributed among three adjacent moiré traps. This three-dimensional excitonic structure enables large in-plane electrical quadrupole moments in addition to the vertical dipole. Upon doping, the quadrupole facilitates the binding of interlayer moiré excitons to the charges in neighbouring moiré cells, forming intercell charged exciton complexes. Our work provides a framework for understanding and engineering emergent exciton many-body states in correlated moiré charge orders.

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Intercell moiré exciton complexes in electron lattices

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