J. Semicond. > 2023, Volume 44 > Issue 1 > 011001, doi: 10.1088/1674-4926/44/1/011001
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REVIEWS

Interface engineering in two-dimensional heterostructures towards novel emitters

Hua Li1, Jinyang Ling1, Jiamin Lin1, Xin Lu2 and Weigao Xu1,

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 Corresponding author: Weigao Xu, xuwg@nju.edu.cn

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Abstract: Two-dimensional (2D) semiconductors have captured broad interest as light emitters, due to their unique excitonic effects. These layer-blocks can be integrated through van der Waals assembly, i.e., fabricating homo- or heterojunctions, which show novel emission properties caused by interface engineering. In this review, we will first give an overview of the basic strategies that have been employed in interface engineering, including changing components, adjusting interlayer gap, and tuning twist angle. By modifying the interfacial factors, novel emission properties of emerging excitons are unveiled and discussed. Generally, well-tailored interfacial energy transfer and charge transfer within a 2D heterostructure cause static modulation of the brightness of intralayer excitons. As a special case, dynamically correlated dual-color emission in weakly-coupled bilayers will be introduced, which originates from intermittent interlayer charge transfer. For homobilayers and type Ⅱ heterobilayers, interlayer excitons with electrons and holes residing in neighboring layers are another important topic in this review. Moreover, the overlap of two crystal lattices forms moiré patterns with a relatively large period, taking effect on intralayer and interlayer excitons. Particularly, theoretical and experimental progresses on spatially modulated moiré excitons with ultra-sharp linewidth and quantum emission properties will be highlighted. Moiré quantum emitter provides uniform and integratable arrays of single photon emitters that are previously inaccessible, which is essential in quantum many-body simulation and quantum information processing. Benefiting from the optically addressable spin and valley indices, 2D heterostructures have become an indispensable platform for investigating exciton physics, designing and integrating novel concept emitters.

Key words: van der Waals assembly, interface interaction, interlayer gap, twist angle, intralayer and interlayer excitons, moiré excitons



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Fig. 1.  (Color online) Features of lattice and band structures of TMD monolayers and heterostructures. (a) 2D hexagonal lattice representing monolayer TMDs. Ri are the vectors connecting nearest metal atoms. (b) Schematic drawing of valley-contrasting splitting at the K and K′ valley of the band structure at the band edges. (c) Spin and valley coupled optical selection rules. K (K′) valley couple to σ+ (σ−) circularly polarized light[15]. Copyright 2012, American Physical Society. (d) Band structures calculated with exchange-correlation energy functions, and the corresponding Brillouin zone (the top right)[31]. Copyright 2013, American Physical Society. (e) Calculated band-edge energies for various TMDs based on ab initio density functional theory calculation using the Perdew-Burke-Ernzerhof functional (blue) and G0W0 (pink), respectively[32]. Copyright 2016, Institute of Physics.

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Fig. 2.  (Color online) Interlayer gap dependence of energy and charge transfer at the 2D interface. (a) The energies of the band-edge states as a function of the interlayer gap in MoS2/WS2 heterostructures[41]. Copyright 2013, American Physical Society. (b, c) Schemes of Fӧrster and Dexter energy transfer mechanism (left), and schemes (right) of representative TMD heterobilayers showing the direction of Fӧrster and Dexter energy transfer[45, 46]. Copyright 2016, American Chemical Society (b) and 2019, American Chemical Society (c). (d) Scheme of WSe2/WS2 heterostructures with different BN intermediate layers. (e) Charge transfer kinetics for heterostructures with different BN layer thicknesses[47]. Copyright 2020, American Chemical Society.

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Fig. 3.  (Color online) Twist-angle-dependent features of the 2D interface. (a) Twist-angle dependence of the average layer distance of the WS2/WSe2 heterobilayer based on AA-stacking (blue) and AB-stacking (red) configurations, calculated by dispersion-corrected DFT. (b) Calculated K–K (blue) and Γ–K (red) transition energies for AB-stacked heterobilayers with different twist angles[56]. Copyright 2021, Oxford University Press. (c–e) Transient kinetics in the MoS2 layer for WSe2/MoS2 heterobilayers with three different twist angles, including a single exponential rise (CT: charge transfer process) and a single exponential decay (CR: charge recombination process). (f) Interfacial charge transfer lifetime and charge recombination lifetime as a function of Δϕ (bottom axis) and momentum change (top axis) in WSe2/MoS2 heterojunctions. Inset shows scheme illustrating the twist angle in momentum space[42]. Copyright 2017, American Chemical Society.

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Fig. 4.  (Color online) Enhanced emission by interfacial interaction in TMD heterostructures. (a, b) Förster energy transfer in MoSe2/WS2 heterobilayers, including photoluminescence excitation intensity map at 78 K where the color scale represents emission intensity (a) and photoluminescence spectra for MoSe2 emission from different heterostructures excited in resonance with A exciton of WS2 (W-A) at 2.00 eV at room temperature (b)[45]. Copyright 2016, American Chemical Society. (c, d) Trion-mediated Förster energy transfer and optical gating effect in WS2/hBN/MoSe2 heterostructures, including the scheme of trion-mediated energy transfer and optical gating effect (c), and photoluminescence spectra at different positions of heterostructures (d)[48]. Copyright 2020, American Chemical Society. (e, f) Dexter energy transfer in WSe2/MoTe2 heterostructures, including photoluminescence spectra of different domains (e) and schematic depiction of near-unity energy transfer of both bright and dark excitons from WSe2 to MoTe2 (f)[46]. Copyright 2019, American Chemical Society. (g, h) Enhanced emission of MoSe2/MoS2 heterostructures by interlayer charge transfer, including a schematic of the band alignment describing the transfer of electrons and holes (g) and photoluminescence intensity maps of the MoSe2/MoS2 with one or two layers h-BNs at the interface. Scale bars are 5 μm[72]. Copyright 2016, American Chemical Society.

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Fig. 5.  (Color online) Fluorescence blinking of 2D emitters. (a) Optical image (left) and fluorescence images (three panels on the right) of a WS2/MoSe2 heterobilayer showing bright, neutral, and dark emission state of WS2 at the heterobilayer region. (b) Spectra of WS2 and MoSe2, and optical image of WS2/MoSe2 heterobilayer (inset). (c) Time-dependent intensity of WS2 (red curve) and MoSe2 (blue curve) emission from the spectra shown in (b)[36]. Copyright 2017, The Authors. (d) Capture of interfacial photocurrent in a blinking WSe2/WS2 circuit at zero bias. The photocurrent and fluorescence intensities are recorded synchronously[39]. Copyright 2021, American Chemical Society.

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Fig. 6.  (Color online) Intralayer moiré excitons in TMD heterostructures. (a) Left: schematic illustration of the moiré superlattice with a twist angle θ and moiré potential period aM. Right: the moiré Brillouin zone corresponding to the moiré unit cell. (b) Schematic diagram of excitons trapped by the periodic moiré potential. (c) Observation of moiré excitons in twisted WS2/WS2 homobilayer superlattices. (d) Linear energy distribution of different peaks fitted by the Lorentzian function[87]. Copyright 2022, American Physical Society. (e, f) Excitons in a reconstructed moiré potential. (e) Scanning electron microscopy image of twisted WSe2 bilayer showing a reconstructed moiré pattern[90]. Copyright 2021, Wiley-VCH GmbH. (f) Photoluminescence spectra at five positions in a WSe2 homobilayer[91]. Copyright 2022, Royal Society of Chemistry.

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Fig. 7.  (Color online) Emission features of interlayer excitons in TMD heterostructures. (a) Photoluminescence of WSe2 and MoSe2 monolayers and the heterobilayers[95]. Copyright 2022, Royal Society of Chemistry. (b) Interlayer exciton energies and calculated transition energies for heterobilayers with different twist angles. (c) Left: band alignment diagram. Right: the misaligned Brillouin zones of MoS2 (blue) and WSe2 (green) where both K–K and Γ–K transitions are k-space indirect[96]. Copyright 2020, Royal Society of Chemistry. (d) Intensity and (e) energy of the interlayer exciton emission versus the twist angle. The inset in (d) shows the schema of MoSe2/WSe2 heterobilayers[97]. Copyright 2017, American Chemical Society. (f, g) Spin-valley polarization of the interlayer exciton in MoSe2/WSe2 heterostructures. (f) Circular polarization-resolved photoluminescence spectra of the interlayer exciton showing the generation of strong valley polarization. (g) Spatial maps of σ+ (left) and σ− (right) interlayer exciton photoluminescence[98]. Copyright 2016, Science.

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Fig. 8.  (Color online) Modulated emissions of interlayer moiré excitons in TMD heterostructures. (a) A moiré superlattice formed by a MoSe2/WSe2 vertical heterostructure, showing three highlighted regions with three-fold rotational symmetry. (b) Optical selection rules of different atomic configurations in K valley. (c) Left: the moiré potential of the interlayer exciton transition, showing a local minimum and maximum at different sites. Right: spatial map of the degree of circular polarization for K-valley excitons[111]. Copyright 2021, Springer Nature. (d, e) Helicity-resolved photoluminescence spectra of trapped interlayer excitons in MoSe2/WSe2 heterobilayers with twist angles of (d) 57° and (e) 2°[112]. Copyright 2021, Royal Society of Chemistry. (f-h), Modulation of interlayer moiré excitons by strain, which changes the moiré patterns. (f, g) Piezoresponse force microscopy (PFM) images at two locations of the heterostructure subjected to stress[113]. Copyright 2021, Wiley‐VCH GmbH. (h) Excitation power-dependent emission spectra of 1D moiré exciton[114]. Copyright 2021, American Chemical Society. (i) Trapped interlayer trions in a moiré superlattice[115]. Copyright 2021, Nature.

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Fig. 9.  (Color online) Quantum emission from moiré excitons. (a) Nano-patterned quantum emitter arrays. Left: distribution of oscillator strength of the interlayer exciton. Right: nanodot confinements at A points, realizing a periodic array of excitonic quantum emitters. Three high-symmetry points corresponding to the moiré superlattices are labeled as A, B, and C, respectively[109]. Copyright 2017, Science. (b) Normalized emission spectra excited by photon energy of 1.55 eV with different excitation power densities[118]. Copyright 2021, American Chemical Society. (c–f) Quantum features of moiré interlayer excitons. (c) Photoluminescence spectrum of MoSe2/WSe2 moiré superlattices at 4 K. (d) Time-resolved normalized PL intensity of the single emitter fitted by single exponential decay fit (red line), which reveals a lifetime of 12.1 ± 0.3 ns. (e) Integrated PL intensity of the same single emission peak (1.401 eV) at different excitation powers. (f) Photon antibunching revealed by second-order photon correlation statistics (g(2)(τ)) of emission with the experimental data (red solid line) and the Poissonian interval error (red shadowed area)[119]. Copyright 2020, Science.

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Table 1.   Primary progresses on novel van der Waals emitters based on interface engineering.

Interface engineering method Interface parameterComponentProperties
Interlayer gap a~ 10 ÅWSe2/MoTe2[46]Dexter energy transfer
< 10 nmMoSe2/WS2[45]Förster energy transfer
2-5 nm, no spacing layerWS2/MoSe2[36]Fluorescence blinking
WS2/WSe2[39]
Twist angle b2°MoSe2/WS2[139]Hybridized exciton
0.5 ± 0.3°WSe2/WS2[85]Intralayer moiré exciton
1.5°WSe2/WS2[87]
< 5°WSe2/WSe2[88]
1.36°WSe2/WSe2[89]
0°/60°MoSe2/WSe2[59]Long-live interlayer exciton
0°–60°MoSe2/WSe2[102]k-space indirect interlayer exciton
MoS2/WSe2[100]
WS2/WSe2[56]
~0°/~60°MoSe2/WSe2[98]Valley polarized interlayer exciton
2°/20°/57°MoSe2/WSe2[126]
58.7°± 0.7°WSe2/MoSe2[140]
2°/20°/57°MoSe2/WSe2[126]Interlayer moiré exciton
~1°MoSe2/WSe2[106]
56.7 ± 0.2°MoSe2/WSe2[115]Interlayer moiré trion
~60°MoSe2/WSe2[117]
57.5°MoSe2/WSe2[105]
0°/60°MoSe2/WSe2 (MoS2/WSe2)[109]Moiré quantum emitter
< 1°MoSe2/WSe2 (MoS2/WS2)[141]
~60°MoSe2/WSe2[119]
a The phenomenon shall be robust for almost all angles.
b In these works, thermal annealing is applied to reach a closely packed state with an estimated interlayer distance of 0.6–0.7 nm.
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    Received: 09 October 2022 Revised: 19 December 2022 Online: Accepted Manuscript: 29 December 2022Uncorrected proof: 29 December 2022Published: 14 January 2023

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      Article Navigation >  Journal of Semiconductors  > 2023  >  44(1): 011001
      Hua Li, Jinyang Ling, Jiamin Lin, Xin Lu, Weigao Xu. Interface engineering in two-dimensional heterostructures towards novel emitters[J]. Journal of Semiconductors, 2023, 44(1): 011001. doi: 10.1088/1674-4926/44/1/011001 H Li, J Y Ling, J M Lin, X Lu, W G Xu. Interface engineering in two-dimensional heterostructures towards novel emitters[J]. J. Semicond, 2023, 44(1): 011001. doi: 10.1088/1674-4926/44/1/011001Export: BibTex EndNote
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      Hua Li, Jinyang Ling, Jiamin Lin, Xin Lu, Weigao Xu. Interface engineering in two-dimensional heterostructures towards novel emitters[J]. Journal of Semiconductors, 2023, 44(1): 011001. doi: 10.1088/1674-4926/44/1/011001

      H Li, J Y Ling, J M Lin, X Lu, W G Xu. Interface engineering in two-dimensional heterostructures towards novel emitters[J]. J. Semicond, 2023, 44(1): 011001. doi: 10.1088/1674-4926/44/1/011001
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      Interface engineering in two-dimensional heterostructures towards novel emitters

      doi: 10.1088/1674-4926/44/1/011001
      • 1.

        Key Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China

      • 2.

        Department of Physics and Engineering Physics, Tulane University, New Orleans, USA

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      • Author Bio:

        Hua Li got her BS degree in 2015 and MS degree in 2018 at Lanzhou University. She then joined Weigao Xu’s group and got her PhD degree in 2021 at Nanjing University. Now she is an associate research fellow at Nanjing University. Her research interest focuses on the optical spectroscopy and microscopic imaging at the interfaces

        Jinyang Ling received his BS degree in Chemistry from Nanjing University in 2021 and is currently pursuing his MS in Physical Chemistry under the supervision of Prof. Weigao Xu at the School of Chemistry and Chemical Engineering in Nanjing University. His research focuses on the excitonic dynamics of 2D layered materials in the in-plane direction, and corresponding excitonic optoelectronic devices

        Jiamin Lin received her BS degree in Materials Science and Engineering from Nanjing University of Science and Technology in 2020 and she is currently pursuing her PhD at institute of Chemistry and Chemical Engineering, Nanjing University, under the supervision of Prof. Weigao Xu. Her research interests include low-dimensional materials and their optothermal transport behavior

        Xin Lu earned her bachelor’s degree from Wuhan University in 2012, and her PhD from Nanyang Technological University in 2017. Subsequently, Lu joined Prof. Ajit Srivastava’s group at Emory University as a postdoctoral researcher. Since January 2021, Lu has started as an Assistant Professor in the Department of Physics and Engineering Physics at Tulane University. Her research focuses on optical spectroscopy of low-dimensional materials

        Weigao Xu got his BS degree in 2008 at Lanzhou University and PhD degree in 2013 at Peking University. Then he joined Qihua Xiong’s group as a postdoc at Nanyang Technological University in Singapore. In March 2018, he joined Nanjing University as a full professor. His research interest focuses on the bottom-up assembly of meso-scale materials from nanomaterial units, the discovery of their optical, electrical, mechanical, and chemical properties, and the development of their functionalities

      • Corresponding author: xuwg@nju.edu.cn
      • Received Date: 2022-10-09
      • Revised Date: 2022-12-19
        • Available Online: 2022-12-29

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