Abstract

Two-dimensional transitional metal dichalcogenides (TMDCs) based lateral heterojunctions have emerged as appealing and intriguing materials for applications in the next generation flexible nanoelectronics. The construction of depletion region near the in-plane interface brings rich opto-electrical dynamics, which is essential for future applications. Due to the synchronous requirement of spatial and time resolution, the study of lateral heterojunction dynamics remains a challenging issue. Herein, with a home-built spatiotemporal femtosecond transient absorption (TAS) spectroscopy platform, we have investigated the ultrafast photocarrier dynamics of monolayer spatial composition-graded WS2xSe2(1−x) lateral heterojunctions. At the alloy interface, the charge transfer (CT) processes have been visualized and referred to occur in 1 ps time scale. The mobility difference between electrons and holes results in the space modulation of the interface and a significant broadening of rising edge on the shell region. Moreover, carrier lifetime near the interface is extraordinarily extended by over 3 times from 153 ps to 678 ps. All these results unveil its great potential in designing future low cost logic devices and ultrafast optical applications.

© 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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2018 (1)

H. Li, X. Zheng, Y. Liu, Z. Zhang, and T. Jiang, “Ultrafast interfacial energy transfer and interlayer excitons in the monolayer WS2/CsPbBr3 quantum dot heterostructure,” Nanoscale. 10, 1650–1659 (2018).
[Crossref]

2017 (13)

Z. Zhang, P. Chen, X. Duan, K. Zang, J. Luo, and X. Duan, “Robust epitaxial growth of two-dimensional heterostructures, multiheterostructures, and superlattices,” Science. 357, 788–792 (2017).
[Crossref] [PubMed]

Z. Ji, H. Hong, J. Zhang, Q. Zhang, W. Huang, T. Cao, R. Qiao, C. Liu, J. Liang, C. Jin, L. Jiao, K. Shi, S. Meng, and K. Liu, “Robust Stacking-Independent Ultrafast Charge Transfer in MoS2/WS2 Bilayers,” ACS Nano 11, 12020–12026 (2017).
[Crossref] [PubMed]

Y. Li, Q. Cui, F. Ceballos, S. D. Lane, Z. Qi, and H. Zhao, “Ultrafast Interlayer Electron Transfer in Incommensurate Transition Metal Dichalcogenide Homobilayers,” Nano Lett. 17, 6661–6666 (2017).
[Crossref] [PubMed]

M. Baranowski, A. Surrente, L. Klopotowski, J. M. Urban, N. Zhang, D. K. Maude, K. Wiwatowski, S. Mackowski, Y. C. Kung, D. Dumcenco, A. Kis, and P. Plochocka, “Probing the Interlayer Exciton Physics in a MoS2/MoSe2/MoS2 van der Waals Heterostructure,” Nano Lett. 17, 6360–6365 (2017).
[Crossref] [PubMed]

B. Miller, A. Steinhoff, B. Pano, J. Klein, F. Jahnke, A. Holleitner, and U. Wurstbauer, “Long-Lived Direct and Indirect Interlayer Excitons in van der Waals Heterostructures,” Nano Lett. 17, 5229–5237 (2017).
[Crossref] [PubMed]

J. Shi, M.-H. Lin, I.-T. Chen, N. Mohammadi Estakhri, X.-Q. Zhang, Y. Wang, H.-Y. Chen, C.-A. Chen, C.-K. Shih, A. Alù, X. Li, Y.-H. Lee, and S. Gwo, “Cascaded exciton energy transfer in a monolayer semiconductor lateral heterostructure assisted by surface plasmon polariton,” Nat. Commun. 8, 35 (2017).
[Crossref] [PubMed]

W. Wei, Y. Dai, and B. Huang, “Straintronics in two-dimensional in-plane heterostructures of transition-metal dichalcogenides,” Phys. Chem. Chem. Phys. 19, 663–672 (2017).
[Crossref]

F. Ullah, Y. Sim, C. T. Le, M.-J. Seong, J. I. Jang, S. H. Rhim, B. C. Tran Khac, K.-H. Chung, K. Park, Y. Lee, K. Kim, H. Y. Jeong, and Y. S. Kim, “Growth and Simultaneous Valleys Manipulation of Two-Dimensional MoSe2-WSe2 Lateral Heterostructure,” ACS Nano 11, 8822–8829 (2017).
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L. Yuan, T. Wang, T. Zhu, M. Zhou, and L. Huang, “Exciton Dynamics, Transport, and Annihilation in Atomically Thin Two-Dimensional Semiconductors,” The J. Phys. Chem. Lett. 8, 3371–3379 (2017).
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F. Nan, Y.-H. Qiu, L. Zhou, and Q.-Q. Wang, “Ultrafast exciton dynamics in chemical heterogenous WSe2 monolayer,” J. Phys. D: Appl. Phys. 50, 485109 (2017).
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J. He, D. He, Y. Wang, and H. Zhao, “Probing effect of electric field on photocarrier transfer in graphene-WS2 van der Waals heterostructures,” Opt. Express 25, 1949–1957 (2017).
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Z. Guo, Y. Wan, M. Yang, J. Snaider, K. Zhu, and L. Huang, “Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy,” Science 356, 59 (2017).
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D. R. Cremons, D. A. Plemmons, and D. J. Flannigan, “Defect-mediated phonon dynamics in TaS2 and WSe2,” Struct. Dyn. 4, 044019 (2017).
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2016 (14)

V. Vega-Mayoral, D. Vella, T. Borzda, M. Prijatelj, I. Tempra, E. A. A. Pogna, S. Dal Conte, P. Topolovsek, N. Vujicic, G. Cerullo, D. Mihailovic, and C. Gadermaier, “Exciton and charge carrier dynamics in few-layer WS2,” Nanoscale. 8, 5428–5434 (2016).
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X. Duan, C. Wang, Z. Fan, G. Hao, L. Kou, U. Halim, H. Li, X. Wu, Y. Wang, and J. Jiang, “Synthesis of WS2xSe2−2x Alloy Nanosheets with Composition-Tunable Electronic Properties,” Nano Lett. 16, 264 (2016).
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K. M. Mccreary, A. T. Hanbicki, G. G. Jernigan, J. C. Culbertson, and B. T. Jonker, “Synthesis of Large-Area WS2 monolayers with Exceptional Photoluminescence,” Sci. Reports 6, 1861–1871 (2016).

T. Y. Jeong, B. M. Jin, S. H. Rhim, L. Debbichi, J. Park, Y. D. Jang, H. R. Lee, D.-H. Chae, D. Lee, Y.-H. Kim, S. Jung, and K. J. Yee, “Coherent Lattice Vibrations in Mono- and Few-Layer WSe2,” ACS Nano 10, 5560–5566 (2016).
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Y. Son, M.-Y. Li, C.-C. Cheng, K.-H. Wei, P. Liu, Q. H. Wang, L.-J. Li, and M. S. Strano, “Observation of Switchable Photoresponse of a Monolayer WSe2/MoS2 Lateral Heterostructure via Photocurrent Spectral Atomic Force Microscopic Imaging,” Nano Lett. 16, 3571–3577 (2016).
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B. Liu, Y. Ma, A. Zhang, L. Chen, A. N. Abbas, Y. Liu, C. Shen, H. Wan, and C. Zhou, “High-Performance WSe2 Field-Effect Transistors via Controlled Formation of In-Plane Heterojunctions,” ACS Nano 10, 5153–5160 (2016).
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K. Bogaert, S. Liu, J. Chesin, D. Titow, S. Gradečak, and S. Garaj, “Diffusion-Mediated Synthesis of MoS2/WS2 Lateral Heterostructures,” Nano Lett. 16, 5129–5134 (2016).
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W. Wei, Y. Dai, and B. Huang, “In-plane interfacing effects of two-dimensional transition-metal dichalcogenide heterostructures,” Phys. Chem. Chem. Phys. 18, 15632–15638 (2016).
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X. Wang, L. Huang, Y. Peng, N. Huo, K. Wu, C. Xia, Z. Wei, S. Tongay, and J. Li, “Enhanced rectification, transport property and photocurrent generation of multilayer ReSe2/MoS2 p–n heterojunctions,” Nano Res. 9, 507–516 (2016).
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J. R. Schaibley, P. Rivera, H. Yu, K. L. Seyler, J. Yan, D. G. Mandrus, T. Taniguchi, K. Watanabe, W. Yao, and X. Xu, “Directional interlayer spin-valley transfer in two-dimensional heterostructures,” Nat. Commun. 7, 13747 (2016).
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K. Wang, B. Huang, M. Tian, F. Ceballos, M.-W. Lin, M. Mahjouri-Samani, A. Boulesbaa, A. A. Puretzky, C. M. Rouleau, M. Yoon, H. Zhao, K. Xiao, G. Duscher, and D. B. Geohegan, “Interlayer Coupling in Twisted WSe2/WS2 Bilayer Heterostructures Revealed by Optical Spectroscopy,” ACS Nano 10, 6612–6622 (2016).
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D. Kozawa, A. Carvalho, I. Verzhbitskiy, F. Giustiniano, Y. Miyauchi, S. Mouri, A. H. Castro Neto, K. Matsuda, and G. Eda, “Evidence for Fast Interlayer Energy Transfer in MoSe2/WS2 Heterostructures,” Nano Lett. 16, 4087–4093 (2016).
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K. Zhang, T. Zhang, G. Cheng, T. Li, S. Wang, W. Wei, X. Zhou, W. Yu, Y. Sun, P. Wang, D. Zhang, C. Zeng, X. Wang, W. Hu, H. J. Fan, G. Shen, X. Chen, X. Duan, K. Chang, and N. Dai, “Interlayer Transition and Infrared Photodetection in Atomically Thin Type-II MoTe2/MoS2 van der Waals Heterostructures,” ACS Nano 10, 3852–3858 (2016).
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X. Duan, C. Wang, Z. Fan, G. Hao, L. Kou, U. Halim, H. Li, X. Wu, Y. Wang, and J. Jiang, “Synthesis of WS2xSe2(1−x) Alloy Nanosheets with Composition-Tunable Electronic Properties,” Nano Lett. 16, 264 (2016).
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2015 (19)

K. Chen, X. Wan, W. Xie, J. Wen, Z. Kang, X. Zeng, H. Chen, and J. Xu, “Lateral Built-In Potential of Monolayer MoS2/WS2 In-Plane Heterostructures by a Shortcut Growth Strategy,” Adv. Mater. 27, 6431–6437 (2015).
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S. Zheng, L. Sun, T. Yin, A. M. Dubrovkin, F. Liu, Z. Liu, Z. X. Shen, and H. J. Fan, “Monolayers of Wx Mo(1 − x)S2 alloy heterostructure with in-plane composition variations,” Appl. Phys. Lett. 106, 063113 (2015).
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Y. Gong, S. Lei, G. Ye, B. Li, Y. He, K. Keyshar, X. Zhang, Q. Wang, J. Lou, Z. Liu, R. Vajtai, W. Zhou, and P. M. Ajayan, “Two-Step Growth of Two-Dimensional WSe2/MoSe2 Heterostructures,” Nano Lett. 15, 6135–6141 (2015).
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P. Rivera, J. R. Schaibley, A. M. Jones, J. S. Ross, S. Wu, G. Aivazian, P. Klement, K. Seyler, G. Clark, N. J. Ghimire, J. Yan, D. G. Mandrus, W. Yao, and X. Xu, “Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures,” Nat. Commun. 6, 6242 (2015).
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F. Ceballos, M. Z. Bellus, H.-Y. Chiu, and H. Zhao, “Probing charge transfer excitons in a MoSe2-WS2 van der Waals heterostructure,” Nanoscale 7, 17523–17528 (2015).
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X. Zhu, N. R. Monahan, Z. Gong, H. Zhu, K. W. Williams, and C. A. Nelson, “Charge Transfer Excitons at van der Waals Interfaces,” J. Am. Chem. Soc. 137, 8313–8320 (2015).
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Y. Zhou, J. Dong, and H. Li, “Electronic transport properties of in-plane heterostructures constructed by MoS2 and WS2 nanoribbons,” RSC Adv. 5, 66852–66860 (2015).
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Y. Yu, S. Hu, L. Su, L. Huang, Y. Liu, Z. Jin, A. A. Purezky, D. B. Geohegan, K. W. Kim, Y. Zhang, and L. Cao, “Equally Efficient Interlayer Exciton Relaxation and Improved Absorption in Epitaxial and Nonepitaxial MoS2/WS2 Heterostructures,” Nano Lett. 15, 486–491 (2015).
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Y.-C. Lin, R. K. Ghosh, R. Addou, N. Lu, S. M. Eichfeld, H. Zhu, M.-Y. Li, X. Peng, M. J. Kim, L.-J. Li, R. M. Wallace, S. Datta, and J. A. Robinson, “Atomically thin resonant tunnel diodes built from synthetic van der Waals heterostructures,” Nat. Commun. 6, 1–10 (2015).
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X.-Q. Zhang, C.-H. Lin, Y.-W. Tseng, K.-H. Huang, and Y.-H. Lee, “Synthesis of Lateral Heterostructures of Semiconducting Atomic Layers,” Nano Lett. 15, 410–415 (2015). : 25494614.
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K. Chen, X. Wan, J. Wen, W. Xie, Z. Kang, X. Zeng, H. Chen, and J.-B. Xu, “Electronic Properties of MoS2/WS2 Heterostructures Synthesized with Two-Step Lateral Epitaxial Strategy,” ACS Nano 9, 9868–9876 (2015).
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J. Kang, H. Sahin, and F. M. Peeters, “Tuning Carrier Confinement in the MoS2/WS2 Lateral Heterostructure,” The J. Phys. Chem. C 119, 9580–9586 (2015).
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B. Liu, M. Fathi, L. Chen, A. Abbas, Y. Ma, and C. Zhou, “Chemical Vapor Deposition Growth of Monolayer WSe2 with Tunable Device Characteristics and Growth Mechanism Study,” Acs Nano 9, 6119 (2015).
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Y. D. Kim, H. Kim, Y. Cho, J. H. Ryoo, C.-H. Park, P. Kim, Y. S. Kim, S. Lee, Y. Li, S.-N. Park, Y. Shim Yoo, D. Yoon, V. E. Dorgan, E. Pop, T. F. Heinz, J. Hone, S.-H. Chun, H. Cheong, S. W. Lee, M.-H. Bae, and Y. D. Park, “Bright visible light emission from graphene,” Nat. Nanotechnol. 10, 676 (2015).
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P. Rivera, J. R. Schaibley, A. M. Jones, J. S. Ross, S. Wu, G. Aivazian, P. Klement, K. Seyler, G. Clark, N. J. Ghimire, J. Yan, D. G. Mandrus, W. Yao, and X. Xu, “Observation of long-lived interlayer excitons in monolayer MoSe2-WSe2 heterostructures,” Nat. Commun. 6, 6242 (2015).
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M. Z. Bellus, F. Ceballos, H.-Y. Chiu, and H. Zhao, “Tightly Bound Trions in Transition Metal Dichalcogenide Heterostructures,” ACS Nano 9, 6459–6464 (2015).
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M. Y. Li, Y. Shi, C. C. Cheng, L. S. Lu, Y. C. Lin, H. L. Tang, M. L. Tsai, C. W. Chu, K. H. Wei, and J. H. He, “NANOELECTRONICS. Epitaxial growth of a monolayer WSe2-MoS2 lateral p-n junction with an atomically sharp interface,” Science 349, 524 (2015).
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W. Yan, Z. Guo, T. Zhu, S. Yan, J. Johnson, and L. Huang, “Cooperative singlet and triplet exciton transport in tetracene crystals visualized by ultrafast microscopy,” Nat. Chem. 7, 785 (2015).
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Z. Guo, J. S. Manser, W. Yan, P. V. Kamat, and L. Huang, “Spatial and temporal imaging of long-range charge transport in perovskite thin films by ultrafast microscopy,” Nat. Commun. 6, 7471 (2015).
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2014 (13)

T. Jiang, H. Liu, D. Huang, S. Zhang, Y. Li, X. Gong, Y.-R. Shen, W.-T. Liu, and S. Wu, “Valley and band structure engineering of folded MoS2 bilayers,” Nat. Nanotechnol. 9, 825–829 (2014).
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Q. Cui, F. Ceballos, N. Kumar, and H. Zhao, “Transient Absorption Microscopy of Monolayer and Bulk WSe2,” ACS Nano 8, 2970–2976 (2014).
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C.-H. Lee, G.-H. Lee, A. M. van der Zande, W. Chen, Y. Li, M. Han, X. Cui, G. Arefe, C. Nuckolls, T. F. Heinz, J. Guo, J. Hone, and P. Kim, “Atomically thin p–n junctions with van der Waals heterointerfaces,” Nat. Nanotechnol. 9, 676–681 (2014).
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C. Huang, S. Wu, A. M. Sanchez, J. J. P. Peters, R. Beanland, J. S. Ross, P. Rivera, W. Yao, D. H. Cobden, and X. Xu, “Lateral heterojunctions within monolayer MoSe2–WSe2 semiconductors,” Nat. Mater. 13, 1096–1101 (2014).
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Y. Gong, J. Lin, X. Wang, G. Shi, S. Lei, Z. Lin, X. Zou, G. Ye, R. Vajtai, B. I. Yakobson, H. Terrones, M. Terrones, B. K. Tay, J. Lou, S. T. Pantelides, Z. Liu, W. Zhou, and P. M. Ajayan, “Vertical and in-plane heterostructures from WS2/MoS2 monolayers,” Nat. Mater. 13, 1135–1142 (2014).
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S. Tongay, W. Fan, J. Kang, J. Park, U. Koldemir, J. Suh, D. S. Narang, K. Liu, J. Ji, J. Li, R. Sinclair, and J. Wu, “Tuning Interlayer Coupling in Large-Area Heterostructures with CVD-Grown MoS2 and WS2 Monolayers,” Nano Lett. 14, 3185–3190 (2014).
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X. Hong, J. Kim, S.-F. Shi, Y. Zhang, C. Jin, Y. Sun, S. Tongay, J. Wu, Y. Zhang, and F. Wang, “Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures,” Nat. Nanotechnol. 9, 682–686 (2014).
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H. Fang, C. Battaglia, C. Carraro, S. Nemsak, B. Ozdol, J. S. Kang, H. A. Bechtel, S. B. Desai, F. Kronast, A. A. Unal, G. Conti, C. Conlon, G. K. Palsson, M. C. Martin, A. M. Minor, C. S. Fadley, E. Yablonovitch, R. Maboudian, and A. Javey, “Strong interlayer coupling in van der Waals heterostructures built from single-layer chalcogenides,” Proc. Natl. Acad. Sci. 111, 6198–6202 (2014).
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F. Ceballos, M. Z. Bellus, H.-Y. Chiu, and H. Zhao, “Ultrafast Charge Separation and Indirect Exciton Formation in a MoS2/MoSe2 van der Waals Heterostructure,” ACS Nano 8, 12717–12724 (2014).
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F. Xia, H. Wang, D. Xiao, M. Dubey, and A. Ramasubramaniam, “Two-dimensional material nanophotonics,” Nat. Photonics 8, 899–907 (2014).
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J. He, N. Kumar, M. Z. Bellus, H.-Y. Chiu, D. He, Y. Wang, and H. Zhao, “Electron transfer and coupling in graphene–tungsten disulfide van der Waals heterostructures,” Nat. Commun. 5, 5622 (2014).
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X. Duan, C. Wang, J. C. Shaw, R. Cheng, Y. Chen, H. Li, X. Wu, Y. Tang, Q. Zhang, A. Pan, J. Jiang, R. Yu, Y. Huang, and X. Duan, “Lateral epitaxial growth of two-dimensional layered semiconductor heterojunctions,” Nat. Nanotechnol. 9, 1024 (2014).
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M. M. Furchi, A. Pospischil, F. Libisch, J. Burgörfer, and T. Mueller, “Photovoltaic Effect in an Electrically Tunable van der Waals Heterojunction,” Nano Lett. 14, 4785–4791 (2014).
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2013 (6)

S. Z. Butler, S. M. Hollen, L. Cao, Y. Cui, J. A. Gupta, H. R. Gutiérrez, T. F. Heinz, S. S. Hong, J. Huang, A. F. Ismach, E. Johnston-Halperin, M. Kuno, V. V. Plashnitsa, R. D. Robinson, R. S. Ruoff, S. Salahuddin, J. Shan, L. Shi, M. G. Spencer, M. Terrones, W. Windl, and J. E. Goldberger, “Progress, Challenges, and Opportunities in Two-Dimensional Materials Beyond Graphene,” ACS Nano 7, 2898–2926 (2013).
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J. Kang, S. Tongay, J. Zhou, J. Li, and J. Wu, “Band offsets and heterostructures of two-dimensional semiconductors,” Appl. Phys. Lett. 102, 012111 (2013).
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L. Britnell, R. M. Ribeiro, A. Eckmann, R. Jalil, B. D. Belle, A. Mishchenko, Y.-J. Kim, R. V. Gorbachev, T. Georgiou, S. V. Morozov, A. N. Grigorenko, A. K. Geim, C. Casiraghi, A. H. C. Neto, and K. S. Novoselov, “Strong Light-Matter Interactions in Heterostructures of Atomically Thin Films,” Science 340, 1311–1314 (2013).
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J. Kang, S. Tongay, J. Li, and J. Wu, “Monolayer semiconducting transition metal dichalcogenide alloys: Stability and band bowing,” J. Appl. Phys. 113, 143703 (2013).
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B. Liu, M. Fathi, L. Chen, A. Abbas, Y. Ma, and C. Zhou, “Chemical Vapor Deposition Growth of Monolayer WSe2 with Tunable Device Characteristics and Growth Mechanism Study,” Acs Nano 9, 6119 (2015).
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Abbas, A. N.

B. Liu, Y. Ma, A. Zhang, L. Chen, A. N. Abbas, Y. Liu, C. Shen, H. Wan, and C. Zhou, “High-Performance WSe2 Field-Effect Transistors via Controlled Formation of In-Plane Heterojunctions,” ACS Nano 10, 5153–5160 (2016).
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Addou, R.

Y.-C. Lin, R. K. Ghosh, R. Addou, N. Lu, S. M. Eichfeld, H. Zhu, M.-Y. Li, X. Peng, M. J. Kim, L.-J. Li, R. M. Wallace, S. Datta, and J. A. Robinson, “Atomically thin resonant tunnel diodes built from synthetic van der Waals heterostructures,” Nat. Commun. 6, 1–10 (2015).
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Aivazian, G.

P. Rivera, J. R. Schaibley, A. M. Jones, J. S. Ross, S. Wu, G. Aivazian, P. Klement, K. Seyler, G. Clark, N. J. Ghimire, J. Yan, D. G. Mandrus, W. Yao, and X. Xu, “Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures,” Nat. Commun. 6, 6242 (2015).
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Y. Gong, S. Lei, G. Ye, B. Li, Y. He, K. Keyshar, X. Zhang, Q. Wang, J. Lou, Z. Liu, R. Vajtai, W. Zhou, and P. M. Ajayan, “Two-Step Growth of Two-Dimensional WSe2/MoSe2 Heterostructures,” Nano Lett. 15, 6135–6141 (2015).
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Y. Gong, J. Lin, X. Wang, G. Shi, S. Lei, Z. Lin, X. Zou, G. Ye, R. Vajtai, B. I. Yakobson, H. Terrones, M. Terrones, B. K. Tay, J. Lou, S. T. Pantelides, Z. Liu, W. Zhou, and P. M. Ajayan, “Vertical and in-plane heterostructures from WS2/MoS2 monolayers,” Nat. Mater. 13, 1135–1142 (2014).
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J. Shi, M.-H. Lin, I.-T. Chen, N. Mohammadi Estakhri, X.-Q. Zhang, Y. Wang, H.-Y. Chen, C.-A. Chen, C.-K. Shih, A. Alù, X. Li, Y.-H. Lee, and S. Gwo, “Cascaded exciton energy transfer in a monolayer semiconductor lateral heterostructure assisted by surface plasmon polariton,” Nat. Commun. 8, 35 (2017).
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Y. D. Kim, H. Kim, Y. Cho, J. H. Ryoo, C.-H. Park, P. Kim, Y. S. Kim, S. Lee, Y. Li, S.-N. Park, Y. Shim Yoo, D. Yoon, V. E. Dorgan, E. Pop, T. F. Heinz, J. Hone, S.-H. Chun, H. Cheong, S. W. Lee, M.-H. Bae, and Y. D. Park, “Bright visible light emission from graphene,” Nat. Nanotechnol. 10, 676 (2015).
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H. Fang, C. Battaglia, C. Carraro, S. Nemsak, B. Ozdol, J. S. Kang, H. A. Bechtel, S. B. Desai, F. Kronast, A. A. Unal, G. Conti, C. Conlon, G. K. Palsson, M. C. Martin, A. M. Minor, C. S. Fadley, E. Yablonovitch, R. Maboudian, and A. Javey, “Strong interlayer coupling in van der Waals heterostructures built from single-layer chalcogenides,” Proc. Natl. Acad. Sci. 111, 6198–6202 (2014).
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F. Ceballos, M. Z. Bellus, H.-Y. Chiu, and H. Zhao, “Probing charge transfer excitons in a MoSe2-WS2 van der Waals heterostructure,” Nanoscale 7, 17523–17528 (2015).
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M. Z. Bellus, F. Ceballos, H.-Y. Chiu, and H. Zhao, “Tightly Bound Trions in Transition Metal Dichalcogenide Heterostructures,” ACS Nano 9, 6459–6464 (2015).
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J. He, N. Kumar, M. Z. Bellus, H.-Y. Chiu, D. He, Y. Wang, and H. Zhao, “Electron transfer and coupling in graphene–tungsten disulfide van der Waals heterostructures,” Nat. Commun. 5, 5622 (2014).
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F. Ceballos, M. Z. Bellus, H.-Y. Chiu, and H. Zhao, “Ultrafast Charge Separation and Indirect Exciton Formation in a MoS2/MoSe2 van der Waals Heterostructure,” ACS Nano 8, 12717–12724 (2014).
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K. Bogaert, S. Liu, J. Chesin, D. Titow, S. Gradečak, and S. Garaj, “Diffusion-Mediated Synthesis of MoS2/WS2 Lateral Heterostructures,” Nano Lett. 16, 5129–5134 (2016).
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Supplementary Material (2)

NameDescription
» Visualization 1       This video illustrates the modulation of the depletion region induced by ultrafast photo-carrier dynamics.
» Visualization 1       This video illustrates the modulation of the depletion region induced by ultrafast photo-carrier dynamics.

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Figures (15)

Fig. 1
Fig. 1 (a) Diagram of the spatiotemporal femtosecond transient absorption system. (b) Energy level diagram of the lateral WS2xSe2(1−x) alloy heterostructures in real space. At the boundary between the core and the shell, WS2xSe2(1−x) alloy interface is formed and thus the energy band transits gradually from WS2 to WSe2. Through fixing the exciting position and scanning the probe light across the interface, the transient exciton density of both sides can be monitored.
Fig. 2
Fig. 2 (a) Optical microscopy image of monolayer WS2xSe2(1−x) alloy lateral heterosjunction. Interface is labeled by white dash line. Spots marked by black, red and blue represent the selected positions of the PL measurement. (b) AFM image and the corresponding phase image. (c) Composition of ternary semiconductor alloys. Inset: PL mapping of the entire monolayer. (d) PL intensities collected from spots marked in (c).
Fig. 3
Fig. 3 (a) Optical microscopy image of heterojunction. Spots marked in black or red are the detection positions. Inset: Synchronous pump-probe mapping at 720 nm wavelength as the probe at 0 ps. (b) Normalized differential reflection signal as a function of delay time. Red and black curves are exponential fits of raw data. The rising time of both core and shell regions are around 400 fs. Gray area is the cross correlation of the pump and probe fitted by Gauss function.
Fig. 4
Fig. 4 (a) Microscope image of the heterojunction with a yellow dash line outlining the heterojunction. The relative position of the excitation spot and the heterojunction is shown in the picture. The red dash line in the middle of the spot represents the scanning direction. (b) Spatiotemporal differential reflection signal as a function of the real space (X-axis) and probe delay. (c) Spatial profile of differential reflection with different probe delays on the X-axis. Solid lines are fitted date by Gauss function. (d) Normalized differential reflection signal with different probe delays.
Fig. 5
Fig. 5 (a) Microscope image of the heterojunction (b) Spatiotemporal differential reflection signal as a function of the real space (X-axis) and probe delay. (c,d) 2D mapping of spatial profile of differential reflection at 0 ps and 0.3 ps. Dash circle represents the pump spot. Red dash line represents the scanning direction in 1D mapping. (e) Peak differential reflection signal of two sides as function of probe delay. (f) Spatial profile of differential reflection signal at 0 ps, 0.3 ps, 2.5 ps along X-axis. (g) Modulation of depletion region extracted from (b) in the first 3 ps.
Fig. 6
Fig. 6 Panel (a,b,c) shows the band structure of the lateral heterojunction and the movement of carriers as a result of Coulomb force originated from the depletion region. (d–h) Carrier density induced modulation of the interface. Pictures are drawing in chronological order.
Fig. 7
Fig. 7 Panel (a,b,c,d) shows the spatiotemporal differential reflection signal with different excitation position. The wavelength of the probe is 720 nm corresponding to the band edge emission of shell region. Pictures on the right side are the spatiotemporal graphs of each left excitation position.
Fig. 8
Fig. 8 (a) Normalized peak differential reflection signal extracted from all four different excitation positions at the shell zone. (b) The magnified rising time of all four curves in (a) and data fitted by Gaussian error function.
Fig. 9
Fig. 9 Time-resolved transient absorption spectrum mapping with different probe wavelengths at 0 ps. The step size is 200 nm. (a) Optical microscopy of composition-graded WS2xSe2(1−x) alloys and its interface marked by yellow dash line. (b,c,d) Mapping images with 670 nm, 700 nm, 720 nm wavelengths serving as probe lights.
Fig. 10
Fig. 10 Polarization-resolved second-harmonic generation(SHG) microscopy measurement of the lateral heterostructure. (a) Optical microscopy of composition-graded WS2xSe2(1−x) alloys. Interface is noted by white dash line. Yellow dash square represents the mapping region. (b) Total SH intensity of points markd in panel (a). (c,d) Polarization-resolved SH mapping of the area enclosed by the yellow dash square in panel (a). (e) Total SH mapping IV + IH. (f) Calculated angle θ between armchair axis and the excitation laser polarization direction. The scale bar for all is 10 μm
Fig. 11
Fig. 11 (a) Photoluminescence (PL) mapping of the entire lateral heterojunction. Each point is described by its peak PL wavelength. The step size is 1 μm. Interface can hardly been observed in this mapping image. (b) PL intensity of points marked in (a). Inset: Magnified PL spectrum with detailed information about points marked by 5,6 and 7. (C) Raman intensity of points marked in (a).
Fig. 12
Fig. 12 (a) Interpolated time-resolved transient absorption spectrum across the junction. The black dash line represents the interface position. (b) time-resolved transient absorption spectral lines across the junction.
Fig. 13
Fig. 13 (a) Linear region measurement of pump fluence. The spot marked in red is the pump fluence we used in our experiment. (b) Measurement of spatial resolution of our spatiotemporal femtosecond transient absorption spectrum system.
Fig. 14
Fig. 14 Solutions of Eq. (8) with different initial value of Δh.
Fig. 15
Fig. 15 Spatiotemporal femtosecond transient absorption spectrum system.

Equations (11)

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Δ R / R 0 = ( R R 0 ) / R 0
Δ p = Δ n + Δ h
d Δ p d t = A ( n p n 0 p 0 ) = A ( n 0 Δ p + p 0 Δ n + Δ p Δ n )
θ = ( 1 / 3 ) tan 1 I V / I H
E g ( x ) = x E gWS 2 + ( 1 x ) E gWSe 2
x = ( 1.97 E g ( x ) ) / 0.34
d Δ p d t = A ( n p n 0 p 0 ) = A ( n 0 Δ p + p 0 Δ n + Δ p Δ n )
d Δ p d t = A [ Δ p 2 + ( p 0 Δ h ) Δ p p 0 Δ h ]
d Δ p d t = A [ Δ p 2 Δ h Δ p ]
d Δ p d t = A Δ p 2
Δ R / R 0 = ( R R 0 ) / R 0

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