Abstract
In recent years, there has been ongoing effort in achieving efficient transport of excitons in monolayer transition metal dichalcogenides subjected to highly non-uniform strain. Here we investigate the transport of excitons and trions in monolayer semiconductor WS2 subjected to controlled non-uniform mechanical strain. An atomic force microscope (AFM)-based setup is applied to actively control and tune the strain profiles by indenting the monolayer with an AFM tip. Optical spectroscopy is used to reveal the dynamics of the excited carriers. The non-uniform strain configuration locally changes the valence and conduction bands of WS2, giving rise to effective forces attracting excitons and trions towards the point of maximum strain underneath the AFM tip. We observe large changes in the photoluminescence spectra of WS2 under strain, which we interpret using a drift–diffusion model. We show that the transport of neutral excitons, a process that was previously thought to be efficient in non-uniformly strained two-dimensional semiconductors and termed as funnelling, is negligible at room temperature, in contrast to previous observations. Conversely, we discover that redistribution of free carriers under non-uniform strain profiles leads to highly efficient conversion of excitons to trions. Conversion efficiency reaches up to about 100% even without electrical gating. Our results explain inconsistencies in previous experiments and pave the way towards new types of optoelectronic devices.
This is a preview of subscription content, access via your institution
Access options
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 print issues and online access
$209.00 per year
only $17.42 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
Data availability
The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.
Change history
27 March 2020
In the HTML version of this Article, Fig. 5 appeared with the caption for Fig. 4 and vice versa; this has now been amended. The PDF version is correct.
References
Mak, K. F., Lee, C., Hone, J., Shan, J. & Heinz, T. F. Atomically thin MoS2: a new direct-gap semiconductor. Phys. Rev. Lett. 105, 136805 (2010).
Zhao, W. et al. Evolution of electronic structure in atomically thin sheets of WS2 and WSe2. ACS Nano 7, 791–797 (2013).
Xu, X., Yao, W., Xiao, D. & Heinz, T. F. Spin and pseudospins in layered transition metal dichalcogenides. Nat. Phys. 10, 343–350 (2014).
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).
Mak, K. F., McGill, K. L., Park, J. & McEuen, P. L. Valleytronics. The valley Hall effect in MoS transistors. Science 344, 1489–1492 (2014).
Tonndorf, P. et al. Single-photon emission from localized excitons in an atomically thin semiconductor. Optica 2, 347–352 (2015).
Chakraborty, C., Kinnischtzke, L., Goodfellow, K. M., Beams, R. & Vamivakas, A. N. Voltage-controlled quantum light from an atomically thin semiconductor. Nat. Nanotechnol. 10, 507–511 (2015).
Koperski, M. et al. Single photon emitters in exfoliated WSe2 structures. Nat. Nanotechnol. 10, 503–506 (2015).
Srivastava, A. et al. Optically active quantum dots in monolayer WSe2. Nat. Nanotechnol. 10, 491–496 (2015).
He, Y.-M. et al. Single quantum emitters in monolayer semiconductors. Nat. Nanotechnol. 10, 497–502 (2015).
Roy, T. et al. Field-effect transistors built from all two-dimensional material components. ACS Nano 8, 6259–6264 (2014).
Lee, C.-H. et al. Atomically thin p–n junctions with van der Waals heterointerfaces. Nat. Nanotechnol. 9, 676–681 (2014).
Jariwala, D., Davoyan, A. R., Wong, J. & Atwater, H. A. Van der Waals materials for atomically-thin photovoltaics: promise and outlook. ACS Photon. 4, 2962–2970 (2017).
Akama, T. et al. Schottky solar cell using few-layered transition metal dichalcogenides toward large-scale fabrication of semitransparent and flexible power generator. Sci. Rep. 7, 11967 (2017).
Liu, K. et al. Elastic properties of chemical-vapor-deposited monolayer MoS2, WS2, and their bilayer heterostructures. Nano Lett. 14, 5097–5103 (2014).
Lee, C. et al. Measurement of the elastic properties and intrinsic strength of monolayer graphene. Science 321, 385–388 (2008).
Roldán, R., Castellanos-Gomez, A., Cappelluti, E. & Guinea, F. Strain engineering in semiconducting two-dimensional crystals. J. Phys. Condens. Matter 27, 313201 (2015).
Feng, J., Qian, X., Huang, C.-W. & Li, J. Strain-engineered artificial atom as a broad-spectrum solar energy funnel. Nat. Photon. 6, 866–872 (2012).
Conley, H. J. et al. Bandgap engineering of strained monolayer and bilayer MoS2. Nano Lett. 13, 3626–3630 (2013).
Niehues, I. et al. Strain control of exciton–phonon coupling in atomically thin semiconductors. Nano Lett. 18, 1751–1757 (2018).
Christiansen, D. et al. Phonon sidebands in monolayer transition metal dichalcogenides. Phys. Rev. Lett. 119, 187402 (2017).
Lloyd, D. et al. Band gap engineering with ultralarge biaxial strains in suspended monolayer MoS2. Nano Lett. 16, 5836–5841 (2016).
Lazić, S. et al. Scalable interconnections for remote indirect exciton systems based on acoustic transport. Phys. Rev. B 89, 085313 (2014).
Manasevit, H. M., Gergis, I. S. & Jones, A. B. Electron mobility enhancement in epitaxial multilayer Si-Si1−xGex alloy films on (100) Si. Appl. Phys. Lett. 41, 464–466 (1982).
People, R. et al. Modulation doping in GexSi1−x/Si strained layer heterostructures. Appl. Phys. Lett. 45, 1231–1233 (1984).
Castellanos-Gomez, A. et al. Local strain engineering in atomically thin MoS2. Nano Lett. 13, 5361–5366 (2013).
Tyurnina, A. V. et al. Strained bubbles in van der Waals heterostructures as local emitters of photoluminescence with adjustable wavelength. ACS Photon. 6, 516–524 (2019).
Castellanos-Gomez, A. et al. Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping. 2D Mater. 1, 011002 (2014).
Dukic, M., Adams, J. D. & Fantner, G. E. Piezoresistive AFM cantilevers surpassing standard optical beam deflection in low noise topography imaging. Sci. Rep. 5, 16393 (2015).
Castellanos-Gomez, A. et al. Elastic properties of freely suspended MoS2 nanosheets. Adv. Mater. 24, 772–775 (2012).
Zhang, R., Koutsos, V. & Cheung, R. Elastic properties of suspended multilayer WSe2. Appl. Phys. Lett. 108, 042104 (2016).
Vella, D. & Davidovitch, B. Indentation metrology of clamped, ultra-thin elastic sheets. Soft Matter 13, 2264–2278 (2017).
Bertolazzi, S., Brivio, J. & Kis, A. Stretching and breaking of ultrathin MoS2. ACS Nano 5, 9703–9709 (2011).
Kulig, M. et al. Exciton diffusion and halo effects in monolayer semiconductors. Phys. Rev. Lett. 120, 207401 (2018).
Ovchinnikov, D., Allain, A., Huang, Y.-S., Dumcenco, D. & Kis, A. Electrical transport properties of single-layer WS2. ACS Nano 8, 8174–8181 (2014).
Siviniant, J., Scalbert, D., Kavokin, A. V., Coquillat, D. & Lascaray, J.-P. Chemical equilibrium between excitons, electrons, and negatively charged excitons in semiconductor quantum wells. Phys. Rev. B 59, 1602–1604 (1999).
Ross, J. S. et al. Electrical control of neutral and charged excitons in a monolayer semiconductor. Nat. Commun. 4, 1474 (2013).
Wang, Y. et al. Strain-induced direct-indirect bandgap transition and phonon modulation in monolayer WS2. Nano Res. 8, 2562–2572 (2015).
Plechinger, G. et al. Identification of excitons, trions and biexcitons in single-layer WS2. Phys. Status Solid. Rap. Res. Lett. 9, 457–461 (2015).
Acknowledgements
We thank R. Netz for fruitful discussions. We also thank K. Höflich for technical support. This work was supported by the European Research Council Starting grant 639739, and DFG CRC/TRR 227.
Author information
Authors and Affiliations
Contributions
M.G.H. and K.I.B. planned and designed the experiment and wrote the paper. M.G.H. and J.N.K. performed the nanoindentation experiments. M.G.H., J.N.K. and M.Q. fabricated the samples. The experiments, data analysis and the theoretical model were done by M.G.H. K.G. contributed to the theoretical model.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Supplementary Information
Supplementary Figs. 1–12 and discussion.
Rights and permissions
About this article
Cite this article
Harats, M.G., Kirchhof, J.N., Qiao, M. et al. Dynamics and efficient conversion of excitons to trions in non-uniformly strained monolayer WS2. Nat. Photonics 14, 324–329 (2020). https://doi.org/10.1038/s41566-019-0581-5
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/s41566-019-0581-5
This article is cited by
-
Twistronics and moiré excitonic physics in van der Waals heterostructures
Frontiers of Physics (2024)
-
Recent progress of exciton transport in two-dimensional semiconductors
Nano Convergence (2023)
-
Tunable interlayer excitons and switchable interlayer trions via dynamic near-field cavity
Light: Science & Applications (2023)
-
Tip-induced excitonic luminescence nanoscopy of an atomically resolved van der Waals heterostructure
Nature Materials (2023)
-
All-optical control of high-purity trions in nanoscale waveguide
Nature Communications (2023)