Nano-spectroscopy of excitons in atomically thin transition metal dichalcogenides

Zhang, Shuai; Li, Baichang; Chen, Xinzhong; Ruta, Francesco L.; Shao, Yinming; Sternbach, Aaron J.; McLeod, A. S.; Sun, Zhiyuan; Xiong, Lin; Moore, S. L.; Xu, Xinyi; Wu, Wenjing; Shabani, Sara; Zhou, Lin; Wang, Zhiying; Mooshammer, Fabian; Ray, Essance; Wilson, Nathan; Schuck, P. J.; Dean, C. R.; Pasupathy, A. N.; Lipson, Michal; Xu, Xiaodong; Zhu, Xiaoyang; Millis, A. J.; Liu, Mengkun; Hone, James C.; Basov, D. N.

doi:10.1038/s41467-022-28117-x

Title: Nano-spectroscopy of excitons in atomically thin transition metal dichalcogenides

Journal Article · 26 January 2022 · Nature Communications

DOI: https://doi.org/10.1038/s41467-022-28117-x · OSTI ID:1842352

;

; Ruta, Francesco L.; Shao, Yinming;

;

; Xiong, Lin;

; Xu, Xinyi; Wu, Wenjing;

;

; Wang, Zhiying;

; Ray, Essance; Wilson, Nathan;

;

Abstract Excitons play a dominant role in the optoelectronic properties of atomically thin van der Waals (vdW) semiconductors. These excitons are amenable to on-demand engineering with diverse control knobs, including dielectric screening, interlayer hybridization, and moiré potentials. However, external stimuli frequently yield heterogeneous excitonic responses at the nano- and meso-scales, making their spatial characterization with conventional diffraction-limited optics a formidable task. Here, we use a scattering-type scanning near-field optical microscope (s-SNOM) to acquire exciton spectra in atomically thin transition metal dichalcogenide microcrystals with previously unattainable 20 nm resolution. Our nano-optical data revealed material- and stacking-dependent exciton spectra of MoSe ₂ , WSe ₂ , and their heterostructures. Furthermore, we extracted the complex dielectric function of these prototypical vdW semiconductors. s-SNOM hyperspectral images uncovered how the dielectric screening modifies excitons at length scales as short as few nanometers. This work paves the way towards understanding and manipulation of excitons in atomically thin layers at the nanoscale.

View Journal Article

Cite

Export

Save

Research Organization:: Columbia Univ., New York, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019443

OSTI ID:: 1842352

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

References (57)

Modern Scattering‐Type Scanning Near‐Field Optical Microscopy for Advanced Material Research Chen, Xinzhong; Hu, Debo; Mescall, Ryan Advanced Materials https://doi.org/10.1002/adma.201804774	journal	April 2019
Enhanced dielectric contrast in scattering-type scanning near-field optical microscopy Knoll, Bernhard; Keilmann, Fritz Optics Communications, Vol. 182, Issue 4-6 https://doi.org/10.1016/S0030-4018(00)00826-9	journal	August 2000
Near-Unity Light Absorption in a Monolayer WS ₂ Van der Waals Heterostructure Cavity Epstein, Itai; Terrés, Bernat; Chaves, André J. Nano Letters, Vol. 20, Issue 5 https://doi.org/10.1021/acs.nanolett.0c00492	journal	April 2020
Nanocavity Clock Spectroscopy: Resolving Competing Exciton Dynamics in WSe ₂ /MoSe ₂ Heterobilayers May, Molly A.; Jiang, Tao; Du, Chenfeng Nano Letters, Vol. 21, Issue 1 https://doi.org/10.1021/acs.nanolett.0c03979	journal	December 2020
Hybrid Tip-Enhanced Nanospectroscopy and Nanoimaging of Monolayer WSe ₂ with Local Strain Control Park, Kyoung-Duck; Khatib, Omar; Kravtsov, Vasily Nano Letters, Vol. 16, Issue 4 https://doi.org/10.1021/acs.nanolett.6b00238	journal	March 2016
Approaching the Intrinsic Limit in Transition Metal Diselenides via Point Defect Control Edelberg, Drew; Rhodes, Daniel; Kerelsky, Alexander Nano Letters, Vol. 19, Issue 7 https://doi.org/10.1021/acs.nanolett.9b00985	journal	June 2019
Probing Evolution of Twist-Angle-Dependent Interlayer Excitons in MoSe ₂ /WSe ₂ van der Waals Heterostructures Nayak, Pramoda K.; Horbatenko, Yevhen; Ahn, Seongjoon ACS Nano, Vol. 11, Issue 4 https://doi.org/10.1021/acsnano.7b00640	journal	April 2017
Nanoscale Spectroscopy of Dielectric Properties of Mica Fali, Alireza; Gamage, Sampath; Howard, Marquez ACS Photonics, Vol. 8, Issue 1 https://doi.org/10.1021/acsphotonics.0c00951	journal	December 2020
Quantitative Measurement of Local Infrared Absorption and Dielectric Function with Tip-Enhanced Near-Field Microscopy Govyadinov, Alexander A.; Amenabar, Iban; Huth, Florian The Journal of Physical Chemistry Letters, Vol. 4, Issue 9 https://doi.org/10.1021/jz400453r	journal	April 2013
Infrared Nanoscopy of Dirac Plasmons at the Graphene–SiO ₂ Interface Fei, Zhe; Andreev, Gregory O.; Bao, Wenzhong Nano Letters, Vol. 11, Issue 11 https://doi.org/10.1021/nl202362d	journal	October 2011
Exciton Radiative Lifetimes in Two-Dimensional Transition Metal Dichalcogenides Palummo, Maurizia; Bernardi, Marco; Grossman, Jeffrey C. Nano Letters, Vol. 15, Issue 5 https://doi.org/10.1021/nl503799t	journal	March 2015
Gate-tuning of graphene plasmons revealed by infrared nano-imaging Fei, Z.; Rodin, A. S.; Andreev, G. O. Nature, Vol. 487, Issue 7405 https://doi.org/10.1038/nature11253	journal	June 2012
Optical nano-imaging of gate-tunable graphene plasmons Chen, Jianing; Badioli, Michela; Alonso-González, Pablo Nature, Vol. 487, Issue 7405 https://doi.org/10.1038/nature11254	journal	June 2012
Large-scale quantum-emitter arrays in atomically thin semiconductors Palacios-Berraquero, Carmen; Kara, Dhiren M.; Montblanch, Alejandro R. -P. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15093	journal	May 2017
Coulomb engineering of the bandgap and excitons in two-dimensional materials Raja, Archana; Chaves, Andrey; Yu, Jaeeun Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15251	journal	May 2017
High-temperature superfluidity with indirect excitons in van der Waals heterostructures Fogler, M. M.; Butov, L. V.; Novoselov, K. S. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5555	journal	July 2014
Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides Moody, Galan; Kavir Dass, Chandriker; Hao, Kai Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9315	journal	September 2015
Resonant internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2 Poellmann, C.; Steinleitner, P.; Leierseder, U. Nature Materials, Vol. 14, Issue 9 https://doi.org/10.1038/nmat4356	journal	July 2015
Magnetic brightening and control of dark excitons in monolayer WSe2 Zhang, Xiao-Xiao; Cao, Ting; Lu, Zhengguang Nature Nanotechnology, Vol. 12, Issue 9 https://doi.org/10.1038/nnano.2017.105	journal	June 2017
Radiative control of dark excitons at room temperature by nano-optical antenna-tip Purcell effect Park, Kyoung-Duck; Jiang, Tao; Clark, Genevieve Nature Nanotechnology, Vol. 13, Issue 1 https://doi.org/10.1038/s41565-017-0003-0	journal	November 2017
Interacting polariton fluids in a monolayer of tungsten disulfide Barachati, Fábio; Fieramosca, Antonio; Hafezian, Soroush Nature Nanotechnology, Vol. 13, Issue 10 https://doi.org/10.1038/s41565-018-0219-7	journal	August 2018
Imaging strain-localized excitons in nanoscale bubbles of monolayer WSe2 at room temperature Darlington, Thomas P.; Carmesin, Christian; Florian, Matthias Nature Nanotechnology, Vol. 15, Issue 10 https://doi.org/10.1038/s41565-020-0730-5	journal	July 2020
Identification of spin, valley and moiré quasi-angular momentum of interlayer excitons Jin, Chenhao; Regan, Emma C.; Wang, Danqing Nature Physics, Vol. 15, Issue 11 https://doi.org/10.1038/s41567-019-0631-4	journal	August 2019
Photonics with hexagonal boron nitride Caldwell, Joshua D.; Aharonovich, Igor; Cassabois, Guillaume Nature Reviews Materials, Vol. 4, Issue 8 https://doi.org/10.1038/s41578-019-0124-1	journal	July 2019
Signatures of moiré-trapped valley excitons in MoSe2/WSe2 heterobilayers Seyler, Kyle L.; Rivera, Pasqual; Yu, Hongyi Nature, Vol. 567, Issue 7746 https://doi.org/10.1038/s41586-019-0957-1	journal	February 2019
Evidence for moiré excitons in van der Waals heterostructures Tran, Kha; Moody, Galan; Wu, Fengcheng Nature, Vol. 567, Issue 7746 https://doi.org/10.1038/s41586-019-0975-z	journal	February 2019
Observation of moiré excitons in WSe2/WS2 heterostructure superlattices Jin, Chenhao; Regan, Emma C.; Yan, Aiming Nature, Vol. 567, Issue 7746 https://doi.org/10.1038/s41586-019-0976-y	journal	February 2019
Resonantly hybridized excitons in moiré superlattices in van der Waals heterostructures Alexeev, Evgeny M.; Ruiz-Tijerina, David A.; Danovich, Mark Nature, Vol. 567, Issue 7746 https://doi.org/10.1038/s41586-019-0986-9	journal	March 2019
Simulation of Hubbard model physics in WSe2/WS2 moiré superlattices Tang, Yanhao; Li, Lizhong; Li, Tingxin Nature, Vol. 579, Issue 7799 https://doi.org/10.1038/s41586-020-2085-3	journal	March 2020
Mott and generalized Wigner crystal states in WSe2/WS2 moiré superlattices Regan, Emma C.; Wang, Danqing; Jin, Chenhao Nature, Vol. 579, Issue 7799 https://doi.org/10.1038/s41586-020-2092-4	journal	March 2020
Strongly correlated electrons and hybrid excitons in a moiré heterostructure Shimazaki, Yuya; Schwartz, Ido; Watanabe, Kenji Nature, Vol. 580, Issue 7804 https://doi.org/10.1038/s41586-020-2191-2	journal	April 2020
Excitonic resonances in thin films of WSe ₂ : from monolayer to bulk material Arora, Ashish; Koperski, Maciej; Nogajewski, Karol Nanoscale, Vol. 7, Issue 23 https://doi.org/10.1039/C5NR01536G	journal	January 2015
Pseudoheterodyne detection for background-free near-field spectroscopy Ocelic, Nenad; Huber, Andreas; Hillenbrand, Rainer Applied Physics Letters, Vol. 89, Issue 10 https://doi.org/10.1063/1.2348781	journal	September 2006
Nanometer-scale dielectric constant of Ge quantum dots using apertureless near-field scanning optical microscopy Ogawa, Y.; Minami, F.; Abate, Yohannes Applied Physics Letters, Vol. 96, Issue 6 https://doi.org/10.1063/1.3309692	journal	February 2010
Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity Bao, Wei; Liu, Xiaoze; Xue, Fei Proceedings of the National Academy of Sciences, Vol. 116, Issue 41 https://doi.org/10.1073/pnas.1909948116	journal	September 2019
Highly confined in-plane propagating exciton-polaritons on monolayer semiconductors Epstein, Itai; Chaves, André J.; Rhodes, Daniel A. 2D Materials, Vol. 7, Issue 3 https://doi.org/10.1088/2053-1583/ab8dd4	journal	June 2020
Near-field spectroscopy of silicon dioxide thin films Zhang, L. M.; Andreev, G. O.; Fei, Z. Physical Review B, Vol. 85, Issue 7 https://doi.org/10.1103/PhysRevB.85.075419	journal	February 2012
Exciton fine structure and spin decoherence in monolayers of transition metal dichalcogenides Glazov, M. M.; Amand, T.; Marie, X. Physical Review B, Vol. 89, Issue 20 https://doi.org/10.1103/PhysRevB.89.201302	journal	May 2014
Measurement of the optical dielectric function of monolayer transition-metal dichalcogenides: MoS 2 , Mo S e 2 , WS 2 , and WS e 2 Li, Yilei; Chernikov, Alexey; Zhang, Xian Physical Review B, Vol. 90, Issue 20 https://doi.org/10.1103/PhysRevB.90.205422	journal	November 2014
Exciton radiative lifetime in transition metal dichalcogenide monolayers Robert, C.; Lagarde, D.; Cadiz, F. Physical Review B, Vol. 93, Issue 20 https://doi.org/10.1103/PhysRevB.93.205423	journal	May 2016
Quantum plasmonic hot-electron injection in lateral WS e 2 / MoS e 2 heterostructures Tang, Chenwei; He, Zhe; Chen, Weibing Physical Review B, Vol. 98, Issue 4 https://doi.org/10.1103/PhysRevB.98.041402	journal	July 2018
Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS 2 Chernikov, Alexey; Berkelbach, Timothy C.; Hill, Heather M. Physical Review Letters, Vol. 113, Issue 7 https://doi.org/10.1103/PhysRevLett.113.076802	journal	August 2014
Experimental Evidence for Dark Excitons in Monolayer WSe 2 Zhang, Xiao-Xiao; You, Yumeng; Zhao, Shu Yang Frank Physical Review Letters, Vol. 115, Issue 25 https://doi.org/10.1103/PhysRevLett.115.257403	journal	December 2015
In-Plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules Wang, G.; Robert, C.; Glazov, M. M. Physical Review Letters, Vol. 119, Issue 4 https://doi.org/10.1103/PhysRevLett.119.047401	journal	July 2017
Large Excitonic Reflectivity of Monolayer MoSe 2 Encapsulated in Hexagonal Boron Nitride Scuri, Giovanni; Zhou, You; High, Alexander A. Physical Review Letters, Vol. 120, Issue 3 https://doi.org/10.1103/PhysRevLett.120.037402	journal	January 2018
Engineering of optical and electronic band gaps in transition metal dichalcogenide monolayers through external dielectric screening Borghardt, Sven; Tu, Jhih-Sian; Winkler, Florian Physical Review Materials, Vol. 1, Issue 5 https://doi.org/10.1103/PhysRevMaterials.1.054001	journal	October 2017
Colloquium : Excitons in atomically thin transition metal dichalcogenides Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M. Reviews of Modern Physics, Vol. 90, Issue 2 https://doi.org/10.1103/RevModPhys.90.021001	journal	April 2018
Nano-optical imaging of monolayer MoSe ₂ -WSe ₂ lateral heterostructure with subwavelength domains Xue, Wenjin; Sahoo, Prasana K.; Liu, Jiru Journal of Vacuum Science & Technology A, Vol. 36, Issue 5 https://doi.org/10.1116/1.5035437	journal	September 2018
Moiré excitons: From programmable quantum emitter arrays to spin-orbit–coupled artificial lattices Yu, Hongyi; Liu, Gui-Bin; Tang, Jianju Science Advances, Vol. 3, Issue 11 https://doi.org/10.1126/sciadv.1701696	journal	November 2017
Transient exciton-polariton dynamics in WSe ₂ by ultrafast near-field imaging Mrejen, M.; Yadgarov, L.; Levanon, A. Science Advances, Vol. 5, Issue 2 https://doi.org/10.1126/sciadv.aat9618	journal	February 2019
Quantum plasmonic control of trions in a picocavity with monolayer WS ₂ He, Zhe; Han, Zehua; Yuan, Jiangtan Science Advances, Vol. 5, Issue 10 https://doi.org/10.1126/sciadv.aau8763	journal	October 2019
Tip-enhanced strong coupling spectroscopy, imaging, and control of a single quantum emitter Park, Kyoung-Duck; May, Molly A.; Leng, Haixu Science Advances, Vol. 5, Issue 7 https://doi.org/10.1126/sciadv.aav5931	journal	July 2019
Exciton Liquid in Coupled Quantum Wells Stern, Michael; Umansky, Vladimir; Bar-Joseph, Israel Science, Vol. 343, Issue 6166 https://doi.org/10.1126/science.1243409	journal	January 2014
Tunable Phonon Polaritons in Atomically Thin van der Waals Crystals of Boron Nitride Dai, S.; Fei, Z.; Ma, Q. Science, Vol. 343, Issue 6175 https://doi.org/10.1126/science.1246833	journal	March 2014
Programmable hyperbolic polaritons in van der Waals semiconductors Sternbach, A. J.; Chae, S. H.; Latini, S. Science, Vol. 371, Issue 6529 https://doi.org/10.1126/science.abe9163	journal	February 2021
Tip-enhanced photoluminescence nano-spectroscopy and nano-imaging Lee, Hyeongwoo; Lee, Dong Yun; Kang, Min Gu Nanophotonics, Vol. 9, Issue 10 https://doi.org/10.1515/nanoph-2020-0079	journal	May 2020
Polariton panorama Basov, D. N.; Asenjo-Garcia, Ana; Schuck, P. James Nanophotonics, Vol. 10, Issue 1 https://doi.org/10.1515/nanoph-2020-0449	journal	November 2020

Similar Records

Dynamic Tuning of Moiré Excitons in a WSe₂/WS₂ Heterostructure via Mechanical Deformation

Journal Article · 2021 · Nano Letters · OSTI ID:1963832

Zhao, Wenyu; Regan, Emma C.; Wang, Danqing; +12 more

Femtosecond exciton dynamics in WSe₂ optical waveguides

Journal Article · 2020 · Nature Communications · OSTI ID:1647310

Sternbach, Aaron J.; Latini, Simone; Chae, Sanghoon; +20 more

Twist Angle-Dependent Interlayer Exciton Lifetimes in van der Waals Heterostructures

Journal Article · 2021 · Physical Review Letters · OSTI ID:1764224

Choi, Junho; Florian, Matthias; Steinhoff, Alexander; +15 more

Related Subjects

71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
electronic properties and materials
nanophotonics and plasmonics
near-infrared spectroscopy
sub-wavelength optics

Title: Nano-spectroscopy of excitons in atomically thin transition metal dichalcogenides

Citation Formats

References (57)

Similar Records

Related Subjects