Anomalous isotope effect on the optical bandgap in a monolayer transition metal dichalcogenide semiconductor

Yu, Yiling; Turkowski, Volodymyr; Hachtel, Jordan A.; Puretzky, Alexander A.; Ievlev, Anton V.; Din, Naseem U.; Harris, Sumner B.; Iyer, Vasudevan; Rouleau, Christopher M.; Rahman, Talat S.; Geohegan, David B.; Xiao, Kai

doi:10.1126/sciadv.adj0758

Anomalous isotope effect on the optical bandgap in a monolayer transition metal dichalcogenide semiconductor

Journal Article · Tue Feb 20 23:00:00 EST 2024 · Science Advances

DOI:https://doi.org/10.1126/sciadv.adj0758· OSTI ID:2317786

^[1]; ^[2]; ^[3]; ^[3]; ^[3]; ^[2]; ^[3]; ^[3]; ^[3]; ^[2]; ^[3]; ^[3]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Wuhan Univ. (China)
Univ. of Central Florida, Orlando, FL (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Isotope effects have received increasing attention in materials science and engineering because altering isotopes directly affects phonons, which can affect both thermal properties and optoelectronic properties of conventional semiconductors. However, how isotopic mass affects the optoelectronic properties in 2D semiconductors remains unclear because of measurement uncertainties resulting from sample heterogeneities. Here, we report an anomalous optical bandgap energy red shift of 13 (±7) milli–electron volts as mass of Mo isotopes is increased in laterally structured ¹⁰⁰MoS₂-⁹²MoS₂ monolayers grown by a two-step chemical vapor deposition that mitigates the effects of heterogeneities. This trend, which is opposite to that observed in conventional semiconductors, is explained by many-body perturbation and time-dependent density functional theories that reveal unusually large exciton binding energy renormalizations exceeding the ground-state renormalization energy due to strong coupling between confined excitons and phonons. The isotope effect on the optical bandgap reported here provides perspective on the important role of exciton-phonon coupling in the physical properties of two-dimensional materials.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: AC05-00OR22725; FG02-07ER46354

OSTI ID:: 2317786

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 8 Vol. 10; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

References (50)

Engineering Substrate Interactions for High Luminescence Efficiency of Transition-Metal Dichalcogenide Monolayers Yu, Yifei; Yu, Yiling; Xu, Chao Advanced Functional Materials, Vol. 26, Issue 26 https://doi.org/10.1002/adfm.201600418	journal	May 2016
Heterogeneities at multiple length scales in 2D layered materials: From localized defects and dopants to mesoscopic heterostructures Cai, Hui; Yu, Yiling; Lin, Yu-Chuan Nano Research, Vol. 14, Issue 6 https://doi.org/10.1007/s12274-020-3047-7	journal	September 2020
Effect of the isotopic mass of gallium on the indirect gap of GaP Meyer, T. A.; Karaiskaj, D.; Thewalt, M. L. W. Solid State Communications, Vol. 126, Issue 3 https://doi.org/10.1016/S0038-1098(03)00030-9	journal	April 2003
Isotope dependence of band-gap energy Plekhanov, V. G.; Plekhanov, N. V. Physics Letters A, Vol. 313, Issue 3 https://doi.org/10.1016/S0375-9601(03)00760-6	journal	June 2003
Isotope Effect in Bilayer WSe ₂ Wu, Wei; Morales-Acosta, Mayra Daniela; Wang, Yongqiang Nano Letters, Vol. 19, Issue 3 https://doi.org/10.1021/acs.nanolett.8b04269	journal	February 2019
An unusual isotope effect in a high-transition-temperature superconductor Gweon, G. -H.; Sasagawa, T.; Zhou, S. Y. Nature, Vol. 430, Issue 6996 https://doi.org/10.1038/nature02731	journal	July 2004
Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides Selig, Malte; Berghäuser, Gunnar; Raja, Archana Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13279	journal	November 2016
The isotopic effects of deuteration on optoelectronic properties of conducting polymers Shao, Ming; Keum, Jong; Chen, Jihua Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4180	journal	January 2014
Ultralong spin coherence time in isotopically engineered diamond Balasubramanian, Gopalakrishnan; Neumann, Philipp; Twitchen, Daniel Nature Materials, Vol. 8, Issue 5 https://doi.org/10.1038/nmat2420	journal	April 2009
Thermal conductivity of isotopically modified graphene Chen, Shanshan; Wu, Qingzhi; Mishra, Columbia Nature Materials, Vol. 11, Issue 3 https://doi.org/10.1038/nmat3207	journal	January 2012
Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei Nature Materials, Vol. 13, Issue 12 https://doi.org/10.1038/nmat4061	journal	August 2014
Isotope engineering of van der Waals interactions in hexagonal boron nitride Vuong, T. Q. P.; Liu, S.; Van der Lee, A. Nature Materials, Vol. 17, Issue 2 https://doi.org/10.1038/nmat5048	journal	December 2017
Strain-engineered growth of two-dimensional materials Ahn, Geun Ho; Amani, Matin; Rasool, Haider Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/s41467-017-00516-5	journal	September 2017
Tuning the Fröhlich exciton-phonon scattering in monolayer MoS2 Miller, Bastian; Lindlau, Jessica; Bommert, Max Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-08764-3	journal	February 2019
Spin coherence in two-dimensional materials Ye, Meng; Seo, Hosung; Galli, Giulia npj Computational Materials, Vol. 5, Issue 1 https://doi.org/10.1038/s41524-019-0182-3	journal	April 2019
Modulating the thermal conductivity in hexagonal boron nitride via controlled boron isotope concentration Yuan, Chao; Li, Jiahan; Lindsay, Lucas Communications Physics, Vol. 2, Issue 1 https://doi.org/10.1038/s42005-019-0145-5	journal	May 2019
Hyperfine interaction in atomically thin transition metal dichalcogenides Avdeev, Ivan D.; Smirnov, Dmitry S. Nanoscale Advances, Vol. 1, Issue 7 https://doi.org/10.1039/C8NA00360B	journal	January 2019
Polaronic and magnetic field effects on the binding energy of an exciton in a quantum well wire Bouhassoune, M.; Charrour, R.; Fliyou, M. Journal of Applied Physics, Vol. 91, Issue 1 https://doi.org/10.1063/1.1419261	journal	January 2002
Unusual isotope effect on thermal transport of single layer molybdenum disulphide Wu, Xufei; Yang, Nuo; Luo, Tengfei Applied Physics Letters, Vol. 107, Issue 19 https://doi.org/10.1063/1.4935603	journal	November 2015
Manipulation of exciton and trion quasiparticles in monolayer WS ₂ via charge transfer Gaur, Anand P. S.; Rivera, Adriana M.; Dash, Saroj P. Applied Physics Letters, Vol. 115, Issue 17 https://doi.org/10.1063/1.5113775	journal	October 2019
Isotopically Controlled Semiconductors Haller, Eugene E. Journal of Nuclear Science and Technology, Vol. 39, Issue 4 https://doi.org/10.1080/18811248.2002.9715208	journal	April 2002
Polaron properties of the Wannier exciton in a quantum well confinement Ercelebi, A.; Ozdincer, U. Journal of Physics: Condensed Matter, Vol. 1, Issue 11 https://doi.org/10.1088/0953-8984/1/11/007	journal	March 1989
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502 https://doi.org/10.1088/0953-8984/21/39/395502	journal	September 2009
Effect of isotopic disorder and mass on the electronic and vibronic properties of three-, two- and one-dimensional solids Cardona, M.; Etchegoin, P.; Fuchs, H. D. Journal of Physics: Condensed Matter, Vol. 5, Issue 33A https://doi.org/10.1088/0953-8984/5/33A/006	journal	August 1993
Bethe-Salpeter equation approach with electron-phonon coupling for exciton binding energies Adamska, Lyudmyla; Umari, Paolo Physical Review B, Vol. 103, Issue 7 https://doi.org/10.1103/PhysRevB.103.075201	journal	February 2021
Perturbative approach to the polaron shift of excitons in transition metal dichalcogenides Henriques, J. C. G.; Peres, N. M. R. Physical Review B, Vol. 103, Issue 16 https://doi.org/10.1103/PhysRevB.103.L161402	journal	April 2021
Theory of exciton-phonon coupling Antonius, Gabriel; Louie, Steven G. Physical Review B, Vol. 105, Issue 8 https://doi.org/10.1103/PhysRevB.105.085111	journal	February 2022
Polaron effects on excitons in GaAs-Ga1−xAlxAs quantum wells Degani, Marcos H.; Hipólito, Oscar Physical Review B, Vol. 35, Issue 9 https://doi.org/10.1103/PhysRevB.35.4507	journal	March 1987
Electronic band structure of isotopically pure germanium: Modulated transmission and reflectivity study Parks, C.; Ramdas, A. K.; Rodriguez, S. Physical Review B, Vol. 49, Issue 20 https://doi.org/10.1103/PhysRevB.49.14244	journal	May 1994
Dependence of the lattice parameters and the energy gap of zinc-blende-type semiconductors on isotopic masses Garro, N.; Cantarero, A.; Cardona, M. Physical Review B, Vol. 54, Issue 7 https://doi.org/10.1103/PhysRevB.54.4732	journal	August 1996
Lattice isotope effects on optical transitions in silicon Hayama, S.; Davies, G.; Tan, J. Physical Review B, Vol. 70, Issue 3 https://doi.org/10.1103/PhysRevB.70.035202	journal	July 2004
Time-dependent density-functional approach for exciton binding energies Turkowski, V.; Leonardo, A.; Ullrich, C. A. Physical Review B, Vol. 79, Issue 23 https://doi.org/10.1103/PhysRevB.79.233201	journal	June 2009
Exciton band structure of monolayer MoS 2 Wu, Fengcheng; Qu, Fanyao; MacDonald, A. H. Physical Review B, Vol. 91, Issue 7 https://doi.org/10.1103/PhysRevB.91.075310	journal	February 2015
Temperature-dependent excitonic effects in the optical properties of single-layer MoS 2 Molina-Sánchez, Alejandro; Palummo, Maurizia; Marini, Andrea Physical Review B, Vol. 93, Issue 15 https://doi.org/10.1103/PhysRevB.93.155435	journal	April 2016
Observation of exciton-phonon coupling in MoSe 2 monolayers Shree, S.; Semina, M.; Robert, C. Physical Review B, Vol. 98, Issue 3 https://doi.org/10.1103/PhysRevB.98.035302	journal	July 2018
Electron-Phonon Renormalization of the Direct Band Gap of Diamond Giustino, Feliciano; Louie, Steven G.; Cohen, Marvin L. Physical Review Letters, Vol. 105, Issue 26 https://doi.org/10.1103/PhysRevLett.105.265501	journal	December 2010
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
Phonon Sidebands in Monolayer Transition Metal Dichalcogenides Christiansen, Dominik; Selig, Malte; Berghäuser, Gunnar Physical Review Letters, Vol. 119, Issue 18 https://doi.org/10.1103/PhysRevLett.119.187402	journal	November 2017
Isotopic Disorder: The Prevailing Mechanism in Limiting the Phonon Lifetime in Hexagonal BN Cuscó, Ramon; Edgar, James H.; Liu, Song Physical Review Letters, Vol. 124, Issue 16 https://doi.org/10.1103/PhysRevLett.124.167402	journal	April 2020
Giant Isotope Effect of Thermal Conductivity in Silicon Nanowires Ci, Penghong; Sun, Muhua; Upadhyaya, Meenakshi Physical Review Letters, Vol. 128, Issue 8 https://doi.org/10.1103/PhysRevLett.128.085901	journal	February 2022
Indirect energy gap ofC13diamond Collins, A. T.; Lawson, S. C.; Davies, Gordon Physical Review Letters, Vol. 65, Issue 7 https://doi.org/10.1103/PhysRevLett.65.891	journal	August 1990
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Anomalous Isotopic Effect Near the Charge-Ordering Quantum Criticality Andergassen, S.; Caprara, S.; Di Castro, C. Physical Review Letters, Vol. 87, Issue 5 https://doi.org/10.1103/PhysRevLett.87.056401	journal	July 2001
Isotope effects on the optical spectra of semiconductors Cardona, Manuel; Thewalt, M. L. W. Reviews of Modern Physics, Vol. 77, Issue 4 https://doi.org/10.1103/RevModPhys.77.1173	journal	November 2005
Dislocation-driven growth of two-dimensional lateral quantum-well superlattices Zhou, Wu; Zhang, Yu-Yang; Chen, Jianyi Science Advances, Vol. 4, Issue 3 https://doi.org/10.1126/sciadv.aap9096	journal	March 2018
Isotopic Homojunction Band Engineering from Diamond Watanabe, H.; Nebel, C. E.; Shikata, S. Science, Vol. 324, Issue 5933 https://doi.org/10.1126/science.1172419	journal	June 2009
Quantum Information Storage for over 180 s Using Donor Spins in a 28Si "Semiconductor Vacuum" Steger, M.; Saeedi, K.; Thewalt, M. L. W. Science, Vol. 336, Issue 6086 https://doi.org/10.1126/science.1217635	journal	June 2012
Quantum and isotope effects in lithium metal Ackland, Graeme J.; Dunuwille, Mihindra; Martinez-Canales, Miguel Science, Vol. 356, Issue 6344 https://doi.org/10.1126/science.aal4886	journal	June 2017
Ultrahigh thermal conductivity in isotope-enriched cubic boron nitride Chen, Ke; Song, Bai; Ravichandran, Navaneetha K. Science, Vol. 367, Issue 6477 https://doi.org/10.1126/science.aaz6149	journal	January 2020
Isotope engineering of silicon and diamond for quantum computing and sensing applications Itoh, Kohei M.; Watanabe, Hideyuki MRS Communications, Vol. 4, Issue 4 https://doi.org/10.1557/mrc.2014.32	journal	November 2014

Similar Records

Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields

Journal Article · Fri Sep 13 00:00:00 EDT 2019 · Nature Communications · OSTI ID:1565907

Exchange-driven intravalley mixing of excitons in monolayer transition metal dichalcogenides

Journal Article · Sun Dec 09 23:00:00 EST 2018 · Nature Physics · OSTI ID:1581333

Related Subjects

36 MATERIALS SCIENCE

Anomalous isotope effect on the optical bandgap in a monolayer transition metal dichalcogenide semiconductor

Citation Formats

References (50)

Similar Records

Related Subjects