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Temperature dependent excitonic transition energies and linewidths of monolayer MoS2 probed by magnetic circular dichroism spectroscopy

Wu Yuan-Jun Shen Chao Tan Qing-Hai Zhang Jun Tan Ping-Heng Zheng Hou-Zhi

Temperature dependent excitonic transition energies and linewidths of monolayer MoS2 probed by magnetic circular dichroism spectroscopy

Wu Yuan-Jun, Shen Chao, Tan Qing-Hai, Zhang Jun, Tan Ping-Heng, Zheng Hou-Zhi
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  • Layered transition metal dichalcogenides (TMDs), as a new class of two-dimensional material, have received wide attention of scientific community due to their peculiar electronic and optical properties. Monolayer TMDs such as MoS2, MoSe2, WS2 and WSe2 are semiconductors with band gap energies in the visible and near-infrared region, which promises the applications in logic nano-devices, ultra-high speed photoelectric detectors and nano-lasers. Temperature has strong influences on the electronic and optical properties of semiconductors, and their applications in photonic and optoelectronic devices. Thus, the research on the temperature dependence of the energy band of monolayer TMDs is important and meaningful. Monolayer MoS2, as a prototype of TMDs, displays a weak absorption line with a strong background in original reflection or absorption spectra. The strong background has a tremendous influence on the determination of excitonic transition energy and linewidth. In this work, we adopt the reflection magnetic circular dichroism (MCD) spectroscopy in which reflection spectra and MCD spectra can be simultaneously obtained. We demonstrate that the background disturbance is eliminated in the MCD spectra, in contrast to the reflectivity spectra. And we discuss the optimization of our home-built experimental setup in detail. Through the elaborate analysis of the MCD theory, we demonstrate that the excitonic transition energy and linewidth can be directly and accurately extracted from the MCD spectrum. We perform the reflection MCD measurements on monolayer MoS2 in a temperature range of 65–300 K. The transition energies and linewidths of A and B excitons of monolayer MoS2 are extracted, respectively. Those functional parameters that describe the temperature dependence of the energy and linewidth of both excitonic transitions are evaluated and analyzed. We find that the broadening of the linewidth is related to the LO phonon scattering, and the linewidth of A exciton is clearly narrower than that of B exciton. The linewidth difference between A and B excitons might result from the stronger inter-valley coupling of B exciton. Our results indicate that MCD spectroscopy, as a modulated spectroscopy by magnetic fields, provides an easy tool to determine the features of monolayer excitons.
      Corresponding author: Shen Chao, shenchao@semi.ac.cn;hzzheng@semi.ac.cn ; Zheng Hou-Zhi, shenchao@semi.ac.cn;hzzheng@semi.ac.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 11404324, 11574305, 51527901).
    [1]

    Novoselov K S, Geim A K, Morozov S V, Jiang D, Zhang Y, Dubonos S V, Grigorieva I V, Firsov A A 2004 Science 306 666

    [2]

    Mak K F, Lee C, Hone J, Shan J, Heinz T F 2010 Phys. Rev. Lett. 105 136805

    [3]

    Eda G, Maier S A 2013 ACS Nano 7 5660

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    Radisavljevic B, Radenovic A, Brivio J, Giacometti V, Kis A 2011 Nat. Nanotechnol. 6 147

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    Britnell L, Gorbachev R V, Jalil R, Belle B D, Schedin F, Mishchenko A, Georgiou T, Katsnelson M I, Eaves L, Morozov S V, Peres N M R, Leist J, Geim A K, Novoselov K S, Ponomarenko L A 2012 Science 335 947

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    Lee C H, Lee G H, van der Zande A M, Chen W, Li Y, Han M, Cui X, Arefe G, Nuckolls C, Heinz T F, Guo J, Hone J, Kim P 2014 Nat. Nanotechnol. 9 676

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    Liu Y, Cheng R, Liao L, Zhou H L, Bai J W, Liu G, Liu L X, Huang Y, Duan X F 2011 Nat. Commun. 2 579

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    Konstantatos G, Badioli M, Gaudreau L, Osmond J, Bernechea M, de Arquer F P G, Gatti F, Koppens F H L 2012 Nat. Nanotechnol. 7 363

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    Liao L, Lin Y C, Bao M, Cheng R, Bai J, Liu Y, Qu Y, Wang K L, Huang Y, Duan X 2010 Nature 467 305

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    Massicotte M, Schmidt P, Vialla F, Schadler K G, Reserbat-Plantey A, Watanabe K, Taniguchi T, Tielrooij K J, Koppens F H 2016 Nat. Nanotechnol. 11 42

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    Wu S, Buckley S, Schaibley J R, Feng L, Yan J, Mandrus D G, Hatami F, Yao W, Vuckovic J, Majumdar A, Xu X 2015 Nature 520 69

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    Wang Q H, Kalantar-Zadeh K, Kis A, Coleman J N, Strano M S 2012 Nat. Nanotechnol. 7 699

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    Lv R, Robinson J A, Schaak R E, Sun D, Sun Y F, Mallouk T E, Terrones M 2015 Acc. Chem. Res. 48 56

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    Bhimanapati G R, Lin Z, Meunier V, Jung Y, Cha J, Das S, Xiao D, Son Y, Strano M S, Cooper V R, Liang L B, Louie S G, Ringe E, Zhou W, Kim S S, Naik R R, Sumpter B G, Terrones H, Xia F N, Wang Y L, Zhu J, Akinwande D, Alem N, Schuller J A, Schaak R E, Terrones M, Robinson J A 2015 ACS Nano 9 11509

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    Kumar A, Ahluwalia P K 2012 Eur. Phys. J. B 85 186

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    Liu G B, Shan W Y, Yao Y, Yao W, Xiao D 2013 Phys. Rev. B 88 085433

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    Chernikov A, Berkelbach T C, Hill H M, Rigosi A, Li Y L, Aslan O B, Reichman D R, Hybertsen M S, Heinz T F 2014 Phys. Rev. Lett. 113 076802

    [18]

    Xiao J, Zhao M, Wang Y, Zhang X 2017 Nanophotonics 6 1309

    [19]

    Aivazian G, Gong Z R, Jones A M, Chu R L, Yan J, Mandrus D G, Zhang C W, Cobden D, Yao W, Xu X 2015 Nat. Phys. 11 148

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    Stier A V, McCreary K M, Jonker B T, Kono J, Crooker S A 2016 Nat. Commun. 7 10643

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    Kioseoglou G, Hanbicki A T, Currie M, Friedman A L, Gunlycke D, Jonker B T 2012 Appl. Phys. Lett. 101 221907

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    Barrows C J, Vlaskin V A, Gamelin D R 2015 J. Phys. Chem. Lett. 6 3076

    [23]

    Muckel F, Yang J, Lorenz S, Baek W, Chang H, Hyeon T, Bacher G, Fainblat R 2016 ACS Nano 10 7135

    [24]

    Wu Y J, Shen C, Tan Q H, Shi J, Liu X F, Wu Z H, Zhang J, Tan P H, Zheng H Z 2018 Appl. Phys. Lett. 112 153105

    [25]

    Li Y, Chernikov A, Zhang X, Rigosi A, Hill H M, van der Zande A M, Chenet D A, Shih E M, Hone J, Heinz T F 2014 Phys. Rev. B 90 205422

    [26]

    Mitioglu A A, Galkowski K, Surrente A, Klopotowski L, Dumcenco D, Kis A, Maude D K, Plochocka P 2016 Phys. Rev. B 93 165412

    [27]

    Lundt N, Klembt S, Cherotchenko E, Betzold S, Iff O, Nalitov A V, Klaas M, Dietrich C P, Kavokin A V, Hofling S, Schneider C 2016 Nat. Commun. 7 13328

    [28]

    Steele D, Whitehead J C, Meares P, Doggett G, Grice R, Hollas J M 1984 J. Chem. Soc. Faraday Trans. 2 80 1503

    [29]

    Liu X L, Wu J B, Luo X D, Tan P H 2017 Acta Phys. Sin. 66 147801 (in Chinese) [(刘雪璐, 吴江滨, 罗向东, 谭平恒 2017 物理学报 66 147801]

    [30]

    Zhang X, Qiao X F, Shi W, Wu J B, Jiang D S, Tan P H 2015 Chem. Soc. Rev. 44 2757

    [31]

    Korn T, Heydrich S, Hirmer M, Schmutzler J, Schuller C 2011 Appl. Phys. Lett. 99 102109

    [32]

    Zhan Y J, Liu Z, Najmaei S, Ajayan P M, Lou J 2012 Small 8 966

    [33]

    Varshni Y P 1967 Physica 34 149

    [34]

    Lautenschlager P, Garriga M, Logothetidis S, Cardona M 1987 Phys. Rev. B 35 9174

    [35]

    Yen P C, Hsu H P, Liu Y T, Huang Y S, Tiong K K 2004 J. Phys. Condens. Matter 16 6995

    [36]

    Tiong K K, Shou T S, Ho C H 2000 J. Phys. Condens. Matter 12 3441

    [37]

    Vina L, Logothetidis S, Cardona M 1984 Phys. Rev. B 30 1979

    [38]

    Bernal-Villamil I, Berghauser G, Selig M, Niehues I, Schmidt R, Schneider R, Tonndorf P, Erhart P, de Vasconcellos S M, Bratschitsch R, Knorr A, Malic E 2018 2D Materials 5 025011

  • [1]

    Novoselov K S, Geim A K, Morozov S V, Jiang D, Zhang Y, Dubonos S V, Grigorieva I V, Firsov A A 2004 Science 306 666

    [2]

    Mak K F, Lee C, Hone J, Shan J, Heinz T F 2010 Phys. Rev. Lett. 105 136805

    [3]

    Eda G, Maier S A 2013 ACS Nano 7 5660

    [4]

    Radisavljevic B, Radenovic A, Brivio J, Giacometti V, Kis A 2011 Nat. Nanotechnol. 6 147

    [5]

    Britnell L, Gorbachev R V, Jalil R, Belle B D, Schedin F, Mishchenko A, Georgiou T, Katsnelson M I, Eaves L, Morozov S V, Peres N M R, Leist J, Geim A K, Novoselov K S, Ponomarenko L A 2012 Science 335 947

    [6]

    Lee C H, Lee G H, van der Zande A M, Chen W, Li Y, Han M, Cui X, Arefe G, Nuckolls C, Heinz T F, Guo J, Hone J, Kim P 2014 Nat. Nanotechnol. 9 676

    [7]

    Liu Y, Cheng R, Liao L, Zhou H L, Bai J W, Liu G, Liu L X, Huang Y, Duan X F 2011 Nat. Commun. 2 579

    [8]

    Konstantatos G, Badioli M, Gaudreau L, Osmond J, Bernechea M, de Arquer F P G, Gatti F, Koppens F H L 2012 Nat. Nanotechnol. 7 363

    [9]

    Liao L, Lin Y C, Bao M, Cheng R, Bai J, Liu Y, Qu Y, Wang K L, Huang Y, Duan X 2010 Nature 467 305

    [10]

    Massicotte M, Schmidt P, Vialla F, Schadler K G, Reserbat-Plantey A, Watanabe K, Taniguchi T, Tielrooij K J, Koppens F H 2016 Nat. Nanotechnol. 11 42

    [11]

    Wu S, Buckley S, Schaibley J R, Feng L, Yan J, Mandrus D G, Hatami F, Yao W, Vuckovic J, Majumdar A, Xu X 2015 Nature 520 69

    [12]

    Wang Q H, Kalantar-Zadeh K, Kis A, Coleman J N, Strano M S 2012 Nat. Nanotechnol. 7 699

    [13]

    Lv R, Robinson J A, Schaak R E, Sun D, Sun Y F, Mallouk T E, Terrones M 2015 Acc. Chem. Res. 48 56

    [14]

    Bhimanapati G R, Lin Z, Meunier V, Jung Y, Cha J, Das S, Xiao D, Son Y, Strano M S, Cooper V R, Liang L B, Louie S G, Ringe E, Zhou W, Kim S S, Naik R R, Sumpter B G, Terrones H, Xia F N, Wang Y L, Zhu J, Akinwande D, Alem N, Schuller J A, Schaak R E, Terrones M, Robinson J A 2015 ACS Nano 9 11509

    [15]

    Kumar A, Ahluwalia P K 2012 Eur. Phys. J. B 85 186

    [16]

    Liu G B, Shan W Y, Yao Y, Yao W, Xiao D 2013 Phys. Rev. B 88 085433

    [17]

    Chernikov A, Berkelbach T C, Hill H M, Rigosi A, Li Y L, Aslan O B, Reichman D R, Hybertsen M S, Heinz T F 2014 Phys. Rev. Lett. 113 076802

    [18]

    Xiao J, Zhao M, Wang Y, Zhang X 2017 Nanophotonics 6 1309

    [19]

    Aivazian G, Gong Z R, Jones A M, Chu R L, Yan J, Mandrus D G, Zhang C W, Cobden D, Yao W, Xu X 2015 Nat. Phys. 11 148

    [20]

    Stier A V, McCreary K M, Jonker B T, Kono J, Crooker S A 2016 Nat. Commun. 7 10643

    [21]

    Kioseoglou G, Hanbicki A T, Currie M, Friedman A L, Gunlycke D, Jonker B T 2012 Appl. Phys. Lett. 101 221907

    [22]

    Barrows C J, Vlaskin V A, Gamelin D R 2015 J. Phys. Chem. Lett. 6 3076

    [23]

    Muckel F, Yang J, Lorenz S, Baek W, Chang H, Hyeon T, Bacher G, Fainblat R 2016 ACS Nano 10 7135

    [24]

    Wu Y J, Shen C, Tan Q H, Shi J, Liu X F, Wu Z H, Zhang J, Tan P H, Zheng H Z 2018 Appl. Phys. Lett. 112 153105

    [25]

    Li Y, Chernikov A, Zhang X, Rigosi A, Hill H M, van der Zande A M, Chenet D A, Shih E M, Hone J, Heinz T F 2014 Phys. Rev. B 90 205422

    [26]

    Mitioglu A A, Galkowski K, Surrente A, Klopotowski L, Dumcenco D, Kis A, Maude D K, Plochocka P 2016 Phys. Rev. B 93 165412

    [27]

    Lundt N, Klembt S, Cherotchenko E, Betzold S, Iff O, Nalitov A V, Klaas M, Dietrich C P, Kavokin A V, Hofling S, Schneider C 2016 Nat. Commun. 7 13328

    [28]

    Steele D, Whitehead J C, Meares P, Doggett G, Grice R, Hollas J M 1984 J. Chem. Soc. Faraday Trans. 2 80 1503

    [29]

    Liu X L, Wu J B, Luo X D, Tan P H 2017 Acta Phys. Sin. 66 147801 (in Chinese) [(刘雪璐, 吴江滨, 罗向东, 谭平恒 2017 物理学报 66 147801]

    [30]

    Zhang X, Qiao X F, Shi W, Wu J B, Jiang D S, Tan P H 2015 Chem. Soc. Rev. 44 2757

    [31]

    Korn T, Heydrich S, Hirmer M, Schmutzler J, Schuller C 2011 Appl. Phys. Lett. 99 102109

    [32]

    Zhan Y J, Liu Z, Najmaei S, Ajayan P M, Lou J 2012 Small 8 966

    [33]

    Varshni Y P 1967 Physica 34 149

    [34]

    Lautenschlager P, Garriga M, Logothetidis S, Cardona M 1987 Phys. Rev. B 35 9174

    [35]

    Yen P C, Hsu H P, Liu Y T, Huang Y S, Tiong K K 2004 J. Phys. Condens. Matter 16 6995

    [36]

    Tiong K K, Shou T S, Ho C H 2000 J. Phys. Condens. Matter 12 3441

    [37]

    Vina L, Logothetidis S, Cardona M 1984 Phys. Rev. B 30 1979

    [38]

    Bernal-Villamil I, Berghauser G, Selig M, Niehues I, Schmidt R, Schneider R, Tonndorf P, Erhart P, de Vasconcellos S M, Bratschitsch R, Knorr A, Malic E 2018 2D Materials 5 025011

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  • Received Date:  08 April 2018
  • Accepted Date:  24 April 2018
  • Published Online:  20 July 2018

Temperature dependent excitonic transition energies and linewidths of monolayer MoS2 probed by magnetic circular dichroism spectroscopy

    Corresponding author: Shen Chao, shenchao@semi.ac.cn;hzzheng@semi.ac.cn
    Corresponding author: Zheng Hou-Zhi, shenchao@semi.ac.cn;hzzheng@semi.ac.cn
  • 1. State Key Laboratory of Superlattices and Microstructures, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083, China;
  • 2. College of Materials Science and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 101408, China
Fund Project:  Project supported by the National Natural Science Foundation of China (Grant Nos. 11404324, 11574305, 51527901).

Abstract: Layered transition metal dichalcogenides (TMDs), as a new class of two-dimensional material, have received wide attention of scientific community due to their peculiar electronic and optical properties. Monolayer TMDs such as MoS2, MoSe2, WS2 and WSe2 are semiconductors with band gap energies in the visible and near-infrared region, which promises the applications in logic nano-devices, ultra-high speed photoelectric detectors and nano-lasers. Temperature has strong influences on the electronic and optical properties of semiconductors, and their applications in photonic and optoelectronic devices. Thus, the research on the temperature dependence of the energy band of monolayer TMDs is important and meaningful. Monolayer MoS2, as a prototype of TMDs, displays a weak absorption line with a strong background in original reflection or absorption spectra. The strong background has a tremendous influence on the determination of excitonic transition energy and linewidth. In this work, we adopt the reflection magnetic circular dichroism (MCD) spectroscopy in which reflection spectra and MCD spectra can be simultaneously obtained. We demonstrate that the background disturbance is eliminated in the MCD spectra, in contrast to the reflectivity spectra. And we discuss the optimization of our home-built experimental setup in detail. Through the elaborate analysis of the MCD theory, we demonstrate that the excitonic transition energy and linewidth can be directly and accurately extracted from the MCD spectrum. We perform the reflection MCD measurements on monolayer MoS2 in a temperature range of 65–300 K. The transition energies and linewidths of A and B excitons of monolayer MoS2 are extracted, respectively. Those functional parameters that describe the temperature dependence of the energy and linewidth of both excitonic transitions are evaluated and analyzed. We find that the broadening of the linewidth is related to the LO phonon scattering, and the linewidth of A exciton is clearly narrower than that of B exciton. The linewidth difference between A and B excitons might result from the stronger inter-valley coupling of B exciton. Our results indicate that MCD spectroscopy, as a modulated spectroscopy by magnetic fields, provides an easy tool to determine the features of monolayer excitons.

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