Abstract

Two-dimensional van der Waals heterostructures (vdWHs) are drawing growing interest in the investigation of their valley polarization properties of localized excitons. However, most of the reported vdWHs were made by micro-mechanical peeling, limiting their large-scale production and practical applications. Furthermore, the circular polarization characters of localized excitons in WSe2/WS2 heterostructures remain elusive. Here, a bidirectional-flow physical vapor deposition technique was employed for the synthesis of the WSe2/WS2 type-II vertical heterostructures. The interfaces of such heterojunctions are sharp and clean, making the neutral excitons of the constituent layers quenched, which significantly highlights the luminescence of the local excitons. The circular polarization of localized excitons in this WSe2/WS2 heterostructure was demonstrated by circularly-polarized PL spectroscopy. The degree of the circular polarization of the localized excitons was determined as 7.17% for σ- detection and 4.78% for σ+ detection. Such local excitons play a critical role in a quantum emitter with enhanced spontaneous emission rate that could lead to the evolution of LEDs. Our observations provide valuable information for the exploration of intriguing excitonic physics and the applications of innovative local exciton devices.

© 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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2020 (5)

Y. Liu, C. Zeng, J. Zhong, J. Ding, Z. M. Wang, and Z. Liu, “Spintronics in Two-Dimensional Materials,” Nano-Micro Lett. 12(1), 93 (2020).
[Crossref]

J. Yu, X. Kuang, Y. Gao, Y. Wang, K. Chen, Z. Ding, J. Liu, C. Cong, J. He, Z. Liu, and Y. Liu, “Direct Observation of the Linear Dichroism Transition in Two-Dimensional Palladium Diselenide,” Nano Lett. 20(2), 1172–1182 (2020).
[Crossref]

J. Yu, J. Zhong, X. Kuang, C. Zeng, L. Cao, Y. Liu, and Z. Liu, “Dynamic Control of High-Range Photoresponsivity in a Graphene Nanoribbon Photodetector,” Nanoscale Res. Lett. 15(1), 124 (2020).
[Crossref]

J. Zhong, J. Yu, L. Cao, C. Zeng, J. Ding, C. Cong, Z. Liu, and Y. Liu, “High-performance polarization-sensitive photodetector based on a few-layered PdSe2 nanosheet,” Nano Res. 13(6), 1780–1786 (2020).
[Crossref]

J. Yu, X. Kuang, J. Zhong, L. Cao, C. Zeng, J. Ding, C. Cong, S. Wang, P. Dai, X. Yue, Z. Liu, and Y. Liu, “Observation of double indirect interlayer exciton in WSe2/WS2 heterostructure,” Opt. Express 28(9), 13260–13268 (2020).
[Crossref]

2019 (4)

Y. Liu, S. Zhang, J. He, Z. M. Wang, and Z. Liu, “Recent Progress in the Fabrication, Properties, and Devices of Heterostructures Based on 2D Materials,” Nano-Micro Lett. 11(1), 13 (2019).
[Crossref]

Y. Liu, Y. Huang, and X. F. Duan, “Van der Waals integration before and beyond two-dimensional materials,” Nature 567(7748), 323–333 (2019).
[Crossref]

Y. Liu, Y. Gao, S. Zhang, J. He, J. Yu, and Z. Liu, “Valleytronics in transition metal dichalcogenides materials,” Nano Res. 12(11), 2695–2711 (2019).
[Crossref]

L. Linhart, M. Paur, V. Smejkal, J. Burgdörfer, T. Mueller, and F. Libisch, “Localized Intervalley Defect Excitons as Single-Photon Emitters in WSe 2,” Phys. Rev. Lett. 123(14), 146401 (2019).
[Crossref]

2018 (10)

S. Refaely-Abramson, D. Y. Qiu, S. G. Louie, and J. B. Neaton, “Defect-Induced Modification of Low-Lying Excitons and Valley Selectivity in Monolayer Transition Metal Dichalcogenides,” Phys. Rev. Lett. 121(16), 167402 (2018).
[Crossref]

W.-T. Hsu, L.-S. Lu, P.-H. Wu, M.-H. Lee, P.-J. Chen, P.-Y. Wu, Y.-C. Chou, H.-T. Jeng, L.-J. Li, M.-W. Chu, and W.-H. Chang, “Negative circular polarization emissions from WSe(2)/MoSe(2) commensurate heterobilayers,” Nat. Commun. 9(1), 1356 (2018).
[Crossref]

G. Moody, K. Tran, X. Lu, T. Autry, J. M. Fraser, R. P. Mirin, L. Yang, X. Li, and K. L. Silverman, “Microsecond Valley Lifetime of Defect-Bound Excitons in Monolayer WSe2,” Phys. Rev. Lett. 121(5), 057403 (2018).
[Crossref]

X. Zhao, T. Huang, S. P. Ping, X. Wu, P. Huang, J. Pan, Y. Wu, and Z. Cheng, “Sensitivity Enhancement in Surface Plasmon Resonance Biochemical Sensor Based on Transition Metal Dichalcogenides/Graphene Heterostructure,” Sensors 18, 2056 (2018).
[Crossref]

Q. Zeng and Z. Liu, “Novel optoelectronic devices: transition-metal-dichalcogenide-based 2D heterostructures,” Adv. Electron. Mater. 4(2), 1700335 (2018).
[Crossref]

L. Zhang, A. Sharma, Y. Zhu, Y. Zhang, B. Wang, M. Dong, H. T. Nguyen, Z. Wang, B. Wen, and Y. Cao, “Efficient and Layer-Dependent Exciton Pumping across Atomically Thin Organic–Inorganic Type-I Heterostructures,” Adv. Mater. 30(40), 1803986 (2018).
[Crossref]

W. Yang, H. Kawai, M. Bosman, B. Tang, J. Chai, W. Le Tay, J. Yang, H. L. Seng, H. Zhu, and H. Gong, “Interlayer interactions in 2D WS 2/MoS 2 heterostructures monolithically grown by in situ physical vapor deposition,” Nanoscale 10(48), 22927–22936 (2018).
[Crossref]

T. Mueller and E. Malic, “Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors,” npj 2D Mater. Appl. 2(1), 29 (2018).
[Crossref]

H. Taghinejad, D. A. Rehn, C. Muccianti, A. A. Eftekhar, M. Tian, T. Fan, X. Zhang, Y. Meng, Y. Chen, and T.-V. Nguyen, “Defect-mediated alloying of monolayer transition-metal dichalcogenides,” ACS Nano 12(12), 12795–12804 (2018).
[Crossref]

Z. Cai, B. Liu, X. Zou, and H.-M. Cheng, “Chemical vapor deposition growth and applications of two-dimensional materials and their heterostructures,” Chem. Rev. 118(13), 6091–6133 (2018).
[Crossref]

2017 (8)

Z. Zhang, P. Chen, X. Duan, K. Zang, J. Luo, and X. Duan, “Robust epitaxial growth of two-dimensional heterostructures, multiheterostructures, and superlattices,” Sci. Bull. 357(6353), 788–792 (2017).
[Crossref]

V. D. Karanikolas and E. Paspalakis, “Localized exciton modes and high quantum efficiency of a quantum emitter close to a MoS 2 nanodisk,” Phys. Rev. B 96(4), 041404 (2017).
[Crossref]

S. Bettis Homan, V. K. Sangwan, I. Balla, H. Bergeron, E. A. Weiss, and M. C. Hersam, “Ultrafast exciton dissociation and long-lived charge separation in a photovoltaic pentacene–MoS2 van der Waals heterojunction,” Nano Lett. 17(1), 164–169 (2017).
[Crossref]

W. Yu, S. Li, Y. Zhang, W. Ma, T. Sun, J. Yuan, K. Fu, and Q. Bao, “Near-Infrared Photodetectors Based on MoTe2/Graphene Heterostructure with High Responsivity and Flexibility,” Small 13(24), 1700268 (2017).
[Crossref]

Y. Li, Y.-L. Li, B. Sa, and R. Ahuja, “Review of two-dimensional materials for photocatalytic water splitting from a theoretical perspective,” Catal. Sci. Technol. 7(3), 545–559 (2017).
[Crossref]

P. Liu and B. Xiang, “2D heterostructures based on transition metal dichalcogenides: fabrication, properties and applications,” Sci. Bull. 62(16), 1148–1161 (2017).
[Crossref]

J. S. Ross, P. Rivera, J. Schaibley, E. Lee-Wong, H. Yu, T. Taniguchi, K. Watanabe, J. Yan, D. Mandrus, and D. Cobden, “Interlayer exciton optoelectronics in a 2D heterostructure p–n junction,” Nano Lett. 17(2), 638–643 (2017).
[Crossref]

S. Gao, L. Yang, and C. D. Spataru, “Interlayer coupling and gate-tunable excitons in transition metal dichalcogenide heterostructures,” Nano Lett. 17(12), 7809–7813 (2017).
[Crossref]

2016 (4)

A. Boulesbaa, K. Wang, M. Mahjouri-Samani, M. Tian, A. A. Puretzky, I. Ivanov, C. M. Rouleau, K. Xiao, B. G. Sumpter, B. G. Sumpter, and D. B. Geohegan, “Ultrafast charge transfer and hybrid exciton formation in 2D/0D heterostructures,” J. Am. Chem. Soc. 138(44), 14713–14719 (2016).
[Crossref]

Y. Ren, Z. Qiao, and Q. Niu, “Topological phases in two-dimensional materials: a review,” Rep. Prog. Phys. 79(6), 066501 (2016).
[Crossref]

W. Shi, M.-L. Lin, Q.-H. Tan, X.-F. Qiao, J. Zhang, and P.-H. Tan, “Raman and photoluminescence spectra of two-dimensional nanocrystallites of monolayer WS2 and WSe2,” 2D Mater. 3(2), 025016 (2016).
[Crossref]

Z. He, X. Wang, W. Xu, Y. Zhou, Y. Sheng, Y. Rong, J. M. Smith, and J. H. Warner, “Revealing Defect-State Photoluminescence in Monolayer WS2 by Cryogenic Laser Processing,” ACS Nano 10(6), 5847–5855 (2016).
[Crossref]

2015 (7)

G. Plechinger, P. Nagler, J. Kraus, N. Paradiso, C. Strunk, C. Schüller, and T. Korn, “Identification of excitons, trions and biexcitons in single-layer WS2,” Phys. Status Solidi RRL 9(8), 457–461 (2015).
[Crossref]

H. Yu, Y. Wang, Q. Tong, X. Xu, and W. Yao, “Anomalous light cones and valley optical selection rules of interlayer excitons in twisted heterobilayers,” Phys. Rev. Lett. 115(18), 187002 (2015).
[Crossref]

A. Srivastava, M. Sidler, A. V. Allain, D. S. Lembke, A. Kis, and A. Imamoğlu, “Optically active quantum dots in monolayer WSe2,” Nat. Nanotechnol. 10(6), 491–496 (2015).
[Crossref]

P. Rivera, J. R. Schaibley, A. M. Jones, J. S. Ross, S. Wu, G. Aivazian, P. Klement, K. Seyler, G. Clark, and N. J. Ghimire, “Observation of long-lived interlayer excitons in monolayer MoSe 2–WSe 2 heterostructures,” Nat. Commun. 6(1), 6242 (2015).
[Crossref]

A. Hanbicki, M. Currie, G. Kioseoglou, A. Friedman, and B. Jonker, “Measurement of high exciton binding energy in the monolayer transition-metal dichalcogenides WS2 and WSe2,” Solid State Commun. 203, 16–20 (2015).
[Crossref]

Y. Gong, S. Lei, G. Ye, B. Li, Y. He, K. Keyshar, X. Zhang, Q. Wang, J. Lou, and Z. Liu, “Two-step growth of two-dimensional WSe2/MoSe2 heterostructures,” Nano Lett. 15(9), 6135–6141 (2015).
[Crossref]

S. Das, J. A. Robinson, M. Dubey, H. Terrones, and M. Terrones, “Beyond graphene: progress in novel two-dimensional materials and van der Waals solids,” Annu. Rev. Mater. Res. 45(1), 1–27 (2015).
[Crossref]

2014 (2)

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(12), 12717–12724 (2014).
[Crossref]

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 MoS 2/WS 2 heterostructures,” Nat. Nanotechnol. 9(9), 682–686 (2014).
[Crossref]

2013 (2)

H. Shi, R. Yan, S. Bertolazzi, J. Brivio, B. Gao, A. Kis, D. Jena, H. G. Xing, and L. Huang, “Exciton dynamics in suspended monolayer and few-layer MoS2 2D crystals,” ACS Nano 7(2), 1072–1080 (2013).
[Crossref]

A. K. Geim and I. V. Grigorieva, “Van der Waals heterostructures,” Nature 499(7459), 419–425 (2013).
[Crossref]

2012 (1)

D. Xiao, G.-B. Liu, W. Feng, X. Xu, and W. Yao, “Coupled spin and valley physics in monolayers of MoS 2 and other group-VI dichalcogenides,” Phys. Rev. Lett. 108(19), 196802 (2012).
[Crossref]

2011 (1)

B. Radisavljevic, A. Radenovic, J. Brivio, V. Giacometti, and A. Kis, “Single-layer MoS2 transistors,” Nat. Nanotechnol. 6(3), 147–150 (2011).
[Crossref]

2005 (1)

S. H. Simon, “Spontaneous interlayer exciton coherence in quantum Hall bilayers at v = 1 and v = 2: a tutorial,” Solid State Commun. 134(1-2), 81–88 (2005).
[Crossref]

1996 (1)

S. Chichibu, T. Azuhata, T. Sota, and S. Nakamura, “Spontaneous emission of localized excitons in InGaN single and multiquantum well structures,” Appl. Phys. Lett. 69(27), 4188–4190 (1996).
[Crossref]

1967 (1)

Y. P. Varshni, “Temperature dependence of the energy gap in semiconductors,” Physica 34(1), 149–154 (1967).
[Crossref]

Ahuja, R.

Y. Li, Y.-L. Li, B. Sa, and R. Ahuja, “Review of two-dimensional materials for photocatalytic water splitting from a theoretical perspective,” Catal. Sci. Technol. 7(3), 545–559 (2017).
[Crossref]

Aivazian, G.

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Y. Gong, S. Lei, G. Ye, B. Li, Y. He, K. Keyshar, X. Zhang, Q. Wang, J. Lou, and Z. Liu, “Two-step growth of two-dimensional WSe2/MoSe2 heterostructures,” Nano Lett. 15(9), 6135–6141 (2015).
[Crossref]

Yu, H.

J. S. Ross, P. Rivera, J. Schaibley, E. Lee-Wong, H. Yu, T. Taniguchi, K. Watanabe, J. Yan, D. Mandrus, and D. Cobden, “Interlayer exciton optoelectronics in a 2D heterostructure p–n junction,” Nano Lett. 17(2), 638–643 (2017).
[Crossref]

H. Yu, Y. Wang, Q. Tong, X. Xu, and W. Yao, “Anomalous light cones and valley optical selection rules of interlayer excitons in twisted heterobilayers,” Phys. Rev. Lett. 115(18), 187002 (2015).
[Crossref]

Yu, J.

J. Yu, X. Kuang, J. Zhong, L. Cao, C. Zeng, J. Ding, C. Cong, S. Wang, P. Dai, X. Yue, Z. Liu, and Y. Liu, “Observation of double indirect interlayer exciton in WSe2/WS2 heterostructure,” Opt. Express 28(9), 13260–13268 (2020).
[Crossref]

J. Yu, J. Zhong, X. Kuang, C. Zeng, L. Cao, Y. Liu, and Z. Liu, “Dynamic Control of High-Range Photoresponsivity in a Graphene Nanoribbon Photodetector,” Nanoscale Res. Lett. 15(1), 124 (2020).
[Crossref]

J. Zhong, J. Yu, L. Cao, C. Zeng, J. Ding, C. Cong, Z. Liu, and Y. Liu, “High-performance polarization-sensitive photodetector based on a few-layered PdSe2 nanosheet,” Nano Res. 13(6), 1780–1786 (2020).
[Crossref]

J. Yu, X. Kuang, Y. Gao, Y. Wang, K. Chen, Z. Ding, J. Liu, C. Cong, J. He, Z. Liu, and Y. Liu, “Direct Observation of the Linear Dichroism Transition in Two-Dimensional Palladium Diselenide,” Nano Lett. 20(2), 1172–1182 (2020).
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Y. Liu, Y. Gao, S. Zhang, J. He, J. Yu, and Z. Liu, “Valleytronics in transition metal dichalcogenides materials,” Nano Res. 12(11), 2695–2711 (2019).
[Crossref]

Yu, W.

W. Yu, S. Li, Y. Zhang, W. Ma, T. Sun, J. Yuan, K. Fu, and Q. Bao, “Near-Infrared Photodetectors Based on MoTe2/Graphene Heterostructure with High Responsivity and Flexibility,” Small 13(24), 1700268 (2017).
[Crossref]

Yuan, J.

W. Yu, S. Li, Y. Zhang, W. Ma, T. Sun, J. Yuan, K. Fu, and Q. Bao, “Near-Infrared Photodetectors Based on MoTe2/Graphene Heterostructure with High Responsivity and Flexibility,” Small 13(24), 1700268 (2017).
[Crossref]

Yue, X.

Zang, K.

Z. Zhang, P. Chen, X. Duan, K. Zang, J. Luo, and X. Duan, “Robust epitaxial growth of two-dimensional heterostructures, multiheterostructures, and superlattices,” Sci. Bull. 357(6353), 788–792 (2017).
[Crossref]

Zeng, C.

J. Yu, X. Kuang, J. Zhong, L. Cao, C. Zeng, J. Ding, C. Cong, S. Wang, P. Dai, X. Yue, Z. Liu, and Y. Liu, “Observation of double indirect interlayer exciton in WSe2/WS2 heterostructure,” Opt. Express 28(9), 13260–13268 (2020).
[Crossref]

J. Yu, J. Zhong, X. Kuang, C. Zeng, L. Cao, Y. Liu, and Z. Liu, “Dynamic Control of High-Range Photoresponsivity in a Graphene Nanoribbon Photodetector,” Nanoscale Res. Lett. 15(1), 124 (2020).
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J. Zhong, J. Yu, L. Cao, C. Zeng, J. Ding, C. Cong, Z. Liu, and Y. Liu, “High-performance polarization-sensitive photodetector based on a few-layered PdSe2 nanosheet,” Nano Res. 13(6), 1780–1786 (2020).
[Crossref]

Y. Liu, C. Zeng, J. Zhong, J. Ding, Z. M. Wang, and Z. Liu, “Spintronics in Two-Dimensional Materials,” Nano-Micro Lett. 12(1), 93 (2020).
[Crossref]

Zeng, Q.

Q. Zeng and Z. Liu, “Novel optoelectronic devices: transition-metal-dichalcogenide-based 2D heterostructures,” Adv. Electron. Mater. 4(2), 1700335 (2018).
[Crossref]

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D. Zhang, Z. Zeng, Q. Tong, Y. Jiang, S. Chen, B. Zheng, J. Qu, F. Li, W. Zheng, and F. Jiang, “Near-Unity Polarization of Valley-Dependent Second-Harmonic Generation in Stacked TMDC Layers and Heterostructures at Room Temperature,” Adv. Mater.1908061 (2020).
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[Crossref]

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Zhao, X.

X. Zhao, T. Huang, S. P. Ping, X. Wu, P. Huang, J. Pan, Y. Wu, and Z. Cheng, “Sensitivity Enhancement in Surface Plasmon Resonance Biochemical Sensor Based on Transition Metal Dichalcogenides/Graphene Heterostructure,” Sensors 18, 2056 (2018).
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D. Zhang, Z. Zeng, Q. Tong, Y. Jiang, S. Chen, B. Zheng, J. Qu, F. Li, W. Zheng, and F. Jiang, “Near-Unity Polarization of Valley-Dependent Second-Harmonic Generation in Stacked TMDC Layers and Heterostructures at Room Temperature,” Adv. Mater.1908061 (2020).
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J. Yu, J. Zhong, X. Kuang, C. Zeng, L. Cao, Y. Liu, and Z. Liu, “Dynamic Control of High-Range Photoresponsivity in a Graphene Nanoribbon Photodetector,” Nanoscale Res. Lett. 15(1), 124 (2020).
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J. Zhong, J. Yu, L. Cao, C. Zeng, J. Ding, C. Cong, Z. Liu, and Y. Liu, “High-performance polarization-sensitive photodetector based on a few-layered PdSe2 nanosheet,” Nano Res. 13(6), 1780–1786 (2020).
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Figures (4)

Fig. 1.
Fig. 1. Growth of the WSe2/WS2 heterostructures. (a) Schematic diagram of the tube furnace used for the growth of the WSe2/WS2 heterostructures in the experiment. The arrows in different colors show two opposite directions of flow, with the green being the forward flow. (b) Schematic diagram of the physical vapor deposition method for the growth of the heterostructures. The top of the diagram shows the deposition process of molecules for the WSe2 layer, while the bottom of the diagram indicates the process of the epitaxial growth of WSe2 on top of the WS2 layer. (c) Optical images of the WSe2/WS2 heterostructures showing the smaller triangular-shaped WSe2 on top of the relatively larger triangular-shaped WS2.
Fig. 2.
Fig. 2. Raman mapping and photoluminescence quenching in the WSe2/WS2 heterostructures. (a) Raman spectra of WSe2 and WS2 and their heterostructure. The red line is a spectrum from the WSe2/WS2, and the blue line is the WS2 spectrum obtained from the edge of the heterostructure where there was no WSe2 present. As a comparison, the Raman spectrum (black line) from a monolayer WSe2 sample is also presented. (b) PL spectra of WSe2, WS2, and their heterostructure. (c)-(e) Raman mapping images of the WSe2/WS2 heterostructures. Mapped with their characteristic peaks, the green regions are WSe2, and the red regions are WS2. The insets are optical images of the WSe2/WS2 heterostructures. (f)-(h) PL mapping images of the WSe2/WS2 heterostructures showing photoluminescence quenching resulting from the band-structure of the type-II heterostructure. The insets in (c)-(h) are the optical images of the WSe2/WS2 heterostructures.
Fig. 3.
Fig. 3. Normalized photoluminescence spectra under variable temperature. (a) The PL spectra of the WS2 region under different temperatures (65K-300K). The dashed line indicates the trends of peak shifting. (b) The PL spectra of the localized excitons in the WSe2/WS2 heterostructures under different temperatures (65K-300K). (c) X- Peak energy as a function of temperature. The solid line indicates a fit using the Varshni equation. (d) Energy level diagram of WS2/WSe2 heterostructure.
Fig. 4.
Fig. 4. Valley polarization of localized excitons. (a) and (c) Polarization-resolved PL spectra for the WSe2/WS2 heterostructures at 65K using σ- excitation. (b) and (d) Polarization-resolved PL spectra for the WSe2/WS2 heterostructures at 65K using σ+ excitation. In (a) and (b), the red line represents the intensity of left-handed light emitted by the heterostructures. The blue line represents the intensity of right-handed light emitted by the heterostructures. The olive-green dotted line indicates the corresponding degree of PL polarization. (e) Schematic diagram of optical selection rules. (f) Schematic diagram of the optical selection rules of the local excitons in WS2. The purple lines indicate defect energy levels.

Equations (2)

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E g ( T ) = E g ( 0 ) α T 2 / ( T + β ) ,
P = I σ I σ + I σ + I σ +