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Exciton spin relaxation dynamics in CdTe quantum dots at room temperature

Zhu Meng-Long Dong Yu-Lan Zhong Hai-Zheng He Jun

Exciton spin relaxation dynamics in CdTe quantum dots at room temperature

Zhu Meng-Long, Dong Yu-Lan, Zhong Hai-Zheng, He Jun
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  • Size-dependent exciton spin relaxation dynamics in CdTe colloidal quantum dots is studied at room temperature with the cross-polarized heterodyne third-order nonlinear transient grating technique The CdTe exciton spin relaxation reveals a mono-exponential decay behavior with a time constant of 0.1-0.5 ps when the pump-probe photon energy is tuned to be in resonance with the lowest exciton absorption transition (1Se-1Sh). The exciton spin relaxation in quantum dot is mainly governed by the hole spin flip process and ascribed to the transitions between bright-dark exciton fine structure states, i.e. J= 1+2. This finding suggests that the exciton spin relaxation rate in CdTe quantum dot is inversely proportional to the fourth power of quantum dot size.
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 61222406, 11174371), the Natural Science Foundation of Hunan Province, China (Grant No. 12JJ1001), the Specialized Research Fund for the Doctoral Program of Higher Education of China (Grant No. 20110162120072), the Program for New Century Excellent Talents in University of Ministry of Education of China (Grant No. NCET-11-0512), and the Fundamental Research Fund for the Central Universities, China.
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    Tong H, Wu M W 2011 Phys. Rev. B 83 235323

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    Tartakovskii A I, Cahill J, Makhonin M N, Whittaker D M, Wells J P R, Fox A M, Mowbray D J, Skolnick M S, Groom K M, Steer M J, Hopkinson M 2004 Phys. Rev. Lett. 93 057401

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    Nair P S, Fritz K P, Scholes G D 2004 Chem. Comm. 18 2084

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    Yu W W, Qu L H, Guo W Z, Peng X G 2003 Chem. Mater. 15 2854

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    Zhong H Z, Nagy M, Jones M, Scholes G D 2009 J. Phys. Chem. C 113 10465

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    An L M, Yang Y Q, Song W S, Su W H, Zeng Q H, Chao K F, Kong X G 2009 Acta Phys. Sin. 58 7914 (in Chinese) [安利民, 杨延强, 宋维斯, 苏文辉, 曾庆辉, 朝克夫, 孔祥贵 2009 物理学报 58 7914]

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    Gerardot B D, Brunner D, Dalgarno P A, Ohberg P, Seidl S, Kroner M, Karrai K, Stoltz N G, Petroff P M, Warburton R J 2008 Nature 451 441

    [13]

    Brunner D, Gerardot B D, Dalgarno P A, Wust G, Laraai K, Stoltz N G, Petroff P M, Warburton R J 2009 Science 325 70

    [14]

    Scholes G D, Kim J, Wong C Y 2006 Phys. Rev. B 73 195325

    [15]

    Huxter V M, Kim J, Lo S S, Lee A, Nair P S, Scholes G D 2010 Chem. Phys. Lett. 491 187

    [16]

    Kim J, Wong C Y, Nair P S, Fritz K P, Kumar S, Scholes G D 2006 J. Phys. Chem. B 110 25371

    [17]

    Scholes G D, Kim J, Wong C Y, Huxter V M, Nair P S, Fritz K P, Kumar S 2006 Nano Lett. 6 1765

    [18]

    He J, Zhong H Z, Scholes G D 2010 Phys. Rev. Lett. 105 046601

    [19]

    He J, Lo S S, Kim J, Scholes G D 2008 Nano Lett. 8 4007

    [20]

    Wong C Y, Kim J, Nair P S, Nagy M C, Scholes G D 2009 J. Phys. Chem. C 113 795

    [21]

    Brus L E 1984 J. Chem. Phys. 80 4403

    [22]

    Efros A L, Rosen M, Kuno M, Nirmal M, Norris D J 1996 Phys. Rev. B 54 4843

    [23]

    Nahalkova P, Sprinzl D, Maly P, Nemec P, Gladilin V N, Devreese J T 2007 Phys. Rev. B 75 113306

    [24]

    Pikus G E, Bir G L 1971 Sov. Phys. JEPT 33 108

    [25]

    Vinattieri A, Shah J, Damen T C, Kim D S, Pfeiffer L N, Maialle M Z, Sham L J 1994 Phys. Rev. B 50 10868

    [26]

    Ma H, Jin Z, Zhang Z, Li G, Ma G 2012 J. Phys. Chem. A 116 2018

    [27]

    He J, Ji W, Ma G H, Tang S H, Elim H L, Sun W X, Zhang Z H, Chin W S 2004 J. Appl. Phys. 95 6381

    [28]

    Viswanatha R, Sapra S, Saha-Dasgupta T, Sarma D D 2005 Phys. Rev. B 72 045333

    [29]

    Atature M, Dreiser J, Badolato A, Hogele A, Karrai K, Imamoglu A 2006 Science 312 551

    [30]

    Gupta J A, Awschalom D D, Efros A L, Rodina A V 2002 Phys. Rev. B 66 125307

    [31]

    Gundogdu K, Hall K C, Koerperick E J, Pryor C E, Flatté M E, Boggess T F 2005 Appl. Phys. Lett. 86 113111

    [32]

    Hall K C, Koerperick E J, Boggess T F, Shchekin O B 2007 Appl. Phys. Lett. 90 053109

    [33]

    Fischer J, Loss D 2009 Science 324 1277

    [34]

    Kolodrubetz M H, Petta J R 2009 Science 325 42

  • [1]

    Gupta J A, Knobel R, Samarth N, Awschalom D D 2001 Science 292 2458

    [2]

    Ouyang M, Dabid D, Awschalom D D 2003 Science 301 1074

    [3]

    Ramsay A J 2010 Semi. Sci. Technol. 25 103001

    [4]

    Tong H, Wu M W 2011 Phys. Rev. B 83 235323

    [5]

    Ma S S, Dou X M, Chang X Y, Sun B Q, Xiong Y H, Niu Z C, Ni H Q 2009 Chin. Phys. Lett. 26 117201

    [6]

    Gupta J A, Awschalom D D, Peng X, Alivisatos A P 1999 Phys. Rev. B 59 R10421

    [7]

    Tartakovskii A I, Cahill J, Makhonin M N, Whittaker D M, Wells J P R, Fox A M, Mowbray D J, Skolnick M S, Groom K M, Steer M J, Hopkinson M 2004 Phys. Rev. Lett. 93 057401

    [8]

    Nair P S, Fritz K P, Scholes G D 2004 Chem. Comm. 18 2084

    [9]

    Yu W W, Qu L H, Guo W Z, Peng X G 2003 Chem. Mater. 15 2854

    [10]

    Zhong H Z, Nagy M, Jones M, Scholes G D 2009 J. Phys. Chem. C 113 10465

    [11]

    An L M, Yang Y Q, Song W S, Su W H, Zeng Q H, Chao K F, Kong X G 2009 Acta Phys. Sin. 58 7914 (in Chinese) [安利民, 杨延强, 宋维斯, 苏文辉, 曾庆辉, 朝克夫, 孔祥贵 2009 物理学报 58 7914]

    [12]

    Gerardot B D, Brunner D, Dalgarno P A, Ohberg P, Seidl S, Kroner M, Karrai K, Stoltz N G, Petroff P M, Warburton R J 2008 Nature 451 441

    [13]

    Brunner D, Gerardot B D, Dalgarno P A, Wust G, Laraai K, Stoltz N G, Petroff P M, Warburton R J 2009 Science 325 70

    [14]

    Scholes G D, Kim J, Wong C Y 2006 Phys. Rev. B 73 195325

    [15]

    Huxter V M, Kim J, Lo S S, Lee A, Nair P S, Scholes G D 2010 Chem. Phys. Lett. 491 187

    [16]

    Kim J, Wong C Y, Nair P S, Fritz K P, Kumar S, Scholes G D 2006 J. Phys. Chem. B 110 25371

    [17]

    Scholes G D, Kim J, Wong C Y, Huxter V M, Nair P S, Fritz K P, Kumar S 2006 Nano Lett. 6 1765

    [18]

    He J, Zhong H Z, Scholes G D 2010 Phys. Rev. Lett. 105 046601

    [19]

    He J, Lo S S, Kim J, Scholes G D 2008 Nano Lett. 8 4007

    [20]

    Wong C Y, Kim J, Nair P S, Nagy M C, Scholes G D 2009 J. Phys. Chem. C 113 795

    [21]

    Brus L E 1984 J. Chem. Phys. 80 4403

    [22]

    Efros A L, Rosen M, Kuno M, Nirmal M, Norris D J 1996 Phys. Rev. B 54 4843

    [23]

    Nahalkova P, Sprinzl D, Maly P, Nemec P, Gladilin V N, Devreese J T 2007 Phys. Rev. B 75 113306

    [24]

    Pikus G E, Bir G L 1971 Sov. Phys. JEPT 33 108

    [25]

    Vinattieri A, Shah J, Damen T C, Kim D S, Pfeiffer L N, Maialle M Z, Sham L J 1994 Phys. Rev. B 50 10868

    [26]

    Ma H, Jin Z, Zhang Z, Li G, Ma G 2012 J. Phys. Chem. A 116 2018

    [27]

    He J, Ji W, Ma G H, Tang S H, Elim H L, Sun W X, Zhang Z H, Chin W S 2004 J. Appl. Phys. 95 6381

    [28]

    Viswanatha R, Sapra S, Saha-Dasgupta T, Sarma D D 2005 Phys. Rev. B 72 045333

    [29]

    Atature M, Dreiser J, Badolato A, Hogele A, Karrai K, Imamoglu A 2006 Science 312 551

    [30]

    Gupta J A, Awschalom D D, Efros A L, Rodina A V 2002 Phys. Rev. B 66 125307

    [31]

    Gundogdu K, Hall K C, Koerperick E J, Pryor C E, Flatté M E, Boggess T F 2005 Appl. Phys. Lett. 86 113111

    [32]

    Hall K C, Koerperick E J, Boggess T F, Shchekin O B 2007 Appl. Phys. Lett. 90 053109

    [33]

    Fischer J, Loss D 2009 Science 324 1277

    [34]

    Kolodrubetz M H, Petta J R 2009 Science 325 42

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  • Received Date:  16 February 2014
  • Accepted Date:  14 April 2014
  • Published Online:  20 June 2014

Exciton spin relaxation dynamics in CdTe quantum dots at room temperature

  • 1. Hunan Key Laboratory for Super-Microstructure and Ultrafast Process, Institute of Super-Microstructure and Ultrafast Process in Advanced Materials, School of Physics and Electronics, Central South University, Changsha 410083, China;
  • 2. School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Fund Project:  Project supported by the National Natural Science Foundation of China (Grant Nos. 61222406, 11174371), the Natural Science Foundation of Hunan Province, China (Grant No. 12JJ1001), the Specialized Research Fund for the Doctoral Program of Higher Education of China (Grant No. 20110162120072), the Program for New Century Excellent Talents in University of Ministry of Education of China (Grant No. NCET-11-0512), and the Fundamental Research Fund for the Central Universities, China.

Abstract: Size-dependent exciton spin relaxation dynamics in CdTe colloidal quantum dots is studied at room temperature with the cross-polarized heterodyne third-order nonlinear transient grating technique The CdTe exciton spin relaxation reveals a mono-exponential decay behavior with a time constant of 0.1-0.5 ps when the pump-probe photon energy is tuned to be in resonance with the lowest exciton absorption transition (1Se-1Sh). The exciton spin relaxation in quantum dot is mainly governed by the hole spin flip process and ascribed to the transitions between bright-dark exciton fine structure states, i.e. J= 1+2. This finding suggests that the exciton spin relaxation rate in CdTe quantum dot is inversely proportional to the fourth power of quantum dot size.

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