Synthesis and optical properties of ultra-small Tin doped CsPbBr<sub>3</sub> blue luminescence quantum dots

Zeng Fan-Ju; Tan Yong-Qian; Hu Wei; Tang Xiao-Sheng; Zhang Xiao-Mei; Yin Hai-Feng

doi:10.7498/aps.71.20211895

Abstract

All-inorganic perovskite CsPbX₃ (X = Cl, Br and I) quantum dots (QDs) have been wildly utilized in optoelectronic devices due to their tunable photoluminescence, high photoluminescence quantum yield (PLQY), and narrow-line width photoluminescence. However, the blue luminescence PLQY of CsPbX₃ perovskite quantum dots is still lower than their red and green luminescence counterparts (PLQYs nearly 100%). Here in this work, we present a handy strategy to synthesise the ultra-small blue luminescence Tin-doped CsPbBr₃ perovskite QDs by supersaturated recrystallization synthetic approach at room temperature, and the particle size of as-prepared QDs is lower than 4 nm. The crystal structure and optical property of Tin doped CsPbBr₃ QDs are characterized by XRD, TEM, ultraviolet-visible spectrophotometer, and fluorescence spectrophotometer. The results show that the particle size of as-prepared QDs is slightly shrunk from 3.33 nm (SnBr₂ 0.03 mmol) to 2.23 nm (SnBr₂ 0.06 mmol) as the SnBr₂ adding quantity increases, but there is no obvious change in the lattice spacing of doped QDs. The partial substitution of Pb for Tin leads the optical spectra to blue-shift from 490 nm (SnBr₂ 0.03 mmol) to 472 nm (SnBr₂ 0.06 mmol). The highest PLQY and the strongest XRD diffraction of ultra-small Tin doped CsPbBr₃blue luminescence QDs are obtained by adding SnBr₂ 0.05 mmol, and the blue luminescence peak is located at 472 nm with the PLQY of 53.4%. There is no any change in PL peak of Tin doped CsPbBr₃ QDs (SnBr₂ 0.05 mmol) by storing it under the ambient atmosphere for 15 days, and the PLQY of Sn²⁺ doped QDs is still 80% of the initial after 15 days. It is concluded that the crystallization and optical property can be effectively improved in Tin doped CsPbBr₃ QDs by partially replacing appropriate quantity of Pb by Tin.

Keywords:

Authors and contacts

1.
School of Big Data Engineering, Kaili University, Kaili 556011, China
2.
College of Optoelectronic Engineering, Chongqing University, Chongqing 400044, China
3.
College of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China

Corresponding author: Zeng Fan-Ju, zengfanju@cqu.edu.cn ; Hu Wei, weihu@cqu.edu.cn ; Tang Xiao-Sheng, xstang@cqu.edu.cn ;

Funds: Project supported by Science and Technology Program of Guizhou Province, China (grant No. ZK[2021]245), the National Natural Science Foundation of China (Grant Nos.61975023, 61875211, 51602033, 61520106012), the Doctoral Project of Kaili University (Grant Nos. BS202004, BS201301), the Academic New Seedling Cultivation and Innovation Exploration Special Project of Kaili University (Grant No. Qian Ke He Ping Tai Ren Cai [2019]01-4), and the Major Research Projects of Innovative Groups in Education Department of Guizhou Province of China (Grant No. Qian Jiao He KY[2018]035).

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References

[1]	Li C L, Han C, Zhang Y B, Zang Z G, Wang M, Tang X S, Du J 2017 Sol. Energy Mater. Sol. Cells 172 341 Google Scholar
[2]	Li C L, Zang Z G, Han C, Hu Z P, Tang X S, Du J, Leng Y X, Sun K 2017 Nano Energy 40 195 Google Scholar
[3]	Song J Z, Tao F, Li J H, Xu L M, Zhang F J, Han B N, Shan Q S, Zeng H B 2018 Adv. Mater. 30 1805409 Google Scholar
[4]	Tang X S, Hu Z P, Chen W W, Xing X, Zang Z G, Hu W, Qiu J, Du J, Leng Y X, Jiang X F, Mai L Q 2016 Nano Energy 28 462 Google Scholar
[5]	Zhang X, Lin H, Huang H, Reckmeier C, Zhang Y, Choy W C, Rogach A L 2016 Nano Lett. 16 1415 Google Scholar
[6]	瞿子涵, 储泽马, 张兴旺, 游经碧 2019 物理学报 68 158504 Google Scholar Qu Z H, Chu Z M, Zhang X W, You J B 2019 Acta Phys. Sin. 68 158504 Google Scholar
[7]	Shirasaki Y, Supran G J, Bawendi M G, Bulović V 2012 Nat. Photon. 7 13
[8]	Protesescu L, Yakunin S, Bodnarchuk M I, Krieg F, Caputo R, Hendon C H, Yang R X, Walsh A, Kovalenko M V 2015 Nano Lett. 15 3692 Google Scholar
[9]	Liu F, Zhang Y H, Ding C, Kobayashi S, Izuishi T, Nakazawa N, Toyoda T, Ohta T, Hayase S, Minemoto T, Yoshino K, Dai S, Shen Q 2017 ACS Nano 11 10373 Google Scholar
[10]	段聪聪, 程露, 殷垚, 朱琳 2019 物理学报 68 158503 Google Scholar Duan C C, Cheng L, Yin Y, Zhu L 2019 Acta Phys. Sin. 68 158503 Google Scholar
[11]	石文奇, 田宏, 陆玉新, 朱虹, 李芬, 王小霞, 刘燕文 2021 物理学报 70 087303 Google Scholar Shi W Q, Tian H, Lu Y X, Zhu H, Li F, Wang X X, Liu Y W 2021 Acta Phys. Sin. 70 087303 Google Scholar
[12]	Chen W W, Xin X, Zang Z G, Tang X S, Li C L, Hu W, Zhou M, Du J 2017 J. Solid State Chem. 255 115 Google Scholar
[13]	Guner T, Demir M M 2018 Phys. Status Solidi A 215 1800120 Google Scholar
[14]	Li X M, Wu Y, Zhang S L, Cai B, Gu Y, Song J Z, Zeng H B 2016 Adv. Funct. Mater. 26 2435 Google Scholar
[15]	Bi C H, Wang S X, Li Q, Kershaw S V, Tian J J, Rogach A L 2019 J. Phys. Chem. Lett. 10 943 Google Scholar
[16]	Liu H W, Wu Z N, Shao J R, Yao D, Gao H, Liu Y, Yu W L, Zhang H, Yang B 2017 ACS Nano 11 2239 Google Scholar
[17]	van der Stam W, Geuchies J J, Altantzis T, van den Bos K H, Meeldijk J D, Van Aert S, Bals S, Vanmaekelbergh D, de Mello Donega C 2017 J. Am. Chem. Soc. 139 4087 Google Scholar
[18]	Liu M, Zhong G H, Yin Y M, Miao J S, Li K, Wang C Q, Xu X R, Shen C, Meng H 2017 Adv. Sci. 4 1700335 Google Scholar
[19]	Li M, Zhang X, Matras-Postolek K, Chen H S, Yang P 2018 J. Mater. Chem. C 6 5506 Google Scholar
[20]	Pradeep K R, Chakraborty S, Viswanatha R 2019 Mater. Res. Express 6 114004 Google Scholar
[21]	Wang H C, Wang W G, Tang A C, Tsai H Y, Bao Z, Ihara T, Yarita N, Tahara H, Kanemitsu Y, Chen S M, Liu R S 2017 Angew. Chem. Int. Edit. 56 13650 Google Scholar
[22]	Zhang X T, Wang H, Hu Y, Pei Y X, Wang S X, Shi Z F, Colvin V L, Wang S N, Zhang Y, Yu W W 2019 J. Phys. Chem. Lett. 10 1750 Google Scholar
[23]	Zhang X L, Cao W Y, Wang W G, Xu B, Liu S, Dai H T, Chen S M, Wang K, Sun X W 2016 Nano Energy 30 511 Google Scholar
[24]	Veldhuis S A, Boix P P, Yantara N, Li M, Sum T C, Mathews N, Mhaisalkar S G 2016 Adv. Mater. 28 6804 Google Scholar
[25]	Wang H C, Bao Z, Tsai H Y, Tang A C, Liu R S 2018 Small 14 1702433 Google Scholar
[26]	Huang H, Susha A S, Kershaw S V, Hung T F, Rogach A L 2015 Adv. Sci. 2 1500194 Google Scholar
[27]	Pan G C, Bai X, Xu W, Chen X, Zhai Y, Zhu J Y, Shao H, Ding N, Xu L, Dong B, Mao Y L, Song H W 2020 ACS Appl. Mater. Interfaces 12 14195 Google Scholar
[28]	Wang S X, Wang Y, Zhang Y, Zhang X T, Shen X Y, Zhuang X W, Lu P, Yu W W, Kershaw S V, Rogach A L 2019 J. Phys. Chem. Lett. 10 90 Google Scholar

Cited By

图 1 锡掺杂CsPbBr₃量子点的XRD谱

Figure 1. XRD patterns of tin doped CsPbBr₃ quantum dots.

DownLoad: Full-Size Img PowerPoint

图 2 锡掺杂CsPbBr₃量子点的TEM图谱(标尺为20 nm) (a) SnBr₂为0.03 mmol; (b) SnBr₂为0.05 mmol; (c) SnBr₂为0.06 mmol. (a) (b)中插图为对应TEM图量子点的HRTEM图谱(标尺为2 nm)

Figure 2. TEM images of tin doped CsPbBr₃ quantum dots (scale bars represent 20 nm): (a) SnBr₂ is 0.03 mmol; (b) SnBr₂ is 0.05 mmol; (c) SnBr₂ is 0.06 mmol. Inset pictures show the HRTEM of corresponding quantum dots (scale bars represent 2 nm).

DownLoad: Full-Size Img PowerPoint

图 3 锡掺杂CsPbBr₃量子点的Cs, Pb, Br和Sn元素的元素映射图像(SnBr₂ 为0.05 mmol), 标尺为50 nm

Figure 3. Cs, Pb, Br, and Sn element mapping images of tin doped CsPbBr₃ quantum dots (SnBr₂ is 0.05 mmol). The scale bars represent 50 nm.

DownLoad: Full-Size Img PowerPoint

图 4 锡掺杂CsPbBr₃量子点的EDS(SnBr₂为0.05 mmol)

Figure 4. EDS of tin doped CsPbBr₃ quantum dots (SnBr₂ 0.05 mmol).

DownLoad: Full-Size Img PowerPoint

图 5 锡掺杂CsPbBr₃量子点的　(a)吸收光谱; (b)荧光光谱; (c) PLQY

Figure 5. (a) Absorption spectra; (b) emission spectra; (c) PLQY of tin doped CsPbBr₃ quantum dots.

DownLoad: Full-Size Img PowerPoint

图 6 锡离子掺杂CsPbBr₃量子点的荧光衰减图

Figure 6. Time-resolved PL decays of tin doped CsPbBr₃ quantum dots.

DownLoad: Full-Size Img PowerPoint

图 7 锡离子掺杂CsPbBr₃量子点大气氛围存放1—15 d的荧光峰位置及PLQY变化

Figure 7. PL peak and PLQY of tin doped CsPbBr₃ quantum dots from 1 to 15 days.

DownLoad: Full-Size Img PowerPoint

表 1 锡掺杂CsPbBr₃量子点的衰减曲线拟合参数

Table 1. Fitting results fitted by time-resolved PL decays curve of tin doped CsPbBr₃ quantum dots.

SnBr₂/
mmol A₁/
% τ₁/
ns A₂/
% τ₂/
ns A₃/
% τ₃/
ns τ_avg/
ns

0.03 12.36 3.60 69.05 9.33 18.59 26.17 16.09
0.04 4.52 1.83 69.01 9.16 26.48 22.92 15.81
0.05 7.43 2.09 63.97 8.96 28.60 25.07 17.73
0.06 4.42 1.65 69.56 8.10 26.03 21.64 14.78

DownLoad: CSV

表 2 τ_r, τ_nr, κ_r和κ_nr计算结果

Table 2. Calculate results of τ_r, τ_nr, κ_r和κ_nr.

SnBr₂/
mmol τ_avg/
ns PLQY/
% τ_r/
ns τ_nr/
ns κ_r×10⁷/
s^–1 κ_nr×10⁷/
s^–1

0.03 16.09 43.4 37.07 28.43 2.70 3.52
0.04 15.81 32.3 48.95 23.35 2.04 4.28
0.05 17.73 53.4 33.20 38.05 3.01 2.63
0.06 14.78 21.7 68.11 18.88 1.47 5.30

DownLoad: CSV

[1]	Li C L, Han C, Zhang Y B, Zang Z G, Wang M, Tang X S, Du J 2017 Sol. Energy Mater. Sol. Cells 172 341 Google Scholar
[2]	Li C L, Zang Z G, Han C, Hu Z P, Tang X S, Du J, Leng Y X, Sun K 2017 Nano Energy 40 195 Google Scholar
[3]	Song J Z, Tao F, Li J H, Xu L M, Zhang F J, Han B N, Shan Q S, Zeng H B 2018 Adv. Mater. 30 1805409 Google Scholar
[4]	Tang X S, Hu Z P, Chen W W, Xing X, Zang Z G, Hu W, Qiu J, Du J, Leng Y X, Jiang X F, Mai L Q 2016 Nano Energy 28 462 Google Scholar
[5]	Zhang X, Lin H, Huang H, Reckmeier C, Zhang Y, Choy W C, Rogach A L 2016 Nano Lett. 16 1415 Google Scholar
[6]	瞿子涵, 储泽马, 张兴旺, 游经碧 2019 物理学报 68 158504 Google Scholar Qu Z H, Chu Z M, Zhang X W, You J B 2019 Acta Phys. Sin. 68 158504 Google Scholar
[7]	Shirasaki Y, Supran G J, Bawendi M G, Bulović V 2012 Nat. Photon. 7 13
[8]	Protesescu L, Yakunin S, Bodnarchuk M I, Krieg F, Caputo R, Hendon C H, Yang R X, Walsh A, Kovalenko M V 2015 Nano Lett. 15 3692 Google Scholar
[9]	Liu F, Zhang Y H, Ding C, Kobayashi S, Izuishi T, Nakazawa N, Toyoda T, Ohta T, Hayase S, Minemoto T, Yoshino K, Dai S, Shen Q 2017 ACS Nano 11 10373 Google Scholar
[10]	段聪聪, 程露, 殷垚, 朱琳 2019 物理学报 68 158503 Google Scholar Duan C C, Cheng L, Yin Y, Zhu L 2019 Acta Phys. Sin. 68 158503 Google Scholar
[11]	石文奇, 田宏, 陆玉新, 朱虹, 李芬, 王小霞, 刘燕文 2021 物理学报 70 087303 Google Scholar Shi W Q, Tian H, Lu Y X, Zhu H, Li F, Wang X X, Liu Y W 2021 Acta Phys. Sin. 70 087303 Google Scholar
[12]	Chen W W, Xin X, Zang Z G, Tang X S, Li C L, Hu W, Zhou M, Du J 2017 J. Solid State Chem. 255 115 Google Scholar
[13]	Guner T, Demir M M 2018 Phys. Status Solidi A 215 1800120 Google Scholar
[14]	Li X M, Wu Y, Zhang S L, Cai B, Gu Y, Song J Z, Zeng H B 2016 Adv. Funct. Mater. 26 2435 Google Scholar
[15]	Bi C H, Wang S X, Li Q, Kershaw S V, Tian J J, Rogach A L 2019 J. Phys. Chem. Lett. 10 943 Google Scholar
[16]	Liu H W, Wu Z N, Shao J R, Yao D, Gao H, Liu Y, Yu W L, Zhang H, Yang B 2017 ACS Nano 11 2239 Google Scholar
[17]	van der Stam W, Geuchies J J, Altantzis T, van den Bos K H, Meeldijk J D, Van Aert S, Bals S, Vanmaekelbergh D, de Mello Donega C 2017 J. Am. Chem. Soc. 139 4087 Google Scholar
[18]	Liu M, Zhong G H, Yin Y M, Miao J S, Li K, Wang C Q, Xu X R, Shen C, Meng H 2017 Adv. Sci. 4 1700335 Google Scholar
[19]	Li M, Zhang X, Matras-Postolek K, Chen H S, Yang P 2018 J. Mater. Chem. C 6 5506 Google Scholar
[20]	Pradeep K R, Chakraborty S, Viswanatha R 2019 Mater. Res. Express 6 114004 Google Scholar
[21]	Wang H C, Wang W G, Tang A C, Tsai H Y, Bao Z, Ihara T, Yarita N, Tahara H, Kanemitsu Y, Chen S M, Liu R S 2017 Angew. Chem. Int. Edit. 56 13650 Google Scholar
[22]	Zhang X T, Wang H, Hu Y, Pei Y X, Wang S X, Shi Z F, Colvin V L, Wang S N, Zhang Y, Yu W W 2019 J. Phys. Chem. Lett. 10 1750 Google Scholar
[23]	Zhang X L, Cao W Y, Wang W G, Xu B, Liu S, Dai H T, Chen S M, Wang K, Sun X W 2016 Nano Energy 30 511 Google Scholar
[24]	Veldhuis S A, Boix P P, Yantara N, Li M, Sum T C, Mathews N, Mhaisalkar S G 2016 Adv. Mater. 28 6804 Google Scholar
[25]	Wang H C, Bao Z, Tsai H Y, Tang A C, Liu R S 2018 Small 14 1702433 Google Scholar
[26]	Huang H, Susha A S, Kershaw S V, Hung T F, Rogach A L 2015 Adv. Sci. 2 1500194 Google Scholar
[27]	Pan G C, Bai X, Xu W, Chen X, Zhai Y, Zhu J Y, Shao H, Ding N, Xu L, Dong B, Mao Y L, Song H W 2020 ACS Appl. Mater. Interfaces 12 14195 Google Scholar
[28]	Wang S X, Wang Y, Zhang Y, Zhang X T, Shen X Y, Zhuang X W, Lu P, Yu W W, Kershaw S V, Rogach A L 2019 J. Phys. Chem. Lett. 10 90 Google Scholar

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Synthesis and optical properties of ultra-small Tin doped CsPbBr₃ blue luminescence quantum dots

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Authors and contacts

Corresponding author: Zeng Fan-Ju, zengfanju@cqu.edu.cn ; Hu Wei, weihu@cqu.edu.cn ; Tang Xiao-Sheng, xstang@cqu.edu.cn ;

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SnBr₂/ mmol	A₁/ %	τ₁/ ns	A₂/ %	τ₂/ ns	A₃/ %	τ₃/ ns	τ_avg/ ns
0.03	12.36	3.60	69.05	9.33	18.59	26.17	16.09
0.04	4.52	1.83	69.01	9.16	26.48	22.92	15.81
0.05	7.43	2.09	63.97	8.96	28.60	25.07	17.73
0.06	4.42	1.65	69.56	8.10	26.03	21.64	14.78

SnBr₂/ mmol	τ_avg/ ns	PLQY/ %	τ_r/ ns	τ_nr/ ns	κ_r×10⁷/ s^–1	κ_nr×10⁷/ s^–1
0.03	16.09	43.4	37.07	28.43	2.70	3.52
0.04	15.81	32.3	48.95	23.35	2.04	4.28
0.05	17.73	53.4	33.20	38.05	3.01	2.63
0.06	14.78	21.7	68.11	18.88	1.47	5.30

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Synthesis and optical properties of ultra-small Tin doped CsPbBr3 blue luminescence quantum dots

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Authors and contacts

Corresponding author: Zeng Fan-Ju, zengfanju@cqu.edu.cn ; Hu Wei, weihu@cqu.edu.cn ; Tang Xiao-Sheng, xstang@cqu.edu.cn ;

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Synthesis and optical properties of ultra-small Tin doped CsPbBr₃ blue luminescence quantum dots