Abstract

Perovskites have emerged as a class of cutting-edge light-emitting materials; however, their poor stability, due to the high sensitivity to moisture in the ambient environment, severely hinders their further application. Here, to obtain stable perovskite-based laser with excellent optical performance, all-inorganic perovskite CsPbBr3 quantum dots (QDs) evenly distributed into sub-micro silica sphere (CsPbBr3-SiO2) have been used as laser gain medium. The single silica sphere embedded by plentiful CsPbBr3 QDs demonstrates frequency up-converted lasing with compounded mode of random and whispering-gallery-mode (WGM) at room temperature. Furthermore, by incorporating the CsPbBr3-SiO2 spheres into a microtubule, the frequency up-converted WGM lasing has been successfully achieved under two-photon excitation. Notably, the CsPbBr3-SiO2 microtubule resonator exhibits a low lasing threshold of 430 μJ/cm2, mostly due to the enhanced gain for CsPbBr3 QDs inside the silica sphere. Moreover, stable WGM lasing is observed under continuous optical pump for 140 min, benefited from the protection of silica shells, which isolate the QDs from the environmental conditions. The enhanced lasing performance provides an effective way for further exploration and application of perovskite-based micro/nano photonic devices.

© 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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References

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2019 (1)

2018 (5)

K. Wei, T. Jiang, Z. Xu, J. Zhou, J. You, Y. Tang, H. Li, R. Chen, X. Zheng, S. Wang, K. Yin, Z. Wang, J. Wang, and X. Cheng, “Ultrafast carrier transfer promoted by interlayer coulomb coupling in 2D/3D perovskite heterostructures,” Laser Photonics Rev. 12(10), 1800128 (2018).
[Crossref]

Z. Liu, J. Yang, J. Du, Z. Hu, T. Shi, Z. Zhang, Y. Liu, X. Tang, Y. Leng, and R. Li, “Robust subwavelength single-mode perovskite nanocuboid laser,” ACS Nano 12(6), 5923–5931 (2018).
[Crossref] [PubMed]

F. Mathies, P. Brenner, G. Hernandez-Sosa, I. A. Howard, U. W. Paetzold, and U. Lemmer, “Inkjet-printed perovskite distributed feedback lasers,” Opt. Express 26(2), A144–A152 (2018).
[Crossref] [PubMed]

A. Gharajeh, R. Haroldson, Z. Li, J. Moon, B. Balachandran, W. Hu, A. Zakhidov, and Q. Gu, “Continuous-wave operation in directly patterned perovskite distributed feedback light source at room temperature,” Opt. Lett. 43(3), 611–614 (2018).
[Crossref] [PubMed]

Z. Hu, Z. Liu, Y. Bian, S. Li, X. Tang, J. Du, Z. Zang, M. Zhou, W. Hu, Y. Tian, and Y. Leng, “Enhanced two-photon-pumped emission from in situ synthesized nonblinking CsPbBr3/SiO2 nanocrystals with excellent stability,” Adv. Opt. Mater. 6(3), 1700997 (2018).
[Crossref]

2017 (6)

R. K. Ratnesh and M. S. Mehata, “Investigation of biocompatible and protein sensitive highly luminescent quantum dots/nanocrystals of CdSe, CdSe/ZnS and CdSe/CdS,” Spectrochim. Acta A Mol. Biomol. Spectrosc. 179, 201–210 (2017).
[Crossref] [PubMed]

X. Li, Y. Wang, H. Sun, and H. Zeng, “Amino-mediated anchoring perovskite quantum dots for stable and low-threshold random lasing,” Adv. Mater. 29(36), 1701185 (2017).
[Crossref] [PubMed]

J. Gong, Y. Wang, S. Liu, P. Zeng, X. Yang, R. Liang, Q. Ou, X. Wu, and S. Zhang, “All-inorganic perovskite-based distributed feedback resonator,” Opt. Express 25(24), A1154–A1161 (2017).
[Crossref] [PubMed]

C. Y. Huang, C. Zou, C. Mao, K. L. Corp, Y. C. Yao, Y. J. Lee, C. W. Schlenker, A. K. Y. Jen, and L. Y. Lin, “CsPbBr3 perovskite quantum dot vertical cavity lasers with low threshold and high stability,” ACS Photonics 4(9), 2281–2289 (2017).
[Crossref]

Y. Wang, X. Li, V. Nalla, H. Zeng, and H. Sun, “Solution-processed low threshold vertical cavity surface emitting lasers from all-inorganic perovskite nanocrystals,” Adv. Funct. Mater. 27(13), 1605088 (2017).
[Crossref]

M. V. Kovalenko, L. Protesescu, and M. I. Bodnarchuk, “Properties and potential optoelectronic applications of lead halide perovskite nanocrystals,” Science 358(6364), 745–750 (2017).
[Crossref] [PubMed]

2016 (7)

X. Tang, Z. Hu, W. Chen, X. Xing, Z. Zang, W. Hu, J. Qiu, J. Du, Y. Leng, X. Jiang, and L. Mai, “Room temperature single-photon emission and lasing for all-inorganic colloidal perovskite quantum dots,” Nano Energy 28, 462–468 (2016).
[Crossref]

Y. Xu, Q. Chen, C. Zhang, R. Wang, H. Wu, X. Zhang, G. Xing, W. W. Yu, X. Wang, Y. Zhang, and M. Xiao, “Two-photon-pumped perovskite semiconductor nanocrystal lasers,” J. Am. Chem. Soc. 138(11), 3761–3768 (2016).
[Crossref] [PubMed]

K. Wei, Z. Xu, R. Chen, X. Zheng, X. Cheng, and T. Jiang, “Temperature-dependent excitonic photoluminescence excited by two-photon absorption in perovskite CsPbBr3 quantum dots,” Opt. Lett. 41(16), 3821–3824 (2016).
[Crossref] [PubMed]

A. Swarnkar, A. R. Marshall, E. M. Sanehira, B. D. Chernomordik, D. T. Moore, J. A. Christians, T. Chakrabarti, and J. M. Luther, “Quantum dot-induced phase stabilization of α-CsPbI3 perovskite for high-efficiency photovoltaics,” Science 354(6308), 92–95 (2016).
[Crossref] [PubMed]

M. Wu, D. N. Congreve, M. W. B. Wilson, J. Jean, N. Geva, M. Welborn, T. Van Voorhis, V. Bulović, M. G. Bawendi, and M. A. Baldo, “Solid-state infrared-to-visible upconversion sensitized by colloidal nanocrystals,” Nat. Photonics 10(1), 31–34 (2016).
[Crossref]

Y. Wang, X. Li, X. Zhao, L. Xiao, H. Zeng, and H. Sun, “Nonlinear absorption and low-threshold multiphoton pumped stimulated emission from all-inorganic perovskite nanocrystals,” Nano Lett. 16(1), 448–453 (2016).
[Crossref] [PubMed]

S. Huang, Z. Li, L. Kong, N. Zhu, A. Shan, and L. Li, “Enhancing the stability of CH3NH3PbBr3 quantum dots by embedding in silica spheres derived from tetramethyl orthosilicate in “waterless” toluene,” J. Am. Chem. Soc. 138(18), 5749–5752 (2016).
[Crossref] [PubMed]

2015 (8)

H. Zhu, Y. Fu, F. Meng, X. Wu, Z. Gong, Q. Ding, M. V. Gustafsson, M. T. Trinh, S. Jin, and X.-Y. Zhu, “Lead halide perovskite nanowire lasers with low lasing thresholds and high quality factors,” Nat. Mater. 14(6), 636–642 (2015).
[Crossref] [PubMed]

B. Zhou, B. Shi, D. Jin, and X. Liu, “Controlling upconversion nanocrystals for emerging applications,” Nat. Nanotechnol. 10(11), 924–936 (2015).
[Crossref] [PubMed]

B. Guzelturk, Y. Kelestemur, K. Gungor, A. Yeltik, M. Z. Akgul, Y. Wang, R. Chen, C. Dang, H. Sun, and H. V. Demir, “Stable and low-threshold optical gain in CdSe/CdS quantum dots: An all-colloidal frequency up-converted laser,” Adv. Mater. 27(17), 2741–2746 (2015).
[Crossref] [PubMed]

S. Yakunin, L. Protesescu, F. Krieg, M. I. Bodnarchuk, G. Nedelcu, M. Humer, G. De Luca, M. Fiebig, W. Heiss, and M. V. Kovalenko, “Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites,” Nat. Commun. 6(1), 8056 (2015).
[Crossref] [PubMed]

Y. Wang, X. Li, J. Song, L. Xiao, H. Zeng, and H. Sun, “All-inorganic colloidal perovskite quantum dots: A new class of lasing materials with favorable characteristics,” Adv. Mater. 27(44), 7101–7108 (2015).
[Crossref] [PubMed]

J. Song, J. Li, X. Li, L. Xu, Y. Dong, and H. Zeng, “Quantum dot light-emitting diodes based on inorganic perovskite cesium lead halides (CsPbX3),” Adv. Mater. 27(44), 7162–7167 (2015).
[Crossref] [PubMed]

C. Zhang, C. L. Zou, Y. Zhao, C. H. Dong, C. Wei, H. Wang, Y. Liu, G. C. Guo, J. Yao, and Y. S. Zhao, “Organic printed photonics: From microring lasers to integrated circuits,” Sci. Adv. 1(8), e1500257 (2015).
[Crossref] [PubMed]

A. Swarnkar, R. Chulliyil, V. K. Ravi, M. Irfanullah, A. Chowdhury, and A. Nag, “Colloidal CsPbBr3 perovskite nanocrystals: Luminescence beyond traditional quantum dots,” Angew. Chem. Int. Ed. Engl. 54(51), 15424–15428 (2015).
[Crossref] [PubMed]

2014 (1)

B. R. Sutherland, S. Hoogland, M. M. Adachi, C. T. O. Wong, and E. H. Sargent, “Conformal organohalide perovskites enable lasing on spherical resonators,” ACS Nano 8(10), 10947–10952 (2014).
[Crossref] [PubMed]

2013 (3)

C. Grivas, C. Li, P. Andreakou, P. Wang, M. Ding, G. Brambilla, L. Manna, and P. Lagoudakis, “Single-mode tunable laser emission in the single-exciton regime from colloidal nanocrystals,” Nat. Commun. 4(1), 2376 (2013).
[Crossref] [PubMed]

J. Yu, Y. Cui, H. Xu, Y. Yang, Z. Wang, B. Chen, and G. Qian, “Confinement of pyridinium hemicyanine dye within an anionic metal-organic framework for two-photon-pumped lasing,” Nat. Commun. 4(1), 2719 (2013).
[Crossref] [PubMed]

S. Jun, J. Lee, and E. Jang, “Highly luminescent and photostable quantum dot-silica monolith and its application to light-emitting diodes,” ACS Nano 7(2), 1472–1477 (2013).
[Crossref] [PubMed]

2012 (2)

C. Dang, J. Lee, C. Breen, J. S. Steckel, S. Coe-Sullivan, and A. Nurmikko, “Red, green and blue lasing enabled by single-exciton gain in colloidal quantum dot films,” Nat. Nanotechnol. 7(5), 335–339 (2012).
[Crossref] [PubMed]

B. Piccione, C. H. Cho, L. K. van Vugt, and R. Agarwal, “All-optical active switching in individual semiconductor nanowires,” Nat. Nanotechnol. 7(10), 640–645 (2012).
[Crossref] [PubMed]

2011 (1)

J. H. Im, C. R. Lee, J. W. Lee, S. W. Park, and N. G. Park, “6.5% efficient perovskite quantum-dot-sensitized solar cell,” Nanoscale 3(10), 4088–4093 (2011).
[Crossref] [PubMed]

2009 (1)

L. Pan and D. B. Bogy, “Heat-assisted magnetic recording,” Nat. Photonics 3(4), 189–190 (2009).
[Crossref]

2008 (2)

2005 (2)

P. T. Snee, Y. H. Chan, D. G. Nocera, and M. G. Bawendi, “Whispering-gallery-mode lasing from a semiconductor nanocrystal/microsphere resonator composite,” Adv. Mater. 17(9), 1131–1136 (2005).
[Crossref]

S. T. Selvan, T. T. Tan, and J. Y. Ying, “Robust, non-cytotoxic, silica-coated CdSe quantum cots with efficient photoluminescence,” Adv. Mater. 17(13), 1620–1625 (2005).
[Crossref]

2002 (1)

A. V. Malko, A. A. Mikhailovsky, M. A. Petruska, J. A. Hollingsworth, H. Htoon, M. G. Bawendi, and V. I. Klimov, “From amplified spontaneous emission to microring lasing using nanocrystal quantum dot solids,” Appl. Phys. Lett. 81(7), 1303–1305 (2002).
[Crossref]

2000 (3)

D. Wiersma, “The smallest random laser,” Nature 406(6792), 133 (2000).
[Crossref] [PubMed]

V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science 290(5490), 314–317 (2000).
[Crossref] [PubMed]

H. Cao, J. Y. Xu, E. W. Seelig, and R. P. H. Chang, “Microlaser made of disordered media,” Appl. Phys. Lett. 76(21), 2997–2999 (2000).
[Crossref]

Adachi, M. M.

B. R. Sutherland, S. Hoogland, M. M. Adachi, C. T. O. Wong, and E. H. Sargent, “Conformal organohalide perovskites enable lasing on spherical resonators,” ACS Nano 8(10), 10947–10952 (2014).
[Crossref] [PubMed]

Agarwal, R.

B. Piccione, C. H. Cho, L. K. van Vugt, and R. Agarwal, “All-optical active switching in individual semiconductor nanowires,” Nat. Nanotechnol. 7(10), 640–645 (2012).
[Crossref] [PubMed]

Akgul, M. Z.

B. Guzelturk, Y. Kelestemur, K. Gungor, A. Yeltik, M. Z. Akgul, Y. Wang, R. Chen, C. Dang, H. Sun, and H. V. Demir, “Stable and low-threshold optical gain in CdSe/CdS quantum dots: An all-colloidal frequency up-converted laser,” Adv. Mater. 27(17), 2741–2746 (2015).
[Crossref] [PubMed]

Andreakou, P.

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M. V. Kovalenko, L. Protesescu, and M. I. Bodnarchuk, “Properties and potential optoelectronic applications of lead halide perovskite nanocrystals,” Science 358(6364), 745–750 (2017).
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J. H. Im, C. R. Lee, J. W. Lee, S. W. Park, and N. G. Park, “6.5% efficient perovskite quantum-dot-sensitized solar cell,” Nanoscale 3(10), 4088–4093 (2011).
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Z. Liu, J. Yang, J. Du, Z. Hu, T. Shi, Z. Zhang, Y. Liu, X. Tang, Y. Leng, and R. Li, “Robust subwavelength single-mode perovskite nanocuboid laser,” ACS Nano 12(6), 5923–5931 (2018).
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X. Li, Y. Wang, H. Sun, and H. Zeng, “Amino-mediated anchoring perovskite quantum dots for stable and low-threshold random lasing,” Adv. Mater. 29(36), 1701185 (2017).
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C. Y. Huang, C. Zou, C. Mao, K. L. Corp, Y. C. Yao, Y. J. Lee, C. W. Schlenker, A. K. Y. Jen, and L. Y. Lin, “CsPbBr3 perovskite quantum dot vertical cavity lasers with low threshold and high stability,” ACS Photonics 4(9), 2281–2289 (2017).
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B. Zhou, B. Shi, D. Jin, and X. Liu, “Controlling upconversion nanocrystals for emerging applications,” Nat. Nanotechnol. 10(11), 924–936 (2015).
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A. Swarnkar, A. R. Marshall, E. M. Sanehira, B. D. Chernomordik, D. T. Moore, J. A. Christians, T. Chakrabarti, and J. M. Luther, “Quantum dot-induced phase stabilization of α-CsPbI3 perovskite for high-efficiency photovoltaics,” Science 354(6308), 92–95 (2016).
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V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H. Eisler, and M. G. Bawendi, “Optical gain and stimulated emission in nanocrystal quantum dots,” Science 290(5490), 314–317 (2000).
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A. V. Malko, A. A. Mikhailovsky, M. A. Petruska, J. A. Hollingsworth, H. Htoon, M. G. Bawendi, and V. I. Klimov, “From amplified spontaneous emission to microring lasing using nanocrystal quantum dot solids,” Appl. Phys. Lett. 81(7), 1303–1305 (2002).
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C. Y. Huang, C. Zou, C. Mao, K. L. Corp, Y. C. Yao, Y. J. Lee, C. W. Schlenker, A. K. Y. Jen, and L. Y. Lin, “CsPbBr3 perovskite quantum dot vertical cavity lasers with low threshold and high stability,” ACS Photonics 4(9), 2281–2289 (2017).
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A. Swarnkar, A. R. Marshall, E. M. Sanehira, B. D. Chernomordik, D. T. Moore, J. A. Christians, T. Chakrabarti, and J. M. Luther, “Quantum dot-induced phase stabilization of α-CsPbI3 perovskite for high-efficiency photovoltaics,” Science 354(6308), 92–95 (2016).
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Y. Wang, X. Li, V. Nalla, H. Zeng, and H. Sun, “Solution-processed low threshold vertical cavity surface emitting lasers from all-inorganic perovskite nanocrystals,” Adv. Funct. Mater. 27(13), 1605088 (2017).
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P. T. Snee, Y. H. Chan, D. G. Nocera, and M. G. Bawendi, “Whispering-gallery-mode lasing from a semiconductor nanocrystal/microsphere resonator composite,” Adv. Mater. 17(9), 1131–1136 (2005).
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J. H. Im, C. R. Lee, J. W. Lee, S. W. Park, and N. G. Park, “6.5% efficient perovskite quantum-dot-sensitized solar cell,” Nanoscale 3(10), 4088–4093 (2011).
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R. K. Ratnesh and M. S. Mehata, “Investigation of biocompatible and protein sensitive highly luminescent quantum dots/nanocrystals of CdSe, CdSe/ZnS and CdSe/CdS,” Spectrochim. Acta A Mol. Biomol. Spectrosc. 179, 201–210 (2017).
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X. Li, Y. Wang, H. Sun, and H. Zeng, “Amino-mediated anchoring perovskite quantum dots for stable and low-threshold random lasing,” Adv. Mater. 29(36), 1701185 (2017).
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A. Swarnkar, A. R. Marshall, E. M. Sanehira, B. D. Chernomordik, D. T. Moore, J. A. Christians, T. Chakrabarti, and J. M. Luther, “Quantum dot-induced phase stabilization of α-CsPbI3 perovskite for high-efficiency photovoltaics,” Science 354(6308), 92–95 (2016).
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S. T. Selvan, T. T. Tan, and J. Y. Ying, “Robust, non-cytotoxic, silica-coated CdSe quantum cots with efficient photoluminescence,” Adv. Mater. 17(13), 1620–1625 (2005).
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Figures (4)

Fig. 1
Fig. 1 (a) Schematic of the CsPbBr3-SiO2 formation. (b) TEM image of pure CsPbBr3 QDs. The scale bar is 50 nm. (c) TEM image of single CsPbBr3/SiO2 sphere. The scale bar is 1 μm. (d) Magnified TEM image at edge of CsPbBr3-SiO2 sphere embedded by an ocean of QDs. The scale bar is 100 nm. (e) XRD patterns of the CsPbBr3, and CsPbBr3-SiO2 sphere, respectively. (f) UV−vis extinction and PL emission spectrum of CsPbBr3 (blue color) QDs and CsPbBr3-SiO2 (red color) sphere, respectively.
Fig. 2
Fig. 2 (a) EDS of the CsPbBr3-SiO2 sphere. (b)-(d) Element mapping images obtained from EDS for elements Cs, Pb, and Br, respectively. All the scale bar is 500 nm.
Fig. 3
Fig. 3 (a) Schematic diagram for measuring CsPbBr3-SiO2 QDs lasing. The green circle and gradient arrows indicate the light propagation inside the cavity. (b) Emission spectra with increasing pump intensity under two-photon excitation. The inset shows the magnified view of the lasing spectra and the arrow indicates a regular peak with slight blue shift. (c) Log–log plot of the output intensity as a function of pump intensity.
Fig. 4
Fig. 4 (a) Lasing image of a cylindrical microtubule incorporated with CsPbBr3/SiO2 QDs. The inset shows the WGM supported by the micro-ring resonator. (b) Emission spectra with increasing pump intensity. (c) Log–log plot of the output integral intensity as a function of pump intensity. (d) Lasing modes estimated with the WGM model. (e) Gauss fitting of a selected lasing peak with FWHM ~0.35 nm, corresponding Q ~1532. (f) Lasing intensity as a function of operated time or excitation shots under 800 nm.

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