Abstract

Black phosphorus (BP) has recently attracted significant attention for its brilliant physical and chemical features. The remarkable strong light-matter interaction and tunable direct wide range band-gap make it an ideal candidate in various application regions, especially saturable absorbers. In this paper, ultrasmall black phosphorus quantum dots (BPQDs), a unique form of phosphorus nanostructures, with average size of 5.7 ± 0.8 nm are synthesized. Compared with BP nanosheets (BPNs) with similar thickness, the ultrafast nonlinear optical (NLO) absorption properties and excited carrier dynamics are investigated in wide spectra. Beyond the saturation absorption (SA), giant two photon absorption (TPA) is observed in BPQDs. BPQDs exhibit quite different excitation intensity and wavelength dependent nonlinear optical (NLO) response from BPNs, which is attributed to the quantum confinement and edge effects. The BPQDs show broadband photon-induced absorption (PIA) under the probe wavelength from 470 nm to 850 nm and a fast and a slow decay time are obtained as long as 92 ± 10 ps and 1100 ± 100 ps, respectively. The substantial independence for ultra-long time scales of pump intensity and temperature reveals that the carrier recombination mechanism may be attributed to a defect-assisted Auger capture process. These findings will help to develop optoelectronic and photonic devices operating in the infrared and visible wavelength region.

© 2017 Optical Society of America

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2016 (9)

D. Mao, B. Du, D. Yang, S. Zhang, Y. Wang, W. Zhang, X. She, H. Cheng, H. Zeng, and J. Zhao, “Nonlinear saturable absorption of liquid-exfoliated molybdenum/tungsten ditelluride nanosheets,” Small 12(11), 1489–1497 (2016).
[Crossref] [PubMed]

Y. Xu, Z. Wang, Z. Guo, H. Huang, Q. Xiao, H. Zhang, and X. Yu, “Solvothermal synthesis and ultrafast photonics of black phosphorus quantum dots,” Adv. Opt. Mater. 4(8), 1223–1229 (2016).
[Crossref]

K. Wang, B. M. Szydłowska, G. Wang, X. Zhang, J. J. Wang, J. J. Magan, L. Zhang, J. N. Coleman, J. Wang, and W. J. Blau, “Ultrafast nonlinear excitation dynamics of black phosphorus nanosheets from visible to mid-infrared,” ACS Nano 10(7), 6923–6932 (2016).
[Crossref] [PubMed]

L. Kong, Z. Qin, G. Xie, Z. Guo, H. Zhang, P. Yuan, and L. Qian, “Black phosphorus as broadband saturable absorber for pulsed lasers from 1 μm to 2.7 μm wavelength,” Laser Phys. Lett. 13(4), 045801 (2016).
[Crossref]

R. Long, W. Fang, and A. V. Akimov, “Nonradiative electron–hole recombination rate is greatly reduced by defects in monolayer black phosphorus: Ab initio time domain study,” J. Phys. Chem. Lett. 7(4), 653–659 (2016).
[Crossref] [PubMed]

X. Niu, Y. Li, H. Shu, and J. Wang, “Anomalous size dependence of optical properties in black phosphorus quantum dots,” J. Phys. Chem. Lett. 7(3), 370–375 (2016).
[Crossref] [PubMed]

K. Wei, X. Zheng, X. Cheng, C. Shen, and T. Jiang, “Observation of ultrafast exciton–exciton annihilation in CsPbBr3 quantum dots,” Adv. Opt. Mater.  4(12), 1993–1997 (2016).

H. Yu, X. Zheng, K. Yin, X. Cheng, and T. Jiang, “Nanosecond passively Q-switched thulium/holmium-doped fiber laser based on black phosphorus nanoplatelets,” Opt. Mater. Express 6(2), 603–609 (2016).
[Crossref]

R. Chen, Y. Tang, X. Zheng, and T. Jiang, “Giant nonlinear absorption and excited carrier dynamics of black phosphorus few-layer nanosheets in broadband spectra,” Appl. Opt. 55(36), 10307–10312 (2016).
[Crossref] [PubMed]

2015 (11)

S. B. Lu, L. L. Miao, Z. N. Guo, X. Qi, C. J. Zhao, H. Zhang, S. C. Wen, D. Y. Tang, and D. Y. Fan, “Broadband nonlinear optical response in multi-layer black phosphorus: an emerging infrared and mid-infrared optical material,” Opt. Express 23(9), 11183–11194 (2015).
[Crossref] [PubMed]

X. Zheng, R. Chen, G. Shi, J. Zhang, Z. Xu, X. Cheng, and T. Jiang, “Characterization of nonlinear properties of black phosphorus nanoplatelets with femtosecond pulsed Z-scan measurements,” Opt. Lett. 40(15), 3480–3483 (2015).
[Crossref] [PubMed]

A. A. Bui, A. B. Stilgoe, N. Khatibzadeh, T. A. Nieminen, M. W. Berns, and H. Rubinsztein-Dunlop, “Escape forces and trajectories in optical tweezers and their effect on calibration,” Opt. Express 23(19), 24317–24330 (2015).
[Crossref] [PubMed]

H. Yu, X. Zheng, K. Yin, X. Cheng, and T. Jiang, “Thulium/holmium-doped fiber laser passively mode locked by black phosphorus nanoplatelets-based saturable absorber,” Appl. Opt. 54(34), 10290–10294 (2015).
[Crossref] [PubMed]

S. Zhang, N. Dong, N. McEvoy, M. O’Brien, S. Winters, N. C. Berner, C. Yim, Y. Li, X. Zhang, Z. Chen, L. Zhang, G. S. Duesberg, and J. Wang, “Direct observation of degenerate two-photon absorption and its saturation in WS2 and MoS2 monolayer and few-layer films,” ACS Nano 9(7), 7142–7150 (2015).
[Crossref] [PubMed]

J. He, D. He, Y. Wang, Q. Cui, M. Z. Bellus, H. Y. Chiu, and H. Zhao, “Exceptional and anisotropic transport properties of photocarriers in black phosphorus,” ACS Nano 9(6), 6436–6442 (2015).
[Crossref] [PubMed]

S. Ge, C. Li, Z. Zhang, C. Zhang, Y. Zhang, J. Qiu, Q. Wang, J. Liu, S. Jia, J. Feng, and D. Sun, “Dynamical evolution of anisotropic response in black phosphorus under ultrafast photoexcitation,” Nano Lett. 15(7), 4650–4656 (2015).
[Crossref] [PubMed]

H. R. Mu, S. H. Lin, Z. C. Wang, S. Xiao, P. F. Li, Y. Chen, H. Zhang, H. F. Bao, S. P. Lau, C. X. Pan, D. Y. Fan, and Q. L. Bao, “Black phosphorus–polymer composites for pulsed lasers,” Adv. Opt. Mater. 3(10), 1447–1453 (2015).
[Crossref]

Y. Wang, G. Huang, H. Mu, S. Lin, J. Chen, S. Xiao, Q. Bao, and J. He, “Ultrafast recovery time and broadband saturable absorption properties of black phosphorus suspension,” Appl. Phys. Lett. 107(9), 091905 (2015).
[Crossref]

D. Hanlon, C. Backes, E. Doherty, C. S. Cucinotta, N. C. Berner, C. Boland, K. Lee, A. Harvey, P. Lynch, Z. Gholamvand, S. Zhang, K. Wang, G. Moynihan, A. Pokle, Q. M. Ramasse, N. McEvoy, W. J. Blau, J. Wang, G. Abellan, F. Hauke, A. Hirsch, S. Sanvito, D. D. O’Regan, G. S. Duesberg, V. Nicolosi, and J. N. Coleman, “Liquid exfoliation of solvent-stabilized few-layer black phosphorus for applications beyond electronics,” Nat. Commun. 6, 8563 (2015).
[Crossref] [PubMed]

Z. Sun, H. Xie, S. Tang, X. F. Yu, Z. Guo, J. Shao, H. Zhang, H. Huang, H. Wang, and P. K. Chu, “Ultrasmall black phosphorus quantum dots: Synthesis and use as photothermal agents,” Angew. Chem. Int. Ed. Engl. 54(39), 11526–11530 (2015).
[Crossref] [PubMed]

2014 (4)

L. Li, Y. Yu, G. J. Ye, Q. Ge, X. Ou, H. Wu, D. Feng, X. H. Chen, and Y. Zhang, “Black phosphorus field-effect transistors,” Nat. Nanotechnol. 9(5), 372–377 (2014).
[Crossref] [PubMed]

H. O. H. Churchill and P. Jarillo-Herrero, “Two-dimensional crystals: Phosphorus joins the family,” Nat. Nanotechnol. 9(5), 330–331 (2014).
[Crossref] [PubMed]

J. Dai and X. C. Zeng, “Bilayer phosphorene: effect of stacking order on bandgap and its potential applications in thin-film solar cells,” J. Phys. Chem. Lett. 5(7), 1289–1293 (2014).
[Crossref] [PubMed]

L. Kou, T. Frauenheim, and C. Chen, “Phosphorene as a superior gas sensor: Selective adsorption and distinct I–V response,” J. Phys. Chem. Lett. 5(15), 2675–2681 (2014).
[Crossref] [PubMed]

2013 (2)

K. Wang, J. Wang, J. Fan, M. Lotya, A. O’Neill, D. Fox, Y. Feng, X. Zhang, B. Jiang, Q. Zhao, H. Zhang, J. N. Coleman, L. Zhang, and W. J. Blau, “Ultrafast saturable absorption of two-dimensional MoS2 nanosheets,” ACS Nano 7(10), 9260–9267 (2013).
[Crossref] [PubMed]

L. Britnell, R. M. Ribeiro, A. Eckmann, R. Jalil, B. D. Belle, A. Mishchenko, Y. J. Kim, R. V. Gorbachev, T. Georgiou, S. V. Morozov, A. N. Grigorenko, A. K. Geim, C. Casiraghi, A. H. Castro Neto, and K. S. Novoselov, “Strong light-matter interactions in heterostructures of atomically thin films,” Science 340(6138), 1311–1314 (2013).
[Crossref] [PubMed]

2012 (1)

X. Huang, X. Qi, F. Boey, and H. Zhang, “Graphene-based composites,” Chem. Soc. Rev. 41(2), 666–686 (2012).
[Crossref] [PubMed]

2009 (1)

K. A. Ritter, J. W. Lyding, F. Fossard, A. L. P. Heureux, N. Y.-W. Tang, P. L. Lévesque, A. Loiseau, R. Leonelli, S. Francoeur, and R. Martel, “The influence of edge structure on the electronic properties of graphene quantum dots and nanoribbons,” Nat. Mater. 8(3), 235–242 (2009).
[Crossref] [PubMed]

2008 (1)

J. A. McGuire, J. Joo, J. M. Pietryga, R. D. Schaller, and V. I. Klimov, “New aspects of carrier multiplication in semiconductor nanocrystals,” Acc. Chem. Res. 41(12), 1810–1819 (2008).
[Crossref] [PubMed]

2005 (1)

K. S. Novoselov, A. K. Geim, S. V. Morozov, D. Jiang, M. I. Katsnelson, I. V. Grigorieva, S. V. Dubonos, and A. A. Firsov, “Two-dimensional gas of massless Dirac fermions in graphene,” Nature 438(7065), 197–200 (2005).
[Crossref] [PubMed]

1991 (1)

M. Baba, Y. Nakamura, K. Shibata, and A. Morita, “Photoconduction of black phosphorus in the infrared region,” J. Appl. Phys. 30(2), 1178 (1991).
[Crossref]

1990 (1)

M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26(4), 760–769 (1990).
[Crossref]

1985 (1)

S. Schmitt-Rink, D. S. Chemla, and D. A. Miller, “Theory of transient excitonic optical nonlinearities in semiconductor quantum-well structures,” Phys. Rev. B Condens. Matter 32(10), 6601–6609 (1985).
[Crossref] [PubMed]

1980 (1)

D. J. Robbins and P. T. Landsberg, “Impact ionisation and auger recombination involving traps in semiconductors,” J. Phys. C Solid State Phys. 13(12), 2425–2439 (1980).
[Crossref]

1963 (1)

D. Warschauer, “Electrical and optical properties of crystalline black phosphorus,” J. Appl. Phys. 34(7), 1853–1860 (1963).
[Crossref]

1960 (1)

M. Lax, “Cascade capture of electrons in solids,” Phys. Rev. 119(5), 1502–1523 (1960).
[Crossref]

Abellan, G.

D. Hanlon, C. Backes, E. Doherty, C. S. Cucinotta, N. C. Berner, C. Boland, K. Lee, A. Harvey, P. Lynch, Z. Gholamvand, S. Zhang, K. Wang, G. Moynihan, A. Pokle, Q. M. Ramasse, N. McEvoy, W. J. Blau, J. Wang, G. Abellan, F. Hauke, A. Hirsch, S. Sanvito, D. D. O’Regan, G. S. Duesberg, V. Nicolosi, and J. N. Coleman, “Liquid exfoliation of solvent-stabilized few-layer black phosphorus for applications beyond electronics,” Nat. Commun. 6, 8563 (2015).
[Crossref] [PubMed]

Akimov, A. V.

R. Long, W. Fang, and A. V. Akimov, “Nonradiative electron–hole recombination rate is greatly reduced by defects in monolayer black phosphorus: Ab initio time domain study,” J. Phys. Chem. Lett. 7(4), 653–659 (2016).
[Crossref] [PubMed]

Baba, M.

M. Baba, Y. Nakamura, K. Shibata, and A. Morita, “Photoconduction of black phosphorus in the infrared region,” J. Appl. Phys. 30(2), 1178 (1991).
[Crossref]

Backes, C.

D. Hanlon, C. Backes, E. Doherty, C. S. Cucinotta, N. C. Berner, C. Boland, K. Lee, A. Harvey, P. Lynch, Z. Gholamvand, S. Zhang, K. Wang, G. Moynihan, A. Pokle, Q. M. Ramasse, N. McEvoy, W. J. Blau, J. Wang, G. Abellan, F. Hauke, A. Hirsch, S. Sanvito, D. D. O’Regan, G. S. Duesberg, V. Nicolosi, and J. N. Coleman, “Liquid exfoliation of solvent-stabilized few-layer black phosphorus for applications beyond electronics,” Nat. Commun. 6, 8563 (2015).
[Crossref] [PubMed]

Bao, H. F.

H. R. Mu, S. H. Lin, Z. C. Wang, S. Xiao, P. F. Li, Y. Chen, H. Zhang, H. F. Bao, S. P. Lau, C. X. Pan, D. Y. Fan, and Q. L. Bao, “Black phosphorus–polymer composites for pulsed lasers,” Adv. Opt. Mater. 3(10), 1447–1453 (2015).
[Crossref]

Bao, Q.

Y. Wang, G. Huang, H. Mu, S. Lin, J. Chen, S. Xiao, Q. Bao, and J. He, “Ultrafast recovery time and broadband saturable absorption properties of black phosphorus suspension,” Appl. Phys. Lett. 107(9), 091905 (2015).
[Crossref]

Bao, Q. L.

H. R. Mu, S. H. Lin, Z. C. Wang, S. Xiao, P. F. Li, Y. Chen, H. Zhang, H. F. Bao, S. P. Lau, C. X. Pan, D. Y. Fan, and Q. L. Bao, “Black phosphorus–polymer composites for pulsed lasers,” Adv. Opt. Mater. 3(10), 1447–1453 (2015).
[Crossref]

Belle, B. D.

L. Britnell, R. M. Ribeiro, A. Eckmann, R. Jalil, B. D. Belle, A. Mishchenko, Y. J. Kim, R. V. Gorbachev, T. Georgiou, S. V. Morozov, A. N. Grigorenko, A. K. Geim, C. Casiraghi, A. H. Castro Neto, and K. S. Novoselov, “Strong light-matter interactions in heterostructures of atomically thin films,” Science 340(6138), 1311–1314 (2013).
[Crossref] [PubMed]

Bellus, M. Z.

J. He, D. He, Y. Wang, Q. Cui, M. Z. Bellus, H. Y. Chiu, and H. Zhao, “Exceptional and anisotropic transport properties of photocarriers in black phosphorus,” ACS Nano 9(6), 6436–6442 (2015).
[Crossref] [PubMed]

Berner, N. C.

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M. Sheik-Bahae, A. A. Said, T. H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26(4), 760–769 (1990).
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Y. Xu, Z. Wang, Z. Guo, H. Huang, Q. Xiao, H. Zhang, and X. Yu, “Solvothermal synthesis and ultrafast photonics of black phosphorus quantum dots,” Adv. Opt. Mater. 4(8), 1223–1229 (2016).
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L. Li, Y. Yu, G. J. Ye, Q. Ge, X. Ou, H. Wu, D. Feng, X. H. Chen, and Y. Zhang, “Black phosphorus field-effect transistors,” Nat. Nanotechnol. 9(5), 372–377 (2014).
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Yu, H.

Yu, X.

Y. Xu, Z. Wang, Z. Guo, H. Huang, Q. Xiao, H. Zhang, and X. Yu, “Solvothermal synthesis and ultrafast photonics of black phosphorus quantum dots,” Adv. Opt. Mater. 4(8), 1223–1229 (2016).
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Z. Sun, H. Xie, S. Tang, X. F. Yu, Z. Guo, J. Shao, H. Zhang, H. Huang, H. Wang, and P. K. Chu, “Ultrasmall black phosphorus quantum dots: Synthesis and use as photothermal agents,” Angew. Chem. Int. Ed. Engl. 54(39), 11526–11530 (2015).
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L. Li, Y. Yu, G. J. Ye, Q. Ge, X. Ou, H. Wu, D. Feng, X. H. Chen, and Y. Zhang, “Black phosphorus field-effect transistors,” Nat. Nanotechnol. 9(5), 372–377 (2014).
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L. Kong, Z. Qin, G. Xie, Z. Guo, H. Zhang, P. Yuan, and L. Qian, “Black phosphorus as broadband saturable absorber for pulsed lasers from 1 μm to 2.7 μm wavelength,” Laser Phys. Lett. 13(4), 045801 (2016).
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[Crossref]

Z. Sun, H. Xie, S. Tang, X. F. Yu, Z. Guo, J. Shao, H. Zhang, H. Huang, H. Wang, and P. K. Chu, “Ultrasmall black phosphorus quantum dots: Synthesis and use as photothermal agents,” Angew. Chem. Int. Ed. Engl. 54(39), 11526–11530 (2015).
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[Crossref] [PubMed]

S. Zhang, N. Dong, N. McEvoy, M. O’Brien, S. Winters, N. C. Berner, C. Yim, Y. Li, X. Zhang, Z. Chen, L. Zhang, G. S. Duesberg, and J. Wang, “Direct observation of degenerate two-photon absorption and its saturation in WS2 and MoS2 monolayer and few-layer films,” ACS Nano 9(7), 7142–7150 (2015).
[Crossref] [PubMed]

K. Wang, J. Wang, J. Fan, M. Lotya, A. O’Neill, D. Fox, Y. Feng, X. Zhang, B. Jiang, Q. Zhao, H. Zhang, J. N. Coleman, L. Zhang, and W. J. Blau, “Ultrafast saturable absorption of two-dimensional MoS2 nanosheets,” ACS Nano 7(10), 9260–9267 (2013).
[Crossref] [PubMed]

Zhang, S.

D. Mao, B. Du, D. Yang, S. Zhang, Y. Wang, W. Zhang, X. She, H. Cheng, H. Zeng, and J. Zhao, “Nonlinear saturable absorption of liquid-exfoliated molybdenum/tungsten ditelluride nanosheets,” Small 12(11), 1489–1497 (2016).
[Crossref] [PubMed]

S. Zhang, N. Dong, N. McEvoy, M. O’Brien, S. Winters, N. C. Berner, C. Yim, Y. Li, X. Zhang, Z. Chen, L. Zhang, G. S. Duesberg, and J. Wang, “Direct observation of degenerate two-photon absorption and its saturation in WS2 and MoS2 monolayer and few-layer films,” ACS Nano 9(7), 7142–7150 (2015).
[Crossref] [PubMed]

D. Hanlon, C. Backes, E. Doherty, C. S. Cucinotta, N. C. Berner, C. Boland, K. Lee, A. Harvey, P. Lynch, Z. Gholamvand, S. Zhang, K. Wang, G. Moynihan, A. Pokle, Q. M. Ramasse, N. McEvoy, W. J. Blau, J. Wang, G. Abellan, F. Hauke, A. Hirsch, S. Sanvito, D. D. O’Regan, G. S. Duesberg, V. Nicolosi, and J. N. Coleman, “Liquid exfoliation of solvent-stabilized few-layer black phosphorus for applications beyond electronics,” Nat. Commun. 6, 8563 (2015).
[Crossref] [PubMed]

Zhang, W.

D. Mao, B. Du, D. Yang, S. Zhang, Y. Wang, W. Zhang, X. She, H. Cheng, H. Zeng, and J. Zhao, “Nonlinear saturable absorption of liquid-exfoliated molybdenum/tungsten ditelluride nanosheets,” Small 12(11), 1489–1497 (2016).
[Crossref] [PubMed]

Zhang, X.

K. Wang, B. M. Szydłowska, G. Wang, X. Zhang, J. J. Wang, J. J. Magan, L. Zhang, J. N. Coleman, J. Wang, and W. J. Blau, “Ultrafast nonlinear excitation dynamics of black phosphorus nanosheets from visible to mid-infrared,” ACS Nano 10(7), 6923–6932 (2016).
[Crossref] [PubMed]

S. Zhang, N. Dong, N. McEvoy, M. O’Brien, S. Winters, N. C. Berner, C. Yim, Y. Li, X. Zhang, Z. Chen, L. Zhang, G. S. Duesberg, and J. Wang, “Direct observation of degenerate two-photon absorption and its saturation in WS2 and MoS2 monolayer and few-layer films,” ACS Nano 9(7), 7142–7150 (2015).
[Crossref] [PubMed]

K. Wang, J. Wang, J. Fan, M. Lotya, A. O’Neill, D. Fox, Y. Feng, X. Zhang, B. Jiang, Q. Zhao, H. Zhang, J. N. Coleman, L. Zhang, and W. J. Blau, “Ultrafast saturable absorption of two-dimensional MoS2 nanosheets,” ACS Nano 7(10), 9260–9267 (2013).
[Crossref] [PubMed]

Zhang, Y.

S. Ge, C. Li, Z. Zhang, C. Zhang, Y. Zhang, J. Qiu, Q. Wang, J. Liu, S. Jia, J. Feng, and D. Sun, “Dynamical evolution of anisotropic response in black phosphorus under ultrafast photoexcitation,” Nano Lett. 15(7), 4650–4656 (2015).
[Crossref] [PubMed]

L. Li, Y. Yu, G. J. Ye, Q. Ge, X. Ou, H. Wu, D. Feng, X. H. Chen, and Y. Zhang, “Black phosphorus field-effect transistors,” Nat. Nanotechnol. 9(5), 372–377 (2014).
[Crossref] [PubMed]

Zhang, Z.

S. Ge, C. Li, Z. Zhang, C. Zhang, Y. Zhang, J. Qiu, Q. Wang, J. Liu, S. Jia, J. Feng, and D. Sun, “Dynamical evolution of anisotropic response in black phosphorus under ultrafast photoexcitation,” Nano Lett. 15(7), 4650–4656 (2015).
[Crossref] [PubMed]

Zhao, C. J.

Zhao, H.

J. He, D. He, Y. Wang, Q. Cui, M. Z. Bellus, H. Y. Chiu, and H. Zhao, “Exceptional and anisotropic transport properties of photocarriers in black phosphorus,” ACS Nano 9(6), 6436–6442 (2015).
[Crossref] [PubMed]

Zhao, J.

D. Mao, B. Du, D. Yang, S. Zhang, Y. Wang, W. Zhang, X. She, H. Cheng, H. Zeng, and J. Zhao, “Nonlinear saturable absorption of liquid-exfoliated molybdenum/tungsten ditelluride nanosheets,” Small 12(11), 1489–1497 (2016).
[Crossref] [PubMed]

Zhao, Q.

K. Wang, J. Wang, J. Fan, M. Lotya, A. O’Neill, D. Fox, Y. Feng, X. Zhang, B. Jiang, Q. Zhao, H. Zhang, J. N. Coleman, L. Zhang, and W. J. Blau, “Ultrafast saturable absorption of two-dimensional MoS2 nanosheets,” ACS Nano 7(10), 9260–9267 (2013).
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Zheng, X.

Acc. Chem. Res. (1)

J. A. McGuire, J. Joo, J. M. Pietryga, R. D. Schaller, and V. I. Klimov, “New aspects of carrier multiplication in semiconductor nanocrystals,” Acc. Chem. Res. 41(12), 1810–1819 (2008).
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ACS Nano (4)

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Figures (6)

Fig. 1
Fig. 1 TEM of the (a) BPQDs and (b) BPNs. Insets are photographs of BPQDs and BPNs in glass vials, respectively. (c) AFM image of BPQDs. (d) Height profile of the red line marked in (c). (e) Statistical analysis of the height of 85 BPQDs determined by AFM. (f) Magnified TEM image. (g) Statistical analysis of the sizes of 100 BPQDs measured from TEM images (h) UV/Vis Absorbance spectrum of BPQDs prepared in this paper. Raman spectra of (i) BPQDs and (j) BPNs [15].
Fig. 2
Fig. 2 (a) OA Z-Scan results for BPQDs, Inset: the photograph of the laser spot at focus. The scatters are experimental data and the solid lines show theoretical fit generated by the theory of Z-scan. (b) NLO absorption coefficient under different excitation irradiance at 1160 nm of BPQDs. Inset: Schematic of TPA process in BPQDs.
Fig. 3
Fig. 3 Schematics of the single photon SA process of BPNs under the excitation of 1160 nm pulsed laser at (a) low excitation irradiance, (b) middle excitation irradiance, (c) high excitation energy and the schematics of TPA process of BPQDs under the excitation of 1160 nm pulsed laser at (d) low excitation irradiance, (e) middle excitation irradiance and (f) high excitation energy.
Fig. 4
Fig. 4 Z-Scan results of BPQDs at (a) 800nm, (b) 1300nm, (c) 1550nm and (d) 2μm pulsed laser under different excitation irradiances. The scatters are experimental data and the solid lines show theoretical fit.
Fig. 5
Fig. 5 (a) Differential absorption (ΔA/A0) map of BPQDs as a function of both delay time and probe photon wavelength with a pump wavelength of 400 nm at average power of 500 μW (pump fluence = 160 μJ/cm2) and probe with the supercontinum white light at the temperature of 77 K. (b) Time evolution of the photon-induced differential absorption (ΔA/A0) as a function of probe delay at wavelength of 545 nm, 601 nm, 657 nm and 716 nm. Inset: Max value of ΔA/A0 as the function of probe photon wavelength, showing that ΔA/A0 is strongest when the probe photon wavelength is ~546 nm (2.27 eV). (c) ΔA/A0 measured with pump power from 200μW to 800μW (pump fluence from 64 to 256 μJ/cm2). The red arrow points out the pump power increasing direction. The inset shows a linear relation between the peak signal and the pump intensity. (d) Schematic of the photon-induced intraband absorption process of BPQDs in pump-probe experiments.
Fig. 6
Fig. 6 (a) Carrier lifetime of BPQDs (exciton recombination time) under different pump power at the temperature of 77K. Inset: ΔA/A0 spectra of BPQDs under different temperature, showing a redshift of the spectra peak with the increasing temperature. (b) Carrier lifetime of BPQDs at different experimental temperature, where the pump power is 200 μW (pump fluence = 64 μJ/cm2). (c) shows three different temporal regions: (1) ΔA/A0 reaches its positive maximum value within ~3 ps. (2) A fast decay of the positive ΔA/A0 then occurs within ~100 ps. (3) Finally, a slow decay of the positive ΔA/A0 lasts for more than 1000 ps. (d) Schematic of defect-assisted Auger carrier capture process in the two temporal regions: (1) After photoexcitation, the carriers thermalize and cool and form a correlated electron−hole plasma. (2) Most of the holes and the electrons are captured by the fast defects within 100 ps time scale. (3) After all the photoexcited holes have been captured and the electrons have filled the traps completely, the direct and indirect electron-hole radiative recombination process then domains and lasts more than 1000 ps.

Tables (1)

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Table 1 Linear and NLO absorption coefficients of BPNs [15] and BPQDs Using Z-Scan Technique

Equations (3)

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T open (z)=1 1 2 2 α NL I 0 L eff 1+ (z/ z 0 ) 2
E abs =1.46+0.30/ r 2 +1.31/r
Im χ 3 = 10 7 cλ n 2 96 π 2 α NL

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