Abstract

We have studied the two- and three-photon absorption (2PA and 3PA) properties of Mn-doped CsPbCl3 two-dimensional nanoplatelets (2D NPs) and cubic nanocrystals. Compared with their cubic counterparts, the Mn-doped 2D NPs exhibit stronger quantum confinement effects that can more efficiently enhance their dopant-carrier exchange interactions and multiphoton absorption. More specifically, the maximum volume-normalized 2PA and 3PA cross sections of the 2D NPs were 6.8 and 7.2 times greater than those of their cubic counterparts, respectively, reaching up to 1237  GM/nm3 in the visible light band and 2.24×1078  cm6·s2·photon2/nm3 in the second biological window, respectively.

© 2018 Chinese Laser Press

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References

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    [Crossref]
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2018 (8)

Q. A. Akkerman, G. Rainò, M. V. Kovalenko, and L. Manna, “Genesis, challenges and opportunities for colloidal lead halide perovskite nanocrystals,” Nat. Mater. 17, 394–405 (2018).
[Crossref]

X. X. Sheng, G. Y. Chen, C. Wang, W. Q. Wang, J. F. Hui, Q. Zhang, K. H. Yu, W. Wei, M. D. Yi, M. Zhang, Y. Deng, P. Wang, X. X. Xu, Z. H. Dai, J. C. Bao, and X. Wang, “Polarized optoelectronics of CsPbX3 (X = Cl, Br, I) perovskite nanoplates with tunable size and thickness,” Adv. Funct. Mater. 28, 1800283 (2018).
[Crossref]

J. Li, C. Ren, X. Qiu, X. Lin, R. Chen, C. Yin, and T. He, “Ultrafast optical nonlinearity of blue-emitting perovskite nanocrystals,” Photon. Res. 6, 554–559 (2018).
[Crossref]

J. Yao, J. Ge, B. Han, K. Wang, H. Yao, H. Yu, J. Li, B. Zhu, J. Song, C. Chen, Q. Zhang, H. Zeng, Y. Luo, and S. Yu, “Ce3+-doping to modulate photoluminescence kinetics for efficient CsPbBr3 nanocrystals based light-emitting diodes,” J. Am. Chem. Soc. 140, 3626–3634 (2018).
[Crossref]

T. He, C. Ren, Z. Li, S. Xiao, J. Li, X. Lin, C. Ye, J. Zhang, L. Guo, W. Hu, and R. Chen, “Thermally activated delayed fluorescence organic dots for two-photon fluorescence lifetime imaging,” Appl. Phys. Lett. 112, 211102 (2018).
[Crossref]

Y. Dong, T. Qiao, D. Kim, D. Parobek, D. Rossi, and D. H. Son, “Precise control of quantum confinement in cesium lead halide perovskite quantum dots via thermodynamic equilibrium,” Nano Lett. 18, 3716–3722 (2018).
[Crossref]

B. J. Bohn, Y. Tong, M. Gramlich, M. L. Lai, M. Döblinger, K. Wang, R. L. Z. Hoye, P. Müller-Buschbaum, S. D. Stranks, A. S. Urban, L. Polavarapu, and J. Feldmann, “Boosting tunable blue luminescence of halide perovskite nanoplatelets through postsynthetic surface trap repair,” Nano Lett. 18, 5231–5238 (2018).
[Crossref]

T. He, J. Li, X. Qiu, S. Xia, C. Yin, and X. Lin, “Highly enhanced normalized-volume multiphoton absorption in CsPbBr3 2D nanoplates,” Adv. Opt. Mater. 2018, 1800843 (2018).
[Crossref]

2017 (14)

C. Huang, Y. G. Shuai, W. Zhang, N. Yia, S. Xiao, and Q. Song, “Giant blueshifts of excitonic resonances in two-dimensional lead halide perovskite,” Nano Energy 41, 320–326 (2017).
[Crossref]

O. Saouma, C. C. Stoumpos, J. Wong, M. G. Kanatzidis, and J. I. Jang, “Selective enhancement of optical nonlinearity in two-dimensional organic-inorganic lead iodide perovskites,” Nat. Commun. 8, 742 (2017).
[Crossref]

J. Butkus, P. Vashishtha, K. Chen, J. K. Gallaher, S. K. K. Prasad, D. Z. Metin, G. Laufersky, N. Gaston, J. E. Halpert, and J. M. Hodgkiss, “The evolution of quantum confinement in CsPbBr3 perovskite nanocrystals,” Chem. Mater. 29, 3644–3652 (2017).
[Crossref]

D. Rossi, D. Parobek, Y. Dong, and D. H. Son, “Dynamics of exciton-Mn energy transfer in Mn-doped CsPbCl3 perovskite nanocrystals,” J. Phys. Chem. C 121, 17143–17149 (2017).
[Crossref]

S. Das Adhikari, S. K. Dutta, A. Dutta, A. K. Guria, and N. Pradhan, “Chemically tailoring the dopant emission in manganese-doped CsPbCl3 perovskite nanocrystals,” Angew. Chem. (Int. Ed.) 56, 8746–8750 (2017).
[Crossref]

T. He, J. Li, C. Ren, S. Xiao, Y. Li, R. Chen, and X. Lin, “Strong two-photon absorption of Mn-doped CsPbCl3 perovskite nanocrystals,” Appl. Phys. Lett. 111, 211105 (2017).
[Crossref]

J. Chen, K. Žídek, P. Chábera, D. Liu, P. Cheng, L. Nuuttila, M. J. Al-Marri, H. Lehtivuori, M. E. Messing, K. Han, K. Zheng, and T. Pullerits, “Size- and wavelength-dependent two-photon absorption cross-section of CsPbBr3 perovskite quantum dots,” J. Phys. Chem. Lett. 8, 2316–2321 (2017).
[Crossref]

J. Zhu, X. Yang, Y. Zhu, Y. Wang, J. Cai, J. Shen, L. Sun, and C. Li, “Room-temperature synthesis of Mn-doped cesium lead halide quantum dots with high Mn substitution ratio,” J. Phys. Chem. Lett. 8, 4167–4171 (2017).
[Crossref]

W. J. Mir, M. Jagadeeswararao, S. Das, and A. Nag, “Colloidal Mn-doped cesium lead halide perovskite nanoplatelets,” ACS Energy Lett. 2, 537–543 (2017).
[Crossref]

A. Swarnkar, V. Kumar Ravi, and A. Nag, “Beyond colloidal cesium lead halide perovskite nanocrystals: analogous metal halides and doping,” ACS Energy Lett. 2, 1089–1098 (2017).
[Crossref]

J. Chen, P. Chábera, T. Pascher, M. E. Messing, R. Schaller, S. Canton, K. Zheng, and T. Pullerits, “Enhanced size selection in two-photon excitation for CsPbBr3 perovskite nanocrystals,” J. Phys. Chem. Lett. 8, 5119–5124 (2017).
[Crossref]

J. Kang and L. Wang, “High defect tolerance in lead halide perovskite CsPbBr3,” J. Phys. Chem. Lett. 8, 489–493 (2017).
[Crossref]

T. He, J. Li, X. Li, C. Ren, Y. Luo, F. Zhao, R. Chen, X. Lin, and J. Zhang, “Spectroscopic studies of chiral perovskite nanocrystals,” Appl. Phys. Lett. 111, 151102 (2017).
[Crossref]

I. Levchuk, A. Osvet, X. Tang, M. Brandl, J. D. Perea, F. Hoegl, G. J. Matt, R. Hock, M. Batentschuk, and C. J. Brabec, “Brightly luminescent and color-tunable formamidinium lead halide perovskite FAPbX3 (X = Cl, Br, I) colloidal nanocrystals,” Nano Lett. 17, 2765–2770 (2017).
[Crossref]

2016 (3)

X. Li, Y. Wu, S. Zhang, B. Cai, Y. Cui, J. Song, and H. Zeng, “CsPbX3 quantum dots for lighting and displays: room-temperature synthesis, photoluminescence superiorities, underlying origins and white light-emitting diodes,” Adv. Funct. Mater. 26, 2435–2445 (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, 448–453 (2016).
[Crossref]

D. Parobek, B. J. Roman, Y. Dong, H. Jin, E. Lee, M. Sheldon, and D. H. Son, “Exciton-to-dopant energy transfer in Mn-doped cesium lead halide perovskite nanocrystals,” Nano Lett. 16, 7376–7380 (2016).
[Crossref]

2015 (5)

L. Protesescu, S. Yakunin, M. I. Bodnarchuk, F. Krieg, R. Caputo, C. H. Hendon, R. X. Yang, A. Walsh, and M. V. Kovalenko, “Nanocrystals of cesium lead halide perovskites (CsPbX3, X=Cl, Br, and I): novel optoelectronic materials showing bright emission with wide color gamut,” Nano Lett. 15, 3692–3696 (2015).
[Crossref]

R. Scott, A. W. Achtstein, A. Prudnikau, A. Antanovich, S. Christodoulou, I. Moreels, M. Artemyev, and U. Woggon, “Two photon absorption in II-VI semiconductors: the influence of dimensionality and size,” Nano Lett. 15, 4985–4992 (2015).
[Crossref]

A. W. Achtstein, A. Antanovich, A. Prudnikau, R. Scott, U. Woggon, and M. Artemyev, “Linear absorption in CdSe nanoplates: thickness and lateral size dependency of the intrinsic absorption,” J. Phys. Chem. C 119, 20156–20161 (2015).
[Crossref]

A. W. Achtstein, A. Ballester, J. L. Movilla, J. Hennig, J. I. Climente, A. Prudnikau, A. Antanovich, R. Scott, M. V. Artemyev, J. Planelles, and U. Woggon, “One- and two-photon absorption in CdS nanodots and wires: the role of dimensionality in the one- and two-photon luminescence excitation spectrum,” J. Phys. Chem. C 119, 1260–1267 (2015).
[Crossref]

A. K. Mandal, S. Sreejith, T. He, S. K. Maji, X. Wang, S. L. Ong, J. Joseph, H. Sun, and Y. Zhao, “Three-photon-excited luminescence from unsymmetrical cyanostilbene aggregates: morphology tuning and targeted bioimaging,” ACS Nano 9, 4796–4805 (2015).
[Crossref]

2014 (1)

T. He, R. Chen, Z. B. Lim, D. Rajwar, L. Ma, Y. Wang, Y. Gao, A. C. Grimsdale, and H. Sun, “Efficient energy transfer under two-photon excitation in a 3D, supramolecular, Zn(II)-coordinated, self-assembled organic network,” Adv. Opt. Mater. 2, 40–47 (2014).
[Crossref]

2013 (3)

P. Wu and X. Yan, “Doped quantum dots for chemo/biosensing and bioimaging,” Chem. Soc. Rev. 42, 5489–5521 (2013).
[Crossref]

R. Subha, V. Nalla, J. H. Yu, S. W. Jun, K. Shin, T. Hyeon, C. Vijayan, and W. Ji, “Efficient photoluminescence of Mn2+-doped ZnS quantum dots excited by two-photon absorption in near-infrared window II,” J. Phys. Chem. C 117, 20905–20911 (2013).
[Crossref]

J. H. Yu, S. Kwon, Z. Petrášek, O. K. Park, S. Woojoo Jun, K. Shin, M. Choi, Y. Il Park, K. Park, H. B. Na, N. Lee, D. W. Lee, J. H. Kim, P. Schwille, and T. Hyeon, “High-resolution three-photon biomedical imaging using doped ZnS nanocrystals,” Nat. Mater. 12, 359–366 (2013).
[Crossref]

2012 (1)

J. Qian, D. Wang, F. Cai, W. Xi, L. Peng, Z. Zhu, H. He, M. Hu, and S. He, “Observation of multiphoton-induced fluorescence from graphene oxide nanoparticles and applications in vivo functional bioimaging,” Angew. Chem. (Int. Ed.) 51, 10570–10575 (2012).
[Crossref]

2011 (1)

L. A. Padilha, G. Nootz, P. D. Olszak, S. Webster, D. J. Hagan, E. W. Van Stryland, L. Levina, V. Sukhovatkin, L. Brzozowski, and E. H. Sargent, “Optimization of band structure and quantum-size-effect tuning for two-photon absorption enhancement in quantum dots,” Nano Lett. 11, 1227–1231 (2011).
[Crossref]

2008 (1)

G. S. He, L. S. Tan, Q. Zheng, and P. N. Prasad, “Multiphoton absorbing materials: molecular designs, characterizations, and applications,” Chem. Rev. 108, 1245–1330 (2008).
[Crossref]

2007 (1)

R. S. S. Kumar, S. V. Rao, L. Giribabu, and D. N. Rao, “Femtosecond and nanosecond nonlinear optical properties of alkyl phthalocyanines studied using Z-scan technique,” Chem. Phys. Lett. 447, 274–278 (2007).
[Crossref]

1995 (2)

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, 760–769 (1990).
[Crossref]

Achtstein, A. W.

R. Scott, A. W. Achtstein, A. Prudnikau, A. Antanovich, S. Christodoulou, I. Moreels, M. Artemyev, and U. Woggon, “Two photon absorption in II-VI semiconductors: the influence of dimensionality and size,” Nano Lett. 15, 4985–4992 (2015).
[Crossref]

A. W. Achtstein, A. Antanovich, A. Prudnikau, R. Scott, U. Woggon, and M. Artemyev, “Linear absorption in CdSe nanoplates: thickness and lateral size dependency of the intrinsic absorption,” J. Phys. Chem. C 119, 20156–20161 (2015).
[Crossref]

A. W. Achtstein, A. Ballester, J. L. Movilla, J. Hennig, J. I. Climente, A. Prudnikau, A. Antanovich, R. Scott, M. V. Artemyev, J. Planelles, and U. Woggon, “One- and two-photon absorption in CdS nanodots and wires: the role of dimensionality in the one- and two-photon luminescence excitation spectrum,” J. Phys. Chem. C 119, 1260–1267 (2015).
[Crossref]

Akkerman, Q. A.

Q. A. Akkerman, G. Rainò, M. V. Kovalenko, and L. Manna, “Genesis, challenges and opportunities for colloidal lead halide perovskite nanocrystals,” Nat. Mater. 17, 394–405 (2018).
[Crossref]

Al-Marri, M. J.

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Adv. Opt. Mater. (2)

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Figures (6)

Fig. 1.
Fig. 1. HR-TEM micrographs depicting the atomic resolution of both (a) flat-lying and stacked Mn-doped CsPbCl3 2D NPs and (b) cubic NCs. Subfigures (c), (d), and (e) show the distribution of the lengths, widths, and thicknesses of the 2D NPs, respectively, while (f) shows the edge size distribution of the cubic NCs.
Fig. 2.
Fig. 2. (a) UV-vis absorption and PL spectra of the 2D NPs and the cubic NCs. (b) Time-dependent PL intensity of Mn2+ at 592 nm measured from the 2D NPs and the cubic NCs. The insets show their colloidal solutions under UV illumination (λ=365  nm).
Fig. 3.
Fig. 3. (a) fs-TA data for the Mn-doped 2D NPs and cubic NCs pumped at 350 nm. (b) Recovery curves of the bleaching process at 383 nm for the 2D NPs and that at 387 nm for the cubic NCs. (c), (d) The excitation-intensity-dependent GSB signal amplitude at a time delay of 1 ns is shown for the 2D NPs and the cubic NCs. The curves are the best fit lines calculated based on Eq. (5).
Fig. 4.
Fig. 4. (a) PL spectra for the 2D NPs and cubic NCs excited by fs pulses at 680 nm. The inset shows the PL emissions of the 2D NPs and cubic NCs. (b) PL intensity versus excitation intensity with log–log plot slopes of 1.95 and 2.02, respectively. (c) 2PA and linear absorption spectra of the 2D NPs and cubic NCs plotted over the two- and one-photon energies. (d) Photo-induced energy transfer process from the host (CsPbCl3) to Mn2+ in the Mn-doped 2D NPs and cubic NCs under two-photon excitation.
Fig. 5.
Fig. 5. (a) PL spectra for the 2D NPs and cubic NCs excited by fs pulses at 1300 nm. The inset shows the PL emissions of the Mn-doped 2D NPs and cubic NCs. (b) PL intensity of the 2D NPs and cubic NCs versus the optical intensity with log–log plot slopes of 2.98 and 3.02, respectively. (c) 3PA spectra of the 2D NPs and cubic NCs. The inset shows solutions of the 2D NPs and cubic NCs in a pure host (CsPbCl3) under the same excitation intensity used for the inset of (a). (d) One-photon excitation spectra of the 2D NPs and cubic NCs detected at 592 nm. The inset shows the direct 3PA process from the A16 state to the T14 state in the Mn2+ of the 2D NPs and cubic NCs.
Fig. 6.
Fig. 6. Comparison of the maximum VN 2PA and 3PA cross sections of Mn-doped CsPbCl3 2D NPs and cubic NCs, as well as Mn-doped ZnS spherical NCs.

Equations (5)

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ΔT(2PA)=11+α2(1eα0Lα0){I0/[1+(z/z0)2]},
ΔT(3PA)=1{1+2α3(1e2α0L2α0){I0/[1+(z/z0)2]}2}0.5,
σ2=α2hνNAd0×103,
σ3=α3(hν)2NAd0×103.
A(I/I0)=Amax[1e(I/I0)·σlin·I0],

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