Abstract

Black phosphorus (BP), a typical mono-elemental and two-dimensional (2D) material, has gathered significant attention owing to its distinct optoelectronic properties and promising applications, despite its main obstacle of long-term stability. Consequently, BP-analog materials with long-term chemical stability show additional potential. In this contribution, tin sulfide (SnS), a novel two-elemental and 2D structural BP-analog monochalcogenide, has been demonstrated to show enhanced stability under ambient conditions. The broadband nonlinear optical properties and carrier dynamics have been systematically investigated via Z-scan and transient absorption approaches. The excellent nonlinear absorption coefficient of 50.5×103  cm/GW, 1 order of magnitude larger than that of BP, endows the promising application of SnS in ultrafast laser generation. Two different decay times of τ1873  fs and τ296.9  ps allow the alteration between pure Q switching and continuous-wave (CW) mode locking in an identical laser resonator. Both mode-locked and Q-switched operations have been experimentally demonstrated using an SnS saturable absorber at the telecommunication window. Femtosecond laser pulses with tunable wavelength and high stability are easily obtained, suggesting the promising potential of SnS as an efficient optical modulator for ultrafast photonics. This primary investigation may be considered an important step towards stable and high-performance BP-analog material-based photonic devices.

© 2019 Chinese Laser Press

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2018 (11)

S. Tan, I. Abdelwahab, L. Chu, S. M. Poh, Y. Liu, J. Lu, W. Chen, and K. P. Loh, “Quasi-monolayer black phosphorus with high mobility and air stability,” Adv. Mater. 30, 1704619 (2018).
[Crossref]

M. Qiu, D. Wang, W. Liang, L. Liu, Y. Zhang, X. Chen, D. K. Sang, C. Xing, Z. Li, and B. Dong, “Novel concept of the smart NIR-light-controlled drug release of black phosphorus nanostructure for cancer therapy,” Proc. Natl. Acad. Sci. 115, 501–506 (2018).
[Crossref]

C. Chang, M. Wu, D. He, Y. Pei, C. Wu, X. Wu, H. Yu, F. Zhu, K. Wang, Y. Chen, and L. Huang, “3D charge and 2D phonon transports leading to high out-of-plane ZT in N-type SnSe crystals,” Science 360, 778–783 (2018).
[Crossref]

Z. Xie, D. Wang, T. Fan, C. Xing, Z. Li, W. Tao, L. Liu, D. Fan, and H. Zhang, “Black phosphorus analogue tin sulfide nanosheets: synthesis and application as near-infrared photothermal agents and drug delivery platforms for cancer therapy,” J. Mater. Chem. B 6, 4747–4755 (2018).
[Crossref]

S. Hwang, Z. Yao, L. Zhang, M. Fu, K. He, L. Mai, C. Wolverton, and D. Su, “Multistep lithiation of tin sulfide: an investigation using in situ electron microscopy,” ACS Nano 12, 3638–3645 (2018).
[Crossref]

H. Wu, X. Lu, G. Wang, K. Peng, H. Chi, B. Zhang, Y. Chen, C. Li, Y. Yan, L. Guo, and C. Uher, “Sodium-doped tin sulfide single crystal: a nontoxic earth-abundant material with high thermoelectric performance,” Adv. Energy Mater. 8, 1800087 (2018).
[Crossref]

K. Szendrei‐Temesi, O. Sanchez‐Sobrado, S. B. Betzler, K. M. Durner, T. Holzmann, and B. V. Lotsch, “Lithium tin sulfide—a high‐refractive‐index 2D material for humidity‐responsive photonic crystals,” Adv. Funct. Mater. 28, 1705740 (2018).
[Crossref]

H. Wang, D. Chao, J. Liu, J. Lin, and Z. Shen, “Nanoengineering of 2D tin sulfide nanoflake arrays incorporated on polyaniline nanofibers with boosted capacitive behavior,” 2D Mater. 5, 031005 (2018).
[Crossref]

W. Cheng, N. Singh, W. Elliott, J. Lee, A. Rassoolkhani, X. Jin, E. W. Mcfarland, and S. Mubeen, “Earth‐abundant tin sulfide‐based photocathodes for solar hydrogen production,” Adv. Sci. 5, 1700362 (2018).
[Crossref]

X. Jiang, S. Liu, W. Liang, S. Luo, Z. He, Y. Ge, H. Wang, R. Cao, F. Zhang, and Q. Wen, “Broadband nonlinear photonics in few‐layer MXene Ti3C2Tx (T = F, O, or OH),” Laser Photon. Rev. 12, 1700229 (2018).
[Crossref]

L. Lu, Z. Liang, L. Wu, Y. X. Chen, Y. Song, S. C. Dhanabalan, J. S. Ponraj, B. Dong, Y. Xiang, and F. Xing, “Few‐layer bismuthene: sonochemical exfoliation, nonlinear optics and applications for ultrafast photonics with enhanced stability,” Laser Photon. Rev. 12, 1700221 (2018).
[Crossref]

2017 (8)

Y. Song, Z. Liang, X. Jiang, Y. Chen, Z. Li, L. Lu, Y. Ge, K. Wang, J. Zheng, and S. Lu, “Few-layer antimonene decorated microfiber: ultra-short pulse generation and all-optical thresholding with enhanced long term stability,” 2D Mater. 4, 045010 (2017).
[Crossref]

C. Xing, Z. Xie, Z. Liang, W. Liang, T. Fan, J. S. Ponraj, S. C. Dhanabalan, D. Fan, and H. Zhang, “Selenium nanosets: 2D nonlayered selenium nanosheets: facile synthesis, photoluminescence, and ultrafast photonics,” Adv. Opt. Mater. 5, 1700884 (2017).
[Crossref]

C. Zhu, F. Wang, Y. Meng, X. Yuan, F. Xiu, H. Luo, Y. Wang, J. Li, X. Lv, and L. He, “A robust and tuneable mid-infrared optical switch enabled by bulk Dirac fermions,” Nat. Commun. 8, 14111 (2017).
[Crossref]

L. Peng, C. Wang, Q. Qian, C. Bi, S. Wang, and Y. Huang, “Complete separation of carriers in the GeS/SnS lateral heterostructure by uniaxial tensile strain,” ACS Appl. Mater. Interfaces 9, 40969–40977 (2017).
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C. Xing, G. Jing, X. Liang, M. Qiu, Z. Li, R. Cao, X. Li, D. Fan, and H. Zhang, “Graphene oxide/black phosphorus nanoflake aerogels with robust thermo-stability and significantly enhanced photothermal properties in air,” Nanoscale 9, 8096–8101 (2017).
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T. Xian, W. Liang, J. Zhao, Z. Li, Q. Meng, T. Fan, C. S. Luo, Z. Ye, L. Yu, and Z. Guo, “Fluorinated phosphorene: electrochemical synthesis, atomistic fluorination, and enhanced stability,” Small 13, 1702739 (2017).
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Y. Zhao, Q. Zhou, Q. Li, X. Yao, and J. Wang, “Passivation of black phosphorus via self-assembled organic monolayers by van der Waals epitaxy,” Adv. Mater. 29, 1603990 (2017).
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Z. Guo, S. Chen, Z. Wang, Z. Yang, F. Liu, Y. Xu, J. Wang, Y. Yi, H. Zhang, and L. Liao, “Metal-ion-modified black phosphorus with enhanced stability and transistor performance,” Adv. Mater. 29, 1703811 (2017).
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2016 (14)

C. R. Ryder, J. D. Wood, S. A. Wells, Y. Yang, D. Jariwala, T. J. Marks, G. C. Schatz, and M. C. Hersam, “Covalent functionalization and passivation of exfoliated black phosphorus via aryl diazonium chemistry,” Nat. Chem. 8, 597–602 (2016).
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Y. Zhao, H. Wang, H. Huang, Q. Xiao, Y. Xu, Z. Guo, H. Xie, J. Shao, Z. Sun, and W. Han, “Surface coordination of black phosphorus for robust air and water stability,” Angew. Chemie 55, 5003–5007 (2016).
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S. Lin, S. Liu, Z. Yang, Y. Li, T. W. Ng, Z. Xu, Q. Bao, J. Hao, C. Lee, and C. Surya, “Solution‐processable ultrathin black phosphorus as an effective electron transport layer in organic photovoltaics,” Adv. Funct. Mater. 26, 864–871 (2016).
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D. Li, A. E. D. R. Castillo, H. Jussila, G. Ye, Z. Ren, J. Bai, X. Chen, H. Lipsanen, Z. Sun, and F. Bonaccorso, “Black phosphorus polycarbonate polymer composite for pulsed fibre lasers,” Appl. Mater. Today 4, 17–23 (2016).
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S. Zhang, N. Wang, S. Liu, S. Huang, W. Zhou, B. Cai, M. Xie, Q. Yang, X. Chen, and H. Zeng, “Two-dimensional GeS with tunable electronic properties via external electric field and strain,” Nanotechnology 27, 274001 (2016).
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C. Xin, J. Zheng, Y. Su, S. Li, B. Zhang, Y. Feng, and F. Pan, “Few-layer tin sulfide: a new black-phosphorus-analogue 2D material with a sizeable band gap, odd–even quantum confinement effect, and high carrier mobility,” J. Phys. Chem. C 120, 22663–22669 (2016).
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Z. Tian, C. Guo, M. Zhao, R. Li, and J. Xue, “Two-dimensional SnS: a phosphorene analogue with strong in-plane electronic anisotropy,” ACS Nano 11, 2219–2226 (2016).
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A. Rodin, L. Gomes, A. Carvalho, and A. Castro Neto, “Valley physics in tin (II) sulfide,” Phys. Rev. B 93, 045431 (2016).
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M. Wu and X. C. Zeng, “Intrinsic ferroelasticity and/or multiferroicity in two-dimensional phosphorene and phosphorene analogues,” Nano Lett. 16, 3236–3241 (2016).
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R. Fei, W. Kang, and L. Yang, “Ferroelectricity and phase transitions in monolayer group-IV monochalcogenides,” Phys. Rev. Lett. 117, 097601 (2016).
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J. Xia, D. Zhu, X. Li, L. Wang, L. Tian, J. Li, J. Wang, X. Huang, and X. Meng, “Epitaxy of layered orthorhombic SnS–SnSxSe(1–x) core–shell heterostructures with anisotropic photoresponse,” Adv. Funct. Mater. 26, 4673–4679 (2016).
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C. B. de Araújo, A. S. Gomes, and G. Boudebs, “Techniques for nonlinear optical characterization of materials: a review,” Rep. Prog. Phys. Phys. Soc. 79, 036401 (2016).
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E. Sani and A. Dell’Oro, “Spectral optical constants of ethanol and isopropanol from ultraviolet to far infrared,” Opt. Mater. (Amsterdam) 60, 137–141 (2016).
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J. Ma, H. Huang, K. Ning, X. Xu, G. Xie, L. Qian, K. P. Loh, and D. Tang, “Generation of 30  fs pulses from a diode-pumped graphene mode-locked Yb:CaYAlO4 laser,” Opt. Lett. 41, 890–893 (2016).
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2015 (15)

Y. Chen, G. Jiang, S. Chen, Z. Guo, X. Yu, C. Zhao, H. Zhang, Q. Bao, S. Wen, and D. Tang, “Mechanically exfoliated black phosphorus as a new saturable absorber for both Q-switching and mode-locking laser operation,” Opt. Express 23, 12823–12833 (2015).
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P. Sinsermsuksakul, L. Sun, S. W. Lee, H. H. Park, S. B. Kim, C. Yang, and R. G. Gordon, “Overcoming efficiency limitations of SnS‐based solar cells,” Adv. Energy Mater. 4, 1400496 (2015).
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L. D. Zhao, G. Tan, S. Hao, J. He, Y. Pei, H. Chi, H. Wang, S. Gong, H. Xu, and V. P. Dravid, “Ultrahigh power factor and thermoelectric performance in hole-doped single-crystal SnSe,” Science 351, 141–144 (2015).
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N. K. Reddy, M. Devika, and E. S. R. Gopal, “Review on tin (II) sulfide (SnS) material: synthesis, properties, and applications,” Crit. Rev. Solid State Mater. Sci. 40, 1–37 (2015).
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J. R. Brent, D. J. Lewis, T. Lorenz, E. A. Lewis, N. Savjani, S. J. Haigh, G. Seifert, B. Derby, and P. O’Brien, “Tin(II) sulfide (SnS) nanosheets by liquid-phase exfoliation of herzenbergite: IV-VI main group two-dimensional atomic crystals,” J. Am. Chem. Soc. 137, 12689–12696 (2015).
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M. Mehboudi, A. M. Dorio, W. Zhu, Zande, A. van der Zande, H. O. H. Churchill, A. A. Pachecosanjuan, E. O. Harriss, P. Kumar, and S. Barrazalopez, “Two-dimensional disorder in black phosphorus and monochalcogenide monolayers,” Nano Lett. 16, 1704–1712 (2015).
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R. Fei, W. Li, J. Li, and L. Yang, “Giant piezoelectricity of monolayer group IV monochalcogenides,” Appl. Phys. Lett. 107, 173104 (2015).
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J. Xia, X. Z. Li, X. Huang, N. Mao, D. D. Zhu, L. Wang, H. Xu, and X. M. Meng, “Physical vapor deposition synthesis of two-dimensional orthorhombic SnS flakes with strong angle/temperature-dependent Raman responses,” Nanoscale 8, 2063–2070 (2015).
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C. Zhao, D. Fan, D. Tang, G. Jiang, H. Zhang, Q. Bao, S. Wen, S. Chen, X. Yu, and Y. Chen, “Mechanically exfoliated black phosphorus as a new saturable absorber for both Q-switching and mode-locking laser operation,” Opt. Express 23, 12823–12833 (2015).
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H. Mu, S. Lin, Z. Wang, S. Xiao, P. Li, Y. Chen, H. Zhang, H. Bao, P. L. Shu, and C. Pan, “Pulsed lasers: black phosphorus–polymer composites for pulsed lasers,” Adv. Opt. Mater. 3, 1447–1453 (2015).
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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, 091905 (2015).
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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, 11183–11194 (2015).
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R. A. Doganov, E. C. O’Farrell, S. P. Koenig, Y. Yeo, A. Ziletti, A. Carvalho, D. K. Campbell, D. F. Coker, K. Watanabe, and T. Taniguchi, “Transport properties of pristine few-layer black phosphorus by van der Waals passivation in an inert atmosphere,” Nat. Commun. 6, 6647 (2015).
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A. Favron, E. Gaufrès, F. Fossard, A. L. Phaneuf-L’Heureux, Y. W. Tang, P. L. Lévesque, A. Loiseau, R. Leonelli, S. Francoeur, and R. Martel, “Photooxidation and quantum confinement effects in exfoliated black phosphorus,” Nat. Mater. 14, 826–832 (2015).
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A. Avsar, I. J. Veramarun, J. Y. Tan, K. Watanabe, T. Taniguchi, A. H. C. Neto, and B. Özyilmaz, “Air-stable transport in graphene-contacted, fully encapsulated ultrathin black phosphorus-based field-effect transistors,” ACS Nano 9, 4138–4145 (2015).
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2014 (16)

J. D. Wood, S. A. Wells, D. Jariwala, K. S. Chen, E. Cho, V. K. Sangwan, X. Liu, L. J. Lauhon, T. J. Marks, and M. C. Hersam, “Effective passivation of exfoliated black phosphorus transistors against ambient degradation,” Nano Lett. 14, 6964–6970 (2014).
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M. Buscema, D. J. Groenendijk, S. I. Blanter, G. A. Steele, H. S. J. van der Zant, and A. Castellanosgomez, “Fast and broadband photoresponse of few-layer black phosphorus field-effect transistors,” Nano Lett. 14, 3347–3352 (2014).
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X. Chen, Y. Wu, Z. Wu, Y. Han, S. Xu, L. Wang, W. Ye, T. Han, Y. He, and Y. Cai, “High-quality sandwiched black phosphorus heterostructure and its quantum oscillations,” Nat. Commun. 6, 7315 (2014).
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F. Xia, H. Wang, and Y. Jia, “Rediscovering black phosphorus as an anisotropic layered material for optoelectronics and electronics,” Nat. Commun. 5, 4458 (2014).
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V. Tran, R. Soklaski, Y. Liang, and L. Yang, “Layer-controlled band gap and anisotropic excitons in few-layer black phosphorus,” Phys. Rev. B 89, 235319 (2014).
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J. O. Island, G. A. Steele, H. S. J. van der Zant, and A. Castellanos-Gomez, “Environmental instability of few-layer black phosphorus,” 2D Mater. 2, 11002 (2014).
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A. Castellanosgomez, L. Vicarelli, E. Prada, J. O. Island, K. L. Narasimhaacharya, S. I. Blanter, D. J. Groenendijk, M. Buscema, G. A. Steele, and J. V. Alvarez, “Isolation and characterization of few-layer black phosphorus,” 2D Mater. 1, 25001 (2014).
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S. M. Herron, J. T. Tanskanen, K. E. Roelofs, and S. F. Bent, “Highly textured tin(II) sulfide thin films formed from sheetlike nanocrystal inks,” Chem. Mater. 26, 7106–7113 (2014).
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R. E. Banai, L. A. Burton, S. G. Choi, F. Hofherr, T. Sorgenfrei, A. Walsh, B. To, A. Cröll, and J. R. S. Brownson, “Ellipsometric characterization and density-functional theory analysis of anisotropic optical properties of single-crystal α-SnS,” J. Appl. Phys. 116, 013511 (2014).
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L. D. Zhao, S. H. Lo, Y. Zhang, H. Sun, G. Tan, C. Uher, C. Wolverton, V. P. Dravid, and M. G. Kanatzidis, “Ultralow thermal conductivity and high thermoelectric figure of merit in SnSe crystals,” Nature 508, 373–377 (2014).
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J. Na, Y. T. Lee, J. A. Lim, D. K. Hwang, G. T. Kim, W. K. Choi, and Y. W. Song, “Few-layer black phosphorus field-effect transistors with reduced current fluctuation,” ACS Nano 8, 11753–11762 (2014).
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A. M. Tripathi and S. Mitra, “Tin sulfide (SnS) nanorods: structural, optical and lithium storage property study,” RSC Adv. 4, 10358–10366 (2014).
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V. Steinmann, R. Jaramillo, K. Hartman, R. Chakraborty, R. E. Brandt, J. R. Poindexter, Y. S. Lee, L. Sun, A. Polizzotti, and H. H. Park, “3.88% efficient tin sulfide solar cells using congruent thermal evaporation,” Adv. Mater. 26, 7488–7492 (2014).
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T. Zhou, W. K. Pang, C. Zhang, J. Yang, Z. Chen, H. K. Liu, and Z. Guo, “Enhanced sodium-ion battery performance by structural phase transition from two-dimensional hexagonal-SnS2 to orthorhombic-SnS,” ACS Nano 8, 8323–8333 (2014).
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K. Wang, Y. Ju, J. He, L. Zhang, Y. Chen, W. J. Blau, and J. Wang, “Nonlinear optical propagation in a tandem structure comprising nonlinear absorption and scattering materials,” Appl. Phys. Lett. 104, 021110 (2014).
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S. Wang, H. Yu, H. Zhang, A. Wang, M. Zhao, Y. Chen, L. Mei, and J. Wang, “Broadband few-layer MoS2 saturable absorbers,” Adv. Mater. 26, 3538–3544 (2014).
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2013 (1)

L. Li, Z. Chen, Y. Hu, X. Wang, T. Zhang, W. Chen, and Q. Wang, “Single-layer single-crystalline SnSe nanosheets,” J. Am. Chem. Soc. 135, 1213–1216 (2013).
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2012 (3)

D. Xue, J. Tan, J. Hu, W. Hu, Y. Guo, and L. Wan, “Anisotropic photoresponse properties of single micrometer‐sized GeSe nanosheet,” Adv. Mater. 24, 4528–4533 (2012).
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C. Ruckebusch, M. Sliwa, P. Pernot, Juan, A. De, and R. Tauler, “Comprehensive data analysis of femtosecond transient absorption spectra: a review,” J. Photochem. Photobiol. C Photochem. Rev. 13, 1–27 (2012).
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J. Chao, Z. Wang, X. Xu, Q. Xiang, W. Song, G. Chen, J. Hu, and D. Chen, “Tin sulfide nanoribbons as high performance photoelectrochemical cells, flexible photodetectors and visible-light-driven photocatalysts,” RSC Adv. 3, 2746–2753 (2012).
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2010 (1)

Q. Bao, Z. Han, W. Yu, Z. Ni, Y. Yan, Z. X. Shen, K. P. Loh, and Y. T. Ding, “Atomic‐layer graphene as a saturable absorber for ultrafast pulsed lasers,” Adv. Funct. Mater. 19, 3077–3083 (2010).
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2005 (1)

H. Zhu, D. Yang, Y. Ji, Z. Hui, and X. Shen, “Two-dimensional SnS nanosheets fabricated by a novel hydrothermal method,” J. Mater. Sci. 40, 591–595 (2005).
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2003 (1)

U. Keller, “Recent developments in compact ultrafast lasers,” Nature 424, 831–838 (2003).
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2001 (1)

R. Paschotta and U. Keller, “Passive mode locking with slow saturable absorbers,” Appl. Phys. B 73, 653–662 (2001).
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1988 (1)

M. Sharon and K. Basavaswaran, “Photoelectrochemical behaviour of tin monosulphide,” Sol. Cells 25, 97–107 (1988).
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S. Tan, I. Abdelwahab, L. Chu, S. M. Poh, Y. Liu, J. Lu, W. Chen, and K. P. Loh, “Quasi-monolayer black phosphorus with high mobility and air stability,” Adv. Mater. 30, 1704619 (2018).
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Alvarez, J. V.

A. Castellanosgomez, L. Vicarelli, E. Prada, J. O. Island, K. L. Narasimhaacharya, S. I. Blanter, D. J. Groenendijk, M. Buscema, G. A. Steele, and J. V. Alvarez, “Isolation and characterization of few-layer black phosphorus,” 2D Mater. 1, 25001 (2014).
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Avsar, A.

A. Avsar, I. J. Veramarun, J. Y. Tan, K. Watanabe, T. Taniguchi, A. H. C. Neto, and B. Özyilmaz, “Air-stable transport in graphene-contacted, fully encapsulated ultrathin black phosphorus-based field-effect transistors,” ACS Nano 9, 4138–4145 (2015).
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Bai, J.

D. Li, A. E. D. R. Castillo, H. Jussila, G. Ye, Z. Ren, J. Bai, X. Chen, H. Lipsanen, Z. Sun, and F. Bonaccorso, “Black phosphorus polycarbonate polymer composite for pulsed fibre lasers,” Appl. Mater. Today 4, 17–23 (2016).
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Banai, R. E.

R. E. Banai, L. A. Burton, S. G. Choi, F. Hofherr, T. Sorgenfrei, A. Walsh, B. To, A. Cröll, and J. R. S. Brownson, “Ellipsometric characterization and density-functional theory analysis of anisotropic optical properties of single-crystal α-SnS,” J. Appl. Phys. 116, 013511 (2014).
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Bao, H.

H. Mu, S. Lin, Z. Wang, S. Xiao, P. Li, Y. Chen, H. Zhang, H. Bao, P. L. Shu, and C. Pan, “Pulsed lasers: black phosphorus–polymer composites for pulsed lasers,” Adv. Opt. Mater. 3, 1447–1453 (2015).
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Bao, Q.

S. Lin, S. Liu, Z. Yang, Y. Li, T. W. Ng, Z. Xu, Q. Bao, J. Hao, C. Lee, and C. Surya, “Solution‐processable ultrathin black phosphorus as an effective electron transport layer in organic photovoltaics,” Adv. Funct. Mater. 26, 864–871 (2016).
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Y. Chen, G. Jiang, S. Chen, Z. Guo, X. Yu, C. Zhao, H. Zhang, Q. Bao, S. Wen, and D. Tang, “Mechanically exfoliated black phosphorus as a new saturable absorber for both Q-switching and mode-locking laser operation,” Opt. Express 23, 12823–12833 (2015).
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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, 091905 (2015).
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C. Zhao, D. Fan, D. Tang, G. Jiang, H. Zhang, Q. Bao, S. Wen, S. Chen, X. Yu, and Y. Chen, “Mechanically exfoliated black phosphorus as a new saturable absorber for both Q-switching and mode-locking laser operation,” Opt. Express 23, 12823–12833 (2015).
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Q. Bao, Z. Han, W. Yu, Z. Ni, Y. Yan, Z. X. Shen, K. P. Loh, and Y. T. Ding, “Atomic‐layer graphene as a saturable absorber for ultrafast pulsed lasers,” Adv. Funct. Mater. 19, 3077–3083 (2010).
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M. Mehboudi, A. M. Dorio, W. Zhu, Zande, A. van der Zande, H. O. H. Churchill, A. A. Pachecosanjuan, E. O. Harriss, P. Kumar, and S. Barrazalopez, “Two-dimensional disorder in black phosphorus and monochalcogenide monolayers,” Nano Lett. 16, 1704–1712 (2015).
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Basavaswaran, K.

M. Sharon and K. Basavaswaran, “Photoelectrochemical behaviour of tin monosulphide,” Sol. Cells 25, 97–107 (1988).
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Bent, S. F.

S. M. Herron, J. T. Tanskanen, K. E. Roelofs, and S. F. Bent, “Highly textured tin(II) sulfide thin films formed from sheetlike nanocrystal inks,” Chem. Mater. 26, 7106–7113 (2014).
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K. Szendrei‐Temesi, O. Sanchez‐Sobrado, S. B. Betzler, K. M. Durner, T. Holzmann, and B. V. Lotsch, “Lithium tin sulfide—a high‐refractive‐index 2D material for humidity‐responsive photonic crystals,” Adv. Funct. Mater. 28, 1705740 (2018).
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L. Peng, C. Wang, Q. Qian, C. Bi, S. Wang, and Y. Huang, “Complete separation of carriers in the GeS/SnS lateral heterostructure by uniaxial tensile strain,” ACS Appl. Mater. Interfaces 9, 40969–40977 (2017).
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M. Buscema, D. J. Groenendijk, S. I. Blanter, G. A. Steele, H. S. J. van der Zant, and A. Castellanosgomez, “Fast and broadband photoresponse of few-layer black phosphorus field-effect transistors,” Nano Lett. 14, 3347–3352 (2014).
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A. Castellanosgomez, L. Vicarelli, E. Prada, J. O. Island, K. L. Narasimhaacharya, S. I. Blanter, D. J. Groenendijk, M. Buscema, G. A. Steele, and J. V. Alvarez, “Isolation and characterization of few-layer black phosphorus,” 2D Mater. 1, 25001 (2014).
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K. Wang, Y. Ju, J. He, L. Zhang, Y. Chen, W. J. Blau, and J. Wang, “Nonlinear optical propagation in a tandem structure comprising nonlinear absorption and scattering materials,” Appl. Phys. Lett. 104, 021110 (2014).
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D. Li, A. E. D. R. Castillo, H. Jussila, G. Ye, Z. Ren, J. Bai, X. Chen, H. Lipsanen, Z. Sun, and F. Bonaccorso, “Black phosphorus polycarbonate polymer composite for pulsed fibre lasers,” Appl. Mater. Today 4, 17–23 (2016).
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C. B. de Araújo, A. S. Gomes, and G. Boudebs, “Techniques for nonlinear optical characterization of materials: a review,” Rep. Prog. Phys. Phys. Soc. 79, 036401 (2016).
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V. Steinmann, R. Jaramillo, K. Hartman, R. Chakraborty, R. E. Brandt, J. R. Poindexter, Y. S. Lee, L. Sun, A. Polizzotti, and H. H. Park, “3.88% efficient tin sulfide solar cells using congruent thermal evaporation,” Adv. Mater. 26, 7488–7492 (2014).
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J. R. Brent, D. J. Lewis, T. Lorenz, E. A. Lewis, N. Savjani, S. J. Haigh, G. Seifert, B. Derby, and P. O’Brien, “Tin(II) sulfide (SnS) nanosheets by liquid-phase exfoliation of herzenbergite: IV-VI main group two-dimensional atomic crystals,” J. Am. Chem. Soc. 137, 12689–12696 (2015).
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R. E. Banai, L. A. Burton, S. G. Choi, F. Hofherr, T. Sorgenfrei, A. Walsh, B. To, A. Cröll, and J. R. S. Brownson, “Ellipsometric characterization and density-functional theory analysis of anisotropic optical properties of single-crystal α-SnS,” J. Appl. Phys. 116, 013511 (2014).
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R. E. Banai, L. A. Burton, S. G. Choi, F. Hofherr, T. Sorgenfrei, A. Walsh, B. To, A. Cröll, and J. R. S. Brownson, “Ellipsometric characterization and density-functional theory analysis of anisotropic optical properties of single-crystal α-SnS,” J. Appl. Phys. 116, 013511 (2014).
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A. Castellanosgomez, L. Vicarelli, E. Prada, J. O. Island, K. L. Narasimhaacharya, S. I. Blanter, D. J. Groenendijk, M. Buscema, G. A. Steele, and J. V. Alvarez, “Isolation and characterization of few-layer black phosphorus,” 2D Mater. 1, 25001 (2014).
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M. Buscema, D. J. Groenendijk, S. I. Blanter, G. A. Steele, H. S. J. van der Zant, and A. Castellanosgomez, “Fast and broadband photoresponse of few-layer black phosphorus field-effect transistors,” Nano Lett. 14, 3347–3352 (2014).
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Cai, B.

S. Zhang, N. Wang, S. Liu, S. Huang, W. Zhou, B. Cai, M. Xie, Q. Yang, X. Chen, and H. Zeng, “Two-dimensional GeS with tunable electronic properties via external electric field and strain,” Nanotechnology 27, 274001 (2016).
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Cai, Y.

X. Chen, Y. Wu, Z. Wu, Y. Han, S. Xu, L. Wang, W. Ye, T. Han, Y. He, and Y. Cai, “High-quality sandwiched black phosphorus heterostructure and its quantum oscillations,” Nat. Commun. 6, 7315 (2014).
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R. A. Doganov, E. C. O’Farrell, S. P. Koenig, Y. Yeo, A. Ziletti, A. Carvalho, D. K. Campbell, D. F. Coker, K. Watanabe, and T. Taniguchi, “Transport properties of pristine few-layer black phosphorus by van der Waals passivation in an inert atmosphere,” Nat. Commun. 6, 6647 (2015).
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X. Jiang, S. Liu, W. Liang, S. Luo, Z. He, Y. Ge, H. Wang, R. Cao, F. Zhang, and Q. Wen, “Broadband nonlinear photonics in few‐layer MXene Ti3C2Tx (T = F, O, or OH),” Laser Photon. Rev. 12, 1700229 (2018).
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C. Xing, G. Jing, X. Liang, M. Qiu, Z. Li, R. Cao, X. Li, D. Fan, and H. Zhang, “Graphene oxide/black phosphorus nanoflake aerogels with robust thermo-stability and significantly enhanced photothermal properties in air,” Nanoscale 9, 8096–8101 (2017).
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A. Rodin, L. Gomes, A. Carvalho, and A. Castro Neto, “Valley physics in tin (II) sulfide,” Phys. Rev. B 93, 045431 (2016).
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R. A. Doganov, E. C. O’Farrell, S. P. Koenig, Y. Yeo, A. Ziletti, A. Carvalho, D. K. Campbell, D. F. Coker, K. Watanabe, and T. Taniguchi, “Transport properties of pristine few-layer black phosphorus by van der Waals passivation in an inert atmosphere,” Nat. Commun. 6, 6647 (2015).
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Figures (9)

Fig. 1.
Fig. 1. Typical characterizations of the SnS NSs. (a) TEM image; (b) AFM image; (c) crystal lattice shown by HRTEM image and corresponding FFT; (d) crystalline features shown by SAED; (e) XRD pattern; (f) Raman spectra of bulk SnS and exfoliated SnS NSs; (g) element distribution mapping via STEM.
Fig. 2.
Fig. 2. Stability of SnS NSs in ambient conditions characterized by (a) absorbance, (b)XRD, (c) Raman, and (d) XPS spectra, respectively.
Fig. 3.
Fig. 3. (a) Linear optical absorption spectrum of SnS NSs from the UV to NIR region in IPA solution. The baseline of IPA has been removed. (b) Corresponding Tauc plot of the linear optical absorption spectrum.
Fig. 4.
Fig. 4. Normalized transmittance versus z axis at different pulse energies [(a) 800 nm, (c) 1550 nm], and the corresponding intensity-dependent transmittance fitted via a two-level energy model [(b) 800 nm, (d) 1550 nm].
Fig. 5.
Fig. 5. (a) TA spectra of the SnS sample in the time scale of 0–5.0 ps; (b) 2D mapping of the TA spectrum from 1000 to 1500 nm; (c) principal dynamic figured out by singular value decomposition; (d) decay time τ1 and τ2 versus the probe wavelength.
Fig. 6.
Fig. 6. Q-switched pulse trains at different pump powers. (a) 275 mW with repetition rate of 36.36 kHz; (b) 300 mW with repetition rate of 38.91 kHz; (c) 325 mW with repetition rate of 41.32 kHz; (d) 400 mW with repetition rate of 49.43 kHz; (e) 500 mW with repetition rate of 65.19 kHz; (f) long-term stability of the Q-switched state.
Fig. 7.
Fig. 7. (a) Evolution of averaged output power and pulse repetition rate as the pump power increases; (b) RF spectrum under the pump power of 325 mW.
Fig. 8.
Fig. 8. Mode-locked performance. (a) Optical spectrum; (b) pulse train; (c) autocorrelation trace; (d) RF spectrum.
Fig. 9.
Fig. 9. (a) Long-term operation of SnS NSs-based mode locking and (b) its tunable wavelength.

Tables (1)

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Table 1. Value of LT, ΔT, Tns, Is, β, Im χ(3) for SnS@800 nm, 1550 nm and BP@800 nm under the pulse energy of 1.3 μJ/pulse and 1.0 μJ/pulse

Equations (5)

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α=α0+αNL,
Tnorm(z)=ln[1+q0(z)]/q0(z),
I=I0/(1+z2/z02).
T=1ΔT×exp(I/Is)Tns,
ΔA=A1exp(t/τ1)+A2exp(t/τ2),

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