非传统溶液外延法在金属硫化物纳米片表面生长有机无机杂化钙钛矿纳米晶（英文）
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摘要
基于外延异质结构的有机-无机杂化钙钛矿/二维纳米片复合材料在光电领域具有很好的应用前景,但目前使用的固相制备方法大大限制了这一目标的实现.我们通过精细调节溶剂环境,成功利用外延沉积的方式实现了在三角/六方相MoS_2纳米片表面生长立方相MAPbBr_3(MA=CH_3NH~+_3)钙钛矿纳米晶.虽然MAPbBr_3与MoS_2存在较大的晶格不匹配度,但是由于MoS_2纳米片性质柔软且表面缺失悬挂键,可以在两条不同方向上观察到较高容忍度(～1%错位)的外延生长关系.这种外延界面的形成有利于MAPbBr_3与MoS_2之间有效的能量转移,因此基于MAPbBr_3/MoS_2异质结的纸质器件与MAPbBr_3或MoS_2器件相比具有更优异的光电性能.此外,除了提高光吸收能力和能量传递, MoS_2纳米片的存在还为离散的MAPbBr_3纳米晶提供柔性和连续的基底,从而改善了MAPbBr_3纳米晶粒的成膜能力.这种液相外延法可用于高性能的有机无机杂化钙钛矿与二维材料的异质结构材料的大规模制备,将推动异质结构材料在光电领域的广泛使用.
Epitaxial heterostructures based on organicinorganic hybrid perovskites and two-dimensional materials hold great promises in optoelectronics, but they have been prepared only via solid-state methods that restricted their practical applications. Herein, we report cubic-phased MAPbBr_3(MA=CH_3NH_3~+) nanocrystals were epitaxially deposited on trigonal/hexagonal-phased MoS_2 nanosheets in solution by facilely tuning the solvation conditions. In spite of the mismatched lattice symmetry between the square MAPbBr_3(001) overlayer and the hexagonal MoS2(001) substrate, two different aligning directions with lattice mismatch of as small as 1% were observed based on the domainmatching epitaxy. This was realized most likely due to the flexible nature and absence of surface dangling bonds of MoS_2 nanosheets. The formation of the epitaxial interface affords an effective energy transfer from MAPbBr_3 to MoS_2, and as a result, paper-based photodetectors facilely fabricated from these solution-dispersible heterostructures showed better performance compared to those based on MoS_2 or MAPbBr_3 alone. In addition to the improved energy transfer and light adsorption, the use of MoS_2 nanosheets provided flexible and continuous substrates to connect the otherwise discrete MAPbBr_3 nanocrystals and achieved the better film forming ability. Our work suggests that the scalable preparation of heterostructures based on organic-inorganic hybrid perovskites and 2D materials via solution-phase epitaxy may bring about more opportunities for expanding their optoelectronic applications.
Epitaxial heterostructures based on organicinorganic hybrid perovskites and two-dimensional materials hold great promises in optoelectronics, but they have been prepared only via solid-state methods that restricted their practical applications. Herein, we report cubic-phased MAPbBr_3(MA=CH_3NH_3~+) nanocrystals were epitaxially deposited on trigonal/hexagonal-phased MoS_2 nanosheets in solution by facilely tuning the solvation conditions. In spite of the mismatched lattice symmetry between the square MAPbBr_3(001) overlayer and the hexagonal MoS2(001) substrate, two different aligning directions with lattice mismatch of as small as 1% were observed based on the domainmatching epitaxy. This was realized most likely due to the flexible nature and absence of surface dangling bonds of MoS_2 nanosheets. The formation of the epitaxial interface affords an effective energy transfer from MAPbBr_3 to MoS_2, and as a result, paper-based photodetectors facilely fabricated from these solution-dispersible heterostructures showed better performance compared to those based on MoS_2 or MAPbBr_3 alone. In addition to the improved energy transfer and light adsorption, the use of MoS_2 nanosheets provided flexible and continuous substrates to connect the otherwise discrete MAPbBr_3 nanocrystals and achieved the better film forming ability. Our work suggests that the scalable preparation of heterostructures based on organic-inorganic hybrid perovskites and 2D materials via solution-phase epitaxy may bring about more opportunities for expanding their optoelectronic applications.
引文
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2 Huang X,Zeng Z,Zhang H.Metal dichalcogenide nanosheets:preparation,properties and applications.Chem Soc Rev,2013,42:1934-1946
3 Geim AK,Novoselov KS.The rise of graphene.Nat Mater,2007,6:183-191
4 Karunadasa HI,Montalvo E,Sun Y,et al.A molecular MoS2edge site mimic for catalytic hydrogen generation.Science,2012,335:698-702
5 Yu WJ,Li Z,Zhou H,et al.Vertically stacked multi-heterostructures of layered materials for logic transistors and complementary inverters.Nat Mater,2013,12:246-252
6 Yu WJ,Liu Y,Zhou H,et al.Highly efficient gate-tunable photocurrent generation in vertical heterostructures of layered materials.Nat Nanotechnol,2013,8:952-958
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13 Esmaeili-Rad MR,Salahuddin S.High performance molybdenum disulfide amorphous silicon heterojunction photodetector.Sci Rep,2013,3:2345
14 Jariwala D,Sangwan VK,Wu CC,et al.Gate-tunable carbon nanotube-MoS2heterojunction p-n diode.Proc Natl Acad Sci USA,2013,110:18076-18080
15 Noel NK,Stranks SD,Abate A,et al.Lead-free organic-inorganic tin halide perovskites for photovoltaic applications.Energy Environ Sci,2014,7:3061-3068
16 Jeon T,Kim SJ,Yoon J,et al.Hybrid perovskites:effective crystal growth for optoelectronic applications.Adv Energy Mater,2017,7:1602596
17 Sum TC,Mathews N.Advancements in perovskite solar cells:photophysics behind the photovoltaics.Energy Environ Sci,2014,7:2518-2534
18 Yang WS,Noh JH,Jeon NJ,et al.High-performance photovoltaic perovskite layers fabricated through intramolecular exchange.Science,2015,348:1234-1237
19 Chiang CH,Nazeeruddin MK,Gr?tzel M,et al.The synergistic effect of H2O and DMF towards stable and 20%efficiency inverted perovskite solar cells.Energy Environ Sci,2017,10:808-817
20 Saliba M,Matsui T,Domanski K,et al.Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance.Science,2016,354:206-209
21 Xing G,Mathews N,Sun S,et al.Long-range balanced electronand hole-transport lengths in organic-inorganic CH3NH3PbI3.Science,2013,342:344-347
22 Stranks SD,Eperon GE,Grancini G,et al.Electron-hole diffusion lengths exceeding 1 micrometer in an organometal trihalide perovskite absorber.Science,2013,342:341-344
23 Green MA,Ho-Baillie A,Snaith HJ.The emergence of perovskite solar cells.Nat Photonics,2014,8:506-514
24 Schmidt LC,Pertegás A,González-Carrero S,et al.Nontemplate synthesis of CH3NH3PbBr3perovskite nanoparticles.J Am Chem Soc,2014,136:850-853
25 Pathak S,Sakai N,Wisnivesky Rocca Rivarola F,et al.Perovskite crystals for tunable white light emission.Chem Mater,2015,27:8066-8075
26 Gonzalez-Carrero S,Galian RE,Pérez-Prieto J.Maximizing the emissive properties of CH3NH3PbBr3perovskite nanoparticles.JMater Chem A,2015,3:9187-9193
27 Huang H,Zhao F,Liu L,et al.Emulsion synthesis of size-tunable CH3NH3PbBr3quantum dots:an alternative route toward efficient light-emitting diodes.ACS Appl Mater Interfaces,2015,7:28128-28133
28 Zhu F,Men L,Guo Y,et al.Shape evolution and single particle luminescence of organometal halide perovskite nanocrystals.ACSNano,2015,9:2948-2959
29 Jang DM,Kim DH,Park K,et al.Ultrasound synthesis of lead halide perovskite nanocrystals.J Mater Chem C,2016,4:10625-10629
30 Xing J,Yan F,Zhao Y,et al.High-efficiency light-emitting diodes of organometal halide perovskite amorphous nanoparticles.ACSNano,2016,10:6623-6630
31 Im JH,Lee CR,Lee JW,et al.6.5%Efficient perovskite quantumdot-sensitized solar cell.Nanoscale,2011,3:4088-4093
32 Niu L,Liu X,Cong C,et al.Controlled synthesis of organic/inorganic van der Waals solid for tunable light-matter interactions.Adv Mater,2015,27:7800-7808
33 Cheng HC,Wang G,Li D,et al.van der Waals heterojunction devices based on organohalide perovskites and two-dimensional materials.Nano Lett,2015,16:367-373
34 Lu J,Carvalho A,Liu H,et al.Hybrid bilayer WSe2-CH3NH3PbI3organolead halide perovskite as a high-performance photodetector.Angew Chem Int Ed,2016,55:11945-11949
35 Ma C,Shi Y,Hu W,et al.Heterostructured WS2/CH3NH3PbI3photoconductors with suppressed dark current and enhanced photodetectivity.Adv Mater,2016,28:3683-3689
36 Kang DH,Pae SR,Shim J,et al.An ultrahigh-performance photodetector based on a perovskite-transition-metal-dichalcogenide hybrid structure.Adv Mater,2016,28:7799-7806
37 Wang Y,Fullon R,Acerce M,et al.Solution-processed MoS2/organolead trihalide perovskite photodetectors.Adv Mater,2017,29:1603995
38 Zhang F,Zhong H,Chen C,et al.Brightly luminescent and colortunable colloidal CH3NH3PbX3(X=Br,I,Cl)quantum dots:potential alternatives for display technology.ACS Nano,2015,9:4533-4542
39 Zhang F,Huang S,Wang P,et al.Colloidal synthesis of air-stable CH3NH3PbI3quantum dots by gaining chemical insight into the solvent effects.Chem Mater,2017,29:3793-3799
40 Zeng Z,Yin Z,Huang X,et al.Single-layer semiconducting nanosheets:high-yield preparation and device fabrication.Angew Chem Int Ed,2011,50:11093-11097
41 Li H,Wu J,Yin Z,et al.Preparation and applications of mechanically exfoliated single-layer and multilayer MoS2and WSe2nanosheets.Acc Chem Res,2014,47:1067-1075
42 Heising J,Kanatzidis MG.Exfoliated and restacked MoS2and WS2:ionic or neutral species?Encapsulation and ordering of hard Electropositive cations.J Am Chem Soc,1999,121:11720-11732
43 Peng W,Wang L,Murali B,et al.Solution-grown monocrystalline hybrid perovskite films for hole-transporter-free solar cells.Adv Mater,2016,28:3383-3390
44 Brunetti B,Cavallo C,Ciccioli A,et al.On the thermal and thermodynamic(in)stability of methylammonium lead halide perovskites.Sci Rep,2016,6:31896
45 Kappera R,Voiry D,Yalcin SE,et al.Phase-engineered low-resistance contacts for ultrathin MoS2transistors.Nat Mater,2014,13:1128-1134
46 Eda G,Yamaguchi H,Voiry D,et al.Photoluminescence from chemically exfoliated MoS2.Nano Lett,2011,11:5111-5116
47 Voiry D,Salehi M,Silva R,et al.Conducting MoS2nanosheets as catalysts for hydrogen evolution reaction.Nano Lett,2013,13:6222-6227
48 Narayan J,Larson BC.Domain epitaxy:A unified paradigm for thin film growth.J Appl Phys,2003,93:278-285
49 Huang X,Zeng Z,Bao S,et al.Solution-phase epitaxial growth of noble metal nanostructures on dispersible single-layer molybdenum disulfide nanosheets.Nat Commun,2013,4:1444
50 Lin Z,Yin A,Mao J,et al.Scalable solution-phase epitaxial growth of symmetry-mismatched heterostructures on two-dimensional crystal soft template.Sci Adv,2016,2:e1600993
51 Jin M,Zhang H,Wang J,et al.Copper can still be epitaxially deposited on palladium nanocrystals to generate core-shell nanocubes despite their large lattice mismatch.ACS Nano,2012,6:2566-2573
52 Fan FR,Liu DY,Wu YF,et al.Epitaxial growth of heterogeneous metal nanocrystals:from gold nano-octahedra to palladium and silver nanocubes.J Am Chem Soc,2008,130:6949-6951
53 Geim AK,Grigorieva IV.van der Waals heterostructures.Nature,2013,499:419-425
54 Schulz P,Edri E,Kirmayer S,et al.Interface energetics in organometal halide perovskite-based photovoltaic cells.Energy Environ Sci,2014,7:1377-1381
55 Yang D,Yang R,Zhang J,et al.High efficiency flexible perovskite solar cells using superior low temperature TiO2.Energy Environ Sci,2015,8:3208-3214
56 Fang H,Li J,Ding J,et al.An origami perovskite photodetector with spatial recognition ability.ACS Appl Mater Interfaces,2017,9:10921-10928
57 Lin CH,Tsai DS,Wei TC,et al.Highly deformable origami paper photodetector arrays.ACS Nano,2017,11:10230-10235
58 Cai C,Ma Y,Jeon J,et al.Epitaxial growth of large-grain NiSe films by solid-state reaction for high-responsivity photodetector arrays.Adv Mater,2017,29:1606180
59 Lopez-Sanchez O,Lembke D,Kayci M,et al.Ultrasensitive photodetectors based on monolayer MoS2.Nat Nanotechnol,2013,8:497-501
60 Stranks SD,Snaith HJ.Metal-halide perovskites for photovoltaic and light-emitting devices.Nat Nanotechnol,2015,10:391-402
61 Fan X,Xu P,Zhou D,et al.Fast and efficient preparation of exfoliated 2H MoS2nanosheets by sonication-assisted lithium intercalation and infrared laser-induced 1T to 2H phase reversion.Nano Lett,2015,15:5956-5960
2 Huang X,Zeng Z,Zhang H.Metal dichalcogenide nanosheets:preparation,properties and applications.Chem Soc Rev,2013,42:1934-1946
3 Geim AK,Novoselov KS.The rise of graphene.Nat Mater,2007,6:183-191
4 Karunadasa HI,Montalvo E,Sun Y,et al.A molecular MoS2edge site mimic for catalytic hydrogen generation.Science,2012,335:698-702
5 Yu WJ,Li Z,Zhou H,et al.Vertically stacked multi-heterostructures of layered materials for logic transistors and complementary inverters.Nat Mater,2013,12:246-252
6 Yu WJ,Liu Y,Zhou H,et al.Highly efficient gate-tunable photocurrent generation in vertical heterostructures of layered materials.Nat Nanotechnol,2013,8:952-958
7 Amani M,Lien DH,Kiriya D,et al.Near-unity photoluminescence quantum yield in MoS2.Science,2015,350:1065-1068
8 Eda G,Maier SA.Two-dimensional crystals:managing light for optoelectronics.ACS Nano,2013,7:5660-5665
9 Zhang W,Chuu CP,Huang JK,et al.Ultrahigh-gain photodetectors based on atomically thin graphene-MoS2heterostructures.Sci Rep,2014,4:3826
10 Tan H,Xu W,Sheng Y,et al.Lateral graphene-contacted vertically stacked WS2/MoS2hybrid photodetectors with large gain.Adv Mater,2017,29:1702917
11 Lin J,Li H,Zhang H,et al.Plasmonic enhancement of photocurrent in MoS2field-effect-transistor.Appl Phys Lett,2013,102:203109
12 Yu SH,Lee Y,Jang SK,et al.Dye-sensitized MoS2photodetector with enhanced spectral photoresponse.ACS Nano,2014,8:8285-8291
13 Esmaeili-Rad MR,Salahuddin S.High performance molybdenum disulfide amorphous silicon heterojunction photodetector.Sci Rep,2013,3:2345
14 Jariwala D,Sangwan VK,Wu CC,et al.Gate-tunable carbon nanotube-MoS2heterojunction p-n diode.Proc Natl Acad Sci USA,2013,110:18076-18080
15 Noel NK,Stranks SD,Abate A,et al.Lead-free organic-inorganic tin halide perovskites for photovoltaic applications.Energy Environ Sci,2014,7:3061-3068
16 Jeon T,Kim SJ,Yoon J,et al.Hybrid perovskites:effective crystal growth for optoelectronic applications.Adv Energy Mater,2017,7:1602596
17 Sum TC,Mathews N.Advancements in perovskite solar cells:photophysics behind the photovoltaics.Energy Environ Sci,2014,7:2518-2534
18 Yang WS,Noh JH,Jeon NJ,et al.High-performance photovoltaic perovskite layers fabricated through intramolecular exchange.Science,2015,348:1234-1237
19 Chiang CH,Nazeeruddin MK,Gr?tzel M,et al.The synergistic effect of H2O and DMF towards stable and 20%efficiency inverted perovskite solar cells.Energy Environ Sci,2017,10:808-817
20 Saliba M,Matsui T,Domanski K,et al.Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance.Science,2016,354:206-209
21 Xing G,Mathews N,Sun S,et al.Long-range balanced electronand hole-transport lengths in organic-inorganic CH3NH3PbI3.Science,2013,342:344-347
22 Stranks SD,Eperon GE,Grancini G,et al.Electron-hole diffusion lengths exceeding 1 micrometer in an organometal trihalide perovskite absorber.Science,2013,342:341-344
23 Green MA,Ho-Baillie A,Snaith HJ.The emergence of perovskite solar cells.Nat Photonics,2014,8:506-514
24 Schmidt LC,Pertegás A,González-Carrero S,et al.Nontemplate synthesis of CH3NH3PbBr3perovskite nanoparticles.J Am Chem Soc,2014,136:850-853
25 Pathak S,Sakai N,Wisnivesky Rocca Rivarola F,et al.Perovskite crystals for tunable white light emission.Chem Mater,2015,27:8066-8075
26 Gonzalez-Carrero S,Galian RE,Pérez-Prieto J.Maximizing the emissive properties of CH3NH3PbBr3perovskite nanoparticles.JMater Chem A,2015,3:9187-9193
27 Huang H,Zhao F,Liu L,et al.Emulsion synthesis of size-tunable CH3NH3PbBr3quantum dots:an alternative route toward efficient light-emitting diodes.ACS Appl Mater Interfaces,2015,7:28128-28133
28 Zhu F,Men L,Guo Y,et al.Shape evolution and single particle luminescence of organometal halide perovskite nanocrystals.ACSNano,2015,9:2948-2959
29 Jang DM,Kim DH,Park K,et al.Ultrasound synthesis of lead halide perovskite nanocrystals.J Mater Chem C,2016,4:10625-10629
30 Xing J,Yan F,Zhao Y,et al.High-efficiency light-emitting diodes of organometal halide perovskite amorphous nanoparticles.ACSNano,2016,10:6623-6630
31 Im JH,Lee CR,Lee JW,et al.6.5%Efficient perovskite quantumdot-sensitized solar cell.Nanoscale,2011,3:4088-4093
32 Niu L,Liu X,Cong C,et al.Controlled synthesis of organic/inorganic van der Waals solid for tunable light-matter interactions.Adv Mater,2015,27:7800-7808
33 Cheng HC,Wang G,Li D,et al.van der Waals heterojunction devices based on organohalide perovskites and two-dimensional materials.Nano Lett,2015,16:367-373
34 Lu J,Carvalho A,Liu H,et al.Hybrid bilayer WSe2-CH3NH3PbI3organolead halide perovskite as a high-performance photodetector.Angew Chem Int Ed,2016,55:11945-11949
35 Ma C,Shi Y,Hu W,et al.Heterostructured WS2/CH3NH3PbI3photoconductors with suppressed dark current and enhanced photodetectivity.Adv Mater,2016,28:3683-3689
36 Kang DH,Pae SR,Shim J,et al.An ultrahigh-performance photodetector based on a perovskite-transition-metal-dichalcogenide hybrid structure.Adv Mater,2016,28:7799-7806
37 Wang Y,Fullon R,Acerce M,et al.Solution-processed MoS2/organolead trihalide perovskite photodetectors.Adv Mater,2017,29:1603995
38 Zhang F,Zhong H,Chen C,et al.Brightly luminescent and colortunable colloidal CH3NH3PbX3(X=Br,I,Cl)quantum dots:potential alternatives for display technology.ACS Nano,2015,9:4533-4542
39 Zhang F,Huang S,Wang P,et al.Colloidal synthesis of air-stable CH3NH3PbI3quantum dots by gaining chemical insight into the solvent effects.Chem Mater,2017,29:3793-3799
40 Zeng Z,Yin Z,Huang X,et al.Single-layer semiconducting nanosheets:high-yield preparation and device fabrication.Angew Chem Int Ed,2011,50:11093-11097
41 Li H,Wu J,Yin Z,et al.Preparation and applications of mechanically exfoliated single-layer and multilayer MoS2and WSe2nanosheets.Acc Chem Res,2014,47:1067-1075
42 Heising J,Kanatzidis MG.Exfoliated and restacked MoS2and WS2:ionic or neutral species?Encapsulation and ordering of hard Electropositive cations.J Am Chem Soc,1999,121:11720-11732
43 Peng W,Wang L,Murali B,et al.Solution-grown monocrystalline hybrid perovskite films for hole-transporter-free solar cells.Adv Mater,2016,28:3383-3390
44 Brunetti B,Cavallo C,Ciccioli A,et al.On the thermal and thermodynamic(in)stability of methylammonium lead halide perovskites.Sci Rep,2016,6:31896
45 Kappera R,Voiry D,Yalcin SE,et al.Phase-engineered low-resistance contacts for ultrathin MoS2transistors.Nat Mater,2014,13:1128-1134
46 Eda G,Yamaguchi H,Voiry D,et al.Photoluminescence from chemically exfoliated MoS2.Nano Lett,2011,11:5111-5116
47 Voiry D,Salehi M,Silva R,et al.Conducting MoS2nanosheets as catalysts for hydrogen evolution reaction.Nano Lett,2013,13:6222-6227
48 Narayan J,Larson BC.Domain epitaxy:A unified paradigm for thin film growth.J Appl Phys,2003,93:278-285
49 Huang X,Zeng Z,Bao S,et al.Solution-phase epitaxial growth of noble metal nanostructures on dispersible single-layer molybdenum disulfide nanosheets.Nat Commun,2013,4:1444
50 Lin Z,Yin A,Mao J,et al.Scalable solution-phase epitaxial growth of symmetry-mismatched heterostructures on two-dimensional crystal soft template.Sci Adv,2016,2:e1600993
51 Jin M,Zhang H,Wang J,et al.Copper can still be epitaxially deposited on palladium nanocrystals to generate core-shell nanocubes despite their large lattice mismatch.ACS Nano,2012,6:2566-2573
52 Fan FR,Liu DY,Wu YF,et al.Epitaxial growth of heterogeneous metal nanocrystals:from gold nano-octahedra to palladium and silver nanocubes.J Am Chem Soc,2008,130:6949-6951
53 Geim AK,Grigorieva IV.van der Waals heterostructures.Nature,2013,499:419-425
54 Schulz P,Edri E,Kirmayer S,et al.Interface energetics in organometal halide perovskite-based photovoltaic cells.Energy Environ Sci,2014,7:1377-1381
55 Yang D,Yang R,Zhang J,et al.High efficiency flexible perovskite solar cells using superior low temperature TiO2.Energy Environ Sci,2015,8:3208-3214
56 Fang H,Li J,Ding J,et al.An origami perovskite photodetector with spatial recognition ability.ACS Appl Mater Interfaces,2017,9:10921-10928
57 Lin CH,Tsai DS,Wei TC,et al.Highly deformable origami paper photodetector arrays.ACS Nano,2017,11:10230-10235
58 Cai C,Ma Y,Jeon J,et al.Epitaxial growth of large-grain NiSe films by solid-state reaction for high-responsivity photodetector arrays.Adv Mater,2017,29:1606180
59 Lopez-Sanchez O,Lembke D,Kayci M,et al.Ultrasensitive photodetectors based on monolayer MoS2.Nat Nanotechnol,2013,8:497-501
60 Stranks SD,Snaith HJ.Metal-halide perovskites for photovoltaic and light-emitting devices.Nat Nanotechnol,2015,10:391-402
61 Fan X,Xu P,Zhou D,et al.Fast and efficient preparation of exfoliated 2H MoS2nanosheets by sonication-assisted lithium intercalation and infrared laser-induced 1T to 2H phase reversion.Nano Lett,2015,15:5956-5960