J. Semicond. > Volume 39 > Issue 1 > Article Number: 014002

Interfacial engineering of printable bottom back metal electrodes for full-solution processed flexible organic solar cells

Hongyu Zhen 1, 2, , , Kan Li 1, 3, , Yaokang Zhang 1, , Lina Chen 1, , Liyong Niu 1, , Xiaoling Wei 1, , Xu Fang 4, , Peng You 5, , Zhike Liu 5, , Dongrui Wang 1, , Feng Yan 5, and Zijian Zheng 1, ,

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Abstract: Printing of metal bottom back electrodes of flexible organic solar cells (FOSCs) at low temperature is of great significance to realize the full-solution fabrication technology. However, this has been difficult to achieve because often the interfacial properties of those printed electrodes, including conductivity, roughness, work function, optical and mechanical flexibility, cannot meet the device requirement at the same time. In this work, we fabricate printed Ag and Cu bottom back cathodes by a low-temperature solution technique named polymer-assisted metal deposition (PAMD) on flexible PET substrates. Branched polyethylenimine (PEI) and ZnO thin films are used as the interface modification layers (IMLs) of these cathodes. Detailed experimental studies on the electrical, mechanical, and morphological properties, and simulation study on the optical properties of these IMLs are carried out to understand and optimize the interface of printed cathodes. We demonstrate that the highest power conversion efficiency over 3.0% can be achieved from a full-solution processed OFSC with the device structure being PAMD-Ag/PEI/P3HT:PC61BM/PH1000. This device also acquires remarkable stability upon repeating bending tests.

Key words: polymer-assisted metal depositionfull-solution processedflexible organic solar cellsprinted electrodesinterface modification layers

Abstract: Printing of metal bottom back electrodes of flexible organic solar cells (FOSCs) at low temperature is of great significance to realize the full-solution fabrication technology. However, this has been difficult to achieve because often the interfacial properties of those printed electrodes, including conductivity, roughness, work function, optical and mechanical flexibility, cannot meet the device requirement at the same time. In this work, we fabricate printed Ag and Cu bottom back cathodes by a low-temperature solution technique named polymer-assisted metal deposition (PAMD) on flexible PET substrates. Branched polyethylenimine (PEI) and ZnO thin films are used as the interface modification layers (IMLs) of these cathodes. Detailed experimental studies on the electrical, mechanical, and morphological properties, and simulation study on the optical properties of these IMLs are carried out to understand and optimize the interface of printed cathodes. We demonstrate that the highest power conversion efficiency over 3.0% can be achieved from a full-solution processed OFSC with the device structure being PAMD-Ag/PEI/P3HT:PC61BM/PH1000. This device also acquires remarkable stability upon repeating bending tests.

Key words: polymer-assisted metal depositionfull-solution processedflexible organic solar cellsprinted electrodesinterface modification layers



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Takei K, Takahashi T, Ho J C, et al. Nanowire active-matrix circuitry for low-voltage macroscale artificial skin. Nat Mater, 2010, 9: 821

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Schwartz G, Tee B C K, Mei J, et al. Flexible polymer transistors with high pressure sensitivity for application in electronic skin and health monitoring. Nat Commun, 2013, 4: 1859

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Xiao F, Li Y, Zan X, et al. Growth of metal–metal oxide nanostructures on freestanding graphene paper for flexible biosensors. Adv Funct Mater, 2012, 22: 2487

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Kwak Y H, Choi D S, Kim Y N, et al. Flexible glucose sensor using CVD-grown graphene-based field effect transistor. Biosensors Bioelectron, 2012, 37: 82

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Shin D Y, Jung M, Chun S. Resistivity transition mechanism of silver salts in the next generation conductive ink for a roll-to-roll printed film with a silver network. J Mater Chem A, 2012, 22: 11755

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Zhang J, Li Y, Zhang B, et al. Flexible indium–gallium– zinc–oxide Schottky diode operating beyond 2.45 GHz. Nat Commun, 2015, 6: 1

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Kaltenbrunner M, White M S, Głowacki E D, et al. Ultrathin and lightweight organic solar cells with high flexibility. Nat Commun, 2012, 3: 770

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Zbiri M, Haverkate L A, Kearley G J, et al. Organic solar cells. In: Neutron applications in materials for energy. Springer, 2015

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Hoppe H, Sariciftci N S. Organic solar cells: an overview. J Mater Res, 2004, 19: 1924

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Lungenschmied C, Dennler G, Neugebauer H, et al. Flexible, long-lived, large-area, organic solar cells. Sol Energy Mater Sol Cells, 2007, 91: 379

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Kaltenbrunner M, White M S, Głowacki E D, et al. Ultrathin and lightweight organic solar cells with high flexibility. Nat Commun, 2012, 3: 770

[13]

Zhen H, Li K, Huang Z, et al. Inverted indium-tin-oxide-free cone-shaped polymer solar cells for light trapping. Appl Phys Lett, 2012, 100: 213901

[14]

Nie W, Tsai H, Asadpour R, et al. High-efficiency solution-processed perovskite solar cells with millimeter-scale grains. Science, 2015, 347: 522

[15]

Yang W S, Noh J H, Jeon N J, et al. High-performance photovoltaic perovskite layers fabricated through intramolecular exchange. Science, 2015, 348: 1234

[16]

He Z, Xiao B, Liu F, et al. Single-junction polymer solar cells with high efficiency and photovoltage. Nat Photonics, 2015, 9: 174

[17]

You J, Dou L, Yoshimura K, et al. A polymer tandem solar cell with 10.6% power conversion efficiency. Nat Commun, 2013, 4: 1446

[18]

Huang J, Li C Z, Chueh C C, et al. 10.4% Power conversion efficiency of ITO-free organic photovoltaics through enhanced light trapping configuration. Adv Energy Mater, 2015, 5: 3599

[19]

Zhao W, Qian D, Zhang S, et al. Fullerene-free polymer solar cells with over 11% efficiency and excellent thermal stability. Adv Mater, 2016, 28: 4734

[20]

Huang J, Carpenter J H, Li C Z, et al. Highly efficient organic solar cells with improved vertical donor–acceptor compositional gradient via an inverted off-center spinning method. Adv Mater, 2015, 28, 5: 967

[21]

Liao S H, Jhuo H J, Yeh P N, et al. Single junction inverted polymer solar cell reaching power conversion efficiency 10.31% by employing dual-doped zinc oxide nano-film as cathode interlayer. Sci Rep, 2014, 4: 6813

[22]

Nian L, Zhang W, Zhu N, et al. Photoconductive cathode interlayer for highly efficient inverted polymer solar cells. J Am Chem Soc, 2015, 137: 6995

[23]

Zhang S, Ye L, Hou J. Breaking the 10% efficiency barrier in organic photovoltaics: morphology and device optimization of well-known PBDTTT polymers. Adv Energy Mater, 2016, 6: 1502529

[24]

Krebs, F. All solution roll-to-roll processed polymer solar cells free from indium-tin-oxide and vacuum coating steps. Org Electron, 2009, 10: 761

[25]

Krantz J, Forberich K, Kubis P, et al. Printing high performance reflective electrodes for organic solar cells. Org Electron, 2015, 17: 334

[26]

Andersen T R, Dam H F, Hösel M, et al. Scalable, ambient atmosphere roll-to-roll manufacture of encapsulated large area, flexible organic tandem solar cell modules. Energy Environ Sci, 2014, 7: 2925

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Zhou Y, Fuentes-Hernandez C, Shim J, et al. A universal method to produce low-work function electrodes for organic electronics. Science, 2012, 336: 327

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Van Franeker J J, Voorthuijzen W P, Gorter H, et al. All-solution-processed organic solar cells with conventional architecture. Sol Energy Mater Sol, 2013, 117: 267

[29]

Guo F, Zhu X, Forberich K, et al. ITO-free and fully solution-processed semitransparent organic solar cells with high fill factors. Adv Energy Mater, 2013, 3: 1062

[30]

Guo F, Li N, Radmilović V V, et al. Fully printed organic tandem solar cells using solution-processed silver nanowires and opaque silver as charge collecting electrodes. Energy Environ Sci, 2015, 8: 1690

[31]

Cheng P, Lin Y, Zawacka N K, et al. Comparison of additive amount used in spin-coated and roll-coated organic solar cells. J Mater Chem A, 2014, 2: 19542

[32]

Li K, Zhen H, Niu L, et al. Full-solution processed flexible organic solar cells using low-cost printable copper electrodes. Adv Mater, 2014, 26: 7271

[33]

Yim J H, Joe S Y, Pang C, et al. Fully solution-processed semitransparent organic solar cells with a silver nanowire cathode and a conducting polymer anode. ACS Nano, 2014, 8: 2857

[34]

Carlé J E, Helgesen M, Zawacka N K, et al. A comparative study of fluorine substituents for enhanced stability of flexible and ITO-free high-performance polymer solar cells. J Polym Sci B, 2014, 52: 893

[35]

Helgesen M, Carlé J E, Krebs F C. Slot-die coating of a high performance copolymer in a readily scalable roll process for polymer solar cells. Adv Energy Mater, 2013, 3: 1664

[36]

Helgesen M, Carlé J E, dos Reis Benatto G A, et al. Making ends meet: flow synthesis as the answer to reproducible high-performance conjugated polymers on the scale that roll-to-roll processing demands. Adv Energy Mater, 2015, 5(9): 1401996

[37]

Nickel F, Haas T, Wegner E, et al. Mechanically robust, ITO-free, 4.8% efficient, all-solution processed organic solar cells on flexible PET foil. Sol Energy Mater Sol, 2014, 130: 317

[38]

Zhang Y K, Wu Z W, Li P, et al. Efficient organic solar cells with solution-processed silver nanowire electrodes. Adv Mater, 2011, 23: 4371

[39]

Kang M G, Xu T, Park H J, et al. Full-solution-processed TCO-free semi-transparent perovskite solar cells for tandem and flexible applications. Adv Energy Mater, 2017: 1701569

[40]

Yim J H, Joe S Y, Pang C, et al. Fully solution-processed semitransparent organic solar cells with a silver nanowire cathode and a conducting polymer anode. ACS Nano, 2014, 8: 2857

[41]

Wu H, Hu L, Rowell M W, Kong D, et al. Electrospun metal nanofiber webs as high-performance transparent electrode. Nano Lett, 2010, 10: 4242

[42]

Chen H Y, Hou J, Zhang S, et al. Polymer solar cells with enhanced open-circuit voltage and efficiency. Nat Photonics, 2009, 3: 649

[43]

He Z, Zhong C, Su S, et al. Enhanced power-conversion efficiency in polymer solar cells using an inverted device structure. Nat Photonics, 2012, 6: 591

[44]

Espinosa N, Lenzmann F O, Ryley S, et al. OPV for mobile applications: an evaluation of roll-to-roll processed indium and silver free polymer solar cells through analysis of life cycle, cost and layer quality using inline optical and functional inspection tools. J Mater Chem A, 2013, 1: 7037

[45]

Kyaw A K K, Wang D H, Gupta V, et al. Efficient solution-processed small-molecule solar cells with inverted structure. Adv Mater, 2013, 25: 2397

[46]

Yu G, Gao J, Hummelen J C, et al. Polymer photovoltiac cells: enhanced efficiencies via a network of internal donor-acceptor heterojunctions. Science, 1995, 270: 1789

[47]

Guo R, Yu Y, Xie Z, et al. Matrix-assisted catalytic printing for the fabrication of multiscale, flexible, foldable, and stretchable metal conductors. Adv Mater, 2013, 25: 3343

[48]

Liu X, Chang H, Li Y, et al. Polyelectrolyte-bridged metal/cotton hierarchical structures for highly durable conductive yarns. ACS Appl Mater Interfaces, 2010, 2: 529

[49]

Yu Y, Zeng J, Chen C, et al. Three-dimensional compressible and stretchable conductive composites. Adv Mater, 2014, 26: 810

[50]

Yu Y, Xiao X, Zhang Y, et al. Photoreactive and metal-platable copolymer inks for high-throughput, room-temperature printing of flexible metal electrodes for thin-film electronics. Adv Mater, 2016, 28: 4926

[51]

Duan C, Zhong C, Huang F, et al. Interface engineering for high performance bulk-heterojunction polymeric solar cells. London: Springer, 2013: 43

[52]

Steim R, Kogler F R, Brabec C J. Interface materials for organic solar cells. J Mater Chem, 2010, 20: 2499

[53]

Chen L M, Xu Z, Hong Z, et al. Interface investigation and engineering–achieving high performance polymer photovoltaic devices. J Mater Chem, 2010, 20: 2575

[54]

Po R, Carbonera C, Bernardi A, et al. The role of buffer layers in polymer solar cells. Energy Environ Sci, 2011, 4: 285

[55]

Pacholski C, Kornowski A, Weller H. Self-assembly of ZnO: from nanodots to nanorods. Angew Chem Int Ed, 2002, 41: 1188

[56]

Hsu C H, Yeh M C, Lo K L, et al. Application of microcontact printing to electroless plating for the fabrication of microscale silver patterns on glass. Langmuir, 2007, 23: 12111

[57]

Park H, Chang S, Zhou X, et al. Flexible graphene electrode-based organic photovoltaics with record-high efficiency. Nano Lett, 2014, 14: 5148

[58]

Wang Z Z, Zhang C F, Chen D Z, et al. Flexible ITO-free organic solar cells based on MoO3/Ag anodes. IEEE Photonics J, 2015, 7: 8400109

[1]

Mannsfeld S C, Tee B C, Stoltenberg R M, et al. Highly sensitive flexible pressure sensors with microstructured rubber dielectric layers. Nat Mater, 2010, 9: 859

[2]

Takei K, Takahashi T, Ho J C, et al. Nanowire active-matrix circuitry for low-voltage macroscale artificial skin. Nat Mater, 2010, 9: 821

[3]

Schwartz G, Tee B C K, Mei J, et al. Flexible polymer transistors with high pressure sensitivity for application in electronic skin and health monitoring. Nat Commun, 2013, 4: 1859

[4]

Xiao F, Li Y, Zan X, et al. Growth of metal–metal oxide nanostructures on freestanding graphene paper for flexible biosensors. Adv Funct Mater, 2012, 22: 2487

[5]

Kwak Y H, Choi D S, Kim Y N, et al. Flexible glucose sensor using CVD-grown graphene-based field effect transistor. Biosensors Bioelectron, 2012, 37: 82

[6]

Shin D Y, Jung M, Chun S. Resistivity transition mechanism of silver salts in the next generation conductive ink for a roll-to-roll printed film with a silver network. J Mater Chem A, 2012, 22: 11755

[7]

Zhang J, Li Y, Zhang B, et al. Flexible indium–gallium– zinc–oxide Schottky diode operating beyond 2.45 GHz. Nat Commun, 2015, 6: 1

[8]

Kaltenbrunner M, White M S, Głowacki E D, et al. Ultrathin and lightweight organic solar cells with high flexibility. Nat Commun, 2012, 3: 770

[9]

Zbiri M, Haverkate L A, Kearley G J, et al. Organic solar cells. In: Neutron applications in materials for energy. Springer, 2015

[10]

Hoppe H, Sariciftci N S. Organic solar cells: an overview. J Mater Res, 2004, 19: 1924

[11]

Lungenschmied C, Dennler G, Neugebauer H, et al. Flexible, long-lived, large-area, organic solar cells. Sol Energy Mater Sol Cells, 2007, 91: 379

[12]

Kaltenbrunner M, White M S, Głowacki E D, et al. Ultrathin and lightweight organic solar cells with high flexibility. Nat Commun, 2012, 3: 770

[13]

Zhen H, Li K, Huang Z, et al. Inverted indium-tin-oxide-free cone-shaped polymer solar cells for light trapping. Appl Phys Lett, 2012, 100: 213901

[14]

Nie W, Tsai H, Asadpour R, et al. High-efficiency solution-processed perovskite solar cells with millimeter-scale grains. Science, 2015, 347: 522

[15]

Yang W S, Noh J H, Jeon N J, et al. High-performance photovoltaic perovskite layers fabricated through intramolecular exchange. Science, 2015, 348: 1234

[16]

He Z, Xiao B, Liu F, et al. Single-junction polymer solar cells with high efficiency and photovoltage. Nat Photonics, 2015, 9: 174

[17]

You J, Dou L, Yoshimura K, et al. A polymer tandem solar cell with 10.6% power conversion efficiency. Nat Commun, 2013, 4: 1446

[18]

Huang J, Li C Z, Chueh C C, et al. 10.4% Power conversion efficiency of ITO-free organic photovoltaics through enhanced light trapping configuration. Adv Energy Mater, 2015, 5: 3599

[19]

Zhao W, Qian D, Zhang S, et al. Fullerene-free polymer solar cells with over 11% efficiency and excellent thermal stability. Adv Mater, 2016, 28: 4734

[20]

Huang J, Carpenter J H, Li C Z, et al. Highly efficient organic solar cells with improved vertical donor–acceptor compositional gradient via an inverted off-center spinning method. Adv Mater, 2015, 28, 5: 967

[21]

Liao S H, Jhuo H J, Yeh P N, et al. Single junction inverted polymer solar cell reaching power conversion efficiency 10.31% by employing dual-doped zinc oxide nano-film as cathode interlayer. Sci Rep, 2014, 4: 6813

[22]

Nian L, Zhang W, Zhu N, et al. Photoconductive cathode interlayer for highly efficient inverted polymer solar cells. J Am Chem Soc, 2015, 137: 6995

[23]

Zhang S, Ye L, Hou J. Breaking the 10% efficiency barrier in organic photovoltaics: morphology and device optimization of well-known PBDTTT polymers. Adv Energy Mater, 2016, 6: 1502529

[24]

Krebs, F. All solution roll-to-roll processed polymer solar cells free from indium-tin-oxide and vacuum coating steps. Org Electron, 2009, 10: 761

[25]

Krantz J, Forberich K, Kubis P, et al. Printing high performance reflective electrodes for organic solar cells. Org Electron, 2015, 17: 334

[26]

Andersen T R, Dam H F, Hösel M, et al. Scalable, ambient atmosphere roll-to-roll manufacture of encapsulated large area, flexible organic tandem solar cell modules. Energy Environ Sci, 2014, 7: 2925

[27]

Zhou Y, Fuentes-Hernandez C, Shim J, et al. A universal method to produce low-work function electrodes for organic electronics. Science, 2012, 336: 327

[28]

Van Franeker J J, Voorthuijzen W P, Gorter H, et al. All-solution-processed organic solar cells with conventional architecture. Sol Energy Mater Sol, 2013, 117: 267

[29]

Guo F, Zhu X, Forberich K, et al. ITO-free and fully solution-processed semitransparent organic solar cells with high fill factors. Adv Energy Mater, 2013, 3: 1062

[30]

Guo F, Li N, Radmilović V V, et al. Fully printed organic tandem solar cells using solution-processed silver nanowires and opaque silver as charge collecting electrodes. Energy Environ Sci, 2015, 8: 1690

[31]

Cheng P, Lin Y, Zawacka N K, et al. Comparison of additive amount used in spin-coated and roll-coated organic solar cells. J Mater Chem A, 2014, 2: 19542

[32]

Li K, Zhen H, Niu L, et al. Full-solution processed flexible organic solar cells using low-cost printable copper electrodes. Adv Mater, 2014, 26: 7271

[33]

Yim J H, Joe S Y, Pang C, et al. Fully solution-processed semitransparent organic solar cells with a silver nanowire cathode and a conducting polymer anode. ACS Nano, 2014, 8: 2857

[34]

Carlé J E, Helgesen M, Zawacka N K, et al. A comparative study of fluorine substituents for enhanced stability of flexible and ITO-free high-performance polymer solar cells. J Polym Sci B, 2014, 52: 893

[35]

Helgesen M, Carlé J E, Krebs F C. Slot-die coating of a high performance copolymer in a readily scalable roll process for polymer solar cells. Adv Energy Mater, 2013, 3: 1664

[36]

Helgesen M, Carlé J E, dos Reis Benatto G A, et al. Making ends meet: flow synthesis as the answer to reproducible high-performance conjugated polymers on the scale that roll-to-roll processing demands. Adv Energy Mater, 2015, 5(9): 1401996

[37]

Nickel F, Haas T, Wegner E, et al. Mechanically robust, ITO-free, 4.8% efficient, all-solution processed organic solar cells on flexible PET foil. Sol Energy Mater Sol, 2014, 130: 317

[38]

Zhang Y K, Wu Z W, Li P, et al. Efficient organic solar cells with solution-processed silver nanowire electrodes. Adv Mater, 2011, 23: 4371

[39]

Kang M G, Xu T, Park H J, et al. Full-solution-processed TCO-free semi-transparent perovskite solar cells for tandem and flexible applications. Adv Energy Mater, 2017: 1701569

[40]

Yim J H, Joe S Y, Pang C, et al. Fully solution-processed semitransparent organic solar cells with a silver nanowire cathode and a conducting polymer anode. ACS Nano, 2014, 8: 2857

[41]

Wu H, Hu L, Rowell M W, Kong D, et al. Electrospun metal nanofiber webs as high-performance transparent electrode. Nano Lett, 2010, 10: 4242

[42]

Chen H Y, Hou J, Zhang S, et al. Polymer solar cells with enhanced open-circuit voltage and efficiency. Nat Photonics, 2009, 3: 649

[43]

He Z, Zhong C, Su S, et al. Enhanced power-conversion efficiency in polymer solar cells using an inverted device structure. Nat Photonics, 2012, 6: 591

[44]

Espinosa N, Lenzmann F O, Ryley S, et al. OPV for mobile applications: an evaluation of roll-to-roll processed indium and silver free polymer solar cells through analysis of life cycle, cost and layer quality using inline optical and functional inspection tools. J Mater Chem A, 2013, 1: 7037

[45]

Kyaw A K K, Wang D H, Gupta V, et al. Efficient solution-processed small-molecule solar cells with inverted structure. Adv Mater, 2013, 25: 2397

[46]

Yu G, Gao J, Hummelen J C, et al. Polymer photovoltiac cells: enhanced efficiencies via a network of internal donor-acceptor heterojunctions. Science, 1995, 270: 1789

[47]

Guo R, Yu Y, Xie Z, et al. Matrix-assisted catalytic printing for the fabrication of multiscale, flexible, foldable, and stretchable metal conductors. Adv Mater, 2013, 25: 3343

[48]

Liu X, Chang H, Li Y, et al. Polyelectrolyte-bridged metal/cotton hierarchical structures for highly durable conductive yarns. ACS Appl Mater Interfaces, 2010, 2: 529

[49]

Yu Y, Zeng J, Chen C, et al. Three-dimensional compressible and stretchable conductive composites. Adv Mater, 2014, 26: 810

[50]

Yu Y, Xiao X, Zhang Y, et al. Photoreactive and metal-platable copolymer inks for high-throughput, room-temperature printing of flexible metal electrodes for thin-film electronics. Adv Mater, 2016, 28: 4926

[51]

Duan C, Zhong C, Huang F, et al. Interface engineering for high performance bulk-heterojunction polymeric solar cells. London: Springer, 2013: 43

[52]

Steim R, Kogler F R, Brabec C J. Interface materials for organic solar cells. J Mater Chem, 2010, 20: 2499

[53]

Chen L M, Xu Z, Hong Z, et al. Interface investigation and engineering–achieving high performance polymer photovoltaic devices. J Mater Chem, 2010, 20: 2575

[54]

Po R, Carbonera C, Bernardi A, et al. The role of buffer layers in polymer solar cells. Energy Environ Sci, 2011, 4: 285

[55]

Pacholski C, Kornowski A, Weller H. Self-assembly of ZnO: from nanodots to nanorods. Angew Chem Int Ed, 2002, 41: 1188

[56]

Hsu C H, Yeh M C, Lo K L, et al. Application of microcontact printing to electroless plating for the fabrication of microscale silver patterns on glass. Langmuir, 2007, 23: 12111

[57]

Park H, Chang S, Zhou X, et al. Flexible graphene electrode-based organic photovoltaics with record-high efficiency. Nano Lett, 2014, 14: 5148

[58]

Wang Z Z, Zhang C F, Chen D Z, et al. Flexible ITO-free organic solar cells based on MoO3/Ag anodes. IEEE Photonics J, 2015, 7: 8400109

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H Y Zhen, K Li, Y K Zhang, L N Chen, L Y Niu, X L Wei, X Fang, P You, Z K Liu, D R Wang, F Yan, Z J Zheng, Interfacial engineering of printable bottom back metal electrodes for full-solution processed flexible organic solar cells[J]. J. Semicond., 2018, 39(1): 014002. doi: 10.1088/1674-4926/39/1/014002.

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History

Manuscript received: 22 June 2017 Manuscript revised: 05 October 2017 Online: Accepted Manuscript: 27 December 2017 Published: 01 January 2018

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