硫化物靶与单质靶制备Cu_2ZnSnS_4薄膜的比较研究
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摘要
为了验证磁控溅射硫化物靶替代单质靶制备Cu_2ZnSnS_4(CZTS)薄膜及太阳电池的可行性与优越性,采用多周期磁控溅射ZnS-Sn-CuS和Zn-Sn-Cu制备CZTS薄膜,并分析了使用不同溅射靶材对薄膜晶体结构、相纯度、表面粗糙度、化学组分、表面、截面形貌及光电特性的影响。按SLG/Mo/CZTS/CdS/i-ZnO/ZnO:Al/Ni-Al结构制成完整的电池器件并测量了J-V曲线。结果显示采用ZnS-Sn-CuS靶制备的CZTS薄膜太阳电池开路电压为611 mV,短路电流密度为21.28mA/cm~2,光电转换效率达5.11%;而以单质靶为基础制备的太阳电池开路电压为594mV,短路电流密度为18.56 mA/cm~2,光电转换效率为4.13%。这归因于采用ZnS-Sn-CuS制备的CZTS薄膜相比于单质靶更加平整致密,纵向生长更好。证明了采用硫化物靶制备CZTS薄膜及太阳电池相较于单质靶的优越性。
To verify feasibility and superiority of preparing Cu_2ZnSnS_4(CZTS) thin films and solar cells by sputtering chalcogenide targets instead of single targets, two kinds of CZTS thin films were synthesized via multi-period sputtering ZnS-Sn-CuS and Zn-Sn-Cu, respectively. Influence of different sputtering targets on crystal structure, phase purity, surface roughness, chemical composition, surface and cross-sectional morphology, and optical-electrical properties of CZTS thin films were investigated in detail. Subsequently, the complete devices were fabricated according to SLG/Mo/CZTS/CdS/i-ZnO/ZnO:Al/Ni-Al and J-V characteristics of cells were measured. The results show that the solar cell made of ZnS-Sn-CuS precursor owns an open-circuit voltage of 611 m V, short-circuit current density of21.28 m A/cm~2 and efficiency of 5.11% while the solar cell based on single targets shows an open-circuit voltage of 594 mV, short-circuit current density of 18.56 mA/cm~2 and an efficiency of 4.13%. It is attributed to the fact that the CZTS thin films prepared by ZnS-Sn-CuS have smoother, denser surface and better longitudinal growth compared with those prepared by single targets. The result confirms the superiority of the CZTS thin film and solar cells prepared using the chalcogenide targets over those from single targets.
To verify feasibility and superiority of preparing Cu_2ZnSnS_4(CZTS) thin films and solar cells by sputtering chalcogenide targets instead of single targets, two kinds of CZTS thin films were synthesized via multi-period sputtering ZnS-Sn-CuS and Zn-Sn-Cu, respectively. Influence of different sputtering targets on crystal structure, phase purity, surface roughness, chemical composition, surface and cross-sectional morphology, and optical-electrical properties of CZTS thin films were investigated in detail. Subsequently, the complete devices were fabricated according to SLG/Mo/CZTS/CdS/i-ZnO/ZnO:Al/Ni-Al and J-V characteristics of cells were measured. The results show that the solar cell made of ZnS-Sn-CuS precursor owns an open-circuit voltage of 611 m V, short-circuit current density of21.28 m A/cm~2 and efficiency of 5.11% while the solar cell based on single targets shows an open-circuit voltage of 594 mV, short-circuit current density of 18.56 mA/cm~2 and an efficiency of 4.13%. It is attributed to the fact that the CZTS thin films prepared by ZnS-Sn-CuS have smoother, denser surface and better longitudinal growth compared with those prepared by single targets. The result confirms the superiority of the CZTS thin film and solar cells prepared using the chalcogenide targets over those from single targets.
引文
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[21]MOUSEL M,SCHWARZ T,DJEMOUR R,et al.Cu-rich precursors improve kesterite solar cells.Advanced Energy Materials,2014,4(2):1300543-1-6.
[22]FERNANDES P A,SALOME P M P,CUNHA A F D.Study of ternary Cu2SnS3 and Cu3SnS4 thin films prepared by sulfurizing stacked metal precursors.Journal of Physics D Applied Physics,2010,43(21):215403-1-11.
[2]KATAGIRI H,SAITOH K,WASHIO T,et al.Development of thin film solar cell based on Cu2ZnSnS4 thin films.Solar Energy Materials and Solar Cells,2011,65(1):141-148.
[3]SHOCKLEY W,QUEISSER H J.Detailed balance limit of efficiency of p-n junction solar cells.Journal of Applied Physics,2004,32(3):510-519.
[4]KATAGIRI H,JIMBO K,MAW W S,et al.Development of CZTS-based thin film solar cells.Thin Solid Films,2009,517(7):2455-2460.
[5]LU FANG-YANG,HUANG JIA-LIANG SUN KAI-WEI et al.Beyond 8%ultrathin kesterite Cu2ZnSnS4 solar cells by interface reaction route controlling and self-organized nanopattern at the back contact.NPG Asia Materials,2017,9(7):e401-1-8.
[6]XU XIN,WANG SHU-RONG,MA XUN,et al.Optimization of sulfurization time for properties of Cu2ZnSnS4 films and cells by sputtering method.Journal of Materials Science:Materials in Electronics,2018,29(22):19137-19146.
[7]WANG K,GUNAWAN O,TODOROV T,et al.Thermally evaporated Cu2ZnSnS4 solar cells.Applied Physics Letters,2010,97(14):2455-1155.
[8]MORIYA K,TANAKA K,UCHIKI H.Fabrication of Cu2ZnSnS4thin-film solar cell prepared by pulsed laser deposition.Japanese Journal of Applied Physics,2014,46(9A):5780-5781.
[9]ChAUDHARI J J,JOSHI U S.Effects of complexing agent on earth-abundant environmentally friendly Cu2ZnSnS4 thin film solar cells prepared by Sol-Gel deposition.Applied Physics A,2018,124(7):465-473.
[10]TAO JIA-HUA,LIU JUN-FENG,CHEN LEI-LEI,et al.7.1%efficienct co-electroplated Cu2ZnSnS4 thin film solar cells with sputtered CdS buffer layers.Green Chemistry,2016,18(2):550-587.
[11]ZENG X,TAI K F,ZHANH T L,et al.Cu2ZnSn(S,Se)4 kesterite solar with 5.1%efficiency using spray pyrolysis of aqueous precursor solution followed by selenization.Solar Energy Materials&Solar Cells,2014,124(5):55-60.
[12]?ZDAL T,KAVAK H.Determination of crystallization threshold temperature for Sol-Gel spin coated Cu2ZnSnS4 thin films.Ceramics International,2018,44(15):18928-1893.
[13]FUKANO T,TAJIMA S,ITO T.Enhancement of conversion efficiency of Cu2ZnSnS4 thin film solar cells by improvement of sulfurization conditions.Applied Physics Express,2013,6(6):062301-1-3.
[14]SHIN B,GUNAWAN O,ZHU Y,et al.Thin film solar cell with8.4%power conversion efficiency using an earth-abundant Cu2Zn Sn S4absorber.Progress in Photovoltaics:Research and Applications,2013,21(1):72-76.
[15]YAN HANG,HUANG JIA-LIANG,LIU FANG-YANG,et al.Cu2ZnSnS4 solar cells with over 10%power conversion efficiency enabled by heterojunction heat treatment.Nature Energy,2018,3(9):764-772.
[16]YANG MIN,WANG SHURONG,JIANG ZHI,et al.Cu2ZnSnS4thin film solar cells prepared by sulfurization of sputtered precursors.Bulletin of the Chinese Ceramic Society,2015,34(Supplement):222-226.
[17]LI ZHI-SHAN,WANG SHU-RONG,JIANG ZHI,et al.Cu2ZnSnS4 thin films prepared by magnetron.Bulletin of the Chinese Ceramic Society,2015,34(Supplement):127-131.
[18]LISCO F,KAMINSKI P M,ABBAS A,et al.High rate deposition of thin film cadmium sulphide by pulsed direct current magnetron sputtering.Thin Solid Films,2015,574(1):43-51.
[19]CHEN S,WANG L W,WALSH A,et al.Abundance of CuZn+SnZn and 2CuZn+SnZn defect clusters in kesterite solar cells.Applied Physics Letters,2012,101(22):223901-1-4.
[20]ZHAO WAN-GEN,WANG GANG,TIAN QING-WEN,et al.Fabrication of Cu2ZnSn(S,Se)4 solar cells via an ethanol-based Sol-Gel route using SnS2 as Sn source.ACS Applied Materials&Interfaces,2014,6(15):12650-12655.
[21]MOUSEL M,SCHWARZ T,DJEMOUR R,et al.Cu-rich precursors improve kesterite solar cells.Advanced Energy Materials,2014,4(2):1300543-1-6.
[22]FERNANDES P A,SALOME P M P,CUNHA A F D.Study of ternary Cu2SnS3 and Cu3SnS4 thin films prepared by sulfurizing stacked metal precursors.Journal of Physics D Applied Physics,2010,43(21):215403-1-11.