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Quaternary sulphides Cu2Zn(Ti, Zr, Hf)S4, the new type of photovoltaic materials

Fan Wei Zeng Zhi

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Quaternary sulphides Cu2Zn(Ti, Zr, Hf)S4, the new type of photovoltaic materials

Fan Wei, Zeng Zhi
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  • Based on the first-principles electronic-structure method, we study the electronic structures, optical properties, and the structural stabilities of the quaternary sulphides Cu2Zn(Ti, Zr, Hf) S4, which are obtained via substituting Ti, Zr, and Hf elements for Sn elements in Cu2ZnSnS4 (CTZS). It is well known that the photovoltaic efficiency of CZTS(Se) will be improved if the Se atoms partially substitute S atoms in CZTS. Our results show that the valence-band top of CZTSe shifts to lower energy and accesses to the valence-band top of Cu(InGa) Se2 (CIGS). Similar to CZTSe, the valenceband tops of Cu2Zn(Ti, Zr, Hf) S4 also shift to lower energies and access to the top of valence-band of CIGS. The high photovoltaic efficiency requires the smooth changes of the valence-band top and energy gap from the window material and the buffer layer to the light-absorption layer. Thus we predict that the photovoltaic efficiency will be improved if Sn atoms are substituted, even partially, by Ti, Zr, Hf atoms in CZTS, just like Se atoms substituting S atoms in CZTS. To obtain some reliable results, we perform the calculations both of PBE functional and HSE06 functional. The changes of valence-band tops from window materials to the light-absorbed materials are similar for PBE functional and HSE06 functional. The absolute values of the valence-band tops with HSE06 are lower in energies compared with PBE functional and the gaps obtained from HSE06 are larger than the gaps from PBE. We also calculate the optical properties of different light-absorbed materials including CZTiS, CZZrS, CZHfS, CZTS and CIGS, in which we mainly focus on the reflectance of different layers from the vacuum to the light-absorbed materials, from the window layers to the buffer layers and from the buffer layers to the light-absorbed layers. For the window layers we consider the ZnO and TiO2, and for the buffer layer we consider the CdS, In2S3, ZnSe and ZnS, etc. respectively. The high-performance solar cell requires low reflectance between the window layer and the buffer layer, the buffer layer and the light-absorbed layer so as to ensure more light transmit to the light-absorbed layer. Our results of reflectance show that ZnO(TiO2)/In2S3(ZnSe)/PVM are possible multilayer structures, with PVM (photovoltaic materials) =CZTS, CIGS, CZTiS, CZZrS, CZHfS. If we replace CdS buffer layer with other n-type semiconductors, the material of the window layer must be replaced accordingly with new materials to reach the lower reflectance. The structural stability of photovoltaics is an important topic in the application of photovoltaics. Our results show that CZTiS, CZZrS and CZHfS are structure-stable at zero temperature in terms of the calculated elastic properties and phonon vibration spectrum. Based on the elastic constants and Poisson-ratio, similar to CdTe, CIGS and CZTS, the CZTiS, CZZrS and CZHfS are ductile materials suitable to be used as the flexible solar cell. Additionally, we have performed the molecular-dynamics simulations at some finite temperatures (100, 800 and 1200 K respectively), calculated the pair-distribution functions and angle-distribution functions. As comparison, we also perform the corresponding molecular dynamics simulations of CZTS and ZnS. Our results show that the structural stabilities of CZTiS, CZZrS, and CZHfS are close to those of CZTS and ZnS. This means that once CZTiS, CZZrS and CZHfS are obtained experimentally, they will be stable. In summary, the novel photovoltaic materials CZTiS, CZZrS and CZHfS studied in detail in this work are potentially the high-performance photovoltaic materials for the solar cell application in the near future.
      Corresponding author: Fan Wei, fan@theory.issp.ac.cn
    • Funds: Project supported by the National Basic Research Program of China (973 Program) (Grant No. 2012CB933702).
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    Shin B, Gunawan O, Zhu Y, Bojarczuk N A, Chey S J, Guha S 2013 Prog. Photovolt: Res.Appl. 21 72

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    Guo Q J, Ford G M, Yang W C, Walker B C, Stach E A, Hillhouse H W, Agrawal R 2010 J. Am. Chem. Soc. 132 17384

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    Guo L, Zhu Y, Gunawan O, Gokmen T, Deline V R, Ahmed S, Romankiw L T, Deligianni H 2014 Prog. Photovolt: Res. Appl. 22 58

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    Wang W, Winkler M T, Gunawan O, Gokmen T, Todorov T K, Zhu Y, Mitzi D B 2014 Adv. Energy Mater. 4 1301465

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    Chen S Y, Walsh A, Gong X G, Wei S H 2013 Adv. Mater. 25 1522

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    Persson C, Zunger A 2005 Appl. Phys. Lett. 87 211904

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    Schmidt S S, Abou-Ras D, Sadewasser S, Yin W J, Feng C B, Yan Y F 2012 Phys. Rev. Lett. 109 095506

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    Yan Y F, Jiang C S, Noufi R, Wei S H, Moutinho H R, Al-Jassim M M 2007 Phys. Rev. Lett. 99 235504

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    Li J W, Mitzi D B, Shenoy V B 2011 ACS Nano 5 8613

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    Xu P, Chen S Y, Huang B, Xiang H J, Gong X G, Wei S H 2013 Phys. Rev. B 88 045427

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    Dong Z Y, Li Y F, Yao B, Ding Z H, Yang G, Deng R, Fang X, Wei Z P, Liu L 2014 J. Phys. D: Appl. Phys. 47 075304

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    Bao W, Ichimura M 2012 Int. J. Photoenergy ArticleID 619812

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    Fan W, Zeng Z 2015 Acta Phys. Sin. 64 238801 (in Chinese) [范巍, 曾雉 2015 物理学报 64 238801]

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    [26]

    Togo A, Oba F, Tanaka I 2008 Phys. Rev. B 78 134106

    [27]

    Romero M J, Du H, Teeter G, Yan Y F, Al-Jassim M M 2011 Phys. Rev. B 84 165324

    [28]

    Grossberg M, Raadik T, Raudoja J, Krustok J 2014 Current Appl. Phys. 14 447

    [29]

    Chen S Y, Yang J H, Gong X G, Walsh A, Wei S H 2010 Phys. Rev. B 81 245204

    [30]

    Yang C Y, Qin M S, Wang Y M, Wan D Y, Huang F Q, Lin J H 2013 Sci. Rep. 3 1286

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    Henkelman G, Arnaldsson A, Jnsson H 2006 Comput. Mater. Sci. 36 354

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    Wang W, Shen H L, Jin J L, Li J Z, Ma Y 2015 Chin. Phys. B 24 056805

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    Gordillo G, Caldern C, Bartolo-Prez P 2014 Appl. Surf. Sci. 305 506

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    Chalapathi U, Uthanna S, Sundara R V 2015 Solar Energy Materials Solar Cells 132 476

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    Levcenko S, Gurieva G, Guc M, Nateprov A 2009 Moldav. J. Phys. Sci. 8 173

    [36]

    Chen Q M, Li Z Q, Ni Y, Cheng S Y, Dou X M 2012 Chin. Phys. B 21 038401

    [37]

    Strohm A, Eisenmann L, Gebhardt R K, Harding A, Schltzer T, Abou-Ras D, Schock H W 2005 Thin Solid Film 480-481 162

    [38]

    Camps I, Coutinho J, Mir M, da Cunha A F, Rayson M J, Briddon P R 2012 Semicond. Sci. Technol. 27 115001

    [39]

    Berlincourt D, Jaffe H, Shiozawa L R 1963 Phys. Rev. 129 1009

    [40]

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    [42]

    Matsushita H, Ichikawa T, Katsui A 2005 J. Mater. Sci. 40 2003

    [43]

    Schorr S, Gonzalez-Aviles G 2009 Phys. Status Solidi A 206 1054

    [44]

    Madelung O 2004 Semiconductors: Data Handbook (Berlin: Springer-Verlag) p205

    [45]

    https://en.wikipedia.org/wiki/Zinc_sulfide

    [46]

    Wang C C, Chen S Y, Yang J H, Lang L, Xiang H J, Gong X G, Walsh A, Wei S H 2014 Chem. Mater. 26 3411

    [47]

    DiSalvo F J, Waszczak J V 1982 Phys. Rev. B 26 2501

    [48]

    Klepp K O, Gurtner D 1996 Journal of Alloys and Compounds 243 19

    [49]

    Liu Y C, Yang Z, Cui D, Ren X D, Sun J K, Liu X J, Zhang J R, Wei Q B, Fan H B, Yu F Y, Zhang X, Zhao C M, Liu S Z 2015 Adv. Mater. 27 5176

    [50]

    Saidaminov M I, Adinolfi V, Comin R, Abdelhady A L, Peng W, Dursun I, Yuan M J, Hoogland S, Sargent E H, Bakr Q M 2015 Nat. Commn. 6 8724

    [51]

    Momma K, Izumi F 2008 J. Appl. Crystallogr. 41 653

  • [1]

    Ito K, Nakazawa T 1988 Jpn. J. Appl. Phys. 27 2094

    [2]

    Shin B, Gunawan O, Zhu Y, Bojarczuk N A, Chey S J, Guha S 2013 Prog. Photovolt: Res.Appl. 21 72

    [3]

    Guo Q J, Ford G M, Yang W C, Walker B C, Stach E A, Hillhouse H W, Agrawal R 2010 J. Am. Chem. Soc. 132 17384

    [4]

    Guo L, Zhu Y, Gunawan O, Gokmen T, Deline V R, Ahmed S, Romankiw L T, Deligianni H 2014 Prog. Photovolt: Res. Appl. 22 58

    [5]

    Wang W, Winkler M T, Gunawan O, Gokmen T, Todorov T K, Zhu Y, Mitzi D B 2014 Adv. Energy Mater. 4 1301465

    [6]

    Xu J X, Yao R H 2012 Acta Phys. Sin. 61 187304 (in Chinese) [许佳雄, 姚若河 2012 物理学报 61 187304]

    [7]

    Chen S Y, Walsh A, Gong X G, Wei S H 2013 Adv. Mater. 25 1522

    [8]

    Yuan Z K, Xu P, Chen S Y 2015 Acta Phys. Sin. 64 186102 (in Chinese) [袁振坤, 许鹏, 陈时友 2015 物理学报 64 186102]

    [9]

    Shu Q, Yang J H, Chen S Y, Huang B, Xiang X J, Gong X G, Wei S H 2013 Phys. Rev. B 87 115208

    [10]

    Zhao H Y, Kumar M, Persson C 2012 Phys. Status Solidi C 9 1600

    [11]

    Persson C, Zunger A 2003 Phys. Rev. Lett. 91 266401

    [12]

    Persson C, Zunger A 2005 Appl. Phys. Lett. 87 211904

    [13]

    Schmidt S S, Abou-Ras D, Sadewasser S, Yin W J, Feng C B, Yan Y F 2012 Phys. Rev. Lett. 109 095506

    [14]

    Yan Y F, Jiang C S, Noufi R, Wei S H, Moutinho H R, Al-Jassim M M 2007 Phys. Rev. Lett. 99 235504

    [15]

    Li J W, Mitzi D B, Shenoy V B 2011 ACS Nano 5 8613

    [16]

    Medvedeva N I, Shalaeva E V, Kuznetsov M V, Yakushev M V 2006 Phys. Rev. B 73 035207

    [17]

    Xu P, Chen S Y, Huang B, Xiang H J, Gong X G, Wei S H 2013 Phys. Rev. B 88 045427

    [18]

    Dong Z Y, Li Y F, Yao B, Ding Z H, Yang G, Deng R, Fang X, Wei Z P, Liu L 2014 J. Phys. D: Appl. Phys. 47 075304

    [19]

    Bao W, Ichimura M 2012 Int. J. Photoenergy ArticleID 619812

    [20]

    Fan W, Zeng Z 2015 Acta Phys. Sin. 64 238801 (in Chinese) [范巍, 曾雉 2015 物理学报 64 238801]

    [21]

    Kresse G, Joubert D 1999 Phys. Rev. B 59 1758

    [22]

    Blchl P E 1994 Phys. Rev. B 50 17953

    [23]

    Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865

    [24]

    Heyd J, Scuseria G E, Ernzerhof M 2003 J. Chem. Phys. 118 8207

    [25]

    Gajdo M, Hummer K, Kresse G, Furthmller J, Bechstedt F 2006 Phys. Rev. B 73 045112

    [26]

    Togo A, Oba F, Tanaka I 2008 Phys. Rev. B 78 134106

    [27]

    Romero M J, Du H, Teeter G, Yan Y F, Al-Jassim M M 2011 Phys. Rev. B 84 165324

    [28]

    Grossberg M, Raadik T, Raudoja J, Krustok J 2014 Current Appl. Phys. 14 447

    [29]

    Chen S Y, Yang J H, Gong X G, Walsh A, Wei S H 2010 Phys. Rev. B 81 245204

    [30]

    Yang C Y, Qin M S, Wang Y M, Wan D Y, Huang F Q, Lin J H 2013 Sci. Rep. 3 1286

    [31]

    Henkelman G, Arnaldsson A, Jnsson H 2006 Comput. Mater. Sci. 36 354

    [32]

    Wang W, Shen H L, Jin J L, Li J Z, Ma Y 2015 Chin. Phys. B 24 056805

    [33]

    Gordillo G, Caldern C, Bartolo-Prez P 2014 Appl. Surf. Sci. 305 506

    [34]

    Chalapathi U, Uthanna S, Sundara R V 2015 Solar Energy Materials Solar Cells 132 476

    [35]

    Levcenko S, Gurieva G, Guc M, Nateprov A 2009 Moldav. J. Phys. Sci. 8 173

    [36]

    Chen Q M, Li Z Q, Ni Y, Cheng S Y, Dou X M 2012 Chin. Phys. B 21 038401

    [37]

    Strohm A, Eisenmann L, Gebhardt R K, Harding A, Schltzer T, Abou-Ras D, Schock H W 2005 Thin Solid Film 480-481 162

    [38]

    Camps I, Coutinho J, Mir M, da Cunha A F, Rayson M J, Briddon P R 2012 Semicond. Sci. Technol. 27 115001

    [39]

    Berlincourt D, Jaffe H, Shiozawa L R 1963 Phys. Rev. 129 1009

    [40]

    Krieger M, Sigg H, Herres N, Bachem K, Kohler K 1995 Appl. Phys. Lett. 66 682

    [41]

    Wortman J J, Evans R A 1965 J. Appl. Phys. 36 153

    [42]

    Matsushita H, Ichikawa T, Katsui A 2005 J. Mater. Sci. 40 2003

    [43]

    Schorr S, Gonzalez-Aviles G 2009 Phys. Status Solidi A 206 1054

    [44]

    Madelung O 2004 Semiconductors: Data Handbook (Berlin: Springer-Verlag) p205

    [45]

    https://en.wikipedia.org/wiki/Zinc_sulfide

    [46]

    Wang C C, Chen S Y, Yang J H, Lang L, Xiang H J, Gong X G, Walsh A, Wei S H 2014 Chem. Mater. 26 3411

    [47]

    DiSalvo F J, Waszczak J V 1982 Phys. Rev. B 26 2501

    [48]

    Klepp K O, Gurtner D 1996 Journal of Alloys and Compounds 243 19

    [49]

    Liu Y C, Yang Z, Cui D, Ren X D, Sun J K, Liu X J, Zhang J R, Wei Q B, Fan H B, Yu F Y, Zhang X, Zhao C M, Liu S Z 2015 Adv. Mater. 27 5176

    [50]

    Saidaminov M I, Adinolfi V, Comin R, Abdelhady A L, Peng W, Dursun I, Yuan M J, Hoogland S, Sargent E H, Bakr Q M 2015 Nat. Commn. 6 8724

    [51]

    Momma K, Izumi F 2008 J. Appl. Crystallogr. 41 653

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Publishing process
  • Received Date:  08 December 2015
  • Accepted Date:  03 January 2016
  • Published Online:  05 March 2016

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