Suppressing the formation of double-layer in Cu2ZnSnSe4(CZTSe) absorber layer by facile heating process through nontoxic selenium atmosphere
Fang-I Lai
Department of Electrical Engineering program C, Yuan-Ze University, Chung-Li, Taiwan
Search for more papers by this authorJui-Fu Yang
Department of Electronic Engineering, Chang Gung University, Taoyuan, Taiwan
Search for more papers by this authorCorresponding Author
Yu-Chao Hsu
School of Medicine, Chang Gung University, Taoyuan, Taiwan
Department of Urology, Chang Gung Memorial Hospital, Taoyuan, Taiwan
Correspondence
Yu-Chao Hsu, School of Medicine, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Taoyuan 333, Taiwan.
Email: [email protected]
Shou-Yi Kuo, Department of Electronic Engineering, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Taoyuan 333, Taiwan.
Email: [email protected]
Search for more papers by this authorCorresponding Author
Shou-Yi Kuo
Department of Electronic Engineering, Chang Gung University, Taoyuan, Taiwan
Department of Urology, Chang Gung Memorial Hospital, Taoyuan, Taiwan
Correspondence
Yu-Chao Hsu, School of Medicine, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Taoyuan 333, Taiwan.
Email: [email protected]
Shou-Yi Kuo, Department of Electronic Engineering, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Taoyuan 333, Taiwan.
Email: [email protected]
Search for more papers by this authorFang-I Lai
Department of Electrical Engineering program C, Yuan-Ze University, Chung-Li, Taiwan
Search for more papers by this authorJui-Fu Yang
Department of Electronic Engineering, Chang Gung University, Taoyuan, Taiwan
Search for more papers by this authorCorresponding Author
Yu-Chao Hsu
School of Medicine, Chang Gung University, Taoyuan, Taiwan
Department of Urology, Chang Gung Memorial Hospital, Taoyuan, Taiwan
Correspondence
Yu-Chao Hsu, School of Medicine, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Taoyuan 333, Taiwan.
Email: [email protected]
Shou-Yi Kuo, Department of Electronic Engineering, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Taoyuan 333, Taiwan.
Email: [email protected]
Search for more papers by this authorCorresponding Author
Shou-Yi Kuo
Department of Electronic Engineering, Chang Gung University, Taoyuan, Taiwan
Department of Urology, Chang Gung Memorial Hospital, Taoyuan, Taiwan
Correspondence
Yu-Chao Hsu, School of Medicine, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Taoyuan 333, Taiwan.
Email: [email protected]
Shou-Yi Kuo, Department of Electronic Engineering, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Taoyuan 333, Taiwan.
Email: [email protected]
Search for more papers by this authorSummary
The Cu2ZnSnSe4 (CZTSe) absorber layer is typically prepared by post-selenization with a metal precursor. In the process of selenization, the loss of SnSex is a common phenomenon, resulting in both an atomic- ratio change and double-layer distribution of the absorber layer. This change affects the film properties. Additionally, excessive deviation from stoichiometry causes the formation of secondary-phase compounds. Moreover, the double-layer distribution reduces the carrier transport between the Mo back electrode and the CZTSe absorber film, inhibiting the effectiveness of the CZTSe solar cell. To address these problems, this study used CuxSe and ZnxSn1−x targets as the sputtering target materials to reduce the loss of SnSex during the selenization of precursor films. In addition, the effect of heating rate on the atomic ratio of the absorber layer was explored by adjusting the heating rate, which is one of the selenization parameters. The results showed that faster heating rates reduced the loss of SnSex, adjusted the Zn/Sn ratio in the absorber layer, and decreased ZnSe-related defects. In this way, the double-layer distribution was improved, air holes were reduced, and crystal structure characteristics of the films were enhanced. Photoluminescence (PL) spectroscopy showed that the signal of the ZnSe-related defect decreased, and the band tail effect became insignificant. The CZTSe absorber layer fabricated under different heating rates is used to prepare the CZTSe solar cell with a photoelectric conversion efficiency ranging from 0.51% to 5.6%.
REFERENCES
- 1 Solar Frontier Press release: Solar Frontier Achieves World Record Thin-Film Solar Cell Efficiency of 23.35%, http://www.solar-frontier.com/eng/news/2017/1220_press.html.
- 2Ramanujam J, Singh U-P. Copper indium gallium selenide based solar cells—a review. Energy Environ Sci. 2017; 10: 1306-1319.
- 3Md A, Hasan M, Bahar A-N. An investigation into the effects of band gap and doping concentration on Cu(In, Ga)Se2 solar cell efficiency. SpringerPlus. 2016; 5: 578.
- 4Malitckaya M, Komsa H-P, Havu V, Puska M-J. Effect of alkali metal atom doping on the CuInSe2-based solar cell absorber. J Phys Chem C. 2017; 121: 15516-15528.
- 5Sun Y, Lin S, Li W, et al. Review on alkali element doping in cu(in, Ga)se 2 thin films and solar cells. Engineering. 2017; 3: 452-459.
- 6Jheng B-T, Liu P-T, Wu M-C. Efficiency enhancement of non-selenized Cu(In,Ga)Se2 solar cells employing scalable low-cost antireflective coating. Nanoscale Res Lett. 2014; 9: 331.
- 7Gour K-S, Karade V, Babar P, et al. Potential role of kesterites in development of earth-abundant elements-based next generation technology. Sol RRL. 2021; 5:2000815.
- 8Wang W, Winkler M-T, Gunawan O, et al. Device characteristics of CZTSSe thin-film solar cells with 12.6% efficiency. Adv Energy Mater. 2014; 4:1301465.
- 9Lee Y-S, Gershon T, Gunawan O, et al. Cu2ZnSnSe4 thin-film solar cells by thermal coevaporation with 11.6% efficiency and improved minority carrier diffusion length. Adv Energy Mater. 2014; 5:1401372.
- 10Taskesen T, Neerken J, Schoneberg J, et al. Device characteristics of an 11.4% CZTSe solar cell fabricated from sputtered precursors. Adv Energy Mater. 2018; 8:1703295.
- 11Ahmed S, Reuter K-B, Gunawan O, Guo L, Romankiw L-T, Deligianni H. A high efficiency electrodeposited Cu2ZnSnS4 solar cell. Adv Energy Mater. 2012; 2: 253-259.
- 12Guo L, Zhu Y, Gunawan O, et al. Electrodeposited Cu2ZnSnSe4 thin film solar cell with 7% power conversion efficiency. Prog Photovolt Res Appl. 2014; 22: 58-68.
- 13Li J, Wang H, Luo M, et al. 10% efficiency Cu2ZnSn(S,se)4 thin film solar cells fabricated by magnetron sputtering with enlarged depletion region width. Sol Energy Mater Sol Cells. 2016; 149: 242-249.
- 14Li J, Kim S, Nam D, et al. Tailoring the defects and carrier density for beyond 10% efficient CZTSe thin film solar cells. Sol Energy Mater Sol Cells. 2017; 159: 447-455.
- 15Zhang Z, Yao L, Zhang Y, et al. Modified back contact interface of CZTSe thin film solar cells: elimination of double layer distribution in absorber layer. Adv Sci. 2018; 5:1700645.
10.1002/advs.201700645 Google Scholar
- 16Yao L, Ao J, Jeng M-J, et al. Reactive mechanism of Cu2ZnSnSe4 thin films prepared by reactive annealing of the Cu/Zn metal layer in a SnSex + se atmosphere. Crystals. 2019; 9: 10.
- 17Lai F-I, Yang J-F, Chen W-C, Kuo S-Y. Cu2ZnSnSe4 thin film solar cell with depth gradient composition prepared by selenization of sputtered novel precursors. ACS Appl Mater Interfaces. 2017; 9: 40224-40234.
- 18Chalapathy R-B-V, Jung G-S, Ahn B-T. Fabrication of Cu2ZnSnS4 films by sulfurization of cu/ZnSn/cu precursor layers in sulfur atmosphere for solar cells. Sol Energy Mater Sol Cells. 2011; 95: 3216-3221.
- 19Katagiri H. Cu2ZnSnS4 thin film solar cells. Thin Solid Films. 2005; 480-481: 426-432.
- 20Redinger A, Siebentritt S. Coevaporation of Cu2ZnSnSe4 thin films. Appl Phys Lett. 2010; 97:092111.
- 21Gour K-S, Singh O-P, Yadav A-K, Parmar R, Singh VN. Effect of NaF evaporation on morphological and structural properties of Cu2ZnSnSe4 (CZTSe) thin film deposited by sputtering from a single compound target. J Alloys Compd. 2017; 718: 231-235.
- 22Gour K-S, Singh O-P, Biplab B, et al. Enhanced photoresponse of Cu2ZnSn(S, Se)4 based photodetector in visible range. J Alloys Compd. 2017; 694: 119-123.
- 23Oh M, Kim W-K. Sn compensation via SnSex binary vapor supply during Cu2ZnSnSe4 formation. J Alloys Compd. 2014; 616: 436-441.
- 24Shin B, Gunawan O, Zhu Y, Bojarczuk N-A, Chey S-J, Guha S. Thin film solar cell with 8.4% power conversion efficiency using an earth-abundant Cu2ZnSnS4 absorber. Prog Photovolt Res Appl Ther. 2013; 21: 72-76.
- 25Chen S, Walsh A, Gong X-G, Wei S-H. Classification of lattice defects in the kesterite Cu2ZnSnS4 and Cu2ZnSnSe4 earth-abundant solar cell absorbers. Adv Mater. 2013; 25: 1522-1539.
- 26Djemour R, Redinger A, Mousel M, et al. The three A symmetry Raman modes of kesterite in Cu2ZnSnSe4. Opt Express. 2013; 21: A695-A703.
- 27Stanchik A-V, Tivanov M-S, Tyukhov I-I, et al. Temperature dependence of Raman scattering in the Cu2ZnSnSe4 thin films on a Ta foil substrate. Sol Energy. 2020; 201: 480-488.
- 28Park D, Nam D, Jung S, et al. Optical characterization of Cu2ZnSnSe4 grown by thermal co-evaporation. Thin Solid Films. 2011; 519: 7386-7389.
- 29Kaur K, Sood M, Kumar N, et al. Critical role of Zn/Sn ratio to enhance Cu-Zn-Sn-S solar cell efficiency by suppressing detrimental Cu2-xS secondary phase. Sol Energy Mater Sol Cells. 2018; 179: 22-30.
- 30Yang K-J, Sim J-H, Son D-H, et al. Effects of the compositional ratio distribution with sulfurization temperatures in the absorber layer on the defect and surface electrical characteristics of Cu2ZnSnS4 solar cells. Prog Photovolt Res Appl. 2015; 23: 1771-1784.
- 31Djemour R, Mousel M, Redinger A, et al. Detecting ZnSe secondary phase in Cu2ZnSnSe4 by room temperature photoluminescence. Appl Phys Lett. 2013; 102: 222108.
- 32Rey G, Larramona G, Bourdais S, et al. On the origin of band-tails in kesterite. Sol Energy Mater Sol Cells. 2018; 179: 142-151.
- 33Zawadzki P, Zakutayev A, Lany S. Entropy-driven clustering in tetrahedrally bonded multinary materials. Phys Rev Appl. 2015; 3:034007.
- 34Scragg J-J-S, Larsen J-K, Kumar M, et al. Cu–Zn disorder and band gap fluctuations in Cu2ZnSn(S, Se)4: theoretical and experimental investigations. Phys Status Solidi (b). 2016; 253(2): 247-254.
- 35Gokmen T, Gunawan O, Todorov T-K, Mitzi D-B. Band tailing and efficiency limitation in kesterite solar cells. Appl Phys Lett. 2013; 103:103506.
- 36Kauk-Kuusik M, Li X-F, Pilvet M, et al. Nano-scale sulfurization of the Cu2ZnSnSe4 crystal surface for photovoltaic applications. J Mater Chem A. 2019; 7: 24884-24890.
- 37Payno D, Sánchez Y, Blázquez O, et al. Partial substitution of the CdS buffer layer with interplay of fullerenes in kesterite solar cells. J Mater Chem C. 2020; 8: 12533.
- 38Wang S, Shen Z, Sun Y, et al. Defects and surface electrical property transformation induced by elemental interdiffusion at the p-n heterojunction via high-temperature annealing. ACS Appl Mater Interfaces. 2021; 13: 12211-12220.
- 39Li S, Lloyd M-A, McCandless B-E, Baxter J-B. Effects of cation composition on carrier dynamics and photovoltaic performance in Cu2ZnSnSe4 monocrystal solar cells. Sol Energy Mater Sol Cells. 2020; 205: 110255.
- 40Ignacio B-R, Diouldé S, Marcel P, et al. Transition-metal oxides for Kesterite solar cells developed on transparent substrates. ACS Appl Mater Interfaces. 2020; 12: 33656-33669.
- 41Saragih AD, Kuo DH. Germanium substitution effect on the property and performance of Cu2ZnSnSe4 thin films and its solar cell having absorber layer made by sputtering with single metallic target plus selenization. Mater Sci Eng B. 2019; 250: 114437.
- 42Valdés M, Sánchez Y, Perelstein G, et al. Influence of co-electrodeposition parameters in the synthesis of kesterite thin films for photovoltaic. J Alloys Compd. 2020; 839: 155679.
- 43Temgoua S, Bodeux R, Mollica F, Naghavi N. Comparative study of Cu2ZnSnSe4 solar cells growth on transparent conductive oxides and molybdenum substrates. Sol Energy. 2019; 194: 121-127.
- 44Nguyen TTH, Tran DH, Dang VAD, et al. Developing highly crystalline, single-phase and copper-poor Cu2ZnSnSe4 nanoparticles for solar cell application. Mater Lett. 2020; 269: 127654.