在本篇論文中，我們提出了以低成本,大量生產及可塗佈的溶液合成方法來合成銅鋅錫硒, 硒化銅銦鎵, 銅鋅錫硫及硫化錫為基礎的光伏材料,並針對反應機制，如晶體結構，薄膜組成，表面形態，光電性質進行探討。
我們開發了使用螯合溶劑聚醚胺,利用溶劑熱回流技術來合成各種多元無機奈米材料,其原料為元素粉末,具有低成本的優點,不須額外添加分散劑,為單一製程,其在兩端的兩個胺基鍵合部位提供了足夠的反應能力，結構中間連續的環氧鏈提供了乳化的作用，使其非常適合於油墨印刷中使用。
對於四元材料CZTSe和CIGSe，我們合成純相CZTSe納米顆粒約為20-24奈米,具有1.42電子伏特的能隙和良好的結晶度,組成為銅窮，鋅富。也成功合成了CIGS奈米顆粒,直徑均在28-46納米範圍內,薄膜組成為銅：銦:鎵：硒= 26.03：15.48：11：48時，能隙約為1.1eV，位於CuIn0.7Ga0.3Se2太陽能電池具有最高能量轉換效率（> 20％）的範圍內。然後，我們研究了根據不同的溶劑其對表面型態的影響,聚醚胺和異佛爾酮二胺的CZTSe納米粒子，其分子結構不同，如胺基團和分子大小，反應性和螯合能力。我們發現，聚醚胺合成具有更為銅窮和富Zn的CZTSe顆粒，更為平坦的表面及球狀顆粒。
由此可知溶液的合成受溶劑的螯合能力很大的影響，因此基於溶液酸鹼值的二元金屬–胺基錯合物的反應機制有了更進一步研究。
我們記錄加入四元材料前後的PH值變化及探討個別元素與之的關聯,來代表元素在聚醚胺中的反應,並探討溫度的效應,最後推導出元素間的氧化還原反應以及CZTSe反應機制。
未經加熱時PH值隨著反應時間的增加而減少,表示金屬與有機溶劑的反應為路易士酸鹼反應,我們可發現四元相 PH值的曲線與銅和鋅的PH曲線非常相似,且PH值皆隨反應時間階段式的變化,這證明CZTSe形成機制是依賴於時間。
加熱後，PH的增加表明還原機制支配CZTSe反應.我們然後比較CZTSe反應的PH值 - 時間曲線之前和加熱之後。首先，加熱後的PH值比以前要高得多，第二，PH值 - 時間曲線梯度加熱後變小，表示反應由金屬-胺錯合物穩定性控制。
為了進一步探討PH值和金屬錯合物形成機制之間的關係，我們以PH最大值和最小值的差的和平均值分別代表它代表金屬在聚醚胺中的反應能力及穩定性。
其中穩定性差異越大的元素將會首先反應,代表二元相的反應路徑。因此，反應性高的CuSe將首先出現，CuSe及SnSe由於穩定性差異大，導致形成Cu2SnSe3。最後反應形成CZTSe。
據我們所知，CZTSe太陽能電池效率仍比CIGS低了許多，這是由於開路電壓損失引起，由於組成偏離劑量比及不均勻所造成的雜質和相關的高缺陷密度引起的。
我們提供了兩個新的方法來克服這些問題.首先，我們直接通過改變前驅物溶液濃度來控制中間相然後再硫化得到完整CTS薄膜。具有良好表面型態,空穴濃度5.23×1017cm-3,遷移率14.2cm2/V-s時，能隙在1.35電子伏特，這是非常適合用於薄膜太陽能電池應用。
值得一提的是我們的實驗合成是在非平衡狀態下,我們證實在此一前驅物狀態下,有利於之後的均勻相變化。由此我們Cu2SnS3為有偏序結構的tetragonal晶體結構，但比規律結構monoclinic更好的電性。
第二，我們通過改變前驅物的銅/錫比和由低溫光致發光來探討改變組成所造成的缺陷性質,其依據能帶與缺陷位之間的載子轉移機制(BI transition)。我們發現在非計量組成下有最大的缺陷發光強度和偏移,尤其是在銅窮的狀態下,我們得到計量比的組成及沒有缺陷峰的存在。這代表在銅窮狀態銅/錫比為1.4的樣品呈現最高遷移率和最低載流子濃度，而銅/錫比2，1.8和1.2具有較高的載流子濃度，如CuSn和VCu。
根據我們的研究，非平衡相非常適合用於進一步退火。我們對CZTSe合成 3小時的樣品進行硒化，中間相由CuSe2，ZnSe,SnSe組成，熱處理後沒有任何其他二次相存在,CZTSe薄膜顯示平坦和更緊湊的結構。
為了實現這個目標，我們設計了單一個區域的結構但具有兩個溫度區來控制硒化處理的退火爐。以這種方式，對於硒氣氛,做為高效反應源，以硒粉溫度來調控;膜固化及相反應所需的熱能，以基板溫度表示;在相變與再結晶基底溫度和原子遷移方面，我們以退火時間表示。
我們提出了長晶與相轉變動態平衡的機制,該方法描述了二元相晶粒生長和轉化以及CZTSe晶粒生長是同時發生且互相競爭的。
因此,銅缺乏，鋅豐富的組成，平坦及均勻的表面型態只有在所有的二元相和CZTSe反應速度達到平衡時發生,硒粉溫度為500℃，基板溫度550℃,熱處理75分鐘。CZTSe具有銅/鋅+錫= 0.91，鋅/錫= 1.12的組成比例，對應於最佳CZTSe太陽能電池。 UV-VIS測量結果表明，在平衡狀態下，我們獲得能隙1.45eV，在合適的太陽光譜範圍。最後霍爾測量還顯示4.25×1017載流子濃度，電洞遷移率41.0941cm2/Vs,適合用於以P-N接面為基礎的光伏應用。
我們進一步製作CZTSe MSM光偵測器,並探討其光響應與表面形態、組成及電性的關係。我們也發現當硒化達到平衡時,硒粉溫度為500℃，基板溫度550℃,熱處理75分鐘具有最高的光響應,高於其他參數將近兩個order,證實了硒化製程穩定性對光電性質有很大的影響。
最後,我們比較了傳統熱處理及快速熱退火的差異並製作太陽能電池元件,由先前雙軌平衡探討可發現硒粉含量對相轉變和顆粒分佈有很大的影響,因此我們以550℃,5min硒粉1g,膜厚約5μm的條件下得到開路電壓580mV,閉路電流5.1mA/cm2,效率為1.06％。我們並發現在快速熱退火下,長晶與相轉變之間的平衡不易達成,故組成為Cu/(Zn+Sn)=1.19,Zn/Sn=1.14且表面較不均勻,這符合先前所述機制。
以上實驗證實我們的聚醚胺製程具有良好潛力來發展低成本,簡易及大面積的多元半導體奈米墨水。

In this essay, the CZTSe、CIGSe、CTS(e) and SnS photovoltaic material based synthesis process、reaction mechanism 、 film properties such as crystal structure、film composition、morphology、optoelectronic properties were fully investigated. We developed a one-step method for the synthesis of well-dispersed multicomponent inorganic semiconductor nanoparticles from elemental powders using a solvent-thermal reflux technique based on chelating solvent polyetheramine, providing two NH2 bonding sites at the ends as well as long, continuous epoxy chains in the center, making it ideally suited to the formation of CZTSe related material for use in ink printing.
For quaternary material CZTSe and CIGSe, we produced pure phase CZTSe nanoparticles approximately 20-24 nm in size with a band gap of 1.42 eV and good crystallinity in a Cu poor, Zn rich composition. CIGS nanoparticles were also successfully synthesized. The as-synthesized of CIGS nanoparticles with diameters were in the range of 28-46 nm with the chemical composition ratios Cu:In:Ga:Se=26.03:15.48:11:48, the optical band gap was approximately 1.1eV,located in the range of the CuIn0.7Ga0.3Se2 solar cells with the highest energy conversion efficiency (>20%).
We then investigated morphology of the CZTSe nanoparticles depending on different solvents polyetheramine and isophorondiamine, which are different in molecular structure such as amine group and molecule size,critical to reactivity and chelating ability to form metal-solvent chelate complexes. We found that the polyetheramine-based process produced particles with far more Cu-poor and Zn-rich composition CZTSe phases, a smoother and closed packed morphology, and a more spherical crystal shape.
We examined reaction mechanism firstly by design a redox reactions by recording the PH values of Cu, Zn, Sn, Se elements in the polyetheramine before and after the addition of thermal energy and compare with the whole quaternary phases solution reaction curve. Without heating, the PH value increased with reaction time. The PH curve was simply a reversal of the PH-time curves of Cu and Zn, which presented a stepwise reaction rate very similar to that of CZTSe. This proves that the CZTSe formation mechanism is time-dependent and stepwise. After heating, the increase in PH over time indicates that the reaction involves reduction.
To further characterize the relationship between PH values and metal complexes formation mechanism, we characterized the PH variation by max and min values interval and average calculation, which represent the indication of the reactivity of metal in polyetheramine, the reaction species most stable existing region.Thus, highly reactive Cu-Se would appear first, and Zn-Se would form later due to its proximity in the stability sequence. The Cu-Se would react with Sn-Se due to a large difference in stability, resulting in the formation of Cu2SnSe3. Finally, Zn-Se would react with Cu-Se-Sn to form CZTSe.
To our knowledge, CZTSe related device efficiency is still lower than CIGS based device, it is due to the fact that Voc loss induced poor efficiency due to the second phase impurities and related high defect density induced poor electrical properties.
We provide two novel methods to overcome these issues. First, we control the phase reactivity directly by synthesizing lower molar concentration of CTS precursor ink then under sulfurization, and we got pure phase CTS and has film electrical properties of hole concentration 5.23×1017cm-3and mobility 14.2cm2/V-s, the optical band-gap energy was measured at 1.35 eV, which are very suitable for thin-film solar cell applications. To be mentioned that our experiment used indicated that the noneqilibrium condition of precursor is beneficial to uniform phase transformation and related electrical properties. As a result, our Cu2SnS3 has crystal structure tetragonal for partial order structure but has superior electrical properties than order monoclinic structure.
Second, we tuned the precursor composition by changing Cu/Sn ratio and convinced the existence and species of defects by low temperature photoluminescence, which obeying the band to impurity transition, indicating an existence of defect based on nonstoichiometric composition. And under Cu poor condition we have shallow defects in low concentration, verifying that Cu poor condition for precursor is easier to get stoichiometric composition product. The sample with a Cu/Sn ratio of 1.4 presented the highest mobility and lowest carrier concentration, whereas samples prepared with Cu/Sn ratios of2, 1.8, and 1.2 have higher carrier concentration due to higher defect density such as CuSn and Vcu.
According our studies, nonequilibrium phases are well suited for further anneal. We selenized CZTSe 3hr sample, composed of intermediate phase such as CuSe2, ZnSe, SnSe. A completely pure CZTSe phase was formed without any other secondary phase existed after selenization. The CZTSe thin films show dense and more compact structure, with grain size about 1-2um.
To accomplish this goal, we designed a one zone structure anneal furnace with two zone temperature control to monitor the selenization process. In this way, efficient reaction source for Se atmosphere, in terms of Se powder temperature; film curing required thermal energy, in terms of substrate temperature and atoms migration for phase transformation and recrystallization, in terms of anneal time.
As a result, we would change the extent of binary phases grain growth and phase transformation into CZTSe. We then proposed a novel bi-path selenization process which describe the binary phases grain growth and transformation as well as CZTSe grain growth. The Cu poor, Zn rich composition with flat, closed pack morphology only occurred while all the binary phases and CZTSe grain reaction rate reached a equilibrium state at Se powder temperature 500℃ and substrate temperature 550℃, 75min. And we got CZTSe film with elemental composition Cu/(Zn+Sn)=0.91, Zn/Sn=1.12, corresponding to optimal CZTSe solar cell composition. UV-VIS measurement shown that at equilibrium state we obtained bandgap 1.45eV, lied in the suitable solar spectrum. Finally Hall measurement also shown a carrier concentration of 4.25×1017, mobility 41.091cm2/Vs, excellent for P-N junction based photovoltaic application.
Then we fabricated CZTSe based MSM photodetector to investigate the relationship between photosensitivity and film morphology, composition and electrical properties. And we found that photosensitivity is nearly two order larger than others for selenization equilibrium state at Se powder temperature 500℃ and substrate temperature 550℃, 75min. Finally, we compared the difference between thermal anneal and rapid thermal anneal. We found that under rapid thermal anneal we have more Cu rich composition Cu/(Zn+Sn)=1.19, Zn/Sn=1.14 and less uniform morphology. This is due to the reason that rapid reaction induced nonequlibrium selenization.
These indicated that stable selenization process has great impact on optoelectronic properties. Finally we fabricated solar cell based on 550℃5min Se powder 1g,film thickness 5μm by RTA, getting Voc 580mV,Isc, and efficiency 1.06％.
In this Dissertation, we proved that polyetheramine based process has great potential for low cost, facile and large area multicomponent nanoink.

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47. S. Bag, O. Gunawan, T. Gokmen, Y. Zhu, T. K. Todorov and D. B. Mitzi, “Low band gap liquid-processed CZTSe solar cell with 10.1% efficiency”, Environ. Eng. Sci. 5, 7060,(2012)
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8. D.H.Kuo, W.D.Haung, Y.S. Huang, J.D. Wu, Y.J. Lin,”Single-step sputtered Cu2SnSe3films using the targets composed of Cu2Se and SnSe2”,Thin Solid Films, 518,7218-7221, (2010)
9. P. Zhao, S. Cheng,”Influence of sulfurization temperature on photoelectric properties Cu2SnS3thin films deposited bymagnetron sputtering”,Adv. Mater.Sci. Eng.,726080, (2013)
10. D.Tiwari, T.K.Chaudhuri, T.Shripathi, U. Deshpande, R.Rawat,”Non-toxic,earth-abundant2%efficientCu2SnS3 solar cellbasedontetragonal films direct-coatedfromsinglemetal-organicprecursorsolution”,Sol.Energ. Mat. Sol. C.,113, 165-170, (2013)
11. S. Dias, S.B. Krupanidhi,”Temperature dependent electrical behavior of Cu2SnS3 films”,Adv. ,4,037121, (2014)
12. A.Kanevce, I.Repins, S.H. Wei,”Impact of bulk properties and local secondary phases on theCu2(Zn,Sn)Se4 solar cells open-circuit voltage“,Sol.Energ.Mater.Sol.C.,133,119-125, (2015)
13. M.Courel, J.A. Andrade-Arvizu, O. Vigil-Galan,”Loss mechanisms influence on Cu2ZnSnS4/CdS-based thin film solar cellperformance”,SolidState Electron.,111, 243-250, (2015)
14. C.J. Wang, S.C.Shei, S.J. Chang,”Synthesis and characterization of CZTSenanoinksusing polyetheramine as solvent”,Opt. Mater. Express,4,1593-1600, (2014)
15. C.J. Wang, S.C.Shei, S.J. Chang,“Novel solutionprocessforsynthesisofCIGSnanoparticlesusingpolyetheramineassolvent”,Mater.Lett.,122,52-54, (2014)
16. C.J. Wang, S.C. Shei, S.J. Chang,“Effect of solvent chelating on crystal growth mechanism of CZTSenanoink in polyetheramine”,IEEE T. Nanotechnology,14,896-903, (2015)
17. R.Xie, M. Rutherford, X.Peng,”Formation of high-quality I-III-VI semiconductornanocrystals by tuning relative reactivity of cationicprecursors”,J. Am. Chem. Soc. ,131,5691-5697, (2009)
18. M. Grossberg, T. Raadik, J. Raudoja, J. Krustok,”Photoluminescence study of defect clusters in Cu2ZnSnS4polycrystals”,Curr. Appl.Phy.,14,447-450, (2014)
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20. M. Grossberg, J. Krustok, J. Raudoja, T. Raadik, “The role of structural properties on deep defect states in Cu2ZnSnS4studied by photoluminescence spectroscopy”,Appl. Phys. Lett. ,101,102102, (2012)
21. K.Tanaka, T.Shinji,H.Uchiki,”PhotoluminescencefromCu2ZnSnS4 thin films withdifferent compositions fabricatedbyasputtering-sulfurizationmethod “,Sol.Energ.Mater.Sol.C.,126,143-148, (2014)
22. M. Grossberg, J. Krustok, K. Timmo, M. Altosaar,”Radiative recombination inCu2ZnSnSe4monograins studied byphotoluminescence spectroscopy”,Thin Solid Films, 517, 2489-2492,(2009)
23. J.H.Yang, X. G. Gong, A. Walsh, S.H. Wei,”Intrinsic point defects and complexes in the quaternary kesterite semiconductor Cu2ZnSnS4”, Phys. Rev. ,B81,245204, (2010)
24. P. Hu, Y. Cao,”Synthesis of rod and lath-shaped CuSe and tremella-shaped Cu2-xSe nanostructures at room temperature, and their optical properties“,J.Nanopart Res. ,14,703, (2012)
25. D. Martínez-Escobar, M.Ramachandran, A. Sánchez-Juárez, J.S.N. Rios,”Optical and electrical properties of SnSe2 and SnSe thin films prepared by Spray pyrolysis”,Thin Solid Films,535,390-393, (2013)
26. S.H. Han, A.M. Hermann, F.S. Hasoon, H.A. Al-Thani, D. H. Levi,”Effect of Cu deficiency on the optical properties and electronic structure of CuInSe2 and CuIn0.8Ga0.2Se2 determined by spectroscopic ellipsometry”,Appl. Phys.Lett.,85,576, (2004)
27. David B.Mitzin, OkiGunawan,TeodorK.Todorov,KejiaWang,SupratikGuha,“The path towards a high-performance solution-processed kesterite solar cell ”,Solar Energy Materials & Solar Cells, 95, 1421–1436,(2011)
28. Wei Wang, Mark T. Winkler, Oki Gunawan, TayfunGokmen, Teodor K. Todorov,Yu Zhu, David B. Mitzi, “Device Characteristics of CZTSSe Thin-Film Solar Cells with 12.6% Effi ciency ”,Advanced Energy Materials, 4, 1301465,1-5, (2014)
29. MahshidAhmadi, Stevin S. Pramana, Sudip K. Batabyal, Chris Boothroyd, Subodh G. Mhaisalkar, Yeng Ming Lam, “Synthesis of Cu2SnSe3 Nanocrystals for Solution Processable Photovoltaic Cells ”,Inorg. Chem., 52, 1722-1728,(2013)
30 Kang Min Kim, Hitoshi Tampo, Hajime Shibata, Shigeru Niki, “Temperature induced phase transformation in coevaporated Cu2SnSe3 thin films”,Materials Letters, 116 , 61–63,(2014)
31. Dong-HauKuo , WalelignWubet, “Mg dopant in Cu2SnSe3 : An n-type former and a promoter of electrical mobility up to 387 cm2v-1s-1”,J. Solid State Chemistry, 218 , 44–49, (2014)
32. Jianjun Wang, Ajay Singh, Pai Liu, Shalini Singh, Claudia Coughlan, YinaGuo, Kevin M Ryan, “Colloidal Synthesis of Cu2SnSe3 Tetrapod Nanocrystals”,J. Am. Chem. Soc., 135, 7835 – 7838,(2013)
33. Michelle E. Norako, Matthew J. Greaney, and Richard L. Brutchey, “Synthesis and Characterization of Wurtzite-Phase Copper Tin Selenide Nanocrystals”,J. Am. Chem.Soc., 134, 23 – 26,(2012)
34. RachmatAdhiWibowo, Stefan Moeckel, HyesunYoo, Astrid Hoelzing, Rainer Hock,Peter J. Wellmann, “Formation of Cu2SnSe3 from stacked elemental layers investigated by combined in situ X-ray diffraction and differential scanning calorimetry techniques ”,Journal of Alloys and Compounds, 588,254–258,(2014)
35. Kang Min Kim , Hitoshi Tampo, Hajime Shibata,ShigeruNiki, “Growth and characterization of coevaporated Cu2SnSe3 thin films forphotovoltaic applications ”,Thin Solid Films, 536,111–114,(2013)
36. Dong-HauKuo , Wei-Di Haung, Ying-Sheng Huang, Jiun-De Wu, Yan-Jih Lin, “Single-step sputtered Cu2SnSe3 films using the targets composed of Cu2Se and SnSe2”,Thin Solid Films, 518 , 7218–7221, (2010)
37. Maria Ib´a~nez, Doris Cadavid, Umberto Anselmi-Tamburini, Reza Zamani, St´ephaneGorsse, Wenhua Li, Antonio M. L´opez, Joan Ramon Morante, JordiArbiol, Andreu Cabot , “Colloidal synthesis and thermoelectric properties of Cu2SnSe3 nanocrystals ”,J. Mater. Chem. A, 1, 1421–1426, (2013)
38. Bin Li, Yi Xie , Jiaxing Huang, YitaiQian , “Synthesis, Characterization, and Properties of Nanocrystalline Cu2SnS3”,Journal of Solid State Chemistry,153, 170 -173,(2000)
39. Wzy Mohammad Harati, JiaJia, Ke´vinGiffard, Kyle Pellarin, Carly Hewson, David A. Love, Woon Ming Lau, Zhifeng Ding, “One-pot electrodeposition, characterization and photoactivity of stoichiometric copper indium gallium diselenide (CIGS) thin films for solar cells “,Phys. Chem. Chem. Phys., 12, 15282–15290, (2010)
40. Fiechter, M. Martinez, G. Schmidt, W. Henrion, Y. Tomm ,“Phase relations and optical properties of semiconducting ternary sulfides in the system Cu–Sn–S”, Journal of Physics and Chemistry of Solids,64 ,1859–1862,(2003)
41. G. Suresh Babu, Y.B. Kishore Kumar, Y. Bharath Kumar Reddy, V. Sundara Raja,”Growth and characterization of Cu2SnSe3 thin films” ,Materials Chemistry and Physics, 96, 442–446,(2006)
42. David Avellaneda, M. T. S. Nair,P. K. Nair, “Cu2SnS3 and Cu4SnS4 Thin Films via Chemical Deposition for Photovoltaic Application” ,Journal of The Electrochemical Society, 157 (6),D346-D352,(2010)
43. N. R. Mathews,J. TamyBenı´tez,F. Paraguay-Delgado , M. Pal , L. Huerta,“Formation of Cu 2 SnS 3 thin film by the heat treatment of electrodeposited SnS–Cu layers”, J Mater Sci: Mater Electron, 24,4060–4067,(2013)
44. RenguoXie, Michael Rutherford, and XiaogangPeng,“Formation of High-Quality I - III - VI Semiconductor Nanocrystals by Tuning Relative Reactivity of Cationic Precursors “,J. AM. CHEM. SOC., 131, 5691–5697, (2009)
45. G. HemaChandra,O. Lakshmana Kumar,R. PrasadaRao, S. Uthanna, “Influence of substrate and selenization temperatures on the growth of Cu2SnSe3 films” ,J. Mater.Sci, 46,6952–6959, (2011)
46. Hao Guan, HonglieShen, Chao Gao,Xiancong He, “The influence of annealing atmosphere on the phase formation of Cu–Sn–S ternary compound by SILAR method” ,Journal of Materials Science: Materials in Electronics, 24(9), 3195-3198,(2013)
47. Ara Cho, SeJinAhn, Jae Ho Yun , JihyeGwak , SeungKyuAhn , Keeshik Shin, JinsuYoo,Hyunjoon Song , Kyunghoon Yoon, “The growth of Cu2−xSe thin films using nanoparticles “,Thin Solid Films, 546,299–307,(2013)
48. Jianjun Wang, Ajay Singh, Pai Liu, Shalini Singh, Claudia Coughlan, YinaGuo, Kevin M. Ryan, “Colloidal Synthesis of Cu2SnSe3 Tetrapod Nanocrystals” ,J. Am. Chem. Soc., 135, 7835 – 7838,(2013)
49. S. Prucnal, F. Jiao, D. Reichel, K. Zhao, S. Cornelius, M. Turek,K. Pyszniak, A. Drozdziel, W. Skorupa, M. Helm, S. Zhou,“Influence of Flash Lamp Annealing on the Optical Properties of CIGS Layer” ,ActaPhysicaPolonica, A., 125(6), 1404,(2014)
50. WilmanSeptina, Shigeru Ikeda,Akio Kyoraiseki, Takashi Harada, Michio Matsumura,”Single-step Electrodeposition of a microcrystalline Cu2ZnSnSe4 thin film With a kesterite Structure”, ElectrochimicaActa,88, 436–442,(2013)
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52. Kuo-Chin Hsu, Yaw-Shyan Fu, Pei-Ying Lin, I-Tseng Tang, Jiunn-Der Liao Hindawi,“Fabrication and Characterization of CuInSe2 Thin Film Applicable for a Solar Energy Light Absorption Material via a Low Temperature Solid State Reaction”, International Journal of Photoenergy, 156964,1-7,(2013)
53. V. Izquierdo-Roca, A. Pérez-Rodríguez, A. Romano-Rodríguez, and J. R. Morante,” Raman microprobe characterization of electrodeposited S-rich CuIn(S,Se)2 for photovoltaic applications: Microstructural analysis”, J. Appl. Phys.,101, 103517,(2007)
54. Jin Chang , Eric R. Waclawik, “Controlled synthesis of CuInS2, Cu2SnS3 and Cu2ZnSnS4 nano-structures: insight into the universal phase-selectivity mechanism”,CrystEngComm, 15, 5612–5619, (2013)
55. C.B. Song, Y.L. Zhao, D.M. Song, L. Zhu, X.Q. Gu, Y.H. Qiang,“Dye-sensitized Solar Cells Based on TiO2 Nanotube/Nanoparticle Composite as Photoanode and Cu2SnSe3 as Counter Electrode” , Int. J. Electrochem. Sci., 9,3158 – 3165, (2014)
56. MahshidAhmadi, Stevin S. Pramana, Sudip K. Batabyal, Chris Boothroyd, Subodh G. Mhaisalkar,Yeng Ming Lam,“Synthesis of Cu2SnSe3 Nanocrystals for Solution Processable Photovoltaic Cells”,Inorg. Chem., 52, 1722−1728,(2013)
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6.1.7 Reference in Chapter 6
1. P. Jackson, D. Hariskos, E. Lotter, S. Paetel, R. Wuerz, R. Menner, W. Wischmann, M. Powalla, “New world record efficiency for Cu(In,Ga)Se2 thin-film solar cells beyond 20%”, Prog. PhotovoltaicsRes.Appl.,19, 894-897, (2011)
2.D.B. Mitzi, O. Gunawan, T.K.Todorov, K. Wang, S. Guha, “The path towards a high-performance solution-processed kesterite solar cell”,Sol. Energy Mater. Sol. Cells, 95, 1421-1436, (2011)
3. S.Siebentritt,S.Schorr, “A challenging material for solar cells”,Prog.PhotovoltaicsRes. Appl.,20, 512-519, (2012)
4.N.Aihara, H. Araki, A. Takeuchi, K.Jimbo, H.Katagiri, “Fabrication of Cu2SnS3 thin films by sulfurization of evaporated Cu-Sn precursors for solar cells”, Phys. Status Solidi C ,10, 1086-1092, (2013)
5. P. Zhao, S. Cheng, “Influence of Sulfurization Temperature on Photoelectric Properties Cu2SnS3 Thin Films Deposited by Magnetron Sputtering”,Adv. Mater. Sci. Eng., 726080-726084, (2013)
6. K. Chino, J. Koike, S.Eguchi, H. Araki,R. Nakamura,K.Jimbo, H.Katagiri, “Preparation of Cu2SnS3 Thin Films by Sulfurization of Cu/Sn Stacked Precursors”, J. J. Appl.Phy.,51, 10NC35, (2012)
7. Y. Tan, Z. Lin, W. Ren, W. Long, Y. Wang, X. Ouyang, “Facile solvothermal synthesis of Cu2SnS3 architectures and their visible-light-driven photocatalytic properties”,Mater.Lett. ,89, 240-242, (2012)
8.T. Nomura, T. Maeda,T. Wada, “Fabrication of Cu2SnS3 solar cells by screen-printing and high-pressure sintering process”,J. J. Appl.Phy.,53 , 05FW01, (2014)
9.J. Han, Y. Zhou, Y.Tian, Z. Huang, X. Wang, J.Zhong, Z. Xia, B. Yang, H. Song, J.Tang, ”Hydrazine processed Cu2SnS3 thin film and their application for photovoltaic devices”,Front.Optoelectron.,7, 37-45, (2014)
10.L.L.Baranowski, P.Zawadzki, S. Christensen, D.Nordlund, S.Lany, A.C.Tamboli, L.Gedvilas, D.S.Ginley, W.Tumas, E.S.Toberer, A.Zakutayev, “Control of Doping in Cu2SnS3 through Defects and Alloying”, Chem. Mater.,26,( 4951-4959, 2014)
11.M.Fiechter, G.Martinez, W.Schmidt, Y.Henrion, J. Tomm, “Phase relations and optical properties of semiconducting ternary sulfides in the system Cu–Sn–S”,J.Phy. Chem. Solids ,64,1859-1862, (2003)
12.P.A.Fernandes, P.M.P. Salomé1, A.F. da Cunha, “Study of Ternary Cu2SnS3 and Cu3SnS4 Thin Films Prepared by Sulfurizing Stacked Metal Precursors”,J. Physics D: Appl.Phy.,43 , 215403, (2010)
13.H.Zhang, M.Xie, S. Zhang, Y.Xiang, “Fabrication of highly crystallized Cu2SnS3 thin films throughsulfurization of Sn-rich metallic precursors”,J. Alloy. Compd.,602,199-203, (2014)
14.D.H.Kuo, W.D.Haung , Y.S. Huang, J.D. Wu, Y.J. Lin, “Single-step sputtered Cu2SnSe3films using the targets composed of Cu2Se and SnSe2”,Thin Solid Films ,518, 7218-7221, (2010)
15.C.J. Wang, S.C.Shei, S.J.Chang, “Synthesis and characterization of CZTSe nanoinks using polyetheramine as solvent”,Opt. Mater. Exp.,4,1593-1600, (2014)
16.R.Xie, M. Rutherford,X.Peng, “Formation of High-Quality I-III-VI Semiconductor Nanocrystals by Tuning Relative Reactivity of Cationic Precursors”, J. Am. Chem. Soc. ,131, 5691-5697, (2009)
17.M. Steichen, R.Djemour, L.Gütay, J.Guillot, S.Siebentritt, P.J. Dale, “Direct Synthesisof Single-Phase p Type SnS by Electrodeposition from a Dicyanamide Ionic Liquid at High Temperature for Thin Film Solar Cells”, J. Phys. Chem. C, 117,4383-4393, (2013)
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7.1.6 Reference in Chapter 7
1. A. de Kergommeaux, J. Faure-Vincent, A.Pron, R. de Bettignies, P. Reiss, “SnS thin films realized from colloidal nanocrystal inks”,Thin Solid Films ,535, 376–379,(2013)
2. S. Hori, T. Suzuki, T. Suzuki, T. Suzuki, S.Nonomura,“Synthesis and characterization of tin monosulfide nanosheets”,J. J. Appl. Phys. ,53,021801,(2014)
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4. S.K. Panda, S. Gorai, S. Chaudhuri, “Shape selective solvothermal synthesis of SnS: Role ofethylenediamine–water solvent system”,Mater. Sci. Eng. B,129, 265–269,(2006)
5. H. Zhu, D. Yang, H. Zhang, “Hydrothermal synthesis, characterization and properties of SnS nanoflowers”,Mater.Lett.,60, 2686–2689,(2006)
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16.J.Xu,Y. Yang,Z.Xie, “Fabrications of SnS thin films and SnS-based heterojunctions
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8.4 Reference in chapter 8
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2. R. B. V. Chalapathy ,Subrata Das1,Jeng-Shin Ma,Jen-Cheng Sung,Chung-Hsin Lu,” Characterization of Cu2ZnSnSe4 (CZTSe) nanoparticles synthesized via solvothermal method for solar cell applications”, J Mater Sci: Mater Electron,26, 7673–7682,(2015)
3. P.M.P. Salomé,J. Malaquias,P.A. Fernandes,M.S. Ferreira,A.F. da Cunha,J.P. LeitãoJ.C. González,F.M. Matinaga,“Growth and characterizationof Cu2ZnSn(S,Se)4 thin films for solar cells”, Solar Energy Materials andSolar Cells, 101, 147–153,2012
4. Carolin M. Fella , Alexander R.Uhl a, Ceri Hammond , Ive Hermans , Yaroslav E.Romanyuk , Ayodhya N. Tiwari ,”Formation mechanism of Cu2ZnSnSe4 absorber layers during selenization of solution deposited metal precursors” , Journal of Alloys and Compounds ,567 ,102–106, (2013)
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