Synthesis of CZTSSe Thin Films from Nanocrystal Inks

Hages, Charles J.

doi:10.1002/9781118437865.ch11

Cited by 10 publications

(13 citation statements)

References 111 publications

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“…Here we characterize notable changes in the grain size upon Ag-incorporation. All films demonstrate dense packing of the grains with no voids, as well as a bi-layer morphology which is commonly reported for selenized nanocrystal-based films [20]. However, a significantly larger average grain size with a reduction in the number of vertical grain boundaries is characterized for the ACZTSe films with increasing Ag-content relative to CZTSeeven with only 5 at.…”

Section: Absorber Characterizationsupporting

confidence: 57%

“…Nanoparticle synthesis described herein follows the procedures described by Miskin et al [19] for CZTS synthesis. Additionally, Ag-incorporation is explored through substitution of silver acetylacetonate (98% Sigma-Aldrich) in place of copper (II) acetylacetonate (97% Sigma-Aldrich) in the nanoparticle synthesis, considered here with While minimal elemental losses are typically characterized for the described nanocrystal-based absorbers following selenization [3,20], EDX analysis on the selenized film with 50 at. % Ag loading was used to verify no notable changes in the atomic ratio exist following the heat treatment.…”

Section: Methodsmentioning

confidence: 99%

“…A mass balance consideration suggests the existence of ZnS in the 50%-ACZTS nanoparticles, though this phase is difficult to distinguish from XRD and nonresonant (w.r.t. ZnS) Raman analysis [20].…”

Section: Nanoparticle Characterizationmentioning

confidence: 99%

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Optoelectronic and material properties of nanocrystal-based CZTSe absorbers with Ag-alloying

Hages

Koeper

Agrawal

2016

Solar Energy Materials and Solar Cells

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127

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In this work, the benefits of Ag-alloying in kesterite solar cells are explored in terms of tunable band gap, improved grain growth, improved minority carrier lifetime, reduced defect formation, and reduced potential fluctuations for (Ag,Cu) 2 ZnSnSe 4 (ACZTSe) absorbers relative to Cu 2 ZnSnSe 4 (CZTSe). The enhanced optoelectronic properties are shown to scale here with the degree of Ag-alloying in ACZTSe. The impacts of these effects on device performance are discussed, with improvement in average device performance/open-circuit voltage reported for ACZTSe (5%-Ag) absorbers relative to CZTSe absorbers with similar band gap. These initial results are promising for the Ag-alloyed ACZTSe material system as V OC limitations are the primary cause of poor device performance in kesterite solar cells, and cation substitution presents a unique method to tune the defect properties of kesterite absorbers. Herein, nanoparticle synthesis and large-grain ACZTSe absorber formation is described followed by material and optoelectronic characterization. Additionally, RTP processing is presented to achieve fully selenized large-grain chalcogenide absorbers from sulfide nanocrystal inks.In addition to modification of the defect properties, Ag-alloying may also be beneficial for band gap tuning/grading of the absorber for improved performance. For CZTSSe, the absorber band gap (E G ) is determined mainly by Cu d orbital and S/Se p orbital anti-bonding (valance band maximum -VBM) and Sn s orbital and S/Se sp

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Section: Absorber Characterizationsupporting

confidence: 57%

Section: Methodsmentioning

confidence: 99%

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Optoelectronic and material properties of nanocrystal-based CZTSe absorbers with Ag-alloying

Hages

Koeper

Agrawal

2016

Solar Energy Materials and Solar Cells

Self Cite

127

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“…Figure 6 shows SEM images taken for a typical thin film, featuring a porous microstructure with low grain growth, high surface roughness, and formation of large gaps or cracks which can extend throughout the thickness of the film, as indicated by the cross-section image in Figure 6b. Although the binary sulfides are expected to provide a reactive sintering environment [36], more analysis is necessary to establish optimal grain growth conditions for this methodology. Low coating density is detrimental to device performance and should be avoided, due to the increased presence of voids and cracks causing surface defects and a film with reduced grain size can result in unfavorable carrier transport [57].…”

Section: Resultsmentioning

confidence: 99%

“…This method of synthesis also removes the need to use the toxic thiourea complexing agent. Another attractive feature of using binary sulfide nanocrystals instead of CZTS nanocrystals is that it can enable a reactive sintering environment without reliance on selenium during the annealing process [36]. Reactive sintering helps to achieve uniform elemental distribution, which reduces the likelihood of forming localized, detrimental secondary phases and grows larger grains which lower the impact of charge carrier trapping and recombination at interfacial features.…”

Section: Introductionmentioning

confidence: 99%

Aqueous-Based Binary Sulfide Nanoparticle Inks for Cu2ZnSnS4 Thin Films Stabilized with Tin(IV) Chalcogenide Complexes

et al. 2019

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Cu2ZnSnS4 (CZTS) is a promising semiconductor material for photovoltaic applications, with excellent optical and electronic properties while boasting a nontoxic, inexpensive, and abundant elemental composition. Previous high-quality CZTS thin films often required either vacuum-based deposition processes or the use of organic ligands/solvents for ink formulation, which are associated with various issues regarding performance or economic feasibility. To address these issues, an alternative method for depositing CZTS thin films using an aqueous-based nanoparticle suspension is demonstrated in this work. Nanoparticles of constituent binary sulfides (CuxS and ZnS) are stabilized in an ink using tin(IV)-based, metal chalcogenide complexes such as [Sn2S6]4−. This research paper provides a systematic study of the nanoparticle synthesis and ink formulation via the enabling role of the tin chalcogenide complexing power, the deposition of high-quality CZTS thin films via spin coating and annealing under sulfur vapor atmosphere, their structural characterization in terms of nanocrystal phase, morphology, microstructure, and densification, and their resultant optoelectronic properties.

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Chemical engineering for a solar economy (2017 P. V. Danckwerts Lecture)

Agrawal

2019

Chemical Engineering Science

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Synthesis of CZTSSe Thin Films from Nanocrystal Inks

Cited by 10 publications

References 111 publications

Optoelectronic and material properties of nanocrystal-based CZTSe absorbers with Ag-alloying

Optoelectronic and material properties of nanocrystal-based CZTSe absorbers with Ag-alloying

Aqueous-Based Binary Sulfide Nanoparticle Inks for Cu2ZnSnS4 Thin Films Stabilized with Tin(IV) Chalcogenide Complexes

Chemical engineering for a solar economy (2017 P. V. Danckwerts Lecture)

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