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Influence of the Cu2ZnSnS4 absorber thickness on thin film solar cells
2015 (English)In: Physica status solidi. A, Applied research, ISSN 0031-8965, E-ISSN 1521-396XArticle in journal (Refereed) Published
Place, publisher, year, edition, pages
2015.
National Category
Engineering and Technology
Identifiers
URN: urn:nbn:se:uu:diva-265420DOI: DOI: 10.1002/pssa.201532311OAI: oai:DiVA.org:uu-265420DiVA: diva2:865605
Available from: 2015-10-28 Created: 2015-10-28 Last updated: 2017-12-01
In thesis
1. Annealing of Cu2ZnSn(S,Se)4 Thin Films: A Study of Secondary Compounds and Their Effects on Solar Cells
Open this publication in new window or tab >>Annealing of Cu2ZnSn(S,Se)4 Thin Films: A Study of Secondary Compounds and Their Effects on Solar Cells
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Kesterite Cu2ZnSnS4 (CZTS) is interesting as a sustainable photovoltaic technology due to its earth-abundant elements and suitable semiconducting properties. To date, a record efficiency of 12.6% has been achieved but further improvements are required to reach high efficiency for industrial implementation. Among the limiting issues is the understanding of the annealing process, which is crucial in promoting high material quality. In particular, the knowledge of the effects of segregated secondary compounds on solar cell performance is lacking.

In contrast to formation of ZnS particles throughout CZTS film, it is notable that SnS forms and usually segregates on the CZTS top and rear surfaces. The influence of SnS on CZTS solar cells was studied by electron beam induced current measurements. It is found that SnS presence on the CZTS surfacecan introduce “dead area”, whereas it seems beneficial for solar cell current when accumulates on the CZTS rear. For SnS passivation and from investigation of the passivation effect from an Al2O3 thin layer at the CZTS rear, improvement in overall device performance could not be demonstrated, due to either poor CZTS bulk or non-optimal device structure. The limitation in CZTS bulk quality was shown from a thickness study where carrier collection saturated already about 700-1000 nm CZTS thickness.

Formation of SnS alongside CZTS implies the anneal is limited by a deficient sulfur partial pressure (PS2). By looking into Sn-S phase transformations in SnS2 films after annealing, we find that PS2 drops rapidly over the annealing time, which could be well-correlated to a series of changes in CZTS material quality including secondary phase formations and defect modifications. It is shown that annealing CZTS under sufficiently high PS2 is critical for CZTS solar cells with high open circuit voltage (upto 783mV was reached), possibly due to the defect modification.

Besides SnS, it is observed that NaxS compounds are also readily formed on CZTS surfaces, due to Na diffusion from the glass substrate during annealing. NaxS negatively affects the formation of the CdS/CZTS interface during chemical bath deposition. It can be removed by an oxidation process or wet chemical etching.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2017. 85 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1476
Keyword
Annealing, sputtering, thin film, CZTS, secondary phases, solar cell
National Category
Engineering and Technology
Research subject
Engineering Science
Identifiers
urn:nbn:se:uu:diva-314975 (URN)978-91-554-9817-7 (ISBN)
Public defence
2017-03-31, Häggsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 13:15 (English)
Opponent
Supervisors
Available from: 2017-03-10 Created: 2017-02-07 Last updated: 2017-03-20
2. Modeling and electrical characterization of Cu(In,Ga)Se2 and Cu2ZnSnS4 solar cells
Open this publication in new window or tab >>Modeling and electrical characterization of Cu(In,Ga)Se2 and Cu2ZnSnS4 solar cells
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In this thesis, modeling and electrical characterization have been performed on Cu(In,Ga)Se2 (CIGS) and Cu2ZnSnS4 (CZTS) thin film solar cells, with the aim to investigate potential improvements to power conversion efficiency for respective technology. The modeling was primarily done in SCAPS, and current-voltage (J-V), quantum efficiency (QE) and capacitance-voltage (C-V) were the primary characterization methods. In CIGS, models of a 19.2 % efficient reference device were created by fitting simulations of J-V and QE to corresponding experimental data. Within the models, single and double GGI = Ga/(Ga+In) gradients through the absorber layer were optimized yielding up to 2 % absolute increase in efficiency, compared to the reference models. For CIGS solar cells of this performance level, electron diffusion length (Ln) is comparable to absorber thickness. Thus, increasing GGI towards the back contact acts as passivation and constitutes largest part of the efficiency increase. For further efficiency increase, majority bottlenecks to improve are optical losses and electron lifetime in the CIGS. In a CZTS model of a 6.7 % reference device, bandgap (Eg) fluctuations and interface recombination were shown to be the majority limit to open circuit voltage (Voc), and Shockley-Read-Hall (SRH) recombination limiting Ln and thus being the majority limit to short-circuit current and fill-factor. Combined, Eg fluctuations and interface recombination cause about 10 % absolute loss in efficiency, and SRH recombination about 9 % loss, compared to an ideal system. Part of the Voc-deficit originates from a cliff-type conduction band offset (CBO) between CZTS and the standard CdS buffer layer, and the energy of the dominant recombination path (EA) is around 1 eV, well below Eg for CZTS. However, it was shown that the CBO could be adjusted and improved with Zn1-xSn­xOy buffer layers. Best results gave EA = 1.36 eV, close to Eg = 1.3-1.35 eV for CZTS as given by photoluminescence, and the Voc-deficit decreased almost 100 mV. Experimentally by varying the absorber layer thickness in CZTS devices, the efficiency saturated at <1 μm, due to short Ln, expected to be 250-500 nm, and narrow depletion width, commonly of the order 100 nm in in-house CZTS. Doping concentration (NA) determines depletion width, but is critical to device performance in general. To better estimate NA with C-V, ZnS and CZTS sandwich structures were created, and in conjunction with simulations it was seen that the capacitance extracted from CZTS is heavily frequency dependent. Moreover, it was shown that C-V characterization of full solar cells may underestimate NA greatly, meaning that the simple sandwich structure might be preferable in this type of analysis. Finally, a model of the Cu2ZnSn(S,Se)4 was created to study the effect of S/(S+Se) gradients, in a similar manner to the GGI gradients in CIGS. With lower Eg and higher mobility for pure selenides, compared to pure sulfides, it was seen that increasing S/(S+Se) towards the back contact improves efficiency with about 1 % absolute, compared to the best ungraded model where S/(S+Se) = 0.25. Minimizing Eg fluctuation in CZTS in conjunction with suitable buffer layers, and improving Ln in all sulfo-selenides, are needed to bring these technologies into the commercial realm.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2017. 86 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1514
National Category
Engineering and Technology
Identifiers
urn:nbn:se:uu:diva-320308 (URN)978-91-554-9909-9 (ISBN)
Public defence
2017-06-08, Polhemsalen, Ångströmlaboratoriet, Läderhyddsvägen 1, Uppsala, 09:15 (English)
Opponent
Supervisors
Funder
Knut and Alice Wallenberg FoundationSwedish Energy AgencySwedish Research Council
Available from: 2017-05-18 Created: 2017-04-18 Last updated: 2017-06-07

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Ren, Yi

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