| 1. |
- Aboulfadl, Hisham, 1986, et al.
(författare)
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Alkali Dispersion in (Ag,Cu)(In,Ga)Se2 Thin Film Solar Cells - Insight from Theory and Experiment
- 2021
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Ingår i: ACS Applied Materials & Interfaces. - : American Chemical Society (ACS). - 1944-8252 .- 1944-8244. ; 13:6, s. 7188-7199
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Tidskriftsartikel (refereegranskat)abstract
- Silver alloying of Cu(In,Ga)Se2 absorbers for thin film photovoltaics offers improvements in open-circuit voltage, especially when combined with optimal alkali-treatments and certain Ga concentrations. The relationship between alkali distribution in the absorber and Ag alloying is investigated here, combining experimental and theoretical studies. Atom probe tomography analysis is implemented to quantify the local composition in grain interiors and at grain boundaries. The Na concentration in the bulk increases up to ∼60 ppm for [Ag]/([Ag] + [Cu]) = 0.2 compared to ∼20 ppm for films without Ag and up to ∼200 ppm for [Ag]/([Ag] + [Cu]) = 1.0. First-principles calculations were employed to evaluate the formation energies of alkali-on-group-I defects (where group-I refers to Ag and Cu) in (Ag,Cu)(In,Ga)Se2 as a function of the Ag and Ga contents. The computational results demonstrate strong agreement with the nanoscale analysis results, revealing a clear trend of increased alkali bulk solubility with the Ag concentration. The present study, therefore, provides a more nuanced understanding of the role of Ag in the enhanced performance of the respective photovoltaic devices.
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| 2. |
- Grini, Sigbjörn, et al.
(författare)
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Strong Interplay between Sodium and Oxygen in Kesterite Absorbers : Complex Formation, Incorporation, and Tailoring Depth Distributions
- 2019
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Ingår i: Advanced Energy Materials. - : WILEY-V C H VERLAG GMBH. - 1614-6832 .- 1614-6840. ; 9:27
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Tidskriftsartikel (refereegranskat)abstract
- Sodium and oxygen are prevalent impurities in kesterite solar cells. Both elements are known to strongly impact performance of the kesterite devices and can be connected to efficiency improvements seen after heat treatments. The sodium distribution in the kesterite absorber is commonly reported, whereas the oxygen distribution has received less attention. Here, a direct relationship between sodium and oxygen in kesterite absorbers is established using secondary ion mass spectrometry and explained by defect analyses within the density functional theory. The calculations reveal a binding energy of 0.76 eV between the substitutional defects Na-Cu and O-S in the nearest neighbor configuration, indicating an abundance of Na Symbol of the Klingon Empire O complexes in kesterite absorbers at relevant temperatures. Oxygen incorporation is studied by introducing isotopic O-18 at different stages of the Cu2ZnSnS4/Mo/soda-lime glass baseline processing. It is observed that oxygen from the Mo back contact and contaminations during the sulfurization are primary contributors to the oxygen distribution. Indeed, unintentional oxygen incorporation leads to immobilization of sodium. This results in a strong correlation between sodium and oxygen, in excellent agreement with the theoretical calculations. Consequently, oxygen availability should be monitored to optimize postdeposition heat treatments to control impurities in kesterite absorbers and ultimately, the solar cell efficiency.
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| 3. |
- Keller, Jan, et al.
(författare)
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On the Paramount Role of Absorber Stoichiometry in (Ag,Cu)(In,Ga)Se2 Wide‐Gap Solar Cells
- 2020
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Ingår i: Solar RRL. - : Wiley. - 2367-198X. ; 4:12
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Tidskriftsartikel (refereegranskat)abstract
- This contribution evaluates the effect of absorber off‐stoichiometry in wide‐gap (Ag,Cu)(In,Ga)Se2 (ACIGS) solar cells. It is found that ACIGS films show an increased tendency to form ordered vacancy compounds (OVCs) with increasing Ga and Ag contents. Very little tolerance to off‐stoichiometry is detected for absorber compositions giving the desired properties of 1) an optimum bandgap (EG) for a top cell in tandem devices (EG = 1.6–1.7 eV) and at the same time 2) a favorable band alignment with a CdS buffer layer. Herein, massive formation of either In‐ or Ga‐enriched OVC patches is found for group I‐poor ACIGS. As a consequence, carrier transport and charge collection are significantly impeded in corresponding solar cells. The transport barrier appears to be increasing with storage time, questioning the long‐term stability of wide‐gap ACIGS solar cells. Furthermore, the efficiency of samples with very high Ga and Ag contents depends on the voltage sweep direction. It is proposed that the hysteresis behavior is caused by a redistribution of mobile Na ions in the 1:1:2 absorber lattice upon voltage bias. Finally, a broader perspective on OVC formation in the ACIGS system is provided and fundamental limitations for wide‐gap ACIGS solar cells are discussed.
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| 4. |
- Keller, Jan, et al.
(författare)
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Wide-gap (Ag,Cu)(In,Ga)Se2 solar cells with different buffer materials—A path to a better heterojunction
- 2020
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Ingår i: Progress in Photovoltaics. - : Wiley. - 1062-7995 .- 1099-159X. ; 28:4, s. 237-250
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Tidskriftsartikel (refereegranskat)abstract
- This contribution concerns the effect of the Ag content in wide-gap AgwCu1-wIn1-xGaxSe2 (ACIGS) absorber films and its impact on solar cell performance. First-principles calculations are conducted, predicting trends in absorber band gap energy (Eg) and band structure across the entire compositional range (w and x). It is revealed that a detrimental negative conduction band offset (CBO) with a CdS buffer can be avoided for all possible absorber band gap values (Eg = 1.0–1.8 eV) by adjusting the Ag alloying level. This opens a new path to reduce interface recombination in wide-gap chalcopyrite solar cells. Indeed, corresponding samples show a clear increase in open-circuit voltage (VOC) if a positive CBO is created by sufficient Ag addition. A further extension of the beneficial compositional range (positive CBO at buffer/ACIGS interface) is possible when exchanging CdS with Zn1-ySnyOz, because of its lower electron affinity (χ). Nevertheless, the experimental results strongly suggest that at present, residual interface recombination still limits the performance of solar cells with optimized CBO, which show an efficiency of up to 15.1% for an absorber band gap of Eg = 1.45 eV.
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| 5. |
- Khavari, Faraz, et al.
(författare)
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Comparison of Sulfur Incorporation into CuInSe(2)and CuGaSe(2)Thin-Film Solar Absorbers
- 2020
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Ingår i: Physica Status Solidi (a) applications and materials science. - : WILEY-V C H VERLAG GMBH. - 1862-6300 .- 1862-6319. ; 217:22
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Tidskriftsartikel (refereegranskat)abstract
- Herein, sulfurization of CuInSe(2)and CuGaSe2(CGSe) absorber layers is compared to improve the understanding of sulfur incorporation into Cu(In,Ga)Se(2)films by annealing in a sulfur atmosphere. It is found for Cu-poor CuInSe(2)that for an annealing temperature of 430 degrees C, sulfur is incorporated into the surface of the absorber and forms an inhomogeneous CuIn(S,Se)(2)layer. In addition, at 530 degrees C, a surface layer of CuInS(2)is formed. In contrast, for Cu-poor CuGaSe(2)samples, S can only be introduced at 530 degrees C, mainly forming an alloy of CuGa(S,Se)(2), where no closed CuGaS(2)layer is found. In Cu-rich CuGaSe(2)samples, however, selenium is substituted by S already at 330 degrees C, which can be explained by a rapid phase transformation of Cu2 - xSe into Cu2 - x(S,Se). This transformation facilitates S in-diffusion and catalyzes CuGa(S,Se)(2)formation, likewise that previously reported to occur in CuInSe2. Finally, the Cu-poor CuInSe(2)solar cell performance is improved by the sulfurization step at 430 degrees C, whereas for the 530 degrees C sample, a decreasing fill factor and short-circuit current density are observed, indicating lower diffusion length accompanied by possible formation of an electron transport barrier. In contrast, the electrical characteristics deteriorate for all sulfurized Cu-poor CuGaSe(2)cells.
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| 6. |
- Khavari, Faraz, et al.
(författare)
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Post‐deposition sulfurization of CuInSe2 solar absorbers by employing sacrificial CuInS2 precursor layers
- 2022
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Ingår i: Physica Status Solidi (a) applications and materials science. - : John Wiley & Sons. - 1862-6300 .- 1862-6319. ; 219:5
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Tidskriftsartikel (refereegranskat)abstract
- Herein, a new route of sulfur grading in CuInSe2 (CISe) thin-film solar absorbers by introducing an ultrathin (<50 nm) sacrificial sputtered CuInS2 (CIS) layer on top of the CISe. Different CIS top layer compositions (Cu-poor to Cu-rich) are analyzed, before and after a high-temperature treatment in selenium (Se)- or selenium+sulfur (SeS)-rich atmospheres. An [S]/([S] + [Se]) grading from the surface into the bulk of the Se- and SeS-treated samples is observed, and evidence of the formation of a mixed CuIn(S,Se)2 phase by Raman analysis and X-ray diffraction is provided. The optical bandgap from quantum efficiency measurements of solar cells is increased from 1.00 eV for the CISe reference to 1.14 and 1.30 eV for the Se- and SeS-treated bilayer samples, respectively. A ≈150 mV higher VOC is observed for the SeS-treated bilayer sample, but the cell exhibits blocking characteristics resulting in lower efficiency as compared with the CISe reference. This blocking is attributed to an internal electron barrier at the interface to the sulfur-rich surface layer. The difference in reaction routes and possible ways to improve the developed sulfurization process are discussed.
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| 7. |
- Larsen, Jes K., et al.
(författare)
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Experimental and Theoretical Study of Stable and Metastable Phases in Sputtered CuInS2
- 2022
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Ingår i: Advanced Science. - : Wiley. - 2198-3844. ; 9:23
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Tidskriftsartikel (refereegranskat)abstract
- The chalcopyrite Cu(In,Ga)S2 has gained renewed interest in recent years due to the potential application in tandem solar cells. In this contribution, a combined theoretical and experimental approach is applied to investigate stable and metastable phases forming in CuInS2 (CIS) thin films. Ab initio calculations are performed to obtain formation energies, X-ray diffraction (XRD) patterns, and Raman spectra of CIS polytypes and related compounds. Multiple CIS structures with zinc-blende and wurtzite-derived lattices are identified and their XRD/Raman patterns are shown to contain overlapping features, which could lead to misidentification. Thin films with compositions from Cu-rich to Cu-poor are synthesized via a two-step approach based on sputtering from binary targets followed by high-temperature sulfurization. It is discovered that several CIS polymorphs are formed when growing the material with this approach. In the Cu-poor material, wurtzite CIS is observed for the first time in sputtered thin films along with chalcopyrite CIS and CuAu-ordered CIS. Once the wurtzite CIS phase has formed, it is difficult to convert into the stable chalcopyrite polymorph. CuIn5S8 and NaInS2 accommodating In-excess are found alongside the CIS polymorphs. It is argued that the metastable polymorphs are stabilized by off-stoichiometry of the precursors, hence tight composition control is required.
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| 8. |
- Larsen, Jes Kipkoech, et al.
(författare)
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Investigation of AgGaSe2 as a Wide Gap Solar Cell Absorber
- 2021
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Ingår i: ACS Applied Energy Materials. - : American Chemical Society (ACS). - 2574-0962. ; 4:2, s. 1805-1814
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Tidskriftsartikel (refereegranskat)abstract
- The compound AgGaSe2 has received limited attention as a potential wide gap solar cell material for tandem applications, despite its suitable band gap. This study aims to investigate the potential of this material by deposition of thin films by co-evaporation and production of solar cell devices. Since AgGaSe2 has a very low tolerance to off-stoichiometry, reference materials of possible secondary phases in the Ag2Se-Ga2Se3 system were also produced. Based on these samples, it was concluded that X-ray diffraction is suited to distinguish the phases in this material system. An attempt to use Raman spectroscopy to identify secondary phases was less successful. Devices were produced using absorbers containing the secondary phases likely formed during co-evaporation. When grown under slightly Ag-rich conditions, the Ag9GaSe6 secondary phase was present along with AgGaSe2, which resulted in devices being shunted under illumination. When absorbers were grown under Ag-deficient conditions, the AgGa5Se8 secondary phase was observed, making the device behavior dependent on the processing route. Deposition with a three-stage evaporation (Ag-poor, Ag-rich, and Ag-poor) resulted in AgGa5Se8 layers at both front and back surfaces, leading to charge carrier blocking in devices. Deposition of the absorber with a one-stage process, on the other hand, caused the formation of AgGa5Se8 locally extended through the entire film, but no continuous layer was found. As a consequence, these devices were not blocking and achieved an efficiency of up to 5.8%, which is the highest reported to date for AgGaSe2 solar cells.
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| 9. |
- Malyi, Oleksandr I., et al.
(författare)
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Energy, Phonon, and Dynamic Stability Criteria of Two-Dimensional Materials
- 2019
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Ingår i: ACS Applied Materials and Interfaces. - : AMER CHEMICAL SOC. - 1944-8244 .- 1944-8252. ; 11:28, s. 24876-24884
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Tidskriftsartikel (refereegranskat)abstract
- First-principles calculations have become a powerful tool to exclude the Edisonian approach in search of novel two-dimensional (2D) materials. However, no universal first-principles criteria to examine the realizability of hypothetical 2D materials have been established in the literature yet. Because of this, and as the calculations are always performed in an artificial simulation environment, one can unintentionally study compounds that do not exist in experiments. Although investigations of physics and chemistry of unrealizable materials can provide some fundamental knowledge, the discussion of their applications can mislead experimentalists for years and increase the gap between experimental and theoretical research. By analyzing energy convex hull, phonon spectra, and structure evolution during ab initio molecular dynamics simulations for a range of synthesized and recently proposed 2D materials, we construct energy, phonon, and dynamic stability filters that need to be satisfied before proposing novel 2D compounds. We demonstrate the power of the suggested filters for several selected 2D systems, revealing that some of them cannot be ever realized experimentally.
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| 10. |
- Malyi, Oleksandr, I, et al.
(författare)
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Noble gas as a functional dopant in ZnO
- 2019
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Ingår i: npj Computational Materials. - : SPRINGERNATURE. - 2057-3960. ; 5
-
Tidskriftsartikel (refereegranskat)abstract
- Owing to fully occupied orbitals, noble gases are considered to be chemically inert and to have limited effect on materials properties under standard conditions. However, using first-principles calculations, we demonstrate herein that the insertion of noble gas (i.e. He, Ne, or Ar) in ZnO results in local destabilization of electron density of the material driven by minimization of an unfavorable overlap of atomic orbitals of the noble gas and its surrounding atoms. Specifically, the noble gas defect (interstitial or substitutional) in ZnO pushes the electron density of its surrounding atoms away from the defect. Simultaneously, the host material confines the electron density of the noble gas. As a consequence, the interaction of He, Ne, or Ar with O vacancies of ZnO in different charge states q (ZnO:V-O(q)) affects the vacancy stability and their electronic structures. Remarkably, we find that the noble gas is a functional dopant that can delocalize the deep in-gap V-O(q) states and lift electrons associated with the vacancy to the conduction band.
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| 11. |
- Saini, Nishant, et al.
(författare)
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Germanium Incorporation in Cu2ZnSnS4 and Formation of a Sn–Ge Gradient
- 2019
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Ingår i: Physica Status Solidi (a) applications and materials science. - : Wiley. - 1862-6300 .- 1862-6319. ; 216:22
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Tidskriftsartikel (refereegranskat)abstract
- Alloying of Cu2ZnSnS4 (CZTS) with Ge can potentially promote grain growth and suppress the formation of Sn‐related defects. Herein, a two‐step fabrication route based on compound co‐sputtering and sulfurization at a high temperature is used to prepare Ge‐incorporated CZTS (Cu2ZnGexSn1 − xS4 [CZGTS]). For Cu2ZnGeS4 (CZGS), films deposited using elemental Ge and binary GeS targets are compared. The recrystallization is shown to be promoted for the absorbers deposited using Ge target, possibly due to lower sulfur content in the precursor suppressing the formation of wurtzite‐like phases during sputtering. The grain growth and crystallinity in CZGTS are slightly improved for x = 0.2 but not for higher concentration of the incorporated Ge. Owing to the composition‐dependent electronic properties, compositionally graded CZGTS films may be beneficial for reducing recombination towards the back contact. Hence, herein, the successful formation of a steep concentration gradient with Ge and Sn is demonstrated by the deposition of a CZGS/CZTS precursor stack followed by sulfurization with varying time periods.
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| 12. |
- Sopiha, Kostiantyn, et al.
(författare)
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Chalcogenide Perovskites : Tantalizing Prospects, Challenging Materials
- 2022
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Ingår i: Advanced Optical Materials. - : John Wiley & Sons. - 2162-7568 .- 2195-1071. ; 10:3
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Tidskriftsartikel (refereegranskat)abstract
- Chalcogenide perovskites have recently emerged into the spotlight as highly robust, earth abundant, and nontoxic candidates for various energy conversion applications, not least photovoltaics (PV). Now, a serious effort is required to determine if they can emulate the PV performance of the better-known, part-organic halide perovskites, in applications such as tandem solar cells. This review summarizes the surprisingly large body of literature pertaining to chalcogenide perovskites, which have been investigated for many years despite only recently being considered for applications. The confusing variety of claims coming from computational materials discovery is clarified, and it is specified which chalcogenide perovskites actually exist and should form the focus of experimental work. The highly interesting optoelectronic and transport properties of the known materials at their current stage of development are summarized, which makes a clear case for investigating them further. The existing synthesis literature is collated, which provides some important and possibly unnoticed clues to experimentalists grappling with these somewhat challenging materials. The authors hope that the highlighting of this information will facilitate further exciting studies, better approaches, and new progress for chalcogenide perovskites.
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| 13. |
- Sopiha, Kostiantyn, et al.
(författare)
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Chemistry of Oxygen Ionosorption on SnO2 Surfaces
- 2021
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 13:28, s. 33664-33676
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Tidskriftsartikel (refereegranskat)abstract
- Ionosorbed oxygen is the key player in reactions on metal-oxide surfaces. This is particularly evident for chemiresistive gas sensors, which operate by modulating the conductivity of active materials through the formation/removal of surface O-related acceptors. Strikingly though, the exact type of species behind the sensing response remains obscure even for the most common material systems. The paradigm for ab initio modeling to date has been centered around charge-neutral surface species, ignoring the fact that molecular adsorbates are required to ionize to induce the sensing response. Herein, we resolve this inconsistency by carrying out a careful analysis of all charged O-related species on three naturally occurring surfaces of SnO2. We reveal that two types of surface acceptors can form spontaneously upon the adsorption of atmospheric oxygen: (i) superoxide O2- on the (110) and the (101) surfaces and (ii) doubly ionized O2- on the (100) facet, with the previous experimental evidence pointing to the latter as the source of sensing response. This species has a unique geometry involving a large displacement of surface Sn, forcing it to attain the coordination resembling that of Sn2+ in SnO, which seems necessary to stabilize O2- and activate metal-oxide surfaces for gas sensing.
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| 14. |
- Sopiha, Kostiantyn, et al.
(författare)
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Off-stoichiometry in I-III-VI2 chalcopyrite absorbers : a comparative analysis of structures and stabilities
- 2022
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Ingår i: Faraday discussions. - : Royal Society of Chemistry (RSC). - 1359-6640 .- 1364-5498. ; 239:0, s. 357-374
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Tidskriftsartikel (refereegranskat)abstract
- Chalcopyrite Cu(In,Ga)Se-2 (CIGSe) solar absorbers are renowned for delivering high solar power conversion efficiency despite containing high concentration of lattice defects amounting to copper deficiencies of several atomic percent. The unique ability to incorporate this deficiency without triggering decomposition (i.e. "tolerance to off-stoichiometry") is viewed by many as the key feature of CIGSe. In principle, this property could benefit any solar absorber, but remarkably little attention has been paid to it so far. In this study, we assess the tolerance to off-stoichiometry of thin-film photovoltaic materials by carrying out ab initio analysis of group-I-poor ordered defect compounds (ODCs) in the extended family of I-III-VI systems (where I = Cu, Ag, III = Al, Ga, In, and VI = S, Se, Te). We analyze convex hulls and structural evolution with respect to group-I content, link them with experimental phase diagrams, and determine two empirical principles for the future identification of solar energy materials with high tolerance to off-stoichiometry. Practical implications for the deposition of I-III-VI absorbers are also discussed in light of our computational results and recent experimental findings.
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| 15. |
- Sopiha, Kostiantyn, et al.
(författare)
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Thermodynamic stability, phase separation and Ag grading in (Ag,Cu)(In,Ga)Se-2 solar absorbers
- 2020
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry. - 2050-7488 .- 2050-7496. ; 8:17, s. 8740-8751
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Tidskriftsartikel (refereegranskat)abstract
- Gallium alloying and grading in Cu(In,Ga)Se-2 (CIGS) are well-established strategies for improving performance of thin-film solar cells by tailoring band profiles within the absorber. Similarly, Ag incorporation is considered to be an effective complementary route towards further advancement of the field. Herein, we explore thermodynamics of the formation of (Ag,Cu)(In,Ga)Se-2 (ACIGS) alloy. Using first-principles methods, we reveal the existence of a miscibility gap in the Ga-rich alloys at temperatures close to those employed for the co-evaporation growth. We demonstrate that this property can result in phase separation and the formation of Ag gradients throughout the film thickness. We prove experimentally that the phase separation can indeed occur during low-temperature growth and/or post-deposition treatments. Furthermore, we uncover the anticorrelation between Ag and Ga contents, and demonstrate thermodynamically-driven formation of [Ag]/([Ag] + [Cu]) gradients in films with a steep [Ga]/([Ga] + [In]) profile. Finally, we discuss how these phenomena can influence solar cell devices. The presented results are expected to provide fundamental insight into the physics of growth and processing of ACIGS absorbers, which could be utilized to further boost the efficiency of thin-film solar cells.
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| 16. |
- Sopiha, Kostiantyn V, et al.
(författare)
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First-Principles Mapping of the Electronic Properties of Two-Dimensional Materials for Strain-Tunable Nanoelectronics
- 2019
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Ingår i: ACS APPLIED NANO MATERIALS. - : American Chemical Society (ACS). - 2574-0970. ; 2:9, s. 5614-5624
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Tidskriftsartikel (refereegranskat)abstract
- Herein, we demonstrate that first-principles calculations can be used for mapping of the electronic properties of two-dimensional (2d) materials with respect to nonuniform strain. By investigating four representative single-layer 2d compounds with different symmetries and bonding characters, namely, 2d-MoS2, phosphorene, alpha-Te, and beta-Te, we reveal that such a mapping can be an effective guidance for advanced strain engineering and the development of strain-tunable nano electronics devices, including transistors, sensors, and photodetectors. Thus, we show that alpha-Te and beta-Te are considerably more elastic compared to the 2d compounds with strong chemical bonding. In the case of beta-Te, mapping uncovers the existence of curious regimes where nonuniform deformations allow one to achieve unique localization of band edges in momentum space that cannot be realized under either uniform or uniaxial deformations. For all other systems, the strain mapping is shown to provide deeper insight into the known trends of band-gap modulation and direct-indirect transitions under strain. Hence, we prove that the standard way of analyzing selected strain directions is insufficient for some 2d systems, and a more general mapping strategy should be employed instead.
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