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Dr. Outman EL KHOUJA

Assistant Researcher

Laboratory of Complex Heterostructures and Multifunctional Materials

outman[DOT]elkhouja[AT]infim[DOT]ro

Resume

Outman El KHOUJA, assistant researcher (since June 2021), born in 1994, graduated from the Faculty of Sciences Ain Chock -Specialization Energy Physics at Hassan II University Casablanca, Morocco, has a MSc degree in Materials engineering and characterization at Ibn Tofail University (UIT), Faculty of Science (FSK), Kenitra, Morocco. PhD degree obtained at FSK, UIT (January, 2024). Work experience: National Institute of Materials Physics (NIMP) (June 2021 – to date), International Center of Theoretical Physics (ICTP) grant (November 2020 to Jun 2021) at NIMP, chemistry and electrochemistry laboratory assistant (2019, 2020) – FSK, Kenitra, Morocco. Main areas of interest/ expertise: Preparation of semiconductor thin films by physical, chemical, and electrochemical methods (magnetron sputtering, electrodeposition, spray pyrolysis, Mist-CVD, Successive Ionic Layer Deposition (SILAR), and Chemical Bath Deposition (CBD)), materials characterization (X-ray diffraction (XRD), Conventional spectroscopies (UV-Vis, IR), SEM-EDS, Raman Spectroscopy, Electrochemistry). Publication (Last Updated May 2024): 15 articles published in Web of Science® (WoS) journals with impact factor (e.g. Ceram. Int., J. Alloy. Compd., Thin Solid Films), Hirsch index: 6, Citations (without self-citations): 60. Professional profile web-links: Brainmap https://brainmap.ro/outman-el-khouja; ORCID ID: 0000-0003-3471-0353; WoS ResearcherID: EUR-9887-2022

Publications

Open Access
1. Exploring the Synthesis of Cu2(Zn,Cd)SnS4 at High Temperatures as a Route for High-Efficiency Solar Cells
Authors: El Khouja, O; Gong, YC; Jimenez-Arguijo, A; Guerra, MJ; Medaille, AG; Scaffidi, R; Basak, A; Radu, C; Flandre, D; Vermang, B; Giraldo, S; Placidi, M; Li-Kao, ZJ; Galca, AC; Saucedo, E

Published: MAY 2025, PROGRESS IN PHOTOVOLTAICS, 33, DOI: 10.1002/pip.3899

The present research explores for the first time the intricate relationship between sulfurization temperature at unusual high temperatures (up to 700 degrees C) and the structural/optoelectronic properties of Cu-2(Zn,Cd)SnS4 (CZCTS) thin films, synthesized via a two-step sequential process involving the precursor film deposition using aprotic molecular ink followed by thermal treatment in sulfur atmosphere. X-ray diffraction patterns confirms the tetragonal structure. Scanning Electron Micrographs revealed significant grain growth, with grain sizes increasing from similar to 0.3 mu m at 620 degrees C to similar to 1.5 mu m at 680 degrees C, effectively reducing grain boundary recombination. Energy dispersive X-ray spectroscopy demonstrated a Cu-poor and Zn-rich composition, with a consistent Cd incorporation of similar to 3.7 at%. Raman spectroscopy showcases the homogeneity and purity of the CZCTS crystalline structure. Precise control of the sulfurization temperature plays a crucial role in determining the photovoltaic characteristics of CZCTS-based solar cells. By increasing the grain size and preventing the thermal decomposition of the CZTS phase, the photovoltaic performance peaked at a sulfurization temperature of 680 degrees C, achieving a power conversion efficiency (PCE) of 10.4%, with an open-circuit voltage of 0.701 V, a short-circuit current density of 24.3 mA/cm(2) and a fill factor of 60.8%. External quantum efficiency reached a maximum of 83.3% at 580 nm. The bandgap of the CZCTS absorber was determined to be 1.48 eV, optimal for photovoltaic applications. However, further increasing the sulfurization temperature to 700 degrees C resulted in a lower PCE of 8.5%, attributed to interface degradation and secondary phase formation. Temperature-dependent current-voltage measurements revealed a reduction in recombination losses, with an activation energy of 1.24 eV at the CZCTS/CdS interface, indicating effective defect passivation by Cd incorporation. The optimized films, sulfurized at 680 degrees C, displayed an absorber thickness of similar to 1.2 mu m after sulfurization, providing efficient light absorption and charge transport. The findings not only emphasize the critical role of sulfurization temperature in engineering CZCTS film and subsequently their functionality but also provide valuable insights for fine tuning their performance in the field of photovoltaic applications.
2. Enhanced photocatalytic performance of V2O5 NRs/RGO nanocomposites for Rhodamine-B decolorization under solar irradiation: Experimental and theoretical study
Authors: Boukhoubza, I; Achehboune, M; El Khouja, O; Basyooni-M Kabates, MA; Mindroc, M; Derkaoui, I; Enculescu, M; Matei, E

Published: JUN 2025, JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS, 201, 112654, DOI: 10.1016/j.jpcs.2025.112654

In the present work, an essential advance in the preparation of novel nanocomposites based on functionalized V2O5 nanostructures with reduced graphene oxide by hydrothermal method, which has great potential for use in photocatalytic processes related to environmental remediation. XRD analysis confirmed V2O5 in an orthorhombic structure. SEM images showed transparent RGO layers well anchored onto the surface of the V2O5 with a homogeneous distribution. Raman spectroscopy further explained the hybridization and interaction between the components. The photocatalytic activity of Rhodamine-B in aqueous solutions has been studied upon irradiation with visible light. A high RhB degradation was obtained using the V2O5/RGO photocatalyst (82 %), compared to the degradation obtained with only V2O5 (60 %). First-principles Density Functional Theory (DFT) simulations reveal a strong interaction between V2O5 molecules and graphene surfaces, with an adsorption energy of -1.673 eV and a significant charge transfer of 0.367 e- to RGO. This interaction modifies the electronic structure, creating semi-metallic behavior near the Fermi level and enhancing catalytic activity through improved charge carrier dynamics and active sites for photocatalytic applications.
Open Access
3. Synthesis of WS2 Ultrathin Films by Magnetron Sputtering Followed by Sulfurization in a Confined Space
Authors: Sava, F; Simandan, ID; Buruiana, AT; Bocirnea, AE; El Khouja, O; Tite, T; Zaki, MY; Mihai, C; Velea, A

Published: MAR 2024, SURFACES, 7, DOI: 10.3390/surfaces7010008

In the quest for advanced materials suitable for next-generation electronic and optoelectronic applications, tungsten disulfide (WS2) ultrathin films have emerged as promising candidates due to their unique properties. However, obtaining WS2 directly on the desired substrate, eliminating the need for transfer, which produces additional defects, poses many challenges. This paper aims to explore the synthesis of WS2 ultrathin films via physical vapor deposition (PVD) followed by sulfurization in a confined space, addressing the challenge of film formation for practical applications. Precursor layers of tungsten and WS2 were deposited by RF magnetron sputtering. Subsequent sulfurization treatments were conducted in a small, closed, graphite box to produce WS2 films. The physical and chemical properties of these precursor and sulfurized layers were thoroughly characterized using techniques such as X-ray reflectometry (XRR), X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). The findings reveal notable distinctions in film thickness, structural orientation, and chemical composition, attributable to the different precursor used. Particularly, the sulfurized layers from the tungsten precursor exhibited a preferred orientation of WS2 crystallites with their (00L) planes parallel to the substrate surface, along with a deviation from parallelism in a small angular range. This study highlights the necessity of precise control over deposition and sulfurization parameters to tailor the properties of WS2 films for specific technological applications.
Open Access
4. Investigation of kesterite to stannite phase transition and band gap engineering in Cu2Zn1-xCoxSnS4 thin films prepared by sol-gel spin coating
Authors: El Mahboub, E; El Khouja, O; Bocirnea, AE; Zakaria, S; Galca, AC; Mansori, M; El Hichou, A

Published: NOV 1 2024, APPLIED SURFACE SCIENCE, 672, 160848, DOI: 10.1016/j.apsusc.2024.160848

In this study, the Cu2Zn1-xCoxSnS4 (CZn1-xCoxTS) films with partial cation substitution of cobalt are synthetized by sol gel spin coating, followed by sulfurization treatment. The incorporation of cobalt cation in the CZTS crystalline lattice as well as the phase transition from kesterite to stannite were confirmed by the X-ray diffraction (XRD) and Raman spectroscopy data. The XRD pattern shows peak-shifting toward higher 2 theta by increasing the Co concentration, indicating a decrease in lattice parameters. The red shift of Raman peaks by increasing x from 0 to 0.6, confirms the phase transition. The CZn1-xCoxTS morphology was observed by scanning electron microscopy, showing large grain size as x increases and a good distribution of elements for all films. Xray photoelectron spectroscopy was employed to study the valence of cations/anions and to probe the chemical bonds. The optical band gap showed a parabolic behavior versus the molar ratio Co/(Co + Zn), this deviation from Vegard's law being induced by the difference in electronegativity between cobalt and zinc. The pure CZTS has a band gap of 1.47 eV, while for CZn0.6Co0.4TS the gap is 1.17 eV, which indicates that the incorporation of cobalt cation produces a red-shift of the band to band transition energy.
Open Access
5. Effect of transition metal ions on the dielectric properties of chromium potassium phosphates
Authors: Mighri, Z; Patru, RE; Leonat, LN; El Khouja, O; Nasri, H; Rostas, AM; Galca, AC

Published: DEC 25 2024, JOURNAL OF ALLOYS AND COMPOUNDS, 1009, 176870, DOI: 10.1016/j.jallcom.2024.176870

Potassium ions are important for developing electrode materials because they have similar properties to lithium and sodium ions. Mixed chromium phosphates (KMIICr(PO4)2) II Cr (PO 4 ) 2 ) with substituted M II sites using divalent elements (M = Ni, Co, Cu) were synthesized using a solid-state reaction method. The samples were analyzed using various techniques such as powder X-ray diffraction, Fourier transform infrared, Raman, and electron paramagnetic resonance spectroscopy. The proposed phosphates had a monoclinic phase structure with a P21/n 1 /n space group, and they contained large tunnels occupied by K+ + cations. The dielectric properties showed that the Ni-based phosphates had slower dielectric relaxation, while the Co and Cu-based phosphates had quicker polarization and depolarization processes. Additionally, the resistance of the grains decreased from Ni to Co to Cu-based phosphates, indicating easier charge movement in each material, consistent with the increase in conductive losses and a.c. conductivity when changing the M II ions.
Open Access
6. Hybrid supercapacitors based on X-site Ba(II) ions substituted by Sr(II) in Langbeinite-type phosphates
Authors: Mighri, Z; Yildirim, ID; Leonat, LN; El Khouja, O; Erdem, E; Nasri, H; Galca, AC; Rostas, AM

Published: AUG 2024, MATERIALIA, 36, 102147, DOI: 10.1016/j.mtla.2024.102147

The compounds KBa 1-x Sr x Cr 2 (PO 4 ) 3 (with x = 0.00; 0.25; 0.50; 0.75; 1.00) were synthesized by a solid-state reaction, and they were thoroughly characterized by different spectroscopic and microscopic techniques. Their structures were indexed in a cubic system with a P2 1 3 space group forming a 3D framework built on CrO 6 octahedra and PO 4 tetrahedra sharing vertices leading to identical Cr 2 P 3 O 18 (U) units. The interconnection between the tetrahedral and octahedral groups leads to the formation of two large closed cavities (K, M II )(1) and (K, M II )(2), statistically occupied by K + and M 2+ (M = Ba, Sr) atoms. Electron paramagnetic resonance spectroscopy confirmed the presence of paramagnetic Cr 3+ ions, showing the effects of substituting the Ba 2+ ions with smaller Sr 2+ ions on the dipolar coupling between the Cr 3+ centers. The obtained materials and active carbon were used as electrode materials in hybrid SC devices. At the same time, their electrochemical properties were assessed by potentiostatic electrochemical impedance spectroscopy, cyclic voltammetry, and galvanostatic charge-discharge measurements, showing promising results with a maximal specific capacitance (3.86 F/g), energy density (343 mWh/kg), and power density (30.9 kW/kg) in the case of KBa 0.5 Sr 0.5 Cr 2 (PO 4 ) 3 , proving them as good candidates for positive and/or negative electrode materials for energy storage applications.
7. Growth and optimization of spray coated Cu 2 BaSnS 4 thin films for solar photovoltaic application
Authors: Kadari, AS; Ech-Chergui, AN; Ghediya, PR; Guendouz, A; Guezzoul, M; El Khouja, O; Bocirnea, AE; Driss-Khodja, K; Amrani, B; Galca, AC

Published: AUG 2024, MATERIALIA, 36, 102178, DOI: 10.1016/j.mtla.2024.102178

Quaternary multicomponent Cu2BaSnS4 (CBTS) has emerged as a potential absorber material due to its abundant and nontoxic constituents, high absorption coefficient (10-4 cm-1) and suitable bandgap (1.5-2.0 eV) for the solar photovoltaic application. In this study, polycrystalline CBTS thin layers have been deposited by a typical spray pyrolysis technique on glass substrates using different substrate temperatures (Ts = 200, 250, 300 and 350 degrees C) followed by annealing in a sulfur-rich atmosphere at 550 degrees C under an argon flow. The (micro-)structural, compositional, and optical properties of both types of films have been studied. Analysis of x-ray diffractogram (XRD) patterns for all acquired films showed the presence of polycrystalline CBTS alongside various secondary phases, including Cu2SnS3 being predominant. Nonetheless, the XRD of the films deposited at 250 degrees C and annealed at 550 degrees C showed only the CBTS phase. Raman spectroscopy confirm the formation of the trigonal phase of CBTS. The presence of Cu, Ba, Sn and S in CBTS thin films was confirmed by X-ray photoelectron spectroscopy and Energy-dispersive X-ray spectroscopy. Scanning electron micrographs show a smooth and dense structure with enhanced crystallinity and improved uniformity. Overall, the physical properties of CBTS thin films were found to be spray deposition temperature dependent. An appropriate optical band gap of 1.6 to 1.8 eV and a compact structure indicate their prospective for solar cell applications.
8. Electrodeposition mechanism of Cu 2 CoSnS 4 thin films onto FTO-coated glass: Effect of some additives
Authors: Layachi, OA; Moujib, A; El Khouja, O; Galca, AC; Boudouma, A; Azmi, S; Nini, M; Nohair, M; Khoumri, E

Published: APR 15 2024, JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 959, 118177, DOI: 10.1016/j.jelechem.2024.118177

In this study, we synthesized thin films of semiconductor Cu 2 CoSnS 4 (CCTS). We investigated the mechanism of CCTS electrodeposition precursor onto fluorine -doped tin oxide (FTO) surface. This investigation utilized various mixed additives (Trisodium citrate, Glycine, and Boric acid) through voltammetric and chronoamperometric techniques. The polarization cathodic indicated that the additives narrowing the potential range for electrodeposition of the four elements. The reduction of S 2 O 3 2- was mainly induced by the effect of metal ions. The current transient was analyzed using the Astley and Scharifker-Hills models. Trisodium citrate electrolyte showed an instantaneous model followed by 3D diffusion -limited growth. Both trisodium citrate mixed with glycine and trisodium citrate mixed with boric acid shifted towards the progressive nucleation model. Trisodium citrate with tartaric acid showed a strong agreement with progressive nucleation. In -situ electrochemical impedance spectroscopy (EIS) evaluated a low charge transfer resistance for CCTS precursor electrodeposition in trisodium citrate electrolyte. The X-ray diffraction and Raman analysis study revealed the stannite structure of the obtained Cu 2 CoSnS 4 thin film. The morphological properties and thickness of the films were investigated using a scanning electron microscope (SEM). The compositions were determined using energy dispersive spectroscopy which indicated different atomic ratios of Cu-Co-Sn-S. The maximum absorption was observed within the 1.5 eV range for the film deposited in the Trisodium citrate bath, as determined by spectroscopic ellipsometry.
9. Unravelling the role of nickel incorporation on the physical properties of CuO thin films deposited by spray pyrolysis and theoretical analysis of nanostructured ZnO/Ni:CuO-based heterojunction solar cells
Authors: Daoudi, O; Jellal, I; Haddout, A; Zimou, J; EL Khouja, O; Nouneh, K; Lharch, M; Fahoume, M; Bendoumou, A

Published: MAR 2023, JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS, 34, 819, DOI: 10.1007/s10854-023-10167-6

Whereas solar photovoltaic cells are promising for proper power production, their wide deployment is hampered by production costs, material availability and toxicity. One of these materials is CuO, which has great chemical stability as well as interesting physical properties, including a direct band gap, a high absorption coefficient, and p-type conductivity. These properties indicate CuO as an exciting semiconducting material to use an absorber layer in thin films solar cells. For this specific reason, this paper focuses on the synthesis of pristine and Ni-incorporated CuO thin films by spray pyrolysis process. Several techniques such as; X-ray diffraction (XRD), Raman spectroscopy, Scanning Electron Microscopy (SEM), Energy dispersive X-ray (EDX) and UV-Visible spectroscopy have been employed to characterize the synthesized samples. The XRD analysis indicated the formation of polycrystalline CuO thin films and the average crystallite size was decreased from 35 to 20 nm for the samples with x = 0-8 at%, respectively. Furthermore, Raman spectroscopy also confirms the single-phase formation of CuO films. The SEM images demonstrated that the incorporation of Ni in the CuO matrix improved the films surface. The EDX analysis and the elemental mapping belay the homogeneous distribution of the elements. Moreover, UV-Visible spectroscopy has shown a significant expansion in optical energy band gap from 1.45 to 1.53 eV with an increase of Ni concentration. On the other hand, to investigate the impact of Ni-incorporated CuO on nanostructure Ni:CuO/ZnO-NRs heterojunction solar cell performance, SCAPS-1D software is used. It has been found that, 8% Ni:CuO layer has been revealed as better for nanostructured solar cells. The results of this contribution will provide some vital guidelines for fabricating higher-efficiency solar cells.
10. Structural and Electrical Properties of Novel Cr/Fe Mixed Transition-Metal Phosphates
Authors: Mighri, Z; Souiwa, K; Rostas, AM; Patru, RE; Bocirnea, AE; Iacob, N; Kuncser, V; El Khouja, O; Leonat, LN; Hidouri, M; Nasri, H; Galca, AC

Published: MAY 24 2023, INORGANIC CHEMISTRY, 62, DOI: 10.1021/acs.inorgchem.2c04389

The phosphate KCoCr-(PO4)(2) and iron-substitutedvariants KCoCr1-x Fe x (PO4)(2) (x =0.25, 0.5, and 0.75) were synthesized by a solid-state reaction route,while a high substitution level of Fe was achieved. Their structureswere refined using powder X-ray diffraction and indexed in a monoclinicsystem with a P2(1)/n spacegroup. A 3D framework with six-sided tunnels parallel to the [101]direction was formed in which the K atoms are located. Mo''ssbauerspectroscopy confirms the exclusive presence of octahedral paramagneticFe(3+) ions, with isomer shifts increasing slightly with x substitution. Electron paramagnetic resonance spectroscopyconfirmed the presence of paramagnetic Cr3+ ions. The activationenergy, determined by dielectric measurements, shows that the iron-containingsamples present higher ionic activity. Relative to the electrochemicalactivity of K, these materials could be good candidates for positiveand/or negative electrode materials for energy storage applications. The synthesized phosphate KCoCr-(PO4)(2) and Fe-substituted variants KCoCr1-x Fe x (PO4)(2) (x = 0.25, 0.5, and 0.75) present a 3D frameworkwith six-sided tunnels in which the K atoms are located. The activationenergy, determined by dielectric measurements, shows that the iron-containingsamples present improved ionic activity, making these materials goodcandidates for positive and/or negative electrode materials for energystorage applications.
11. Growth and characterization of Cu-Ni-Sn-S films electrodeposited at different applied potentials
Authors: El Khouja, O; Nouneh, K; Touhami, ME; Matei, E; Stancu, V; Enculescu, M; Galca, AC

Published: MAR 2023, JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS, 34, 760, DOI: 10.1007/s10854-023-10173-8

Cu2NiSnS4 (CNTS) absorber layers are elaborated by electrodeposition at various applied potentials followed by sulfurization treatment at 450 degrees C under sulfur atmosphere. The microstructural investigations revealed the presence of Cu4SnS4 secondary phases which can be reduced using an applied potential of -1.15 V vs. Ag/AgCl. Using the corresponding cathodic potential for Ni2+, the competing detrimental hydrogen evolution regresses the morphology and composition. The film with the highest Ni concentration has a band gap of 1.44 eV as inferred from diffuse reflectance data. The Randles cell model is probed by electrochemical impedance spectroscopy.
12. Effect of growth temperature on the physical properties of Spray pyrolysis deposited CZTS films
Authors: Khaaissa, Y; Talbi, A; Nouneh, K; El Khouja, O; Ahmoum, H; Fahoume, M

Published: SEP 2022, MATERIALS TODAY-PROCEEDINGS, 66, DOI: 10.1016/j.matpr.2022.04.893

Cu2ZnSnS4 (CZTS) functional thin films have been successfully synthesized using the spray pyrolysis method in a single deposition process and under atmospheric pressure. The samples have been deposited on glass substrates under different growth temperatures ranging from 350 ? to 450 ?. The solution has been prepared using Copper chloride dihydrate, Zinc chloride, Tin chloride dihydrate, and Thiourea as Copper, Zinc, Tin and Sulfur sources respectively. The structural, optical, morphological and electrical properties of CZTS films have been investigated. X-ray diffraction (XRD) and Raman spectroscopy have confirmed the kesterite structure of all samples without any secondary phase. The surface morphology and topography of the samples have been examined by scanning electron microscopy (SEM) and atomic force microscopy (AFM). Data from UV-Vis spectroscopy analysis and Hall effect measurement showed that CZTS films elaborated at 400 ? have an optimum band gap (Eg = 1.5 eV), low resistivity (1.7239 x 10(-2) omega.cm), and high conductivity (58.00 (omega.cm)(-1)). Copyright (c) 2022 Elsevier Ltd. All rights reserved.
13. Evaluation of quinoxaline-2(1H)-one, derivatives as corrosion inhibitors for mild steel in 1.0 M acidic media: Electrochemistry, quantum calculations, dynamic simulations, and surface analysis
Authors: Ech-chebab, A; Missioui, M; Guo, L; El Khouja, O; Lachhab, R; Kharbouch, O; Galai, M; Ouakki, M; Ejbouh, A; Dahmani, K; Dkhireche, N; Touhami, ME

Published: DEC 16 2022, CHEMICAL PHYSICS LETTERS, 809, 140156, DOI: 10.1016/j.cplett.2022.140156

The evaluation of corrosion inhibition of mild steel (M-S) in 1.0 M HCl solution in the absence and the presence of different concentrations of (E)-3-(5-bromo-2-hydroxystyryl)quinoxalin-2(1H)-one (FR178) and (E)-3-(5-fluoro-2-hydroxystyryl)quinoxalin-2(1H)-one (FR179) was studied by electrochemical,and theoretical measurements. These organic inhibitors have proven to be effective corrosion inhibitors for the protection of mild steel. Increasing concentrations of inhibitors contributed to high inhibition efficiencies, which were attributed to the simple blocking action of the anodic and cathodic sites by adsorption of the inhibitors molecules onto the M-S surface. Their inhibition efficiencies can reach about 90.9 % and 91.5 % when the optimal concentration is 10-3M for the two inhibitors FR178 and FR179 respectively.On the other hand, as the temperature rises, the anticorrosion capability of both FR178 and FR179 diminishes slightly and attains 82 % and 84 % respectively at the temperature of 328 K.Potentiodynamique polarization (PDP) and electrochemical impedance spectroscopy (EIS) demonstrated that both inhibitors examined act as mixed-type inhibitors.Furthermore, X-ray diffraction (XRD) and scanning electron microscopy coupled to energy dispersive spectroscopy (SEM/EDS) measurements indicated the formation of a protective layer adsorbed on the mild steel surface. The density functional theory (DFT) and molecular dynamics (MD) simulations were carried out to examine the correlation between molecular and chemical reactivity. The obtained results were found to be consistent with the experimental findings.
14. ZnS stacking order influence on the formation of Zn-poor and Zn-rich Cu2ZnSnS4 phase
Authors: Zaki, MY; El Khouja, O; Nouneh, K; Touhami, ME; Matei, E; Azmi, S; Rusu, MI; Grigorescu, CEA; Briche, S; Boutamart, M; Badica, P; Burdusel, M; Secu, M; Pintilie, L; Galca, AC

Published: MAY 2022, JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS, 33, DOI: 10.1007/s10854-022-08160-6

This paper reports the synthesis and characterization of Cu2ZnSnS4 (CZTS) absorber films, prepared by a two-step electrodeposition of a ZnS (zinc sulfide) binary and a CZT (copper, zinc and tin) ternary precursors on Mo/Ti/Si substrates. The as-electrodeposited ZnS/CZT and CZT/ZnS stacks were thermally treated in a tubular furnace in sulfur environment at 550 degrees C. The role of the ZnS buffer layer is to provide a zinc and sulfur reservoir, needed to complete the formation of kesterite phase. X-ray diffraction and Raman analyses revealed the formation of the CZTS phase. The surface morphology and chemical composition of the films were studied using a scanning electron microscope. The bandgap values inferred from diffuse reflectance data, are discussed with respect to the stoichiometry which is considerably affected by the order of the stacks. Room-temperature photoluminescence of the CZT/ZnS sample showed a board PL band of 1.51 eV. It was found that the film with a ZnS layer on top is preferred for the formation of a Zn-rich single CZTS phase.
Open Access
15. New Chalcogenide Glass-Ceramics Based on Ge-Zn-Se for IR Applications
Authors: Velea, A; Sava, F; Badica, P; Burdusel, M; Mihai, C; Galca, AC; Matei, E; Buruiana, AT; El Khouja, O; Calvez, L

Published: JUL 2022, MATERIALS, 15, 5002, DOI: 10.3390/ma15145002

The consumer market requests infrared (IR) optical components, made of relatively abundant and environmentally friendly materials, to be integrated or attached to smartphones. For this purpose, three new chalcogenides samples, namely Ge23.3Zn30.0Se46.7 (d_GZSe-1), Ge26.7Zn20.0Se53.3 (d_GZSe-2) and Ba4.0Ge12.0Zn17.0Se59.0I8.0 (d_GZSe-3) were obtained by mechanical alloying and processed by spark plasma sintering into dense bulk disks. Obtaining a completely amorphous and homogeneous material proved to be difficult. d_GZSe-2 and d_GZSe-3 are glass-ceramics with the amount of the amorphous phase being 19.7 and 51.4 wt. %, while d_GZSe-1 is fully polycrystalline. Doping with barium and iodine preserves the amorphous phase formed by milling and lowers the sintering temperature from 350 degrees C to 200 degrees C. The main crystalline phase in all of the prepared samples is cubic ZnSe or cubic Zn0.5Ge0.25Se, while in d_GZSe-3 the amorphous phase contains GeSe4 clusters. The color of the first two sintered samples is black (the band gap values are 0.42 and 0.79 eV), while d_GZSe-3 is red (E-g is 1.37 eV) and is transparent in IR domain. These results are promising for future research in IR materials and thin films.
16. Structural and transport properties of Cu2CoSnS4 films prepared by spray pyrolysis
Authors: El Khouja, O; Assahsahi, I; Nouneh, K; Touhami, ME; Secu, M; Talbi, A; Khaaissa, Y; Matei, E; Stancu, V; Galatanu, A; Galca, AC

Published: NOV 1 2022, CERAMICS INTERNATIONAL, 48, DOI: 10.1016/j.ceramint.2022.07.185

In the present work, stannite Cu2CoSnS4 (CCTS) films were elaborated using spray pyrolysis method on soda-lime glass, at different deposition temperatures (T-d = 250, 300, and 350 degrees C), followed by different chosen sulfurization temperatures (T-s = 450, 500, and 550 degrees C). X-ray diffraction (XRD) revealed the nearly single-phase formation of CCTS films at 300 degrees C deposition temperature. After sulfurization in argon flow, the XRD lines become narrower, the average crystallite size expanding above 70 nm. The Raman spectroscopy analysis confirmed the stannite structure formation, as well as the presence CoS2 secondary phases, which reduces at higher sulfurization temperature (550 degrees C). The energy dispersive spectroscopy results indicated atomic ratios of Cu/Co/Sn/S close to the ideal stoichiometric ratio 2:1:1:4. The room temperature photoluminescence emission is recorded with maximum in the 1.35-1.40 eV range. Thermoelectric properties are measured up to 130 degrees C, the films show poor power factor as a result of small positive Seebeck coefficients 10-45 Of K -1 and low electrical conductivity despite of having relatively high carrier concentration (similar to 10(20) cm(-3)).
17. Bulk and surface characteristics of co-electrodeposited Cu2FeSnS4 thin films sulfurized at different annealing temperatures
Authors: El Khouja, O; Negrila, CC; Nouneh, K; Secu, M; Touhami, ME; Matei, E; Stancu, V; Enculescu, M; Kuncser, V; Galca, AC

Published: JUN 15 2022, JOURNAL OF ALLOYS AND COMPOUNDS, 906, 164379, DOI: 10.1016/j.jallcom.2022.164379

In this study, stannite, Cu2FeSnS4 (CFTS), absorber films were obtained by electrodeposition on Molybdenum-coated soda-lime substrates, followed by sulfurization treatment at certain temperatures in the 400-550 degrees C range. The purposes of this work were to control the manufacturing of CFTS films with good stoichiometry, high crystallinity and to study the annealing temperature impact on CFTS films properties. The X-ray diffraction and the Raman spectroscopy measurement distinguished the CFTS phase formation, with a presence of SnS2 secondary phase. The energy dispersive spectroscopy results reveal compositional differences between samples as well as the in-depth gradients. The photoluminescence emission band around 1.35-1.40 eV is slightly below the direct bandgap inferred from the conventional spectroscopy (diffuse reflectance). X-ray photoelectron spectroscopy results indicate clearly a high amount of Sn on the surface. The Conversion Electron Mossbauer unveiled the presence of Fe in the chalcogenide unit cell. The electrochemical characteristics of the synthesized films are also given. (c) 2022 Elsevier B.V. All rights reserved.
18. Experimental and numerical simulation of deposition time effect on ZnS thin films for CZTS-based solar cells
Authors: Khaaissa, Y; Talbi, A; Nouneh, K; El Khouja, O; Ahmoum, H; Galca, AC; Belahmar, A; Li, GJ; Wang, Q

Published: SEP 2021, OPTICAL AND QUANTUM ELECTRONICS, 53, 487, DOI: 10.1007/s11082-021-03143-z

High-quality ZnS thin films as buffer layer have been successfully synthesized and simulated using the low-cost Mist CVD technique and the SCAPS-1D software for different deposition times (30, 40, 50, and 60 min). The structural, morphological, and optical properties of the prepared ZnS films have been investigated using X-ray diffraction (XRD), scanning electronic microscopy (SEM), atomic force microscopy (AFM), and UV-Vis spectrophotometer. The time deposition effect on ZnS films' efficiency as a buffer layer has been evaluated. XRD pattern confirms the hexagonal/cubic structure of the prepared samples, with (111) as preferred orientation. Raman spectra confirm XRD findings by the two peaks located at 348 cm(-1) and 697 cm(-1) which correspond to ZnS samples' cubic and hexagonal structures. Scanning electronic microscopy (SEM) and atomic force microscopy (AFM) images show densely uniform grains with precise shapes and boundaries covering the entire sample's surface with a relative roughness for all deposition times. The optical transmittance shows an average of 78% in the visual field of light with an optical band gap varying between 3.69 and 3.80 eV. Numerical simulation of ZnO:Al/ZnS/CZTS/Mo cell using SCAPS-1D software shows that the sample deposited for 30 min presents the best performance with an efficiency of up to 8.9%.
19. Secondary phases and their influence on optical and electrical properties of electrodeposited Cu2FeSnS4 films
Authors: El Khouja, O; Galca, AC; Zaki, MY; Talbi, A; Ahmoum, H; Nouneh, K; Touhami, ME; Taibi, M; Matei, E; Enculescu, M; Pintilie, L

Published: NOV 2021, APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING, 127, 887, DOI: 10.1007/s00339-021-05038-y

Cu-Fe-Sn-S have been electrodeposited on indium tin oxide coated glass (ITO/glass) substrates, varying only the deposition time, followed by sulfurization in argon atmosphere at a temperature of 500 degrees C. X-ray diffraction patterns confirmed the formation of polycrystalline CFTS and other secondary phases. The Raman spectroscopy results confirm the formation of stannite phase, by the existence of the most intense peak at 330 cm(-1) corresponding to A-symmetry vibrational mode, while the SnS2 surface phase reduces upon increasing deposition time. The inferred bandgaps by specular transmission are in 1.4-1.7 eV range, influenced by the detected orthorhombic Cu4SnS4 and rhodostannite secondary phases. The electrical measurements confirm the p-type nature of the films, while density of free carriers is relatively high (similar to 10(19) cm(-3)), leading to extremely low resistivity in the Omega cm range.
20. Structural, morphological and optical properties of Cu-Fe-Sn-S thin films prepared by electrodeposition at fixed applied potential
Authors: El Khouja, O; Galca, AC; Nouneh, K; Zaki, MY; Touhami, ME; Taibi, M; Matei, E; Negrila, CC; Enculescu, M; Pintilie, L

Published: MAR 1 2021, THIN SOLID FILMS, 721, 138547, DOI: 10.1016/j.tsf.2021.138547

Cu-Fe-Sn-S films were obtained on indium tin oxide / glass substrates by a low-cost electrodeposition using an aqueous solution of CuSO4, FeSO4, SnSO4, and Na2S2O3 at room temperature followed by high-temperature sulfurization (500 degrees C) in argon flow. A range of cathodic potentials have been used for electrodeposition, those being chosen after a preliminary cyclic voltammetry study. The coatings were characterized using X-ray diffraction, Raman spectroscopy, scanning electron microscopy, energy dispersive spectroscopy, X-ray Photoelectron Spectroscopy and conventional spectroscopy (diffuse reflectance and specular transmission). The results are discussed with respect to the used applied potential.
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