To alleviate the limitations of pure sulfide Cu2ZnSnS4 (CZTS) thin film, such as band gaps adjustment, antisite defects, secondary phase and microstructure, Cadmium is introduced into CZTS thin film to replace Zn partially to form Cu2Zn1−xCdxSnS4 (CZCTS) thin film by low‐cost sol–gel method. It is demonstrated that the band gaps and crystal structure of CZCTS thin films are affected by the change in Zn/Cd ratio. In addition, the ZnS secondary phase can be decreased and the grain sizes can be improved to some degree by partial replacement of Zn with Cd in CZCTS thin film. The power conversion efficiency of CZTS solar cell device is enhanced significantly from 5.30% to 9.24% (active area efficiency 9.82%) with appropriate ratio of Zn/Cd. The variation of device parameter as a function of Zn/Cd ratio may be attributed to the change in electronic structure of the bulk CZCTS thin film (i.e., phase change from kesterite to stannite), which in turn affects the band alignment at the CZCTS/buffer interface and the charge separation at this interface.
Recently, considerable attention in the development of Cu 2 ZnSnS 4 (CZTS)-based thin-film solar cells has been given to the reduction of antisite defects via cation substitution. In this Letter, we report the substitution of copper atoms by silver, incorporated into the crystal lattice through a solution processable method. We observe an increase in open-circuit voltage (V OC ) by 50 mV and an accompanying rise in device efficiency from 4.9% to 7.2%. The incorporation of Ag is found to improve the grain size, enhance the depletion width of the pn-junction, and reduce the concentration of antisite defect states. This work demonstrates the promising role of Ag in reducing the V OC deficit of Cu-kesterite thin-film solar cells.
Single-phase Cu2ZnSnS4 (CZTS) is an essential prerequisite toward a high-efficiency thin-film solar cell device. Herein, the selective phase formation of single-phase CZTS nanoparticles by ligand control is reported. Surface-enhanced Raman scattering (SERS) spectroscopy is demonstrated for the first time as a characterization tool for nanoparticles to differentiate the mixed compositional phase (e.g., CZTS, CTS, and ZnS), which cannot be distinguished by X-ray diffraction. Due to the superior selectivity and sensitivity of SERS, the growth mechanism of CZTS nanoparticle formation by hot injection is revealed to involve three growth steps. First, it starts with nucleation of Cu(2-x)S nanoparticles, followed by diffusion of Sn(4+) into Cu(2-x)S nanoparticles to form the Cu3SnS4 (CTS) phase and diffusion of Zn(2+) into CTS nanoparticles to form the CZTS phase. In addition, it is revealed that single-phase CZTS nanoparticles can be obtained via balancing the rate of CTS phase formation and diffusion of Zn(2+) into the CTS phase. We demonstrate that this balance can be achieved by 1 mL of thiol with Cu(OAc)2, Sn(OAc)4, and Zn(acac)2 metal salts to synthesize the CZTS phase without the presence of a detectable binary/ternary phase with SERS.
An analytical platform suitable for trace detection using a small volume of analyte is pertinent to the field of toxin detection and criminology. Plasmonic nanostructures provide surface-enhanced Raman scattering (SERS) that can potentially achieve trace toxins and/or molecules detection. However, the detection of highly diluted, small volume samples remains a challenge. Here, we fabricate a superhydrophobic SERS platform by assembling Ag nanocubes that support strong surface plasmon and chemical functionalization for trace detection with sample volume of just 1 μL. Our strategy integrates the intense electromagnetic field confinement generated by Ag nanocubes with a superhydrophobic surface capable of analyte concentration to lower the molecular detection limit. Single crystalline Ag nanocubes are assembled using the Langmuir-Blodgett technique to create surface roughness. To create a stable superhydrophobic SERS platform, an additional 25 nm Ag coating is evaporated over the Ag nanocubes to "weld" the Ag nanocubes onto the substrate followed by chemical functionalization with perfluorodecanethiol. The resulting substrate has an advancing contact angle of 169° ± 5°. Our superhydrophobic platform confines analyte molecules within a small area and prevents the random spreading of molecules. An analyte concentrating factor of 14-fold is attained, as compared to a hydrophilic surface. Consequently, the detection limit of our superhydrophobic SERS substrate reaches 10(-16) M (100 aM) for rhodamine 6G using 1 μL analyte solutions. An analytical SERS enhancement factor of 10(11) is achieved. Our protocol is a general method that provides a simple, cost-effective approach to develop a stable and uniform superhydrophobic SERS platform for trace molecular sensing.
Interfacial self-assembly of nanoparticles is capable of creating large-area close-packed structures for a variety of applications. However, monolayers of hydrophilic cetyltrimethylammonium bromide (CTAB)-coated Au nanoparticles are challenging to assemble via interfacial self-assembly. This report presents a facile and scalable process to fabricate large-area monolayer films of ultrathin CTAB-coated Au nanoprisms at the air-water interface using the Langmuir-Schaefer technique. This is first achieved by a one-step functionalization of Au nanoprisms with poly(vinylpyrrolidone) (PVP). PVP functionalization is completed within a short time without loss of nanoprisms due to aggregation. Uniform and near close-packed monolayers of the Au nanoprisms formed over large areas (∼1 cm(2)) at the air-water interface can be transferred to substrates with different wettabilities. The inter-prism gaps are tuned qualitatively through the introduction of dodecanethiol and oleylamine. The morphological integrity of the nanoprisms is maintained throughout the entire assembly process, without truncation of the nanoprism tips. The near close-packed arrangement of the nanoprism monolayers generates large numbers of hot spots in the 2D arrays in the tip-to-tip and edge-to-edge inter-particle regions, giving rise to strong surface-enhanced Raman scattering (SERS) signals. When deposited on an Au mirror film, additional hotspots are created in the 3(rd) dimension in the gaps between the 2D nanoprism monolayers and the Au film. SERS enhancement factors reaching 10(4) for non-resonant probe molecules are achieved.
Metal–organic frameworks (MOFs) are a well‐developed field of materials, having a high potential for various applications such as gas storage, water purification, and catalysis. Despite the continuous discoveries of new MOFs, so far there are only a limited number of industrial applications, partially due to their low chemical stability and limited mechanical properties, as well as difficulties in integration within functional devices, Herein, a new approach is presented toward the fabrication of MOF‐based devices, utilizing direct 3D printing. By this method, 3D, flexible, and hydrolytically stable MOF‐embedded polymeric structures are fabricated. It is found that the adsorption capacity of the 3D‐printed MOF is retained, with significantly improved hydrolytic stability of the printed MOFs (copper benzene‐1,3,5‐tricarboxylate) compared to the MOF only. It is expected that applying 3D printing technologies, for the fabrication of functional MOF objects such as filters and matrices for columns and flow reactors, will open the way for utilization of this important class of materials.
Potassium (K) post-treatment on CIGSSe has been shown to yield the highest efficiency reported to date. However, very little is known on the effect of K doping in CZTSSe and the mechanism behind the efficiency improvement. Here we reveal the mechanism by which K enhances the charge separation in CZTSSe. We show that K accumulates at the CdS/CZTSSe, passivating the recombination at the front interface and improving carrier collection. K is also found to accumulate at the CZTSSe/Mo interface and facilitates the diffusion of Cd into the absorber which affects the morphology and grain growth of CZTSSe. As revealed by the C–V, external quantum efficiency, and color J–V test, K doping significantly increases the carrier density, improves carrier collection, and passivates the front interface and grain boundaries, leading to the enhancement of V oc and J sc. The average power conversion efficiency has been promoted from 5% to above 7%, and the best 7.78% efficiency has been achieved for the 1.5 mol % K-doped CZTSSe device. This work offers some new insights into the K doping effects on CZTSSe via solution-based approach and demonstrates the potential of facile control of K doping for further improvement of CZTSSe thin film solar cells.
Figure 4. Optical properties of direct-write colloidal crystals. Photographs of a) small-grain and b) large-grain colloidal crystal imaged under ring lighting around the objective lens. c) Schematic depicting the characterization of optical properties by illuminating the colloidal crystal with collimated light at an angle normal to the crystal and observing the projection of diffracted colors on a hemispherical screen. Photograph of colors projected from the d) smallgrain and g) large-grain colloidal crystal. Colors from the e) small-grain and h) large-grain samples linearly mapped onto azimuthal angle φ and polar angle θ. f) Plot of radiant intensity versus θ for each of the RGB channels, obtained by averaging over all values of φ. i) Plot of radiant intensity versus azimuthal angle φ derived from the blue channel of (h), ranging φ = 0°-60° averaged over the sixfold symmetry regions, at θ = 52°. The solid blue line is the radiant intensity and the shaded region represents standard deviation. The highest peak is from the largest grain, A; the second highest peak is from the second-largest grain, B; and the lowest radiant intensity, denoted by the solid black line, is an estimate of the amount of light from various other small grains, C. The dashed line represents the background illumination of the ping pong ball, measured in a noncolored region. j) Optical image of the illuminated region, with A, B, and C grain structures identified. k) SEM image analysis confirms that the largest grain A and the second-largest grain B are relatively orientated at 19.5°. www.advancedsciencenews.com
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