Se Jin Park

Synthesis of Cu2ZnSnS4 thin films by a precursor solution paste for thin film solar cell applications

Cu2ZnSnS4 (CZTS) is a very promising semiconductor material when used for the absorber layer of thin film solar cells because it consists of only abundant and inexpensive elements. In addition, a low-cost solution process is applicable to the preparation of CZTS absorber films, which reduces the cost when this film is used for the production of thin film solar cells. To fabricate solution-processed CZTS thin film using an easily scalable and relatively safe method, we suggest a precursor solution paste coating method with a two-step heating process (oxidation and sulfurization). The synthesized CZTS film was observed to be composed of grains of a size of ~300 nm, showing an overall densely packed morphology with some pores and voids. A solar cell device with this film as an absorber layer showed the highest efficiency of 3.02% with an open circuit voltage of 556 mV, a short current density of 13.5 mA/cm(2), and a fill factor of 40.3%. We also noted the existence of Cd moieties and an inhomogeneous Zn distribution in the CZTS film, which may have been triggered by the presence of pores and voids in the CZTS film.

A monolithic and standalone solar-fuel device having comparable efficiency to photosynthesis in nature

The need for developing sustainable energy sources has generated academic and industrial attention in artificial photosynthesis, inspired by the natural process. In this study, we demonstrate a highly efficient solar energy to fuel conversion device using CO2 and water as feedstock. We developed a thin film photovoltaic technology for the light absorbing component using a low cost, solution based Cu(InxGa1−x)(SySe1−y)2 (CIGS) module fabrication method to provide sufficient potential for the conversion reactions. Our solar-fuel device uses cobalt oxide (Co3O4) nanoparticle thin film deposited with a low temperature coating method as the water oxidation catalyst and nanostructured gold film as the CO2 reduction to CO generation catalyst. We demonstrated that the integrated monolithic device operated by energy only from sunlight, in an absence of any external energy input. The individual components showed the following abilities: solar-to-power conversion efficiency of 8.58% for the CIGS photovoltaic module photoelectrode, overpotential reduction of water oxidation with the Co3O4 catalyst film by ∼360 mV at 5 mA cm−2, and Faradaic efficiency of over 90% by the nanostructured Au catalyst for CO2 reduction to CO. Remarkably, this is the first demonstration of a monolithic and standalone solar-fuel device whose solar-to-fuel conversion efficiency from CO2 and H2O is 4.23%, which is comparable with that of photosynthesis in nature.

Bulk Heterojunction Formation between Indium Tin Oxide Nanorods and CuInS2 Nanoparticles for Inorganic Thin Film Solar Cell Applications

In this study, we developed a novel inorganic thin film solar cell configuration in which bulk heterojunction was formed between indium tin oxide (ITO) nanorods and CuInS(2) (CIS). Specifically, ITO nanorods were first synthesized by the radio frequency magnetron sputtering deposition method followed by deposition of a dense TiO(2) layer and CdS buffer layer using atomic layer deposition and chemical bath deposition method, respectively. The spatial region between the nanorods was then filled with CIS nanoparticle ink, which was presynthesized using the colloidal synthetic method. We observed that complete gap filling was achieved to form bulk heterojunction between the inorganic phases. As a proof-of-concept, solar cell devices were fabricated by depositing an Au electrode on top of the CIS layer, which exhibited the best photovoltaic response with a V(oc), J(sc), FF, and efficiency of 0.287 V, 9.63 mA/cm(2), 0.364, and 1.01%, respectively.

Printable, wide band-gap chalcopyrite thin films for power generating window applications

Printable, wide band-gap chalcopyrite compound films (CuInGaS2, CIGS) were synthesized on transparent conducting oxide substrates. The wide band-gap and defective nature of the films reveal semi-transparent and bifacial properties that are beneficial for power generating window applications. Importantly, solar cell devices with these films demonstrate a synergistic effect for bifacial illumination resulting in a 5.4–16.3% increase of the apparent power conversion efficiency compared to the simple sum of the efficiencies of the front and rear side illumination only. We also confirmed that this extra output power acquisition due to bifacial irradiation is apparently not influenced by the light intensity of the rear side illumination, which implies that weak light (e.g., indoor light) can be efficiently utilized to improve the overall solar cell efficiency of bifacial devices.

Fabrication of nanocrystal ink based superstrate-type CuInS2 thin film solar cells

A CuInS₂ (CIS) nanocrystal ink was applied to thin film solar cell devices with superstrate-type configuration. Monodispersed CIS nanocrystals were synthesized by a colloidal synthetic route and re-dispersed in toluene to form an ink. A spray method was used to coat CIS films onto conducting glass substrates. Prior to CIS film deposition, TiO₂ and CdS thin films were also prepared as a blocking layer and a buffer layer, respectively. We found that both a TiO₂ blocking layer and a CdS buffer layer are necessary to generate photoresponses in superstrate-type devices. The best power conversion efficiency (∼1.45%) was achieved by the CIS superstrate-type thin film solar cell device with 200 and 100 nm thick TiO₂ and CdS films, respectively.

Chalcogenization-Derived Band Gap Grading in Solution-Processed CuInxGa1–x(Se,S)2 Thin-Film Solar Cells

Significant enhancement of solution-processed CuIn(x)Ga(1-x)(Se,S)2 (CIGSSe) thin-film solar cell performance was achieved by inducing a band gap gradient in the film thickness, which was triggered by the chalcogenization process. Specifically, after the preparation of an amorphous mixed oxide film of Cu, In, and Ga by a simple paste coating method chalcogenization under Se vapor, along with the flow of dilute H2S gas, resulted in the formation of CIGSSe films with graded composition distribution: S-rich top, In- and Se-rich middle, and Ga- and S-rich bottom. This uneven compositional distribution was confirmed to lead to a band gap gradient in the film, which may also be responsible for enhancement in the open circuit voltage and reduction in photocurrent loss, thus increasing the overall efficiency. The highest power conversion efficiency of 11.7% was achieved with J(sc) of 28.3 mA/cm(2), V(oc) of 601 mV, and FF of 68.6%.

Monolithic DSSC/CIGS tandem solar cell fabricated by a solution process

Tandem architecture between organic (dye-sensitized solar cell, DSSC) and inorganic (CuInGaSe2 thin film solar cell, CIGS) single-junction solar cells was constructed particularly based on a solution process. Arc-plasma deposition was employed for the Pt interfacial layer to minimize the damage to the layers of the CIGS bottom cell. Solar cell efficiency of 13% was achieved, which is significant progress from individual single-junction solar cells (e.g., 7.25 and 6.2% for DSSC and CIGS, respectively).

Fabrication of solution processed 3D nanostructured CuInGaS2 thin film solar cells

In this study we demonstrate the fabrication of CuInGaS₂ (CIGS) thin film solar cells with a three-dimensional (3D) nanostructure based on indium tin oxide (ITO) nanorod films and precursor solutions (Cu, In and Ga nitrates in alcohol). To obtain solution processed 3D nanostructured CIGS thin film solar cells, two different precursor solutions were applied to complete gap filling in ITO nanorods and achieve the desirable absorber film thickness. Specifically, a coating of precursor solution without polymer binder material was first applied to fill the gap between ITO nanorods followed by deposition of the second precursor solution in the presence of a binder to generate an absorber film thickness of ∼1.3 μm. A solar cell device with a (Al, Ni)/AZO/i-ZnO/CdS/CIGS/ITO nanorod/glass structure was constructed using the CIGS film, and the highest power conversion efficiency was measured to be ∼6.3% at standard irradiation conditions, which was 22.5% higher than the planar type of CIGS solar cell on ITO substrate fabricated using the same precursor solutions.

Cocktails of Paste Coatings for Performance Enhancement of CuInGaS2 Thin-Film Solar Cells

To fabricate low-cost and printable wide-bandgap CuInxGa1-xS2 (CIGS) thin-film solar cells, a method based on a precursor solution was developed. In particular, under this method, multiple coatings with two pastes with different properties (e.g., viscosity) because of the different binder materials added were applied. Paste A could form a thin, dense layer enabling a high-efficiency solar cell but required several coating and drying cycles for the desired film thickness. On the other hand, paste B could easily form one-micrometer-thick films by means of a one-time spin-coating process but the porous microstructure limited the solar cell performance. Three different configurations of the CIGS films (A + B, B + A, and A + B + A) were realized by multiple coatings with the two pastes to find the optimal stacking configuration for a combination of the advantages of each paste. Solar cell devices using these films showed a notable difference in their photovoltaic characteristics. The bottom dense layer increased the minority carrier diffusion length and enhanced the short-circuit current. The top dense layer could suppress interface recombination but exhibited a low optical absorption, thereby decreasing the photocurrent. As a result, the A + B configuration could be suggested as a desirable simple stacking structure. The solar cell with A + B coating showed a highly improved efficiency (4.66%) compared to the cell with a film prepared by paste B only (2.90%), achieved by simple insertion of a single thin (200 nm), dense layer between the Mo back contact and a thick porous CIGS layer.

Semi-transparent thin film solar cells by a solution process

Easily processed, low cost, and highly efficient solar cells are desirable for photovoltaic conversion of solar energy to electricity. We present the fabrication of precursor solution processed CuInGaS2 (CIGS) thin film solar cells on transparent indium tin oxide (ITO) substrates. The CIGS absorber film was prepared by a spin-coating method, followed by two successive heat treatment processes. The first annealing process was on a hot plate at 300 °C for 30 min in air to remove carbon impurities in the film; this was followed by a sulfurization process at 500 °C in an H2S(1%)/Ar environment to form a polycrystalline CIGS film. The absorber film with an optical band-gap of 1.52 eV and a thickness of about 1.1 µm was successfully synthesized. Because of the usage of a transparent glass substrate, a bifacial CIGS thin film device could be achieved; its power conversion efficiency was measured to be 6.64% and 0.96% for front and rear illumination, respectively, under standard irradiation conditions.