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Despite its growing popularity as a solar material, there is no comprehensive reference to aid with determining various polymorphs of copper zinc tin sulfide (CZTS) in the lab. Understanding the diverse electronic, optical and vibrational properties of these polymorphs is crucial to further enhance the conversion efficiency of CZTS solar cells. Here, findings are presented that suggest the effective hole mass in a monoclinic polymorph, that is likely to form along with the more commonly reported tetragonal variations, is about 10 times heavier than that of its tetragonal counterparts, thereby affecting key attributes such as carrier transport and concentration. Among tetragonal polymorphs, the so‐called primitive mixed CuAu (PMCA) arrangement is likely to undergo a direct‐indirect gap transition due to internal strains. Optical absorption between different polymorphs could also vary by up to 90% in the visible spectrum. Finally, accurate Raman footprint of each polymorph is predicted to help establish a definitive method for their detection. From a modeling perspective, Becke‐Lee‐Yang‐Parr with spin‐orbit coupling is shown to be a superior yet 100X faster alternative to hybrid functionals when applied to studying electronic structure of CZTS. [ABSTRACT FROM AUTHOR]

Kesterite is an earth‐abundant energy material with high predicted power conversion efficiency, making it a sustainable and promising option for photovoltaics. However, a large open circuit voltage Voc deficit due to non‐radiative recombination at intrinsic defects remains a major hurdle, limiting device performance. Incorporating Ge into the kesterite structure emerges as an effective approach for enhancing performance by manipulating defects and morphology. Herein, how different amounts of Ge affect the kesterite growth pathways through the combination of advanced microscopy characterization techniques are systematically investigated. The results demonstrate the significance of incorporating Ge during the selenization process of the CZTSSe thin film. At high temperature, the Ge incorporation effectively delays the selenization process due to the formation of a ZnSe layer on top of the metal alloys through decomposition of the Cu‐Zn alloy and formation of Cu‐Sn alloy, subsequently forming of Cu‐Sn‐Se phase. Such an effect is compounded by more Ge incorporation that further postpones kesterite formation. Furthermore, introducing Ge mitigates detrimental "horizontal" grain boundaries by increasing the grain size on upper layer. The Ge incorporation strategy discussed in this study holds great promise for improving device performance and grain quality in CZTSSe and other polycrystalline chalcogenide solar cells. [ABSTRACT FROM AUTHOR]

Flexible photovoltaics have been and will be increasingly in demand in modern and future society in various applications. Searching for ideal flexible photovoltaic technologies that can perfectly meet these expanding demands has long been an active branch of photovoltaic research. Flexible kesterite Cu2ZnSn(S,Se)4 (CZTSSe) has emerged in recent years owning to its great potential to be an abundant, low-cost, stable, and high-efficiency 'green' photovoltaic material that can be widely deployed with the lowest detrimental environmental impact. Here, we review the recent progress with flexible kesterite solar cells in thin-film and monograin technologies, discuss the key challenges and strategies associated with the flexible substrates, and finally provide the future perspectives on further pushing the efficiency toward commercial-competitive levels. [ABSTRACT FROM AUTHOR]

Kesterite Cu2ZnSn(S,Se)4 (CZTSSe) with earth‐abundant and environmental‐benign constituents has been regarded as a promising solar energy harvesting material for green and cost‐effective photovoltaic applications. The record efficiency of CZTSSe solar cells has recently been refreshed twice after years‐long stagnation, keeping it in the spotlight. Nevertheless, the champion efficiency of 13.6% is still far behind its counterpart Cu(In,Ga)Se2 (CIGS) (23.35%) despite being endowed with a similar electronic structure and nearly‐identical device architecture. In fact, CZTSSe solar cells are more susceptible to non‐radiative recombination at bulk and interfaces, which must be improved for further efficiency advancement. In this review, the state‐of‐art strategies to enhance the power conversion efficiency of CZTSSe solar cells are summarized and discussed, with focus given to three critical device regions i) kesterite absorber, ii) buffer/kesterite interface, and iii) kesterite/back contact interface. With the further elucidation of the latest progress and disclosure of fundamental mechanisms, novel insights toward high‐efficiency kesterite solar cells are proposed. [ABSTRACT FROM AUTHOR]

Effectively incorporating alkali metals or alternative isovalent cations into Cu2ZnSnS4 (CZTS) is considered one of the most promising strategies for realizing a step‐change improvement in the photovoltaic device performance. Herein, the local distribution of Na and Cd by a moisture‐assisted postdeposition annealing (MAPDA) treatment combined with a subsequent heterojunction heat treatment is manipulated. The MAPDA treatment facilitates the controllable reduction of the Na concentration, thus promoting the spontaneous diffusion of Cd into the heterojunction region. A subsequent 150 °C low‐temperature heterojunction heat treatment after MAPDA treatment enables further modification of Cd and Na distributions, leading to significantly enhanced optoelectronic properties at the CZTS/CdS heterojunction and greatly improved device performance with a peak conversion efficiency of 9.40%. The modified heterojunction significantly improves quasi‐Fermi‐level splitting under low‐photon injection, making CZTS solar cells more feasible in low‐light applications. This work provides an effective approach to simultaneously manipulate the distribution of Na and Cd, enabling pronounced modification of the heterojunction quality of CZTS solar cells and boost of conversion efficiencies. Insights gleaned herein may also be applicable to manipulating other critical trace elements in chalcogenide materials in general. [ABSTRACT FROM AUTHOR]

Earth‐abundant and environmentally benign kesterite Cu2ZnSn(S,Se)4 (CZTSSe) is a promising alternative to its cousin chalcopyrite Cu(In,Ga)(S,Se)2 (CIGS) for photovoltaic applications. However, the power conversion efficiency of CZTSSe solar cells has been stagnant at 12.6% for years, still far lower than that of CIGS (23.35%). In this report, insights into the latest cutting‐edge strategies for further advance in the performance of kesterite solar cells is provided, particularly focusing on the postdeposition thermal treatment (for bare absorber, heterojunction, and completed device), alkali doping, and bandgap grading by engineering graded cation and/or anion alloying. These strategies, which have led to the step‐change improvements in the power conversion efficiency of the counterpart CIGS solar cells, are also the most promising ones to achieve further efficiency breakthroughs for kesterite solar cells. Herein, the recent advances in kesterite solar cells along these pathways are reviewed, and more importantly, a comprehensive understanding of the underlying mechanisms is provided, and promising directions for the ongoing development of kesterite solar cells are proposed. [ABSTRACT FROM AUTHOR]

Lithium incorporation in kesterite Cu2ZnSn(S,Se)4 (CZTSSe) materials has been experimentally proven effective in improving electronic quality for application in photovoltaic devices. Herein, a feasible and effective solution‐based lithium post‐deposition treatment (PDT), enabling further efficiency improvement on the high‐performance baseline is reported and the dominant mechanism for this improvement is proposed. In this way, lithium is uniformly incorporated into grain interiors (GIs) without segregation at grain boundaries (GBs), which can occupy the Zn sites with a high solubility in the CZTSSe matrix, producing high density of LiZn antisites with shallower acceptor levels than the intrinsic dominant defect (CuZn antisites). As a result, CZTSSe absorber with better p‐type doping is obtained, leading to a pronounced enhancement in fill factor and a corresponding gain in open‐circuit voltage and short‐circuit current and consequently a significant efficiency boost from 9.3% to 10.7%. This work provides a feasible alternative alkali‐PDT treatment for chalcogenide semiconductors and promotes a better understanding of the mechanism of Li incorporation in kesterite materials. [ABSTRACT FROM AUTHOR]

Abstract: In this research, a new route of surface passivation is reported by introducing hydrogen from the atomic layer deposited (ALD) Al2O3 layer into pure sulfide Cu2ZnSnS4 (CZTS) solar cells. Different amounts of hydrogen are incorporated into the Cu2ZnSnS4/CdS interface through controlling the thickness of the ALD‐Al2O3 layer. The device with three cycles of ALD‐Al2O3 yields the highest efficiency of 8.08% (without antireflection coating) with improved open‐circuit voltage of up to 70 mV. With closer examination on the passivation route of ALD‐Al2O3, it is revealed by the surface chemisty study that the Al2O3 can be etched away by ammonium hydroxide in the CdS buffer deposition process. Instead, the hydrogen is detected within a shallow depth from the CZTS surface, and makes a significant difference in the measured distribution of contact potential difference and device performance. This may be interpreted by the effect of hydrogen passivation of the CZTS surface by curing dangling bonds at the surface of CZTS grains. This work may provide a new direction of further improving the performance of kesterite solar cells. [ABSTRACT FROM AUTHOR]

Sulfurization with various atmosphere and postheat treatments has been reported for earth abundant kesterite Cu2ZnSnS4 (CZTS) preparation as cost-effective material for next-generation solar cells. A full understanding of the nanoscale microstructure and chemistry of CZTS/CdS interface obtained from these different fabrication routes is currently lacking, yet is critical to developing optimal processing routes for high-performance kesterite solar cells. Here, the first detailed investigation of the interfacial microstructure and chemistry of CdS/Cu2ZnSnS4 heterojunctions is presented. For CZTS obtained from sulfurization in a sulfur-only atmosphere where highly defective surfaces are present, air annealing followed by etching in the initial stage of chemical bath deposition (CBD) process can effectively eliminate interfacial defects and allow the epitaxial growth of CBD-CdS, improving the minority lifetime, open circuit voltage ( VOC), and fill factor (FF) of the devices, while blocking Cd diffusion and deteriorating short circuit current ( Jsc). For CZTS from sulfurization in a combined sulfur and SnS atmosphere where CBD-CdS can directly epitaxially grow on CZTS and Cd-diffusion is clearly observed, associated devices show the longest lifetime and the highest efficiency of 8.76%. Epitaxial growth of CdS and Cd diffusion into CZTS are found to be two crucial features minimizing interfacial recombination and achieving high-efficiency devices. This will not only enhance the understanding of the device structure and physics of kesterite based solar cells, but also provide an effective way for designing other chalcogenide heterojunction solar cells. [ABSTRACT FROM AUTHOR]

A kesterite Cu2ZnSnS4 thin film solar cell with efficiency of over 9% is obtained by utilizing Zn1–xCdxS film as a replacement to traditional CdS buffer layer. Zn1–xCdxS film can optimize the conduction band offset between Cu2ZnSnS4 absorber and buffer, forming a minor positive conduction band alignment, thereby alleviating the recombination significantly and improving the open circuit voltage and fill factor efficiently. [ABSTRACT FROM AUTHOR]

Kesterite-based solar cells are attracting considerable attention in recent years, owing to the reduced toxicity and greater abundance of their constituent elements. In this brief review, we discuss the current status of this important technology by focusing on three key aspects of the device: (i) the interface between the kesterite absorber and the Mo back contact, (ii) the kesterite absorber bulk defects and grain boundaries and (iii) the interface between the kesterite absorber and the buffer layer. By identifying key issues to be addressed, we provide suggestions for their potential improvement and future research. Copyright © 2016 John Wiley & Sons, Ltd. [ABSTRACT FROM AUTHOR]

Various characterization methods are implemented to investigate the fundamental properties of a Cu2ZnSnS4 (CZTS) solar cell. The chemical distribution across the CZTS grain boundaries, the surface potential of CZTS absorber, the minority lifetime, the carrier collection length, diode ideality factor, dark saturation current, and series resistance are revealed in the characterization measurement. The short minority lifetime, high defect density, and large series resistance are confirmed and need to be addressed in the future work for further efficiency improvement. [ABSTRACT FROM AUTHOR]

Cd‐free high‐bandgap Cu2ZnSnS4 (CZTS) solar cells are expected to offer green and low‐cost solutions to single‐junction and tandem photovoltaic markets. Despite attracting considerable attention in past years, reported certified efficiency has yet to exceed the 10% threshold. Sn‐related defects, especially those originating from Sn2+ oxidation states, lead to severe recombination loss and limit device performance. Here, the formation of these detrimental defects is suppressed by creating a more benign chemical environment during sulfurization annealing. With dominant Sn4+ states in the source material and the precursor, the oxidation state of Sn remains primarily in its native Sn4+ state during annealing and in the final film. Engineering the Sn‐related defects leads to shallower tail states in bulk CZTS and fewer interfacial defects. As a result, both radiative and non‐radiative recombination losses are alleviated, contributing to a certified 10.7% efficiency of the Cd‐free high‐bandgap CZTS solar cell. This strategy may advance various kesterite materials and other technologies with multivalent constituents. [ABSTRACT FROM AUTHOR]

This paper describes the growth of highly textured Cu 2 ZnSnS 4 (CZTS) thin films on sapphire (0 0 0 1) substrate by radio frequency (RF) magnetron sputtering from a single CZTS target. Working pressure is one of the most important parameters for a one-step RF magnetron sputtering process. The influence of working pressure on the composition and the structural, morphological, and optical properties of CZTS thin films has been investigated is this paper. The properties of Zn-rich and Cu-poor and stoichiometric CZTS thin films are compared to study the effect of film composition. Using photoluminescence (PL) and time-resolved photoluminescence (TRPL) techniques, two PL bands are observed from the Zn-rich and Cu-poor highly textured CZTS. In addition to the band to band transition at 1.39 eV, a PL band at 1.26 eV is ascribed to the donor–acceptor recombination. The band edge transition exhibits a PL lifetime of 17.2 ns. In contrast, the band of donor–acceptor recombination exhibits a much longer lifetime of 177.3 ns. The understanding of the film formation mechanism from single target sputtering may improve the standard preparation method for high quality CZTS absorbers. [ABSTRACT FROM AUTHOR]

Highlights • Cu 2 ZnSnS 4 thin films are fabricated on Si substrates by one-step sputtering. • Cu 2 ZnSnS 4 solar cells on Si with photovoltaic response are fabricated. • The interactions between Cu 2 ZnSnS 4 and Si are studied. Abstract Integrating commercialized Si solar cells with eco-friendly and earth-abundant Cu 2 ZnSnS 4 (CZTS) film is a promising method to increase power conversion efficiency and hence reduce the levelized cost of electricity. However, synthesis of CZTS thin film on Si as well as the study of the interaction between the two materials, which are crucial for good performance of CZTS/Si two-terminal devices, are areas that have been less investigated. Here, we grow polycrystalline CZTS thin films on Si (1 0 0) substrate by sputtering and study the properties of the CZTS thin film and interface between the CZTS and Si. The CZTS shows uniform microstructure and optimal optical properties. A CZTS solar cell which is fabricated on Si shows a photovoltaic response although subjected to high serious resistance, and Cu diffusion was found from CZTS into Si, which caused needle-like dislocations in Si. Therefore, an effective conductive barrier layer between CZTS and Si is desirable to inhibit Cu from diffusing into Si for tandem solar cell purposes. The study offers valuable input for understanding the properties of CZTS thin film sputtered from single target sputtering and the impact on the interfaces and underlying Si, suggesting concerns that manufacturers need to be aware of for its application in tandem solar cells based on Si. [ABSTRACT FROM AUTHOR]

In this work we report the Na incorporation from Na-doped Mo (Mo-Na) back contact for kesterite Cu 2 ZnSnS 4 solar cells on flexible stainless steel substrates. It is demonstrated that Na can be effectively incorporated into CZTS by inserting Mo-Na layer at back contact. Direct contact of CZTS and Mo-Na layer leads to poor homogeneity and adhesion. The thickness of MoS 2 formed at the back contact depends on the presence of Na and whether Mo contacts with CZTS directly. Back contact configuration with a Mo capping layer on Mo-Na layer is found to be helpful to maintain the advantages of Mo back contact and control the thickness of MoS 2 interface. As a result, CZTS device fabricated on this configuration yields higher conversion efficiency of 6.2%. However, this efficiency is still far lower than that on traditional soda lime glass substrate which shows efficiency over 8%. The loss mechanism of device fabricated on stainless steel is investigated and analyzed according to the device performance and electrical parameters. [ABSTRACT FROM AUTHOR]

Short minority carrier lifetime and low open circuit voltage (Voc) are key issues limiting the current efficiency development for Cu 2 ZnSnS 4 (CZTS) thin film solar cells. This work presents the use of Cd ion soaking and post-heat treatment to increase the lifetime and Voc of CZTS. The time-resolved photoluminescence (TRPL) results confirmed that Cd ion soaking and post heat treatment is effective in enhancing the minority lifetime, from ∼10 ns up to ∼28 ns. With analyses of the current density- voltage (J-V) curves and external quantum efficiency (EQE) data, Cd ion soaking and subsequent post heat treatment is found to greatly reduce the recombination and improve the junction quality, contributing to a ∼70 mV Voc enhancement and resulting in the increased device efficiency of 7.6%, from 5.9%. [ABSTRACT FROM AUTHOR]

In this research, we present thermal evaporated MoO 3 layer as a primary back contact for pure sulphide Cu 2 ZnSnS 4 solar cells. The effects of incorporating MoO 3 in primary back contact and its thickness on the Cu 2 ZnSnS 4 device performance are investigated. The MoO 3 layer acts as enhancing sodium diffusion site where sodium is more effectively diffused into CZTS absorber, facilitating the formation of larger CZTS grains during sulfurization process compared to the reference absorber. The power conversion efficiency is improved from 5.2% to 6.2% on average, yielding the highest efficiency of 6.52% by the insertion of 10 nm MoO 3 layer between Cu 2 ZnSnS 4 absorber and molybdenum contact. The major efficiency enhancement arises from open circuit voltage which is improved from 530 to 615 mV. [ABSTRACT FROM AUTHOR]

We report on the fabrication of a 5.2% efficiency Cu 2 ZnSnS 4 (CZTS) solar cell made by pulsed laser deposition (PLD) featuring an ultra-thin absorber layer (less than 450 nm). Solutions to the issues of reproducibility and micro-particulate ejection often encountered with PLD are proposed. At the optimal laser fluence, amorphous CZTS precursors with optimal stoichiometry for solar cells are deposited from a single target. Such precursors do not result in detectable segregation of secondary phases after the subsequent annealing step. In the analysis of the solar cell device, we focus on the effects of the finite thickness of the absorber layer. Depletion region width, carrier diffusion length, and optical losses due to incomplete light absorption and back contact reflection are quantified. We conclude that material- and junction quality is comparable to that of thicker state-of-the-art CZTS devices, even though the efficiency is lower due to optical losses. [ABSTRACT FROM AUTHOR]

Low Voc is the major factor limiting the current efficiency of pure sulfide Cu 2 ZnSnS 4 (CZTS) thin film solar cells. In this work, stacking two CZTS layers with different majority doping levels is employed to increase Voc. With this double-layer structure, the obtained highest efficiency is 7.57% with Voc of 734 mV, Jsc of 15.4 mA/cm 2 and FF of 67.0%. Compared to the traditional device with single CZTS layer (Efficiency: 7.62%, Voc: 665 mV, Jsc: 20.0 mA/cm 2 , FF: 57.3%), the average Voc has been increased by 70–80 mV. However the Jsc was decreased due to voids within the CZTS and severe band tailing problem, limiting the further boost of efficiency for double-layer CZTS solar cell. [ABSTRACT FROM AUTHOR]

In this work we perform comprehensive characterization on a 6.9% pure sulphide Cu 2 ZnSnS 4 (CZTS) device and construct a 2D device model in Sentaurus TCAD to identify possible roots of performance bottlenecks. Electrical and optical parameters of the absorber from comprehensive electrical and optical characterization, together with other necessary parameters from literature, we successfully reproduce measured current density-voltage (J-V) and external quantum efficiency (EQE) curves. Absorption coefficient is extracted by fitting measured internal quantum efficiency (IQE). At the buffer/absorber interface, a surface recombination velocity of 1×10 5 cm/s is identified to adequately describe measured spectral response at the near-interface region. Furthermore, a bulk lifetime of ~29 ns is extracted from effective lifetime modelling in conjunction with time resolved photoluminescence (TRPL) results. The key underlying V oc deficit, ~200 mV, is pinpointed to bandgap fluctuation, which is backed by the simulation study on both QE tail and steady state photoluminescence. [ABSTRACT FROM AUTHOR]

Kesterite Cu 2 ZnSnS 4 (CZTS) thin film solar cells are fabricated based on sputtering and post sulfurization process on stainless steel substrates. NaF layers with different thickness are used as external sodium source to address the lack of Na issue in Na-free steel substrates and 10 nm of NaF layer is proved to be the optimal thickness. Sodium incorporation into CZTS induces the metal element redistribution, facilitates CZTS film recrystallization and promotes the phase evolution. Appropriate amount of sodium is evidenced to yield an enhancement in power conversion efficiency from 3.07% to 4.10% whilst further increase in sodium tends to deteriorate the device efficiency. Device performance deterioration is correlated to the rather small grain size accompanied with a large amount of grain boundaries and unfavorable SnS 2 secondary phase for CZTS samples without sodium, while pinholes and lower carrier density in absorber for CZTS samples with over amount of sodium. [ABSTRACT FROM AUTHOR]

In this work, a thin layer of bismuth (Bi) is pre-deposited on the Mo-coated glass before the deposition of the Cu 2 ZnSnS 4 to optimize the properties of the Cu 2 ZnSnS 4 thin film and the performance of corresponding solar cell. It is found that the pre-deposition of Bi leads to the improvement in the crystallinity of synthesized Cu 2 ZnSnS 4 film as evidenced by large grain sizes and less grain boundaries. Photoluminescence measurement indicates that the recombination in the film is inhibited as the reduction of the boundaries which is always regarded as the recombination centers of the carriers. Besides, the reaction of Zn into CZTS lattice is promoted with the decrease of the second phase ZnS. In addition, the inserted Bi layer blocks the diffusion of S atoms into Mo with the reduced thickness of MoS 2 at CZTS|Mo interface. It decreases the cell series resistance. Because of the improvements above, the performance of the cell with pre-deposited Bi is boosted. [ABSTRACT FROM AUTHOR]

The large open circuit voltage (Voc) deficit (Eg/ q -Voc) is the key factor limiting the current efficiency of pure sulfide Cu 2 ZnSnS 4 (CZTS) thin film solar cells. This present work reports CZTS devices with a Voc of over 710 mV by utilizing either In 2 S 3 buffer or In 2 S 3 /CdS hybrid buffer. The improvement in Voc mainly results from (i) an increased carrier concentration in CZTS due to In-doping when the In 2 S 3 buffer is adjacent to the CZTS absorber and (ii) favorable conduction band alignments at the CZTS/buffer interface. However, devices with In 2 S 3 buffers suffer from having a lower Fill Factor (FF) and short circuit current density (Jsc) when compared with those with CdS buffers. In contrast devices with In 2 S 3 /CdS hybrid buffers not only yield an enhancement in Voc, but also give the same level of FF and an even higher Jsc relative to CdS buffers, thereby increasing the efficiency from 5.5% to 6.6%. These hybrid In 2 S 3 /CdS buffers provide a promising way to reduce the Voc deficit and further boost the efficiency of pure sulfide CZTS solar cells. [ABSTRACT FROM AUTHOR]

Analysis of ZnS segregation behaviour and its influence on the device performance has been made on the Zn-rich Cu 2 ZnSnS 4 thin film solar cells. Cross-sectional transmission electron microscopy images reveal that ZnS is the main secondary phase in the Cu 2 ZnSnS 4 layer obtained from a sulphurised Zn/CuSn metallic stack. The excess Zn diffuses from back contact region to top surface of Cu 2 ZnSnS 4 layer accumulating in the form of ZnS. The solar cell with a higher Zn concentration shows a large quantity of isolated ZnS grains at Cu 2 ZnSnS 4 top surface which is close to CdS/Cu 2 ZnSnS 4 heterojunction interface. Soft X-ray absorption spectroscopy indicates a large spike-like conduction band offset between Cu 2 ZnSnS 4 and ZnS. Consequently, such much ZnS precipitates would increase series resistance and generate lower short-circuit current and external quantum efficiency. However, appropriate amount of ZnS at the space charge region of the solar cell has beneficial effects by reducing the heterojunction interface recombination. Therefore, an improved open-circuit voltage and a higher shunt resistance are achieved. This paper provides a possible method to intentionally segregate ZnS at the space charge region by depositing the Zn layer at the bottom of co-sputtered CuSn layer. Although it is difficult to synthesis a pure phase Cu 2 ZnSnS 4 absorber, we can utilise the ZnS secondary phase to improve the Cu 2 ZnSnS 4 solar performance by controlling the Zn-excess amount. [ABSTRACT FROM AUTHOR]

Highlights: [•] The Mo/Zn/(Cu & Sn) metallic structure was utilized to fabricate CZTS solar cell. [•] Found that Zn rich composition facilitate the formation of large grain. [•] Sn composition is highly correlated Cu content with Cu/Sn ratio of two. [Copyright &y& Elsevier]

• Cu 2 SrSnS 4 (CSTS) thin films synthesized via a sol-gel based solution process. • Morphological, phases and optical properties of CSTS thin films characterized. • 600°C annealing and Sr/Sn atomic ratios of 1.15 were the best preparation conditions. • Champion CSTS solar cell with 0.164% power conversion efficiency obtained. • Feasibility of solar energy harvesting of CSTS material demonstrated. According to theory calculation, the Cu 2 SrSnS 4 (CSTS) become a candidate material for harvesting solar energy via either photovoltaic (PV) or photoelectrochemical (PEC) paths due to its efficient light-absorbing capability (high absorption coefficients above 104 cm−1), earth-abundant, nontoxic constituents, and suitable defect properties. As a new material, there is a long way to accomplish the application of CSTS. Film preparation of CSTS are very critical. In this work, CSTS thin films were synthesized by a sol-gel based solution process. The obtained CSTS films showed trigonal structure with band gap of 1.93 eV and p-type conductivity. By comparing the CSTS thin films synthesized with different annealed temperature and Sr/Sn atomic ratios, we confirmed that sulfurization annealing at 600°C and Sr/Sn atomic ratios of 1.15 yields relatively high quality CSTS films. A PEC cell using the CSTS thin film as working electrode were established and a saturated photocurrent of ∼0.5 mA/cm2 had been achieved. It has also been applied to a PV device, demonstrating open-circuit voltage of 296 mV and power conversion efficiency of 0.164%. Pinholes in the films and reef-like grains at the surface of CSTS films were likely to limit the devices performance. The feasibility of solar energy harvesting of CSTS material was demonstrated. [ABSTRACT FROM AUTHOR]