Sn-deficiency in the electrodeposited ternary CuxSnySz thin films by ECALE

Caporali, Stefano; Tolstogouzov, A.; Teodoro, O.M.N.D.; Innocenti, Massimo; Benedetto, Francesco Di; Cinotti, Serena; Picca, Rosaria Anna; Cioffi, Nicola

doi:10.1016/j.solmat.2015.02.029

Cited by 16 publications

(14 citation statements)

References 46 publications

(55 reference statements)

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“…Copper sulfide thin films have been fabricated by various deposition techniques, such as chemical vapor deposition, sputtering, spray pyrolysis, chemical bath deposition, and electrochemical methods . However, in most cases the required control over the film stoichiometry and phase composition is poorly achieved due to the coexistence of several stable and metastable copper sulfide phases .…”

Section: Introductionmentioning

confidence: 99%

Atomic Layer Deposition of Conducting CuS Thin Films from Elemental Sulfur

Tripathi

Lahtinen

Karppinen

2018

Adv Materials Inter

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Copper sulfide thin films have been fabricated by various deposition techniques, such as chemical vapor deposition, [15] sputtering, spray pyrolysis, [16,17] chemical bath deposition, [18,19] and electrochemical methods. [20][21][22] However, in most cases the required control over the film stoichiometry and phase composition is poorly achieved due to the coexistence of several stable and metastable copper sulfide phases. [23] Moreover, fabrication of continuous copper sulfide coatings with a well-controlled morphology on highaspect-ratio nanostructures has remained a challenge. It is here in particular where the atomic layer deposition (ALD) technique could provide us with clear advantages over the other thin-film technologies for the deposition of high-quality copper sulfide thin films for various advanced applications including the photovoltaics. [17,24,25] Atomic layer deposition is based on sequential and self-limiting gas-surface reactions and is known to yield exceptionally homogeneous coatings in atomic-scale precision independent of the substrate geometry.The vast majority of the metal sulfide ALD processes is based on metal-organic precursors together with hydrogen sulfide H 2 S as the source of sulfur; [26] the same applies to the reported copper sulfide ALD processes as well (see Table 1). The main merit of H 2 S is that it is highly reactive toward common metal precursors. However, H 2 S is a flammable, corrosive, and highly toxic gas, and its incorporation in the ALD technology presents several serious technical challenges. The special precautions required for the safe use of H 2 S may even be one of the reasons why only 16 metal sulfide ALD processes have been so far reported during the half a century long ALD history. [26] Another drawback of the H 2 S-based ALD processes is the slowness of these processes, see, e.g., the growth rate values given in Table 1 for the copper sulfide processes. Moreover, majority of the reported copper sulfide processes yields Cu(I) sulfide as the main phase; hence, there is a clear interest in a new robust and efficient ALD process for high-quality Cu(II) sulfide thin films. [27] Despite the fact that some of the early ALD processes employed elemental sulfur instead of H 2 S as the sulfur source, [35] to the best of our knowledge no sulfur-based ALD processes have been reported for copper sulfide thin films. Here, we present a simple and efficient low-temperature ALD process for the deposition of high-quality p-type conducting CuS thin films from copper acetyl acetonate and elemental sulfur precursors, as a highly viable solution to the challenges discussed above.A facile, yet precisely controlled and efficient atomic layer deposition (ALD) process is reported for high-quality copper(II) sulfide thin films based on elemental solid sulfur as the source for sulfur; Cu(acac) 2 (acac: acetylacetonate) is used as the copper precursor. In the deposition temperature range as low as 140-160 °C, the process proceeds in an essentially ideal ALD manner and yields single-phase C...

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Section: Introductionmentioning

confidence: 99%

Atomic Layer Deposition of Conducting CuS Thin Films from Elemental Sulfur

Tripathi

Lahtinen

Karppinen

2018

Adv Materials Inter

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“…This conundrum has been overcome taking into account two deposition processes that were different with respect to the potential related to a small bump in the CVs: (1) potentiostatic in underpotential conditions and (2) potentiostatic in slightly overpotential conditions. The charge deposited by means of the two procedures to the deposition of the partial atomic layer of Cd over a sulfide substrate [8,37] confirming the process as an effective SLR Cd deposition. Moreover, thanks to the XPS investigations, the occurrence of a complex sample composition (including the eventual presence of ZnS oxidation and/or the alloying between CdS and ZnS) is revealed.…”

Section: Cds/cu X Zn Y Smentioning

confidence: 69%

Operando Structural Characterization of the E-ALD Process Ultra-Thin Films Growth

Giaccherini¹,

Felici²,

Innocenti³

2017

X-Ray Characterization of Nanostructured Energy Materials by Synchrotron Radiation

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Spanning from nanoelectronics to new solar energy materials, technological development in the recent years requested highly controlled nanostructured surfaces, ultra-thin films, and 2D structured materials. In general, although very favorable from a full life cycle assessment (FLCA) standpoint, electrodeposition hardly allows to obtain the high order required by recent technologies. In particular cases, the electrodeposition enables the deposition of atomic layers by means of surface limited reactions (SLRs). By exploiting SLRs, it is possible to define layer-by-layer deposition scheme of different atomic layers; we refer to these schemes as electrochemical atomic layer deposition (E-ALD) and when the growth of the film is epitaxial with the substrate, the techniques are called electrochemical atomic layer epitaxy (ECALE). Aiming at characterizing structure and growth of materials grown by means of E-ALD, surface analysis techniques apply better. In particular, surface X-ray diffraction (SXRD) with high brilliance synchrotron sources enables the operando structural analysis in electrochemical environment. In recent years, several works on the operando surface characterization by means of SXRD have been reported. Thanks to novelties in the field of operando SXRD experiments, semiconducting systems were studied, such as single and multilayer of CdS and Cu 2 S.

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“…Our research involves the use of the ECALE deposition technique for the growth of ultra-thin films of metal sulfide, [22][23][24][25] and other, materials. So far we have been able to successfully develop several films of materials, including CdS, CdTe, CdSe, ZnS, ZnSe, NiS, PbS, CuS, and InAs.…”

Section: 1117/21201512006249 Page 2/3mentioning

confidence: 99%

Fabricating energy devices with low environmental impacts

Innocenti¹,

Benedetto²,

Lavacchi³

et al. 2016

SPIE Newsroom

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Techniques such as electrochemical atomic layer epitaxial deposition can be used to grow high-quality pseudo-2D layers of photovoltaic materials.Efforts to reduce the rate of carbon emissions from industry, 1 as well as the impending economic and social problems that could arise from the depletion of fossil fuels, 2 are the two driving forces for the development of devices that can generate electric power from renewable sources. It is necessary for research and development in this field to satisfy a few major requirements. In the last few decades, the increasing demand for high-tech applications has led to increasing solicitation of mineral deposits and has brought many rare metals to the brink of irreversible depletion. 3 It is therefore necessary for new devices to be based on abundant materials that are available on a global or local scale. The whole 'life cycle' of the materials must also be environmentally friendly (i.e., the materials must be non-toxic and easily recycled). Moreover, the materials must be energetically favorable, i.e., they must involve low-energy consumption processes during all the phases of the life cycle (production, to maintenance, to decommission, to recycling). This final aspect-which can be determined accurately through a full life cycle assessment (LCA)-depends on the energy costs and energy conversion efficiency of the device itself. In a full LCA, several parameters are estimated. These include the payback time (time required to earn the energy costs of the production process), the energy return on energy investment (ratio between the energy produced by and the energy costs of the system along the whole life cycle), 4 and the net energy (the energy delivered to society for discretionary uses after all the energetic costs are subtracted from the energy produced). This last figure of merit (i.e., the net energy) is a crucial parameter for defining energy policy. 4 All these requirements for renewable energy devices can be met satisfactorily by solar cells that are based on pseudo-ternary sulfides, such as stannite (Cu 2 FeSnS 4 ), kuramite (Cu 3 SnS 4 ), and kesterite (Cu 2 ZnSnS 4 ). 5 Kesterite-type semiconductors are Figure 1. Schematic illustration of the electrochemical atomic layer epitaxial deposition (ECALE) technique for the growth of quaternary metallic compound thin films.generally synthesized by high-temperature solidification, in the vapor phase, or under high-vacuum conditions. Other easier and cheaper methods (e.g., from aqueous solutions), however, can also be considered. Electrochemical techniques, for example, are particularly suitable for satisfying the requirements. Indeed, with these methods, a low cost can be achieved with relatively simple instrumentation, low working temperatures, and accurate control of the experimental parameters. 6 Furthermore, morphological, structural, and compositional control of the final deposited film can be obtained.In our work, we use a particular electrochemical techniqueknown as electrochemical atomic layer epitaxial deposition...

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Sn-deficiency in the electrodeposited ternary CuxSnySz thin films by ECALE

Cited by 16 publications

References 46 publications

Atomic Layer Deposition of Conducting CuS Thin Films from Elemental Sulfur

Atomic Layer Deposition of Conducting CuS Thin Films from Elemental Sulfur

Operando Structural Characterization of the E-ALD Process Ultra-Thin Films Growth

Fabricating energy devices with low environmental impacts

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