Si Electrochemical Liquid Phase Epitaxy: Low-Temperature Growth of Hyperdoped Epitaxial Si Films

Downes, Nathanael; DeMuth, Joshua; Waelder, Jacob; Cheek, Quintin; Bartels, Hannah; Maldonado, Stephen

doi:10.1021/acs.chemmater.2c01899

Cited by 6 publications

(13 citation statements)

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“…B. Bartels, H. Maldonado, S. 10.1021/acs.chemmater.2c01899Chem. Mater.2022341086110872 Evidence for Facilitated Surface Transport during Ge Crystal Growth by Indium in Liquid Hg-In Alloys at Room TemperaturePattadarD.CheekQ.SartoriA.ZhaoY.GiriR.…”

Section: Key Referencesmentioning

confidence: 99%

“…We used a pulsed electrodeposition waveform (Figure g) that prevents the accumulation of deleterious side products . Macroscopic Si epifilms with micrometer thicknesses were then readily obtained (Figures h,i).…”

Section: Controlling the Location Of Nucleation And Crystal Growthmentioning

confidence: 99%

“…We used a pulsed electrodeposition waveform (Figure 4g) that prevents the accumulation of deleterious side products. 3 Macroscopic Si epifilms with micrometer thicknesses were then readily obtained (Figures 4h,i). The collected microscopic and diffraction data indicated that the crystal structure of the electrodeposited films was a direct extension of the underlying substrate without any obvious sign of an intervening oxide layer (Figure 4j−l).…”

Section: And Crystal Growthmentioning

confidence: 99%

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Understanding and Expanding the Prospects for Electrosynthesis with Liquid Metal Electrodes

Hazelnis

Maldonado

2023

Acc. Chem. Res.

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Metrics & MoreArticle Recommendations CONSPECTUS: This Account describes and summarizes the latest work from our laboratory on developing and maturing strategies based on low-temperature liquid metals as reaction environments for materials synthesis. The electrochemical liquid−liquid−solid (ec-LLS) crystal growth concept is a hybrid method that combines electrodeposition and melt crystal growth. Using liquid metals as both electrodes and solvents for the purpose of producing inorganic crystals and materials, a simple and environmentally friendly process is possible. The impetus is to address the key deficiency in the inorganic crystalline materials that are the basis of modern optoelectronics and renewable energy capture/conversion systems. Specifically, existing methods for synthesizing crystalline inorganic materials for these purposes are largely energy-and resource-intensive, with a substantial impact on the environment when scaled. A long-term goal of our work with ec-LLS is to realize a materials synthetic process that is matured without requiring intensive resources or negatively impacting the environment. To this end, the factors that both limit and govern ec-LLS processes must be identified and understood. To date, questions regarding the factors that affect crystal nucleation and growth, form factors, and overall composition remain.Previous work established concretely ec-LLS as a versatile method for synthesizing and producing crystalline semiconductors at low temperatures as either particles, nanowires, or microwires. Subsequent experiments have focused on two tiers. First, the microscopic details of the liquid metal and its interfaces that dictate materials synthesis and crystal growth must be identified. Second, strategies that widen the attainable material form factors to facilitate device architectures must be realized. Hence, this Account describes results aimed at answering three questions: (1) What are the consequences of reaching supersaturation by an electrochemical rather than a thermal driving force for crystal growth in ec-LLS? (2) Can the location of nucleation and subsequent crystal growth be controlled? (3) Does the atomic structure of the liquid metal affect product formation in ec-LLS? The science described herein illustrates the value of in situ methods spanning transmission electron microscopy, X-ray diffraction, and X-ray reflectance for revealing the role that liquid metal composition and structure can play in ec-LLS. Additionally, we summarize work that shows for the first time that it is possible to produce both single-crystalline epitaxial films and complex intermetallic compounds through ec-LLS by tuning the cell design, electrochemical excitation waveform, and composition of the liquid metal electrodes.The cumulative findings described here substantially enrich our understanding of the ec-LLS concept while simultaneously motivating further questions moving forward. Is it possible to attain complete control over the crystalline quality and composition of ec-LLS products? Can th...

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Section: Key Referencesmentioning

confidence: 99%

Section: Controlling the Location Of Nucleation And Crystal Growthmentioning

confidence: 99%

Section: And Crystal Growthmentioning

confidence: 99%

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Understanding and Expanding the Prospects for Electrosynthesis with Liquid Metal Electrodes

Hazelnis

Maldonado

2023

Acc. Chem. Res.

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“…Electrochemical cells can support the direct electrification of chemical manufacturing and construction (9)(10)(11)(12)(13)(14). The electrochemical reduction of iron oxide, using electricity sourced from lowcarbon, renewable resources (i.e.…”

Section: Introductionmentioning

confidence: 99%

Electrochemical Chlor-Iron Process for Iron Production from Iron Oxide and Seawater

Noble¹,

Moutarlier²,

Kempler³

2023

Preprint

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The iron and steel industry accounts for ~ 8% of global greenhouse gas emissions. Electrochemical reduction of iron ore to metal for electric arc furnaces can enable sustainable steel production, but existing electrochemical processes require expensive capital or electrolytes. We report a low-temperature, electrochemical cell that consumes low-cost and abundant iron oxide and seawater, while co-producing NaOH and Cl2 with industrially relevant current densities reaching 300 mA cm-2 and current efficiencies >90 %. Freestanding films of phase-pure iron were formed after 4 h of continuous, stable electrolysis. The process can lead to levelized costs of iron that are competitive with iron produced in fossil-fuel-powered blast furnaces (< $500 per metric tonne) and the co-produced NaOH can be used for CO2 mineralization from the air or ocean, creating a net negative-emission process.

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“…The use of liquid metal catalysts for the growth of semiconductor crystals has been introduced to electrochemical systems by Maldonado, , and so-called electrochemical liquid–liquid–solid (ec-LLS) has been applied for the electrochemical growth of various semiconductors such as Ge, GaAs, and Si. , During VLS and ec-LLS growth, the liquid metal catalyst significantly affects all aspects of the Si crystal, such as the growth rate, shape, crystal structure, and doping. , Similarly, the use of a liquid catalyst might be another strategy for the electrochemical growth of high-quality Si. However, its role in the electrochemical growth in molten salt remains uncertain because photoactive Si and a controllable doping can be obtained without a liquid metal catalyst. ,,, In this study, the role of the liquid metal catalyst was investigated thoroughly by comparing the properties of Si grown with and without a liquid metal catalyst.…”

Section: Introductionmentioning

confidence: 99%

Unraveling the Role of Liquid Metal Catalysts in Electrochemical Growth of Solar Si from SiO₂ in CaCl₂-Based Molten Salt: Enhancement of Crystallization, Purity, and Photoresponse

Lee

et al. 2023

ACS Appl. Energy Mater.

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The electrochemical growth of Si has been developed as an alternative method of producing highly crystalline and pure semiconducting solar Si. The use of liquid catalysts for the electrochemical growth of semiconductors has been suggested to improve their quality. In this study, the role of liquid catalysts during the direct electrochemical growth of Si from SiO2 in CaCl2-based molten salts was investigated by comparing the crystallinity, purity, and photoresponse of Si deposited with and without liquid catalysts. A liquid catalyst was introduced into Si via the codeposition of Au or Ag, thereby forming a eutectic liquid mixture with Si during electrochemical growth. The use of liquid catalysts did not affect the growth rate of Si. Conversely, the liquid catalysts cause significant morphological changes associated with an approximately 2-fold increase in the grain size of Si, as estimated from X-ray diffraction and Raman analyses, by offering a low interface energy for Si nucleation. In addition, secondary ion and inductively coupled plasma mass spectroscopy analyses revealed that Al from the SiO2 feedstock was the primary impurity within the Si deposit and that its amount decreased when a liquid catalyst was used to filter the impurities during Si growth. Subsequently, the enhanced crystallization and purification of the liquid catalysts increased the photoresponse of the Si deposit, as confirmed by photoelectrochemical measurements. These results suggest that the electrochemical growth of Si using liquid catalysts can enhance the quality of Si, reflecting its potential to replace the conventional process of Si production.

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Si Electrochemical Liquid Phase Epitaxy: Low-Temperature Growth of Hyperdoped Epitaxial Si Films

Cited by 6 publications

References 88 publications

Understanding and Expanding the Prospects for Electrosynthesis with Liquid Metal Electrodes

Understanding and Expanding the Prospects for Electrosynthesis with Liquid Metal Electrodes

Electrochemical Chlor-Iron Process for Iron Production from Iron Oxide and Seawater

Unraveling the Role of Liquid Metal Catalysts in Electrochemical Growth of Solar Si from SiO₂ in CaCl₂-Based Molten Salt: Enhancement of Crystallization, Purity, and Photoresponse

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Si Electrochemical Liquid Phase Epitaxy: Low-Temperature Growth of Hyperdoped Epitaxial Si Films

Cited by 6 publications

References 88 publications

Understanding and Expanding the Prospects for Electrosynthesis with Liquid Metal Electrodes

Understanding and Expanding the Prospects for Electrosynthesis with Liquid Metal Electrodes

Electrochemical Chlor-Iron Process for Iron Production from Iron Oxide and Seawater

Unraveling the Role of Liquid Metal Catalysts in Electrochemical Growth of Solar Si from SiO2 in CaCl2-Based Molten Salt: Enhancement of Crystallization, Purity, and Photoresponse

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Product

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Unraveling the Role of Liquid Metal Catalysts in Electrochemical Growth of Solar Si from SiO₂ in CaCl₂-Based Molten Salt: Enhancement of Crystallization, Purity, and Photoresponse