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Polymorphic Control of Solution-Processed Cu2SnS3 Films with Thiol-Amine Ink Formulation.

Kristopher M Koskela1, Carlos Mora Perez1, Dmitry B Eremin1,2

  • 1Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States.

Chemistry of Materials : a Publication of the American Chemical Society
|October 17, 2022
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Researchers developed new molecular inks for creating pure semiconductor films. By changing the thiol in thiol-amine solvents, they controlled the specific crystal structure (polymorph) of copper tin sulfide films.

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Area of Science:

  • Materials Science
  • Inorganic Chemistry
  • Solid-State Chemistry

Background:

  • Growing demand for tailored molecular inks for solution-processed semiconductor films.
  • Copper tin sulfide (Cu₂SnS₃) is an I₂-IV-VI₃ semiconductor with multiple polymorphs.
  • Controlling semiconductor film structure is crucial for device performance.

Purpose of the Study:

  • To develop molecular inks for phase-pure solution-processed Cu₂SnS₃ films.
  • To achieve polymorphic control over Cu₂SnS₃ films using thiol-amine solvent mixtures.
  • To understand the relationship between ink formulation and resulting film structure.

Main Methods:

  • Dissolving copper(I) sulfide (Cu₂S) and tin(II) oxide (SnO) precursors in thiol-amine solvents.
  • Utilizing different thiols (1,2-ethanedithiol vs. 2-mercaptoethanol) to influence ink properties.
  • Annealing the inks to form thin films and characterizing their crystalline structure and properties.

Main Results:

  • Free-flowing molecular inks were successfully generated from inexpensive precursors.
  • Phase-pure tetragonal and orthorhombic Cu₂SnS₃ films were obtained by switching the thiol.
  • Polymorph control was linked to molecular metal-thiolate complexes and decomposition pathways.
  • Films exhibited similar p-type semiconducting behavior with direct optical band gaps of 0.94 eV (tetragonal) and 0.88 eV (orthorhombic).
  • Strong photoelectrochemical current responses were observed for both polymorphs.

Conclusions:

  • Thiol-amine ink formulation provides a route for polymorphic control of Cu₂SnS₃.
  • The choice of thiol dictates the formation of specific Cu₂SnS₃ polymorphs.
  • This understanding can guide the development of novel inks for solution-processed semiconductor films.