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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Crystallography

Background:

  • Hybrid metal halides (HMHs) are tunable optoelectronic materials.
  • Pressure can modulate HMH properties, but effects are often reversible.
  • A method for permanent band-structure modification in HMHs is needed.

Purpose of the Study:

  • To investigate pressure-induced polymerization (PIP) as a strategy for irreversible band-structure engineering in HMHs.
  • To explore the effects of PIP on the electronic properties of three specific HMH crystals: (m-APA)2Pb3I8, (m-APA)2PbBr4, and (m-APA)PbCl3.
  • To demonstrate the potential of PIP for permanent functional design of HMHs.

Main Methods:

  • Synthesis and characterization of three HMH crystals: (m-APA)2Pb3I8, (m-APA)2PbBr4, and (m-APA)PbCl3.
  • Application of high pressure to induce polymerization of the m-aminophenylacetylene (m-APA) cation within the HMH structures.
  • Analysis of the resulting polymeric phases using techniques to determine band gaps, band alignments, and cation structures (sp2/sp3-C ratios).

Main Results:

  • Distinct polymerization pathways were observed, yielding novel, ambient-stable polymeric HMH phases.
  • The band gaps were narrowed, and band alignments were reconfigured in the resulting materials.
  • The polymeric cations exhibited varied sp2/sp3-C ratios, tuning electronic coupling and leading to different band alignment transitions (e.g., type I to type II).

Conclusions:

  • Pressure-induced polymerization (PIP) is a viable and general strategy for permanent band-structure engineering in HMHs.
  • PIP enables the creation of novel HMH phases with tailored electronic properties through controlled covalent transformation of organic cations.
  • This approach offers a pathway for the functional design of HMHs with permanently modified electronic structures.