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Mixed-vs-Segregated Stack Polymorphism in the N,N,N',N'-Tetramethylbenzidine-TCNQF4 Charge Transfer Complex.

Elena Ferrari1,2, Francesco Mezzadri1, Matteo Masino1

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Researchers developed a novel organic charge transfer (CT) cocrystal using N-TMB and TCNQF4 that exhibits both mixed and segregated stack structures. This finding expands the understanding of CT crystal polymorphism and material design.

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Area of Science:

  • Materials Science
  • Solid-State Chemistry
  • Crystallography

Background:

  • Organic charge transfer (CT) cocrystals are 1-D materials formed by donor (D) and acceptor (A) molecules.
  • These materials typically exhibit segregated (separate D/A columns) or mixed (alternating D-A) stack motifs.
  • Polymorphism in CT crystals is common, but coexisting mixed and segregated stack phases are rare.

Purpose of the Study:

  • To synthesize and characterize a new organic CT cocrystal exhibiting both mixed and segregated stack phases.
  • To investigate the structural and optical properties of these coexisting phases.
  • To explore potential stack distortions in the segregated phase at low temperatures.

Main Methods:

  • Synthesis of a novel CT complex using N-TMB (donor) and TCNQF4 (acceptor).
  • Single-crystal X-ray diffraction for structural analysis.
  • Polarized infrared (IR) and Raman spectroscopy for optical characterization.

Main Results:

  • A new CT complex of N-TMB and TCNQF4 was successfully synthesized, displaying both mixed and segregated stack motifs.
  • Common structural and optical features were identified between the mixed and segregated phases using spectroscopy and X-ray diffraction.
  • Low-temperature data indicated a stack distortion within the segregated stack phase.

Conclusions:

  • This study presents a rare example of an organic CT cocrystal exhibiting both mixed and segregated stack phases.
  • The findings highlight the potential for designing materials with tunable structural motifs.
  • The observed stack distortion in the segregated phase warrants further investigation into its electronic implications.