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Two-Dimensional Phosphorus Porous Polymorphs with Tunable Band Gaps.

Zhiwen Zhuo1, Xiaojun Wu1, Jinlong Yang1

  • 1CAS Key Laboratory of Materials for Energy Conversion, School of Chemistry and Materials Sciences, and CAS Center for Excellence in Nanoscience, ‡Hefei National Laboratory of Physical Sciences at the Microscale, and §Synergetic Innovation of Quantum Information & Quantum Technology, University of Science and Technology of China , Hefei, Anhui 230026, China.

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Researchers discovered 21 new stable 2D phosphorus allotropes with tunable semiconductor properties. Nine are more stable than white phosphorus and show potential for photocatalysis in water splitting.

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Area of Science:

  • Materials Science
  • Condensed Matter Physics
  • Solid State Chemistry

Background:

  • Two-dimensional (2D) crystalline phosphorus structures, like phosphorene, exhibit unique anisotropic properties and potential for advanced electronic devices.
  • Discovering new stable 2D phosphorus allotropes is crucial for expanding their applications.

Purpose of the Study:

  • To report the discovery and characterization of 21 novel 2D phosphorus allotropes with porous structures.
  • To investigate their stability, mechanical, and electronic properties.
  • To assess their potential for applications in photocatalysis.

Main Methods:

  • Topological modeling and first-principles calculations were employed to design and predict new 2D phosphorus structures.
  • Vibrational spectra and Born-Oppenheimer molecular dynamics simulations were used to confirm dynamic and thermal stability.
  • Electronic band structures were calculated using the HSE06 method.

Main Results:

  • Twenty-one new 2D porous phosphorus allotropes were identified, formed by assembling various phosphorus units (monomer to hexamer).
  • Nine of these structures demonstrate higher stability than white phosphorus, with confirmed dynamic and thermal stability up to 1500 K.
  • These allotropes exhibit isotropic mechanical properties, are softer than phosphorene, and possess tunable semiconductor band gaps (0.15–3.42 eV).
  • Specific allotropes show band edge positions suitable for visible-light-driven water splitting photocatalysis.

Conclusions:

  • The study successfully identified numerous stable 2D porous phosphorus allotropes with diverse electronic and mechanical properties.
  • These novel materials offer promising avenues for high-performance electronic devices and efficient photocatalytic applications, particularly for water splitting.