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Updated: Aug 6, 2025

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Pressure-induced second-order phase transition in fluorine.

Giovani L Rech1, André L Martinotto1, Janete E Zorzi1

  • 1Universidade de Caxias do Sul, 95070-560 Caxias do Sul, RS, Brazil. glrech1@ucs.br.

Physical Chemistry Chemical Physics : PCCP
|March 23, 2023
PubMed
Summary

High-pressure fluorine exhibits a phase transition from the C2/c to the Cmce structure. This transition is driven by the disappearance of dynamical instability in the Cmce phase as pressure increases.

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Area of Science:

  • Solid-state chemistry
  • Computational materials science
  • High-pressure physics

Background:

  • Understanding crystal structure stability is crucial for predicting material properties under extreme conditions.
  • Fluorine's unique electronic properties, specifically the absence of sigma-holes, influence its intermolecular interactions compared to heavier halogens.
  • The high-pressure behavior of molecular solids like fluorine remains an active area of research.

Purpose of the Study:

  • To investigate the relative stability between the ambient alpha-F2 (C2/c) and a proposed high-pressure (Cmce) crystal structure of fluorine.
  • To elucidate the mechanism and nature of the pressure-induced phase transition in fluorine.
  • To compare the structural behavior of fluorine with heavier halogens under pressure.

Main Methods:

  • Density Functional Theory (DFT) calculations using the PBE0+D3(ABC)/TVZP level of theory.
  • Quantum Monte Carlo (QMC) calculations for further assessment of relative energies.
  • Phonon dispersion spectra analysis to identify dynamical instabilities.

Main Results:

  • The C2/c structure is energetically favored over the Cmce structure at ambient pressure.
  • The Cmce phase exhibits a dynamical instability near the Gamma-point at ambient pressure, attributed to repulsive head-to-head interactions between fluorine molecules due to the absence of sigma-holes.
  • This dynamical instability in the Cmce phase disappears with increasing pressure, facilitating the phase transition.

Conclusions:

  • The pressure-induced phase transition from C2/c to Cmce in fluorine is confirmed to be of second-order.
  • The absence of sigma-holes in fluorine is a key factor differentiating its high-pressure behavior from heavier halogens.
  • Computational methods provide valuable insights into the complex phase behavior of elements under pressure.