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Exfoliation and Analysis of Large-area, Air-Sensitive Two-Dimensional Materials

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Published on: January 5, 2019

Second-Order Raman Scattering in Exfoliated Black Phosphorus.

Alexandre Favron¹, Félix Antoine Goudreault¹, Vincent Gosselin¹

¹Département de Physique and Regroupement Québécois sur les Matériaux de Pointe, Université de Montréal , C. P. 6128, Succursale Centre-Ville, Montréal, Québec H3C 3J7, Canada.

|January 12, 2018

Summary

Second-order Raman scattering was observed in black phosphorus (P(black)), revealing new defect-activated modes. These findings enhance understanding of disorder in anisotropic semiconductors.

Keywords:

Black phosphorus anisotropic properties doubly resonant Raman phonon-defect modes

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Area of Science:

Condensed Matter Physics
Materials Science
Nanotechnology

Background:

Second-order Raman scattering is well-studied in carbon nanomaterials, activating normally forbidden modes sensitive to crystal disorder.
First-order Raman processes typically dominate in sp²-hybridized carbon systems, making them an exception.

Purpose of the Study:

To identify and characterize second-order Raman scattering modes in exfoliated black phosphorus (P(black)).
To investigate the nature and origin of these newly observed modes in an anisotropic semiconductor.

Main Methods:

Experimental Raman spectroscopy on exfoliated black phosphorus with varying thickness, excitation wavelength, and defect density.
Ab initio simulations of monolayer black phosphorus to understand scattering mechanisms.

Main Results:

Identification of four new second-order Raman modes (D₁, D₁^', D₂, D₂^') in black phosphorus, dominating at 633 nm excitation.
These modes are defect-activated and involve high-momentum phonons via a doubly resonant Raman process.
Ab initio simulations attribute D' and D modes to intravalley scattering along armchair and zigzag directions, respectively.

Conclusions:

Discovery of defect-activated second-order Raman modes in black phosphorus, challenging previous assumptions for elemental semiconductors.
The high sensitivity of these modes to disorder provides a tool for characterizing defects in black phosphorus.
These findings help resolve discrepancies in existing literature regarding Raman scattering in black phosphorus.