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Electronic Rearrangement in Molecular Plasmons: An Electron Density and Electrostatic Potential-Based Study.

Mishu Paul1, P Balanarayan1

  • 1Department of Chemical Sciences, Indian Institute of Science Education and Research (IISER) Mohali, Sector 81, S.A.S. Nagar, Knowledge City, Mohali, Manauli P.O., Punjab-, 140306, India.

Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry
|January 24, 2018
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Molecular plasmons in polyacenes exhibit minimal electron rearrangement, distinguishing them from single-particle excitations. These plasmonic states closely resemble the ground state based on one-electron properties.

Keywords:
acenesdensity functional calculationselectron densityelectrostatic potentialmolecular plasmon

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Area of Science:

  • Computational Chemistry
  • Molecular Spectroscopy
  • Quantum Mechanics

Background:

  • Molecular plasmons are crucial for understanding light-matter interactions in molecules.
  • Previous methods for identifying plasmonic modes involved scaling electron interactions or analyzing transition dipole moments.
  • Polyacenes display distinct peaks in their electronic absorption spectra.

Purpose of the Study:

  • To analyze the excited states of polyacenes (naphthalene to pentacene) using electron densities and molecular electrostatic potential (MESP) topography.
  • To characterize molecular plasmons by examining electron rearrangement.
  • To compare plasmonic states with single-particle excitations.

Main Methods:

  • Time-dependent density functional theory (TD-DFT) with the B3LYP/cc-pVTZ basis set was employed for calculations.
  • Analysis of electron densities and MESP topography for excited states.
  • Comparison of electron rearrangement in plasmonic versus single-particle excited states.

Main Results:

  • Both low- and high-energy peaks in polyacene spectra arise from similar electronic transitions (HOMO-n to LUMO and HOMO to LUMO+n).
  • Plasmonic states (bright and dark) show the least electron rearrangement compared to other excited states.
  • MESP topography analysis reveals the lowest variance in MESP values and minimal displacement of MESP minima for plasmonic states.

Conclusions:

  • Molecular plasmons represent excited states with the least electron rearrangement, closely resembling the ground state in one-electron properties.
  • This finding holds true for both organic molecules (polyacenes) and inorganic clusters (silver and sodium chains).
  • The study provides a new perspective on characterizing molecular plasmons through electron density and MESP analysis.