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Vibrational Stark Effects: Ionic Influence on Local Fields.

Demelza Wright1, Sara Sangtarash2, Niclas S Mueller1

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|May 27, 2022
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Summary
This summary is machine-generated.

Vibrational Stark shift reporters measure electric fields, but uniform field DFT fails for molecular layers. Ionic movement and electrical double-layer penetration explain observed shifts, controllable by molecular layer composition.

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Area of Science:

  • Physical Chemistry
  • Surface Science
  • Computational Chemistry

Background:

  • Molecules with vibrational Stark shift reporters are used for in situ DC electric field measurements.
  • Density functional theory (DFT) in a uniform electric field is the standard method for theoretical quantification.
  • Existing models struggle to accurately represent complex molecular systems, such as monolayers on electrodes.

Purpose of the Study:

  • To investigate the limitations of uniform field DFT in modeling vibrational Stark shifts in molecular monolayers.
  • To elucidate the role of ionic movement and electrical double-layer effects in observed Stark shifts.
  • To demonstrate a method for controlling and suppressing Stark shifts by modifying the molecular layer.

Main Methods:

  • Combined theoretical and experimental study.
  • Density functional theory (DFT) calculations.
  • Direct modeling of ionic movement within the molecular layer.
  • Experimental manipulation of molecular layer composition.

Main Results:

  • Uniform field DFT cannot simultaneously model the behavior of the three strongest vibrational modes in molecular monolayers.
  • Measured Stark shifts are accurately explained by partial electrical double-layer penetration into the molecular layer.
  • Stark shifts can be experimentally suppressed by creating mixed molecular layers that inhibit ionic penetration.

Conclusions:

  • Standard uniform field DFT is insufficient for accurately predicting Stark shifts in certain molecular systems.
  • Electrical double-layer penetration is a critical factor influencing Stark shifts in molecular monolayers on electrodes.
  • Tailoring the molecular layer composition offers a viable strategy to control and eliminate Stark shifts for precise electric field sensing.