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A Photonic System for Generating Unconditional Polarization-Entangled Photons Based on Multiple Quantum Interference

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Free energy functionals for polarization fluctuations: Pekar factor revisited.

Mohammadhasan Dinpajooh¹, Marshall D Newton², Dmitry V Matyushov³

¹School of Molecular Sciences, Arizona State University, P.O. Box 871604, Tempe, Arizona 85287-1604, USA.

The Journal of Chemical Physics

|February 17, 2017

Summary

Pekar

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Area of Science:

Physical Chemistry
Computational Chemistry
Theoretical Chemistry

Background:

Pekar's theory (70 years ago) separated electronic and nuclear polarization for electron mobility in polarizable media.
This separation introduced the Pekar factor, predicting a significant drop in nuclear solvation free energy.
The Pekar factor is crucial for understanding solvent effects on electron transfer reactions.

Purpose of the Study:

To investigate the separation of fast electronic and slow nuclear polarization modes in polar molecular liquids.
To move beyond the continuum approximation by using atomistic simulations.
To derive a nonlocal free energy functional and analyze solvation free energy and electron transfer reorganization energy.

Main Methods:

Development of a nonlocal free energy functional.
Atomistic numerical simulations to compute electronic and nuclear susceptibilities in reciprocal space.
Extrapolation of finite-size simulation results to the continuum limit (zero wavevector).

Main Results:

The continuum nuclear susceptibility from simulations aligns with the Pekar factor.
A new functionality involving static and high-frequency dielectric constants was derived.
Contrary to Pekar's prediction, nuclear solvation free energy does not significantly drop with increasing liquid polarizability.

Conclusions:

Electron transfer reorganization energy remains constant or increases with solvent polarizability, challenging traditional theories.
The study provides a more accurate, simulation-based understanding of polarization effects in polar liquids.
Findings impact the mechanistic understanding of electron transfer in various solvent environments.