Polariton mediated reservoir energy transfer in disordered photonic wires Público

Abstract

      Strong light-matter interactions are emerging as an innovative way to modify chemical reactions and promote changes in molecular systems. One function of strong light-matter interactions that is still not fully understood is their ability to facilitate efficient and effective intermolecular energy transfer beyond the Förster limit. This work aims to build computational models that represent quantum systems within Fabry-Perot cavities to gain insight into the mechanisms behind polariton-mediated energy transfer and the conditions that maximize its efficiency. Unlike previous works, stochastic fluctuations of the transition energies of molecules within the system were incorporated. Results show a greater than 50% decrease in effectiveness of energy transfer when the energy of the cavity is raised to higher than the molecular transition energies. Results also show a 10-fold increase in the effectiveness of energy transfer when energetic disorder is increased from a standard deviation of 0 eV to 0.13 eV in a Gaussian distribution. Conclusions from this work provide additional insight into some puzzling experimental results, but more complex models will likely be required to gain complete understanding of experimental observations.

Table of Contents

Table of Contents

1. INTRODUCTION 1

1.1. Fabry-Perot Cavities 1

1.2. Strong Light-Matter Coupling Within Cavities 3

1.3. Energy Transfer Within Strong Coupling Regime 5

1.4. Statement of Purpose 6

2. COMPUTATIONAL MODEL 6

2.1. Closed System Quantum Dynamics 10

2.2. Open Quantum System Dynamics via Pauli Master Equation 10

3. CLOSED SYSTEM QUANTUM DYNAMICS 13

3.1. Ideal Model 13

3.2. Energetic Disorder Effects 15

3.3. Comparison to Coulomb Model 17

3.4. Distance Dependence 19

3.5. Relevance of Cavity Detuning 22

4. OPEN QUANTUM SYSTEM DYNAMICS 23

4.1. Classification of Eigenstates 23

4.2. Time Evolution of Energy Transfer 25

4.3. Energy Transfer Efficiency 29

4.4. Intraband Dynamics 32

4.5. Coarse Grained Approach 34

5. CONCLUSION AND FUTURE DIRECTIONS 35

6. REFERENCES 37

7. SUPPLEMENTARY MATERIALS 42

About this Honors Thesis

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School	Emory College
Department	Chemistry
Degree	B.S.
Submission	Honors Thesis
Language	English
Research Field	Chemistry, Physical Chemistry, General
Palabra Clave	Polariton Energy Transfer Microcavity
Committee Chair / Thesis Advisor	Dr. Raphael F. Ribeiro, Emory University
Committee Members	Dr. James T. Kindt, Emory University Dr. Fang Liu, Emory University

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