Keywords

diarylethenes, optical data storage, two-photon absorption, resonance energy transfer, photochromic materials, fluorene derivatives

Abstract

Three-dimensional (3D) optical data storage based on two-photon processes provides highly confined excitation in a recording medium and a mechanism for writing and reading data with less cross talk between multiple memory layers, due to the quadratic dependence of two photon absorption (2PA) on the incident light intensity. The capacity for highly confined excitation and intrinsic 3D resolution affords immense information storage capacity (up to 1012 bits/cm3). Recently, the use of photochromic materials for 3D memory has received intense interest because of several major advantages over current optical systems, including their erasable/rewritable capability, high resolution, and high sensitivity. This work demonstrates a novel two-photon 3D optical storage system based on the modulation of the fluorescence emission of a highly efficient two-photon absorbing fluorescent dye (fluorene derivative) and a photochromic compound (diarylethene). The feasibility of using efficient intermolecular Förster Resonance Energy Transfer (RET) from the non-covalently linked two-photon absorbing fluorescent fluorene derivative to the photochromic diarylethene as a novel read-out method in a two-photon optical data storage system was explored. For the purpose of the development of this novel two-photon 3D optical storage system, linear and two-photon spectroscopic characterization of commercial diarylethenes in solution and in a polymer film and evidence of their cyclization (O→C) and cycloreversion (C→O) reactions induced by two-photon excitation were undertaken. For the development of a readout method, Resonance Energy Transfer (RET) from twophoton absorbing fluorene derivatives to photochromic compounds was investigated under one and two-photon excitation. The Förster's distances and critical acceptor concentrations were determined for non-bound donor-acceptor pairs in homogeneous molecular ensembles. To the best of my knowledge, modulation of the two-photon fluorescence emission of a dye by a photochromic diarylethene has not been reported as a mechanism to read the recorded information in a 3D optical data storage system. This system was demonstrated to be highly stable and suitable for recording data in thick storage media. The proposed RET-based readout method proved to be non-destructive (exhibiting a loss of the initial fluorescence emission less than 20% of the initial emission after 10,000 readout cycles). Potential application of this system in a rewritable-erasable optical data storage system was proved. As part of the strategy for the development of diarylethenes optimized for 3D optical data storage, derivatives containing Ï€-conjugated fluorene molecules were synthesized and characterized. The final part of this reasearch demonstrated the photostability of fluorine derivatives showing strong molecular polarizability and high fluorescence quantum yields. These compounds are quite promising for application in RET-based two-photon 3D optical data storage. Hence, the photostability of these fluorene derivatives is a key parameter to establish, and facilitates their full utility in critical applications.

Notes

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Graduation Date

2007

Semester

Summer

Advisor

Belfield, Kevin

Degree

Doctor of Philosophy (Ph.D.)

College

College of Sciences

Department

Chemistry

Degree Program

Chemistry

Format

application/pdf

Identifier

CFE0001662

URL

http://purl.fcla.edu/fcla/etd/CFE0001662

Language

English

Release Date

April 2008

Length of Campus-only Access

None

Access Status

Doctoral Dissertation (Open Access)

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Included in

Chemistry Commons

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