| Content Provider |
Semantic Scholar |
| Author |
Socolar, Joshua E. S. |
| Copyright Year |
2002 |
| Abstract |
The primary objective of this project was to verify dependence of Forster resonance energy transfer (FRET) on angular separation of chromophore pair. A secondary objective was to investigate the formation of exciplex, a heterodimeric compound that forms as a result of electrostatic interaction between a pair of proximal chromophores with either species in the excited state. In this study, photochemical interaction between a select pair of chromophores was studied. A method based on functionalization of chromophores on oligonucleotides was developed in order to place chromophores in a rigid conformation with respect to distance and angular separation. The method consisted of functionalizing maleimide variants of chromophores to thiolated terminus of oligonucleotides and creating a rigid structure via hybridization of complementary strands. In the close proximity that the chromophores were situated, angular separation becomes the predominant factor behind modulation of transfer efficiency. This phenomenon was verified with FRET pair studies involving three configurations, with two of the three attaching the chromophores to base pairs that were positioned orthogonal to each other. Steady‐state fluorescence measurements were used to interpret the photochemical properties of the structures, while sample temperature was varied in order to investigate the changes in these properties as structure dissociates. Results show that fluorescence of the donor appear to be strongly quenched in the two orthogonal configurations (ΦT = 0.1~0.2), contrary to the other configuration where the two chromophores are placed in close proximity (ΦTmax = ~0.6). However, the formation of exciplex could not be observed from the results obtained in this experiment, primarily due to the difficulties encountered in identifying the contribution of exciplex emission from the total emission of the system. In conclusion, angular dependence of FRET efficiency was observed to be related to the base pair separation of chromophore pair. From a high‐level perspective, this investigation is a step towards synthesizing molecular logic gates using RET logic. Future directions include identifying chromophore pairs that can form exciplexes, as well as studying the effect of tether lengths to the formation of exciplexes between chromophores conjugated to a DNA nanostructure. With two or more exciplex‐forming species with a common acceptor, it is possible to envision a system that selectively interacts with one donor over another, creating a molecular pass gate whose behavior is modulated entirely by electromagnetic waves. Intorduction Using resonance energy transfer as a mechanism for performing logical operations has been studied in the past at Duke Self‐Assembled Systems Group. An important aspect of this enterprise is the characterization of chromophore interactions, which forms the basis of this project. The primary objective of this project was to verify dependence of Forster resonance energy transfer (FRET) on angular separation of chromophore pair. A secondary objective was to investigate the formation of exciplex, a heterodimeric compound that was identified as a potential candidate for use in designing an electromagnetic‐source modulated FRET pass gate. A. Modulation of FRET Efficiency Forster Resonance Energy Transfer (FRET) is a non‐radiative energy transfer mechanism. When a donor molecule is excited by incident EM wave, it may transfer its excited state to an acceptor molecule through a nonradiative dipole‐dipole interaction. In absence of an acceptor, the donor may radiate energy as the excited electron returns to a lower orbital. In case of chromophores as donors, this would result in a release of photons at their characteristic emission wavelengths. In presence of an acceptor however, the excited donor may act like an oscillating dipole and transmit energy directly to the acceptor molecule, resulting in exciting the acceptor as the donor reaches ground state (1). A key feature of this mechanism is its operating distance. FRET takes place between molecules separated by several tens of Angstroms, but its efficiency is strongly attenuated as the separation between chromophores extend beyond a threshold distance. An inverse 6 power law governs transfer efficiency between a given donor and acceptor: Represented graphically, transfer efficiency undergoes a sharp transition when r = R0. |
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10.4135/9781483347660.n134 |
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https://doi.org/10.4135/9781483347660.n134 |
| Language |
English |
| Access Restriction |
Open |
| Content Type |
Text |
| Resource Type |
Article |
