Use of modular nucleic acid scaffolds to create nanoscale energy harvesting and focusing arrays
Inventors
Buckhout-White, Susan • Ancona, Mario • Goldman, Ellen R. • Medintz, Igor L. • Melinger, Joseph S.
Assignees
Publication Number
US-9970049-B2
Publication Date
2018-05-15
Expiration Date
2035-04-14
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Abstract
The invention relates to a nanoscale antenna including a nucleic acid scaffold having a structure selected from the group consisting of a Holliday junction, a star, and a dendrimer; and a plurality of fluorophores attached to the scaffold and configured as a FRET cascade comprising at least three different types of fluorophores, arranged with (a) a plurality of initial donor fluorophores fixed in exterior positions on the structure, (b) a terminal acceptor fluorophore fixed in a central position on the structure, and (c) a plurality of intermediate fluorophores fixed in positions on the scaffold between the initial acceptor fluorophores and the terminal acceptor fluorophores.
Core Innovation
The invention relates to nanoscale antennas comprising a nucleic acid scaffold selected from a Holliday junction, a star, and a dendrimer structures, with multiple fluorophores attached and arranged to form a Förster resonance energy transfer (FRET) cascade. This cascade includes at least three different types of fluorophores arranged such that initial donor fluorophores are fixed at exterior positions, a terminal acceptor fluorophore is fixed centrally, and intermediate fluorophores are positioned in between the donors and acceptor on the scaffold. This configuration enables modular assembly and control of energy transfer through multiple discrete steps.
The invention addresses the need for techniques to focus light excitonic energy and to study FRET phenomena. Existing methods lack flexible modular nanoscale structures capable of directing energy through multiple fluorophores in a controllable, reconfigurable manner. The disclosed nucleic acid scaffolds provide a platform for programmable light energy harvesting and concentrating, with capability for multi-step energy transfer and the ability to modify the energy transfer network by changing the number and types of fluorophores and the scaffold geometry.
Claims Coverage
The patent claims comprise three independent claims covering nanoscale antennas with specified scaffolds and fluorophore arrangements, antennas with dendrimer scaffolds, and methods of using such antennas for sensing applications. The main inventive features focus on the scaffold structures, arrangements of fluorophores forming multi-step FRET cascades, and detachable scaffold portions with toehold sequences for sensing via complementary sequence binding.
Nanoscale antenna with modular nucleic acid scaffolds and FRET cascade arrangement
This feature discloses a nanoscale antenna comprising a nucleic acid scaffold chosen from Holliday junction, star, or dendrimer structures. A plurality of fluorophores are attached forming a FRET cascade with at least three types of fluorophores arranged as initial donors fixed on exterior positions, one or more terminal acceptors fixed centrally, and intermediate fluorophores positioned between donors and terminal acceptors. Additionally, scaffold portions with intermediate fluorophores include toehold sequences enabling detachment upon contact with complementary sequences.
Nanoscale antenna with dendrimer nucleic acid scaffold and detachable intermediate fluorophore segments
This feature specifies a nanoscale antenna having a dendrimer nucleic acid scaffold, with fluorophores arranged as a FRET cascade of at least three types: initial donors at external positions, terminal acceptors centrally fixed, and intermediate fluorophores positioned between. Parts of the scaffold that include intermediate fluorophores have toehold sequences enabling their detachment upon contact with complementary sequences.
Method of using nanoscale antenna for analyte sensing via toehold-mediated scaffold detachment
This method involves providing a nanoscale antenna with a nucleic acid scaffold selected from Holliday junction, star, or dendrimer, and a plurality of fluorophores forming a FRET cascade with initial donors exterior, terminal acceptors central, and intermediates between. The scaffold portions with intermediate fluorophores have toehold sequences detachable upon complementary sequence contact. The antenna is contacted with an analyte, excited with light to activate the FRET cascade, and the resulting response measured to indicate the presence and degree of the complementary sequence in the analyte.
The independent claims cover nanoscale antennas with modular nucleic acid scaffolds having multi-step FRET cascades arranged via specific fluorophore localization, inclusion of toehold sequences permitting scaffold modification upon complementary binding, and methods employing these features for analyte sensing. The inventive features provide molecular architectures and operational methods for controlled energy transfer and biosensing applications.
Stated Advantages
Enables controlled multi-step energy transfer with programmable fluorophore arrangements for tailored light-harvesting.
Allows easy reconfiguration of energy transfer networks by changing the number, type, and spatial arrangement of fluorophores and scaffold geometry.
Supports multiple FRET pathways in parallel, increasing energy transfer efficiency and signal amplification for sensing.
Facilitates site-specific conjugation to biological or abiotic moieties and tethering to surfaces, enhancing integration into devices and sensors.
Assembly utilizes a "one-pot" strategy without requiring purification, applicable for ensemble or single-molecule applications.
High biocompatibility allows use in biological imaging with reduced background and support for various excitation modes including multiphoton and time-gated modalities.
Documented Applications
Energy harvesting and focusing through nanoscale antennas configured by nucleic acid scaffolds with fluorophores arranged for FRET cascades.
Biosensing devices that detect analytes via toehold-mediated detachment of intermediate scaffold portions, resulting in measurable alterations in energy transfer.
Use as research tools for studying light-harvesting and FRET phenomena in synthetic photonic networks and artificial photosynthesis mimics.
Optical coding, information storage, information processing, data encryption, and sensitization for energy conversion through programmable fluorophore arrays.
Biological imaging with enhanced signal sensitivity and potential integration with other optically active materials such as quantum dots and metal chelates.
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