Title: Controlled Organization of Inorganic Materials Using Biological Molecules for Activating Therapeutic Functionalities

Journal Article · · ACS Applied Materials and Interfaces

Precise control over the assembly of biocompatible three-dimensional (3D) nanostructures would allow for programmed interactions within the cellular environment. Nucleic acids can be used as programmable crosslinkers to direct the assembly of quantum dots (QDs) and tuned to demonstrate different interparticle binding strategies. In this work, morphologies of self-assembled QDs are evaluated via gel electrophoresis, transmission electron microscopy, small-angle X-ray scattering, and dissipative particle dynamics simulations, with all results being in good agreement. The controlled assembly of 3D QD organizations is demonstrated in cells via the colocalized emission of multiple assembled QDs, and their immunorecognition is assessed via enzyme-linked immunosorbent assays. RNA interference inducers are also embedded into the interparticle binding strategy to be released in human cells only upon QD assembly, which is demonstrated by specific gene silencing. The programmability and intracellular activity of QD assemblies offer a strategy for nucleic acids to imbue the structure and therapeutic function into the formation of complex networks of nanostructures, while the photoluminescent properties of the material allow for optical tracking in cells in vitro.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
National Institutes of Health (NIH); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0012704
OSTI ID:
1837208
Report Number(s):
BNL-222519-2021-JAAM
Journal Information:
ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 33 Vol. 13; ISSN 1944-8244
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (61)

Control of Nanoparticle Assembly by Using DNA-Modified Diatom Templates journal October 2004
A Free-Running DNA Motor Powered by a Nicking Enzyme journal July 2005
Semiconductor Quantum Dots for Bioanalysis journal September 2008
A Light-Driven DNA Nanomachine for the Efficient Photoswitching of RNA Digestion journal March 2010
Salt Responsive Morphologies of ssDNA‐Based Triblock Polyelectrolytes in Semi‐Dilute Regime: Effect of Volume Fractions and Polyelectrolyte Length journal September 2017
An Implicit Solvent Ionic Strength (ISIS) Method to Model Polyelectrolyte Systems with Dissipative Particle Dynamics: An Implicit Solvent Ionic Strength (ISIS) DPD Method journal August 2014
Fast Parallel Algorithms for Short-Range Molecular Dynamics journal March 1995
Structure-switching allosteric deoxyribozymes journal April 2005
Nucleic acid nanoparticles (NANPs) as molecular tools to direct desirable and avoid undesirable immunological effects journal June 2021
Exosomes as natural delivery carriers for programmable therapeutic nucleic acid nanoparticles (NANPs) journal September 2021
Oligomeric nanoparticles functionalized with NIR-emitting CdTe/CdS QDs and folate for tumor-targeted imaging journal September 2014
Fluorescence imaging using synthetic GFP chromophores journal August 2015
Three-dimensional DNA-programmable nanoparticle superlattices journal June 2020
LAMMPS framework for dynamic bonding and an application modeling DNA journal August 2012
Quantum dots-βcyclodextrin-histidine labeled human adipose stem cells-laden chitosan hydrogel for bone tissue engineering journal July 2020
Exosome mediated delivery of functional nucleic acid nanoparticles (NANPs) journal November 2020
Dissipative particle dynamics journal December 1998
Stimuli-Responsive DNA-Based Hydrogels: From Basic Principles to Applications journal February 2017
Multistrand Structure Prediction of Nucleic Acid Assemblies and Design of RNA Switches journal February 2016
The Use of Minimal RNA Toeholds to Trigger the Activation of Multiple Functionalities journal February 2016
Emulsion-Based RIR-MAPLE Deposition of Conjugated Polymers: Primary Solvent Effect and Its Implications on Organic Solar Cell Performance journal July 2016
Quantum Dot-Functionalized Extracellular Matrices for In Situ Monitoring of Cardiomyocyte Activity journal May 2020
Light-Induced Reversible DNA Ligation of Gold Nanoparticle Superlattices journal April 2019
Aptamers as Modular Components of Therapeutic Nucleic Acid Nanotechnology journal October 2019
Fluorescence Blinking as an Output Signal for Biosensing journal October 2016
Nucleic Acid/Quantum Dots (QDs) Hybrid Systems for Optical and Photoelectrochemical Sensing journal March 2013
Switchable Reconfiguration of Nucleic Acid Nanostructures by Stimuli-Responsive DNA Machines journal March 2014
Binary Heterogeneous Superlattices Assembled from Quantum Dots and Gold Nanoparticles with DNA journal April 2011
Spherical Nucleic Acids journal January 2012
DNA-Functionalized Quantum Dots: Fabrication, Structural, and Physicochemical Properties journal May 2013
Organization of Metallic Nanoparticles Using Tobacco Mosaic Virus Templates journal March 2003
Highly Selective, Electrically Conductive Monolayer of Nanoparticles on Live Bacteria journal April 2004
Controllable Self-Assembly of Nanoparticles for Specific Delivery of Multiple Therapeutic Molecules to Cancer Cells Using RNA Nanotechnology journal September 2005
Multifunctional RNA Nanoparticles journal September 2014
A DNA-fuelled molecular machine made of DNA journal August 2000
Modular Assembly of Cell-targeting Devices Based on an Uncommon G-quadruplex Aptamer journal January 2015
DNA-programmable nanoparticle crystallization journal January 2008
DNA-guided crystallization of colloidal nanoparticles journal January 2008
Dynamic DNA nanotechnology using strand-displacement reactions journal January 2011
NIH Image to ImageJ: 25 years of image analysis journal June 2012
A DNA nanomachine that maps spatial and temporal pH changes inside living cells journal April 2009
DNA-based programming of quantum dot valency, self-assembly and luminescence journal July 2011
Activation of different split functionalities on re-association of RNA–DNA hybrids journal March 2013
Origin and control of blinking in quantum dots journal August 2016
Design and self-assembly of siRNA-functionalized RNA nanoparticles for use in automated nanomedicine journal December 2011
Crystal engineering with DNA journal February 2019
Colloidal diamond journal September 2020
Prediction of solvent-induced morphological changes of polyelectrolyte diblock copolymer micelles journal January 2015
Application of semiconductor quantum dots in bioimaging and biosensing journal January 2017
Co-transcriptional production of RNA–DNA hybrids for simultaneous release of multiple split functionalities journal November 2013
Functionally-interdependent shape-switching nanoparticles with controllable properties journal January 2017
RNA–DNA fibers and polygons with controlled immunorecognition activate RNAi, FRET and transcriptional regulation of NF-κB in human cells journal December 2018
Quantum Dots for Live Cells, in Vivo Imaging, and Diagnostics journal January 2005
Scaling Up Digital Circuit Computation with DNA Strand Displacement Cascades journal June 2011
Statistical Mechanics of Dissipative Particle Dynamics journal May 1995
Quantum dots in imaging, drug delivery and sensor applications journal January 2017
The Interleukin-10 Family of Cytokines and Their Role in the CNS journal November 2018
Fluorogenic RNA Aptamers: A Nano-platform for Fabrication of Simple and Combinatorial Logic Gates journal November 2018
Aptamer-Modified Semiconductor Quantum Dots for Biosensing Applications journal July 2017
Neurogenic Exacerbation of Microglial and Astrocyte Responses to Neisseria meningitidis and Borrelia burgdorferi journal June 2008
ImageJ Plugin for Analysis of Porous Scaffolds used in Tissue Engineering journal January 2015