Nanoscale 3D spatial addressing and valence control of quantum dots using wireframe DNA origami

Chen, Chi; Wei, Xingfei; Parsons, Molly F.; Guo, Jiajia; Banal, James L.; Zhao, Yinong; Scott, Madelyn N.; Schlau‐Cohen, Gabriela S.; Hernandez, Rigoberto; Bathe, Mark

doi:10.1038/s41467-022-32662-w

Cited by 27 publications

(32 citation statements)

References 73 publications

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“…We calculate the relative quantum yield (QY) of our ELP engineered FP by comparing the quantum yield of known FP. − We first prepared serial dilutions of both reference and unknown FP-ELP samples and obtained absorbance values at 435, 465, 475, and 540 nm for BFP, GFP, YFP, and RFP, respectively. The fluorescence spectrum was obtained using the above wavelength to excite each FP fluorophore, and the integrated area under the curve was calculated.…”

Section: Methodsmentioning

confidence: 99%

Elastic Fluorescent Protein-Based Down-Converting Optical Films for Flexible Display

et al. 2022

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Protein-based material design provides great advantages to developing smart biomaterials with tunable structures and desired functions. They have been widely used in many biomedical applications including tissue engineering and drug delivery. However, protein-based materials are not yet widely used in optoelectronic materials despite their excellent optical and tunable mechanical properties. Here, we synthesized engineered fluorescent proteins (FPs) fused with elastic protein for the development of optoelectrical down-converting optical filters for flexible display materials. We synthesized sequencespecific FPs to tune blue, green, yellow, and red colors and fused them with elastic protein to tune mechanical properties. We fabricated flexible self-supporting film materials and characterized mechanical properties and down-converting optical properties. We also fabricated a hybrid light-emitting diode (LED) to down convert blue to desired green, red, and white colors. Furthermore, we constructed a flexible white LED using organic LED as a flexible substrate. Our modular synthesis approach of tunable bio-optoelectrical material approaches will be useful to design future biocompatible and flexible display materials and technologies.

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Section: Methodsmentioning

confidence: 99%

Elastic Fluorescent Protein-Based Down-Converting Optical Films for Flexible Display

et al. 2022

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“…Absorbance spectra were measured using a UV–vis spectrophotometer (Thermo-Fisher) and the PL spectra were measured using a FluoroMax-4C (Horiba Jobin Yvon). The extinction coefficient of QD was estimated using the first extinction absorption peak and calculated according to the empirical formula from refs and . The quantum yield of QD was determined using the relative quantum yield determination method with rhodamine 101 in spectroscopic-grade ethanol as standard in refs and .…”

Section: Methodsmentioning

confidence: 99%

“…Aqueous QD was prepared as described previously. 59 Briefly, 80 μL of QD (5 mg/mL) were incubated with TOPO (1 g/10 mL in chloroform) and chloroform at 25 °C and shacked. After 30 min, TBAB (0.3 M in chloroform) was added to this mixture.…”

Section: Methodsmentioning

confidence: 99%

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Molecular Structure of Single-Stranded DNA on the ZnS Surface of Quantum Dots

et al. 2022

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DNA-based nanoparticle assemblies have emerged as leading candidates in the development of bioimaging materials, photonic devices, and computing materials. Here, we combine atomistic simulations and experiments to characterize the wrapping mechanism of chimeric single-stranded DNA (ssDNA) on CdSe-ZnS (core–shell) quantum dots (QDs) at different ratios of the phosphorothioate (PS) modification of the bases. We use an implicit solvent, all-atom ssDNA model to match the experimentally calculated ssDNA conformation at low salt concentrations. Through simulation, we find that 3-mercaptopropionic acid (MPA) induces electrostatic repulsion and O-(2-mercaptoethyl)-Ó-methyl-hexa (ethylene glycol) (mPEG) induces steric exclusion, and both reduce the binding affinity of ssDNA. In both simulation and experiment, we find that ssDNA is closer to the QD surface when the QD size is larger. The effect of the PS-base ratio on the conformation of ssDNA is also elaborated in this work. We found through MD simulations, and confirmed by transmission electron microscopy, that the maximum valence numbers are 1, 2, and 3 on QDs of 6, 9, and 14 nm in diameter, respectively. We conclude that the maximum ssDNA valence number is linearly related to the QD size, n ∝ R, and justify this finding through an electrostatic repulsion mechanism.

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“…For this reason, most DNA composite materials, including those assembled using short ssDNAs [3] or DNA nanotechnologies [2], employ gold nanoparticles that are easily modified via thiol binding to their surfaces. Very few examples exist of DNA materials incorporating other nanoparticle types (e.g., quantum dots, magnetic nanoparticles, catalysts) [13][14][15], despite potential advantages of such structures in biomedical imaging, optoelectronic, and energy applications. Even when considering thiol-binding chemistries used for gold nanoparticle ssDNA modification, the two main methods employed: salt aging and low pH modification require three days [3] or very precise pH control [16], which hinders their application at commercial scales.…”

Section: Introductionmentioning

confidence: 99%

DNA-caged Nanoparticles via Electrostatic Self-Assembly

Jergens¹,

Fernandes-Junior

Cui

et al. 2022

Preprint

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DNA-modified nanoparticles enable DNA sensing and therapeutics in nanomedicine and are also crucial for nanoparticle self-assembly with DNA-based materials. However, methods to conjugate DNA to nanoparticle surfaces are limited, inefficient, and lack control. Inspired by DNA tile nanotechnology, we demonstrate a new approach to nanoparticle modification based on electrostatic attraction between negatively charged DNA tiles and positively charged nanoparticles. This approach does not disrupt nanoparticle surfaces and leverages the programmability of DNA nanotechnology to control DNA presentation. We demonstrated this approach using a variety of nanoparticles, including polymeric micelles, polystyrene beads, gold nanoparticles, and superparamagnetic iron oxide nanoparticles with sizes ranging from 5-20 nm in diameter. DNA cage formation was confirmed through transmission electron microscopy (TEM), neutralization of zeta potential, and a series of fluorescence experiments. DNA cages present “handle” sequences that can be used for reversible target attachment or self-assembly. Handle functionality was verified in solution, at the solid-liquid interface, and inside fixed cells, corresponding to applications in biosensing, DNA microarrays, and erasable immunocytochemistry. These experiments demonstrate the versatility of the electrostatic DNA caging approach and provide a new pathway to nanoparticle modification with DNA that will empower further applications of these materials in medicine and materials science.

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Nanoscale 3D spatial addressing and valence control of quantum dots using wireframe DNA origami

Cited by 27 publications

References 73 publications

Elastic Fluorescent Protein-Based Down-Converting Optical Films for Flexible Display

Elastic Fluorescent Protein-Based Down-Converting Optical Films for Flexible Display

Molecular Structure of Single-Stranded DNA on the ZnS Surface of Quantum Dots

DNA-caged Nanoparticles via Electrostatic Self-Assembly

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