Light‐Responsive Dynamic DNA‐Origami‐Based Plasmonic Assemblies

Ryssy, Joonas; Natarajan, Ashwin Karthick; Wang, Jinhua; Lehtonen, Arttu J.; Nguyen, Minh‐Kha; Klajn, Rafał; Kuzyk, Anton

doi:10.1002/ange.202014963

Cited by 18 publications

(17 citation statements)

References 56 publications

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“…However, the process of doping azobenzene is time-consuming and expensive. Ryssy et al 133 choose the merocyanine-based photoacid (MCH + ) as a new light-responsive regulator. Upon blue light illumination, the MCH + produced a ring-closing reaction along with the release of H + .…”

Section: Reconfigurable Chiral Arrangements Of Nanoparticles Based On Dynamic Dna Nanotechnologymentioning

confidence: 99%

Progress and perspective on chiral plasmonic nanostructures enabled by DNA programming methodology

Yang

Tang

et al. 2021

Mater. Adv.

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Section: Reconfigurable Chiral Arrangements Of Nanoparticles Based On Dynamic Dna Nanotechnologymentioning

confidence: 99%

Progress and perspective on chiral plasmonic nanostructures enabled by DNA programming methodology

Yang

Tang

et al. 2021

Mater. Adv.

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“…1 Recent advances in DNA nanotechnology have enabled the construction of molecular machines that can respond to specific external triggers. These designs allow precise nanoscale control over chemical processes in dynamic materials, 2 catalytic systems, 3 and controlled-release drug delivery. 4 Most mechanisms use chemical ‘fuel’ ( e .…”

Section: Introductionmentioning

confidence: 99%

A modular intramolecular triplex photo-switching motif that enables rapid and reversible control of aptamer binding activity

Trinh

Thompson

Clark

et al. 2022

Preprint

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DNA switches that can change conformation in response to certain wavelengths of light could enable rapid and non-invasive control of chemical processes for a wide range of applications. However, most current photo-responsive DNA switches are limited either by irreversible switching or reversible switching with impractically slow kinetics. Here, we report the design of an intramolecular triplex photoswitch (TPS) design based on single-stranded DNA that undergoes rapid and reversible photoswitching between folded and unfolded states through isomerization of internal azobenzene modifications. After optimizing the performance of our photoswitch design, we used molecular dynamics (MD) simulations to reveal how individual azobenzenes contribute to the stabilization or destabilization of the triplex depending on their photoisomerization state. By coupling our TPS to an existing aptamer, we can reversibly modulate its binding affinity with less than 15 seconds of UV light exposure. We further demonstrate reproducible shifting in affinity over multiple cycles of UV and blue light irradiation without substantial photobleaching. Given that our TPS can introduce switching functionality to aptamers without manipulating the aptamer sequence itself, we believe our design methodology should offer a versatile means for integrating photo-responsive properties into DNA nanostructures.

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“…The shortest hydrophobic hydrocarbon chain between SP and a permanently charged headgroup known from literature is propyl (C3) [17,45,[47][48][49][50][51][52]56,57]. Amphiphiles with butyl-linked (C4) SP and headgroup were studied by Braunschweig et al [21].…”

Section: Introductionmentioning

confidence: 99%

Spiropyran/Merocyanine Amphiphile in Various Solvents: A Joint Experimental–Theoretical Approach to Photophysical Properties and Self-Assembly

Savchenko¹,

Lomadze²,

Santer³

et al. 2022

Preprint

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This joint experimental-theoretical work focuses on molecular and photophysical properties of the spiropyran-containing amphiphilic molecule in organic and aqueous solutions. Being dissolved in tested organic solvents, the system demonstrates positive photochromism, i.e. upon UV stimulus the colorless spiropyran form is transformed into colorful merocyanine isomer. However, aqueous solution of the amphiphile possesses a negative photochromism: the orange-red merocyanine form turns to be thermodynamically more stable in water, and both UV and vis stimuli lead to the partial or complete photobleaching of the solution. The explanation of this phenomenon is given on the basis of density functional theory calculations and classical modeling including thermodynamic integration. The simulations reveal that stabilization of merocyanine in water proceeds with the energy of ca. 70 kJ mol−1, and that the Helmholtz free energy of hydration of merocyanine form is 100 kJ mol−1 lower as compared to the behavior of SP isomer in water. The explanation of such a difference lies in the molecular properties of the merocyanine: after ring-opening reaction this molecule transforms into a zwitterionic form, as evidenced by the electrostatic potential plotted around the opened form. The presence of three charged groups on the periphery of a flat conjugated backbone stimulates the self-assembly of merocyanine molecules in water, ending up with the formation of elongated associates with stack-like building blocks, as shown in molecular dynamics simulations of the aqueous solution with the concentration above critical micelle concentration. Our quantitative evaluation of the hydrophilicity switching in spiropyran/merocyanine containing surfactants may prompt the search for new systems, including colloidal and polymeric ones, aiming at remote tuning of their morphology, which could give new promising shapes and patterns for the needs of modern nanotechnology.

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Light‐Responsive Dynamic DNA‐Origami‐Based Plasmonic Assemblies

Cited by 18 publications

References 56 publications

Progress and perspective on chiral plasmonic nanostructures enabled by DNA programming methodology

Progress and perspective on chiral plasmonic nanostructures enabled by DNA programming methodology

A modular intramolecular triplex photo-switching motif that enables rapid and reversible control of aptamer binding activity

Spiropyran/Merocyanine Amphiphile in Various Solvents: A Joint Experimental–Theoretical Approach to Photophysical Properties and Self-Assembly

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