Prof. Dr. Tim Liedl

- Functional DNA devices using the DNA origami method
R Yaadav, K Trofymchuk, M Dass, V Behrendt, B Hauer, J Schütz, C Close, M Scheckenbach, G Ferrari, L Mäurer, S Sebina, V Glembockyte, T Liedl, P Tinnefeld
Bringing Attomolar Detection to the Point-of-Care with Nanopatterned DNA Origami Nanoantennas Journal Article
In: Advanced Materials, 2025, ISSN: 0935-9648.
@article{nokey,
title = {Bringing Attomolar Detection to the Point-of-Care with Nanopatterned DNA Origami Nanoantennas},
author = {R Yaadav and K Trofymchuk and M Dass and V Behrendt and B Hauer and J Sch\"{u}tz and C Close and M Scheckenbach and G Ferrari and L M\"{a}urer and S Sebina and V Glembockyte and T Liedl and P Tinnefeld},
url = {\<Go to ISI\>://WOS:001536107000001},
doi = {10.1002/adma.202507407},
issn = {0935-9648},
year = {2025},
date = {2025-07-26},
journal = {Advanced Materials},
abstract = {Creating increasingly sensitive and cost-effective nucleic acid detection methods is critical for enhancing point-of-care (POC) applications. This requires highly specific capture of biomarkers and efficient transduction of capture events. However, the signal from biomarkers present at extremely low amounts often falls below the detection limit of typical fluorescence-based methods, necessitating molecular amplification. Here, we present single-molecule detection of a non-amplified, 151-nucleotide sequence specific to antibiotics-resistant Klebsiella pneumoniae down to attomolar concentrations, using Trident NanoAntennas with Cleared HOtSpots (NACHOS). This NACHOS-diagnostics assay leverages a compact microscope with a large field-of-view, including microfluidic flow to enhance capturing efficiency. Fluorescence enhancement is provided by NanoAntennas, arranged using a combination of nanosphere lithography and site-specific DNA origami placement. This method can detect 200 +/- 50 out of 600 molecules in a 100 mu L sample volume within an hour. This represents a typical number of pathogens in clinical samples commonly detected by Polymerase Chain Reaction. We achieve similar sensitivity in untreated human plasma, enhancing the practical applicability of the system. This platform can be adapted to detect shorter nucleic acid fragments that are not compatible with traditional amplification-based technologies. This provides a robust and scalable solution for sensitive nucleic acid detection in diverse clinical settings.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
H Ijäs, J Trommler, L Nguyen, S Van Rest, P C Nickels, T Liedl, M J Urban
DNA origami signal amplification in lateral flow immunoassays Journal Article
In: Nature Communications, vol. 16, no. 1, pp. 3216, 2025, ISSN: 2041-1723.
@article{nokey,
title = {DNA origami signal amplification in lateral flow immunoassays},
author = {H Ij\"{a}s and J Trommler and L Nguyen and S Van Rest and P C Nickels and T Liedl and M J Urban},
url = {https://doi.org/10.1038/s41467-025-57385-6},
doi = {10.1038/s41467-025-57385-6},
issn = {2041-1723},
year = {2025},
date = {2025-04-04},
journal = {Nature Communications},
volume = {16},
number = {1},
pages = {3216},
abstract = {Lateral flow immunoassays (LFIAs) enable a rapid detection of analytes in a simple, paper-based test format. Despite their multiple advantages, such as low cost and ease of use, their low sensitivity compared to laboratory-based testing limits their use in e.g. many critical point-of-care applications. Here, we present a DNA origami-based signal amplification technology for LFIAs. DNA origami is used as a molecularly precise adapter to connect detection antibodies to tailored numbers of signal-generating labels. As a proof of concept, we apply the DNA origami signal amplification in a sandwich-based LFIA for the detection of cardiac troponin I (cTnI) in human serum. We show a 55-fold improvement of the assay sensitivity with 40-nm gold nanoparticle labels and an adjustable signal amplification of up to 125-fold with fluorescent dyes. The technology is compatible with a wide range of existing analytes, labels, and sample matrices, and presents a modular approach for improving the sensitivity and reliability of lateral flow testing.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
C Sikeler, S Kempter, I Sekulic, S Burger, T Liedl
Chiral Plasmonic Crystals Self-Assembled by DNA Origami Journal Article
In: The Journal of Physical Chemistry C, vol. 129, no. 10, pp. 5116-5121, 2025, ISSN: 1932-7447.
@article{nokey,
title = {Chiral Plasmonic Crystals Self-Assembled by DNA Origami},
author = {C Sikeler and S Kempter and I Sekulic and S Burger and T Liedl},
url = {https://doi.org/10.1021/acs.jpcc.4c08768},
doi = {10.1021/acs.jpcc.4c08768},
issn = {1932-7447},
year = {2025},
date = {2025-03-13},
journal = {The Journal of Physical Chemistry C},
volume = {129},
number = {10},
pages = {5116-5121},
abstract = {Periodic lattices of high refractive index materials manipulate light in exceptional manners. Resulting remarkable properties range from photonic band gaps to chiral active matter, which critically depend on parameters of crystal lattices such as the unit cell, lattice type, and periodicity. In self-assembled materials, the lattice properties are inherited by the geometry and size of the macromolecules or colloidal particles assembling the unit cell. DNA origami allows for excellent control over the size and shape of assembled macromolecules while simultaneously allowing control over the interaction between them and ultimately the crystal’s structure. Here, we present the assembly of chiral, rhombohedral crystals in one, two, and three dimensions built by a DNA origami tensegrity triangle. Subsequent modification of the lattice with gold nanorods converts the lattices into chiral plasmonic metamaterials active in the visible and near-infrared spectral range. We demonstrate their chiral activity and corroborate the experimental results with simulated data.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
J Lee, J Kim, G Posnjak, A Ershova, D Hayakawa, W M Shih, W B Rogers, Y Ke, T Liedl, S Lee
DNA Origami Colloidal Crystals: Opportunities and Challenges Journal Article
In: Nano Letters, vol. 25, no. 1, pp. 16-27, 2025, ISSN: 1530-6984.
@article{nokey,
title = {DNA Origami Colloidal Crystals: Opportunities and Challenges},
author = {J Lee and J Kim and G Posnjak and A Ershova and D Hayakawa and W M Shih and W B Rogers and Y Ke and T Liedl and S Lee},
url = {https://doi.org/10.1021/acs.nanolett.4c05041},
doi = {10.1021/acs.nanolett.4c05041},
issn = {1530-6984},
year = {2025},
date = {2025-01-08},
journal = {Nano Letters},
volume = {25},
number = {1},
pages = {16-27},
abstract = {Over the last three decades, colloidal crystallization has provided an easy-to-craft platform for mesoscale engineering of photonic and phononic crystals. Nevertheless, the crystal lattices achieved thus far with commodity colloids are largely limited to symmetric and densely packed structures, restricting their functionalities. To obtain non-close-packed crystals and the resulting complexity of the available structures, directional binding between “patchy” colloids has been pursued. However, the conventional “patchy” colloids have been restricted to micrometer-scale spherical particles or clusters. In this Mini-Review, we argue that the time has come to widen the scope of the colloidal palette and include particles made using DNA origami. By benefiting from its unprecedented ability to control nanoscale shapes and patch placement and incorporate various nanomaterials, DNA origami enables novel engineering of colloidal crystallization, particularly for photonic and phononic applications. This mini-review summarizes the recent progress on using DNA origami for colloidal crystallization, together with its challenges and opportunities.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
A Ermatov, M Kost, X Yin, P Butler, M Dass, I D Sharp, T Liedl, T Bein, G Posnjak
Fabrication of functional 3D nanoarchitectures via atomic layer deposition on DNA origami crystals Journal Article
In: arXiv preprint arXiv:2410.13393, 2024.
@article{nokey,
title = {Fabrication of functional 3D nanoarchitectures via atomic layer deposition on DNA origami crystals},
author = {A Ermatov and M Kost and X Yin and P Butler and M Dass and I D Sharp and T Liedl and T Bein and G Posnjak},
year = {2024},
date = {2024-10-17},
journal = {arXiv preprint arXiv:2410.13393},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
G Posnjak, X Yin, P Butler, O Bienek, M Dass, S Lee, I D Sharp, T Liedl
Diamond-lattice photonic crystals assembled from DNA origami Journal Article
In: Science, vol. 384, no. 6697, pp. 781-785, 2024.
@article{nokey,
title = {Diamond-lattice photonic crystals assembled from DNA origami},
author = {G Posnjak and X Yin and P Butler and O Bienek and M Dass and S Lee and I D Sharp and T Liedl},
url = {https://www.science.org/doi/abs/10.1126/science.adl2733},
doi = {doi:10.1126/science.adl2733},
year = {2024},
date = {2024-05-16},
journal = {Science},
volume = {384},
number = {6697},
pages = {781-785},
abstract = {Colloidal self-assembly allows rational design of structures on the micrometer and submicrometer scale. One architecture that can generate complete three-dimensional photonic bandgaps is the diamond cubic lattice, which has remained difficult to realize at length scales comparable with the wavelength of visible or ultraviolet light. In this work, we demonstrate three-dimensional photonic crystals self-assembled from DNA origami that act as precisely programmable patchy colloids. Our DNA-based nanoscale tetrapods crystallize into a rod-connected diamond cubic lattice with a periodicity of 170 nanometers. This structure serves as a scaffold for atomic-layer deposition of high\textendashrefractive index materials such as titanium dioxide, yielding a tunable photonic bandgap in the near-ultraviolet. Diamond lattices can generate a complete three-dimensional photonic band gap, but generally have been fabricated by lithography and exhibit infrared and near-infrared band gaps. Two studies now report DNA templating of lattices on a length scale that can create photonic band gaps at optical wavelengths (see the Perspective by Li and Mao). Posnjak et al. designed DNA origami that self-assembled into diamond lattices with a periodicity of 170 nanometers. After coating the surfaces with a high-dielectric material (titanium dioxide), a reflection corresponding to the photonic band gap was seen in the near ultraviolet. Liu et al. developed an inverse design strategy for creating pyrochlore lattices that can exhibit a large and omnidirectional band gap. This approach, which uses octahedral and icosahedral origami, avoids the formation of traps that interfere with the assembly process. \textemdashPhil Szuromi},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
C Sikeler, F Haslinger, I V Martynenko, T Liedl
DNA Origami-Directed Self-Assembly of Gold Nanospheres for Plasmonic Metasurfaces Journal Article
In: Advanced Functional Materials, vol. 34, no. 42, pp. 2404766, 2024, ISSN: 1616-301X.
@article{nokey,
title = {DNA Origami-Directed Self-Assembly of Gold Nanospheres for Plasmonic Metasurfaces},
author = {C Sikeler and F Haslinger and I V Martynenko and T Liedl},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202404766},
doi = {https://doi.org/10.1002/adfm.202404766},
issn = {1616-301X},
year = {2024},
date = {2024-05-10},
journal = {Advanced Functional Materials},
volume = {34},
number = {42},
pages = {2404766},
abstract = {Abstract Plasmonic nanostructures are frequently utilized to create metasurfaces with a large variety of optical effects. Control over shape and positioning of the nanostructures is key to the function of such plasmonic metasurfaces. Next to lithographic means, directed self-assembly is a viable route to create plasmonic structures on surfaces with the necessary precision. Here, a combined approach of DNA origami self-assembly and electron beam lithography is presented for determinate positioning of gold nanospheres on a SiO2 surface. First, DNA origami structures bind to the electron beam-patterned substrate and subsequently, gold nanoparticles attach to a defined binding site on the DNA origami structure via DNA hybridization. A sol-gel reaction is then used to grow a silica layer around the DNA, thereby increasing the stability of the self-assembled metasurface. A mean yield of 74% of single gold nanospheres is achieved located at the determinate positions with a spatial position accuracy of 9 nm. Gold nanosphere dimers and trimers are achieved with a rate of 65% and 60%, respectively. The applicability of this structuring method is demonstrated by the fabrication of metasurfaces whose optical response can be tuned by the polarization of the incoming and the scattered light.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
S Lee, C Fan, A Movsesyan, J Bürger, F J Wendisch, L De S. Menezes, S A Maier, H Ren, T Liedl, L V Besteiro, A O Govorov, E Cortés
Unraveling the Chirality Transfer from Circularly Polarized Light to Single Plasmonic Nanoparticles Journal Article
In: Angewandte Chemie International Edition, vol. 63, no. 11, pp. e202319920, 2024, ISSN: 1433-7851.
@article{nokey,
title = {Unraveling the Chirality Transfer from Circularly Polarized Light to Single Plasmonic Nanoparticles},
author = {S Lee and C Fan and A Movsesyan and J B\"{u}rger and F J Wendisch and L De S. Menezes and S A Maier and H Ren and T Liedl and L V Besteiro and A O Govorov and E Cort\'{e}s},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202319920},
doi = {https://doi.org/10.1002/anie.202319920},
issn = {1433-7851},
year = {2024},
date = {2024-01-18},
journal = {Angewandte Chemie International Edition},
volume = {63},
number = {11},
pages = {e202319920},
abstract = {Abstract Due to their broken symmetry, chiral plasmonic nanostructures have unique optical properties and numerous applications. However, there is still a lack of comprehension regarding how chirality transfer occurs between circularly polarized light (CPL) and these structures. Here, we thoroughly investigate the plasmon-assisted growth of chiral nanoparticles from achiral Au nanocubes (AuNCs) via CPL without the involvement of any chiral molecule stimulators. We identify the structural chirality of our synthesized chiral plasmonic nanostructures using circular differential scattering (CDS) spectroscopy, which is correlated with scanning electron microscopy imaging at both the single-particle and ensemble levels. Theoretical simulations, including hot-electron surface maps, reveal that the plasmon-induced chirality transfer is mediated by the asymmetric distribution of hot electrons on achiral AuNCs under CPL excitation. Furthermore, we shed light on how this plasmon-induced chirality transfer can also be utilized for chiral growth in bimetallic systems, such as Ag or Pd on AuNCs. The results presented here uncover fundamental aspects of chiral light-matter interaction and have implications for the future design and optimization of chiral sensors and chiral catalysis, among others.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
S Lee, C Fan, A Movsesyan, J Bürger, F J Wendisch, L De S. Menezes, S A Maier, H Ren, T Liedl, L V Besteiro, A O Govorov, E Cortés
Unraveling the Chirality Transfer from Circularly Polarized Light to Single Plasmonic Nanoparticles Journal Article
In: Angewandte Chemie International Edition, vol. 63, no. 11, pp. e202319920, 2024, ISSN: 1433-7851.
@article{nokey,
title = {Unraveling the Chirality Transfer from Circularly Polarized Light to Single Plasmonic Nanoparticles},
author = {S Lee and C Fan and A Movsesyan and J B\"{u}rger and F J Wendisch and L De S. Menezes and S A Maier and H Ren and T Liedl and L V Besteiro and A O Govorov and E Cort\'{e}s},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202319920},
doi = {https://doi.org/10.1002/anie.202319920},
issn = {1433-7851},
year = {2024},
date = {2024-01-18},
journal = {Angewandte Chemie International Edition},
volume = {63},
number = {11},
pages = {e202319920},
abstract = {Abstract Due to their broken symmetry, chiral plasmonic nanostructures have unique optical properties and numerous applications. However, there is still a lack of comprehension regarding how chirality transfer occurs between circularly polarized light (CPL) and these structures. Here, we thoroughly investigate the plasmon-assisted growth of chiral nanoparticles from achiral Au nanocubes (AuNCs) via CPL without the involvement of any chiral molecule stimulators. We identify the structural chirality of our synthesized chiral plasmonic nanostructures using circular differential scattering (CDS) spectroscopy, which is correlated with scanning electron microscopy imaging at both the single-particle and ensemble levels. Theoretical simulations, including hot-electron surface maps, reveal that the plasmon-induced chirality transfer is mediated by the asymmetric distribution of hot electrons on achiral AuNCs under CPL excitation. Furthermore, we shed light on how this plasmon-induced chirality transfer can also be utilized for chiral growth in bimetallic systems, such as Ag or Pd on AuNCs. The results presented here uncover fundamental aspects of chiral light-matter interaction and have implications for the future design and optimization of chiral sensors and chiral catalysis, among others.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
A Muravitskaya, A Movsesyan, O Ávalos-Ovando, V A Bahamondes Lorca, M A Correa-Duarte, L V Besteiro, T Liedl, P Yu, Z Wang, G Markovich, A O Govorov
Hot Electrons and Electromagnetic Effects in the Broadband Au, Ag, and Ag–Au Nanocrystals: The UV, visible, and NIR Plasmons Journal Article
In: ACS Photonics, vol. 11, no. 1, pp. 68-84, 2024.
@article{nokey,
title = {Hot Electrons and Electromagnetic Effects in the Broadband Au, Ag, and Ag\textendashAu Nanocrystals: The UV, visible, and NIR Plasmons},
author = {A Muravitskaya and A Movsesyan and O \'{A}valos-Ovando and V A Bahamondes Lorca and M A Correa-Duarte and L V Besteiro and T Liedl and P Yu and Z Wang and G Markovich and A O Govorov},
url = {https://doi.org/10.1021/acsphotonics.3c00951},
doi = {10.1021/acsphotonics.3c00951},
year = {2024},
date = {2024-01-17},
journal = {ACS Photonics},
volume = {11},
number = {1},
pages = {68-84},
abstract = {Energetic and optical properties of plasmonic nanocrystals strongly depend on their sizes, shapes, and composition. Whereas the use of plasmonic nanoparticles in biotesting has become routine, applications of plasmonics in energy are still early in development. Here, we investigate hot-electron (HE) generation and related electromagnetic effects in both mono- and bimetallic nanorods (NRs) and focus on a promising type of bimetallic nanocrystal\textendashcore\textendashshell Au\textendashAg nanorods. The spectra of the NRs are broadband, highly tunable with their geometry, and exhibit few plasmon resonances. In this work, we provide a new quantum formalism describing the HE generation in bimetallic nanostructures. Interestingly, we observe that the HE generation rate at the UV plasmon resonance of Au\textendashAg NRs appears to be very high. These HEs are highly energetic and suitable for carbon-fuel reactions. Simultaneously, the HE generation at the longitudinal plasmon (L-plasmon) peaks, which can be tuned from the yellow to near-IR, depends on the near-field and electromagnetic Mie effects, limiting the HE efficiencies for long and large NRs. These properties of the L-plasmon relate to all kinds of NRs (Au, Ag, and Au\textendashAg). We also consider the generation of the interband d-holes in Au and Ag, since the involvement of the d-band is crucial for the energetic properties of UV plasmons. The proposed formalism is a significant development for the description of bimetallic (or trimetallic, or more complex) nanostructures, and paving the way for the efficient application of the photophysical mechanisms based on the plasmonic HEs and hot holes in sensing, nanotechnology, photocatalysis, and electrophotochemistry.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
I V Martynenko, E Erber, V Ruider, M Dass, G Posnjak, X Yin, P Altpeter, T Liedl
Site-directed placement of three-dimensional DNA origami Journal Article
In: Nature Nanotechnology, vol. 18, no. 12, pp. 1456-1462, 2023, ISSN: 1748-3395.
@article{nokey,
title = {Site-directed placement of three-dimensional DNA origami},
author = {I V Martynenko and E Erber and V Ruider and M Dass and G Posnjak and X Yin and P Altpeter and T Liedl},
url = {https://doi.org/10.1038/s41565-023-01487-z},
doi = {10.1038/s41565-023-01487-z},
issn = {1748-3395},
year = {2023},
date = {2023-12-01},
journal = {Nature Nanotechnology},
volume = {18},
number = {12},
pages = {1456-1462},
abstract = {The combination of lithographic methods with two-dimensional DNA origami self-assembly has led, among others, to the development of photonic crystal cavity arrays and the exploration of sensing nanoarrays where molecular devices are patterned on the sub-micrometre scale. Here we extend this concept to the third dimension by mounting three-dimensional DNA origami onto nanopatterned substrates, followed by silicification to provide hybrid DNA\textendashsilica structures exhibiting mechanical and chemical stability and achieving feature sizes in the sub-10-nm regime. Our versatile and scalable method relying on self-assembly at ambient temperatures offers the potential to three-dimensionally position any inorganic and organic components compatible with DNA origami nanoarchitecture, demonstrated here with gold nanoparticles. This way of nanotexturing could provide a route for the low-cost production of complex and three-dimensionally patterned surfaces and integrated devices designed on the molecular level and reaching macroscopic dimensions.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
F Schuknecht, K Kołątaj, M Steinberger, T Liedl, T Lohmueller
Accessible hotspots for single-protein SERS in DNA-origami assembled gold nanorod dimers with tip-to-tip alignment Journal Article
In: Nature Communications, vol. 14, no. 1, pp. 7192, 2023, ISSN: 2041-1723.
@article{nokey,
title = {Accessible hotspots for single-protein SERS in DNA-origami assembled gold nanorod dimers with tip-to-tip alignment},
author = {F Schuknecht and K Ko\l\k{a}taj and M Steinberger and T Liedl and T Lohmueller},
url = {https://doi.org/10.1038/s41467-023-42943-7},
doi = {10.1038/s41467-023-42943-7},
issn = {2041-1723},
year = {2023},
date = {2023-11-08},
journal = {Nature Communications},
volume = {14},
number = {1},
pages = {7192},
abstract = {The label-free identification of individual proteins from liquid samples by surface-enhanced Raman scattering (SERS) spectroscopy is a highly desirable goal in biomedical diagnostics. However, the small Raman scattering cross-section of most (bio-)molecules requires a means to strongly amplify their Raman signal for successful measurement, especially for single molecules. This amplification can be achieved in a plasmonic hotspot that forms between two adjacent gold nanospheres. However, the small (≈1−2 nm) gaps typically required for single-molecule measurements are not accessible for most proteins. A useful strategy would thus involve dimer structures with gaps large enough to accommodate single proteins, whilst providing sufficient field enhancement for single-molecule SERS. Here, we report on using a DNA origami scaffold for tip-to-tip alignment of gold nanorods with an average gap size of 8 nm. The gaps are accessible to streptavidin and thrombin, which are captured at the plasmonic hotspot by specific anchoring sites on the origami template. The field enhancement achieved for the nanorod dimers is sufficient for single-protein SERS spectroscopy with sub-second integration times. This design for SERS probes composed of DNA origami with accessible hotspots promotes future use for single-molecule biodiagnostics in the near-infrared range.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
G Posnjak, X Yin, P Butler, O Bienek, M Dass, I D Sharp, T Liedl
Diamond photonic crystals assembled from DNA origami Journal Article
In: arXiv preprint arXiv:2310.10884, 2023.
@article{nokey,
title = {Diamond photonic crystals assembled from DNA origami},
author = {G Posnjak and X Yin and P Butler and O Bienek and M Dass and I D Sharp and T Liedl},
url = {https://arxiv.org/abs/2310.10884},
doi = {https://doi.org/10.48550/arXiv.2310.10884},
year = {2023},
date = {2023-10-16},
journal = {arXiv preprint arXiv:2310.10884},
abstract = {Colloidal self-assembly allows rational design of structures on the micron and submicron scale, potentially leading to physical material properties that are rare or non-existent in nature. One of the architectures that can generate complete 3D photonic band gaps is the diamond cubic lattice, which has remained difficult to realize at length scales comparable to the wavelength of visible light. Here, we demonstrate 3D photonic crystals self-assembled from DNA origami that act as precisely programmable patchy colloids. Our DNA-based nanoscale tetrapods crystallize into a rod-connected diamond cubic lattice with a periodicity of 170 nm that serves as a scaffold for atomic layer deposition of high refractive index materials such as TiO2, yielding a tunable photonic band gap in the near UV range.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
I V Martynenko, E Erber, V Ruider, M Dass, G Posnjak, X Yin, P Altpeter, T Liedl
Site-directed placement of three-dimensional DNA origami Journal Article
In: Nature Nanotechnology, vol. 18, no. 12, pp. 1456-1462, 2023, ISSN: 1748-3395.
@article{nokey,
title = {Site-directed placement of three-dimensional DNA origami},
author = {I V Martynenko and E Erber and V Ruider and M Dass and G Posnjak and X Yin and P Altpeter and T Liedl},
url = {https://doi.org/10.1038/s41565-023-01487-z},
doi = {10.1038/s41565-023-01487-z},
issn = {1748-3395},
year = {2023},
date = {2023-08-28},
journal = {Nature Nanotechnology},
volume = {18},
number = {12},
pages = {1456-1462},
abstract = {The combination of lithographic methods with two-dimensional DNA origami self-assembly has led, among others, to the development of photonic crystal cavity arrays and the exploration of sensing nanoarrays where molecular devices are patterned on the sub-micrometre scale. Here we extend this concept to the third dimension by mounting three-dimensional DNA origami onto nanopatterned substrates, followed by silicification to provide hybrid DNA\textendashsilica structures exhibiting mechanical and chemical stability and achieving feature sizes in the sub-10-nm regime. Our versatile and scalable method relying on self-assembly at ambient temperatures offers the potential to three-dimensionally position any inorganic and organic components compatible with DNA origami nanoarchitecture, demonstrated here with gold nanoparticles. This way of nanotexturing could provide a route for the low-cost production of complex and three-dimensionally patterned surfaces and integrated devices designed on the molecular level and reaching macroscopic dimensions.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
M Alarcón-Correa, L Kilwing, F Peter, T Liedl, P Fischer
Platinum-DNA Origami Hybrid Structures in Concentrated Hydrogen Peroxide Journal Article
In: ChemPhysChem, vol. 24, no. 22, pp. e202300294, 2023, ISSN: 1439-4235.
@article{nokey,
title = {Platinum-DNA Origami Hybrid Structures in Concentrated Hydrogen Peroxide},
author = {M Alarc\'{o}n-Correa and L Kilwing and F Peter and T Liedl and P Fischer},
url = {https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/cphc.202300294},
doi = {https://doi.org/10.1002/cphc.202300294},
issn = {1439-4235},
year = {2023},
date = {2023-08-28},
journal = {ChemPhysChem},
volume = {24},
number = {22},
pages = {e202300294},
abstract = {Abstract The DNA origami technique allows fast and large-scale production of DNA nanostructures that stand out with an accurate addressability of their anchor points. This enables the precise organization of guest molecules on the surfaces and results in diverse functionalities. However, the compatibility of DNA origami structures with catalytically active matter, a promising pathway to realize autonomous DNA machines, has so far been tested only in the context of bio-enzymatic activity, but not in chemically harsh reaction conditions. The latter are often required for catalytic processes involving high-energy fuels. Here, we provide proof-of-concept data showing that DNA origami structures are stable in 5 % hydrogen peroxide solutions over the course of at least three days. We report a protocol to couple these to platinum nanoparticles and show catalytic activity of the hybrid structures. We suggest that the presented hybrid structures are suitable to realize catalytic nanomachines combined with precisely engineered DNA nanostructures.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
K Trofymchuk, K Kołątaj, V Glembockyte, F Zhu, G P Acuna, T Liedl, P Tinnefeld
Gold Nanorod DNA Origami Antennas for 3 Orders of Magnitude Fluorescence Enhancement in NIR Journal Article
In: ACS Nano, vol. 17, iss. 2, pp. 1327-1334, 2023, ISSN: 1936-0851.
@article{nokey,
title = {Gold Nanorod DNA Origami Antennas for 3 Orders of Magnitude Fluorescence Enhancement in NIR},
author = {K Trofymchuk and K Ko\l\k{a}taj and V Glembockyte and F Zhu and G P Acuna and T Liedl and P Tinnefeld},
url = {https://doi.org/10.1021/acsnano.2c09577},
doi = {10.1021/acsnano.2c09577},
issn = {1936-0851},
year = {2023},
date = {2023-01-03},
urldate = {2023-01-03},
journal = {ACS Nano},
volume = {17},
issue = {2},
pages = {1327-1334},
abstract = {DNA origami has taken a leading position in organizing materials at the nanoscale for various applications such as manipulation of light by exploiting plasmonic nanoparticles. We here present the arrangement of gold nanorods in a plasmonic nanoantenna dimer enabling up to 1600-fold fluorescence enhancement of a conventional near-infrared (NIR) dye positioned at the plasmonic hotspot between the nanorods. Transmission electron microscopy, dark-field spectroscopy, and fluorescence analysis together with numerical simulations give us insights on the heterogeneity of the observed enhancement values. The size of our hotspot region is ∼12 nm, granted by using the recently introduced design of NAnoantenna with Cleared HotSpot (NACHOS), which provides enough space for placing of tailored bioassays. Additionally, the possibility to synthesize nanoantennas in solution might allow for production upscaling.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
K Trofymchuk, K Kołątaj, V Glembockyte, F Zhu, G P Acuna, T Liedl, P Tinnefeld
Gold Nanorod DNA Origami Antennas for 3 Orders of Magnitude Fluorescence Enhancement in NIR Journal Article
In: ACS Nano, vol. 17, no. 2, pp. 1327-1334, 2023, ISSN: 1936-0851.
@article{nokey,
title = {Gold Nanorod DNA Origami Antennas for 3 Orders of Magnitude Fluorescence Enhancement in NIR},
author = {K Trofymchuk and K Ko\l\k{a}taj and V Glembockyte and F Zhu and G P Acuna and T Liedl and P Tinnefeld},
url = {https://doi.org/10.1021/acsnano.2c09577},
doi = {10.1021/acsnano.2c09577},
issn = {1936-0851},
year = {2023},
date = {2023-01-03},
journal = {ACS Nano},
volume = {17},
number = {2},
pages = {1327-1334},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
K Martens, T Funck, E Y Santiago, A O Govorov, S Burger, T Liedl
Onset of Chirality in Plasmonic Meta-Molecules and Dielectric Coupling Journal Article
In: ACS Nano, vol. 16, no. 10, pp. 16143-16149, 2022, ISSN: 1936-0851.
@article{nokey,
title = {Onset of Chirality in Plasmonic Meta-Molecules and Dielectric Coupling},
author = {K Martens and T Funck and E Y Santiago and A O Govorov and S Burger and T Liedl},
url = {https://doi.org/10.1021/acsnano.2c04729},
doi = {10.1021/acsnano.2c04729},
issn = {1936-0851},
year = {2022},
date = {2022-10-25},
journal = {ACS Nano},
volume = {16},
number = {10},
pages = {16143-16149},
abstract = {Chirality is a fundamental feature in all domains of nature, ranging from particle physics over electromagnetism to chemistry and biology. Chiral objects lack a mirror plane and inversion symmetry and therefore cannot be spatially aligned with their mirrored counterpart, their enantiomer. Both natural molecules and artificial chiral nanostructures can be characterized by their light\textendashmatter interaction, which is reflected in circular dichroism (CD). Using DNA origami, we assemble model meta-molecules from multiple plasmonic nanoparticles, representing meta-atoms accurately positioned in space. This allows us to reconstruct piece by piece the impact of varying macromolecular geometries on their surrounding optical near fields. Next to the emergence of CD signatures in the instance that we architect a third dimension, we design and implement sign-flipping signals through addition or removal of single particles in the artificial molecules. Our data and theoretical modeling reveal the hitherto unrecognized phenomenon of chiral plasmonic\textendashdielectric coupling, explaining the intricate electromagnetic interactions within hybrid DNA-based plasmonic nanostructures.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
K Martens, T Funck, E Y Santiago, A O Govorov, S Burger, T Liedl
Onset of Chirality in Plasmonic Meta-Molecules and Dielectric Coupling Journal Article
In: ACS Nano, vol. 16, no. 10, pp. 16143-16149, 2022, ISSN: 1936-0851.
@article{nokey,
title = {Onset of Chirality in Plasmonic Meta-Molecules and Dielectric Coupling},
author = {K Martens and T Funck and E Y Santiago and A O Govorov and S Burger and T Liedl},
url = {https://doi.org/10.1021/acsnano.2c04729},
doi = {10.1021/acsnano.2c04729},
issn = {1936-0851},
year = {2022},
date = {2022-10-14},
journal = {ACS Nano},
volume = {16},
number = {10},
pages = {16143-16149},
abstract = {Chirality is a fundamental feature in all domains of nature, ranging from particle physics over electromagnetism to chemistry and biology. Chiral objects lack a mirror plane and inversion symmetry and therefore cannot be spatially aligned with their mirrored counterpart, their enantiomer. Both natural molecules and artificial chiral nanostructures can be characterized by their light\textendashmatter interaction, which is reflected in circular dichroism (CD). Using DNA origami, we assemble model meta-molecules from multiple plasmonic nanoparticles, representing meta-atoms accurately positioned in space. This allows us to reconstruct piece by piece the impact of varying macromolecular geometries on their surrounding optical near fields. Next to the emergence of CD signatures in the instance that we architect a third dimension, we design and implement sign-flipping signals through addition or removal of single particles in the artificial molecules. Our data and theoretical modeling reveal the hitherto unrecognized phenomenon of chiral plasmonic\textendashdielectric coupling, explaining the intricate electromagnetic interactions within hybrid DNA-based plasmonic nanostructures.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
V Giegold, K Koła̧Taj, T Liedl, A Hartschuh
Phase-Selective Four-Wave Mixing of Resonant Plasmonic Nanoantennas Journal Article
In: ACS Photonics, 2022.
@article{nokey,
title = {Phase-Selective Four-Wave Mixing of Resonant Plasmonic Nanoantennas},
author = {V Giegold and K Ko\la̧Taj and T Liedl and A Hartschuh},
url = {https://doi.org/10.1021/acsphotonics.2c01362},
doi = {10.1021/acsphotonics.2c01362},
year = {2022},
date = {2022-10-11},
journal = {ACS Photonics},
abstract = {Metallic nanoantennas are key components of a wide range of optical techniques that exploit their plasmonic response for signal amplification and extremely sensitive detection. For nonlinear techniques, the higher-order plasmonic response of a nanoantenna can be predicted by the product of the nanoantenna’s linear susceptibilities, known as Miller’s rule, provided that the spatial field distributions at the fundamental and the nonlinear frequencies are the same. Here, we show that Miller’s rule also holds for ultra-broadband excitation pulses and that it can be utilized to predict the frequency dependence of the near-degenerate four-wave mixing (ND-FWM) intensities generated by individual resonant plasmonic nanoantennas. Importantly, this implies that the nanoantenna’s nonlinear response can be deterministically controlled and further optimized by varying the spectral phase of the laser pulse. We demonstrate this by measuring the chirp dependence of the ND-FWM signal and observe an enhancement of up to 60% depending on the position of the plasmon resonance with respect to the laser spectrum, in agreement with model predictions. Finally, we exploit this phase control for chirp-selective confocal imaging of resonant nanoantennas. Our findings may help improve the sensitivity of nonlinear techniques such as plasmon-enhanced coherent anti-Stokes Raman scattering.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
K Martens, T Funck, E Y Santiago, A O Govorov, S Burger, T Liedl
On the origin of chirality in plasmonic meta-molecules Journal Article
In: arXiv preprint arXiv:2110.06689, 2021.
@article{nokey,
title = {On the origin of chirality in plasmonic meta-molecules},
author = {K Martens and T Funck and E Y Santiago and A O Govorov and S Burger and T Liedl},
url = {https://arxiv.org/abs/2110.06689},
doi = {arXiv:2110.06689v2},
year = {2021},
date = {2021-10-13},
journal = {arXiv preprint arXiv:2110.06689},
abstract = {Chirality is a fundamental feature in all domains of nature, ranging from particle physics over electromagnetism to chemistry and biology. Chiral objects lack a mirror plane and inversion symmetry and therefore cannot be spatially aligned with their mirrored counterpart, their enantiomer. Both natural molecules and artificial chiral nanostructures can be characterized by their light-matter interaction, which is reflected in circular dichroism (CD). Using DNA origami, we assemble model meta-molecules from multiple plasmonic nanoparticles, representing meta-atoms accurately positioned in space. This allows us to reconstruct piece by piece the impact of varying macromolecular geometries on their surrounding optical near fields. Next to the emergence of CD signatures in the instance that we architect a third dimension, we design and implement sign flipping signals through addition or removal of single particles in the artificial molecules. Our data and theoretical modelling reveal the hitherto unrecognized phenomenon of chiral plasmonic-dielectric coupling, explaining the intricate electromagnetic interactions within hybrid DNA-based plasmonic nanostructures.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
K Martens, F Binkowski, L Nguyen, L Hu, A O Govorov, S Burger, T Liedl
Long- and short-ranged chiral interactions in DNA-assembled plasmonic chains Journal Article
In: Nature Communications, vol. 12, no. 1, pp. 2025, 2021, ISSN: 2041-1723.
@article{nokey,
title = {Long- and short-ranged chiral interactions in DNA-assembled plasmonic chains},
author = {K Martens and F Binkowski and L Nguyen and L Hu and A O Govorov and S Burger and T Liedl},
url = {https://doi.org/10.1038/s41467-021-22289-8},
doi = {10.1038/s41467-021-22289-8},
issn = {2041-1723},
year = {2021},
date = {2021-04-01},
journal = {Nature Communications},
volume = {12},
number = {1},
pages = {2025},
abstract = {Circular dichroism (CD) has long been used to trace chiral molecular states and changes of protein configurations. In recent years, chiral plasmonic nanostructures have shown potential for applications ranging from pathogen sensing to novel optical materials. The plasmonic coupling of the individual elements of such metallic structures is a crucial prerequisite to obtain sizeable CD signals. We here identify and implement various coupling entities\textemdashchiral and achiral\textemdashto demonstrate chiral transfer over distances close to 100 nm. The coupling is realized by an achiral nanosphere situated between a pair of gold nanorods that are arranged far apart but in a chiral fashion using DNA origami. The transmitter particle causes a strong enhancement of the CD response, the emergence of an additional chiral feature at the resonance frequency of the nanosphere, and a redshift of the longitudinal plasmonic resonance frequency of the nanorods. Matching numerical simulations elucidate the intricate chiral optical fields in complex architectures.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
L Nguyen, M Dass, M F Ober, L V Besteiro, Z M M Wang, B Nickel, A O Govorov, T Liedl, A Heuer-Jungemann
Chiral Assembly of Gold-Silver Core-Shell Plasmonic Nanorods on DNA Origami with Strong Optical Activity Journal Article
In: Acs Nano, vol. 14, no. 6, pp. 7454-7461, 2020, ISSN: 1936-0851.
@article{,
title = {Chiral Assembly of Gold-Silver Core-Shell Plasmonic Nanorods on DNA Origami with Strong Optical Activity},
author = {L Nguyen and M Dass and M F Ober and L V Besteiro and Z M M Wang and B Nickel and A O Govorov and T Liedl and A Heuer-Jungemann},
url = {\<Go to ISI\>://WOS:000543744100103},
doi = {10.1021/acsnano.0c03127},
issn = {1936-0851},
year = {2020},
date = {2020-06-23},
journal = {Acs Nano},
volume = {14},
number = {6},
pages = {7454-7461},
abstract = {The spatial organization of metal nanoparticles has become an important tool for manipulating light in nanophotonic applications. Silver nanoparticles, particularly silver nanorods, have excellent plasmonic properties but are prone to oxidation and are therefore inherently unstable in aqueous solutions and salt-containing buffers. Consequently, gold nanoparticles have often been favored, despite their inferior optical performance. Bimetallic, i.e., gold-silver core-shell nanoparticles, can resolve this issue. We present a method for synthesizing highly stable gold-silver core-shell NRs that are instantaneously functionalized with DNA, enabling chiral self-assembly on DNA origami. The silver shell gives rise to an enhancement of plasmonic properties, reflected here in strongly increased circular dichroism, as compared to pristine gold nanorods. Gold-silver nanorods are ideal candidates for plasmonic sensing with increased sensitivity as needed in pathogen RNA or antibody testing for nonlinear optics and light-funneling applications in surface enhanced Raman spectroscopy. Furthermore, the control of interparticle orientation enables the study of plasmonic phenomena, in particular, synergistic effects arising from plasmonic coupling of such bimetallic systems.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Y Negrín-Montecelo, M Comesaña-Hermo, L K Khorashad, A Sousa-Castillo, Z Wang, M Pérez-Lorenzo, T Liedl, A O Govorov, M A Correa-Duarte
In: ACS Energy Letters, pp. 395-402, 2019.
@article{,
title = {Photophysical Effects behind the Efficiency of Hot Electron Injection in Plasmon-Assisted Catalysis: The Joint Role of Morphology and Composition},
author = {Y Negr\'{i}n-Montecelo and M Comesa\~{n}a-Hermo and L K Khorashad and A Sousa-Castillo and Z Wang and M P\'{e}rez-Lorenzo and T Liedl and A O Govorov and M A Correa-Duarte},
url = {https://doi.org/10.1021/acsenergylett.9b02478},
doi = {10.1021/acsenergylett.9b02478},
year = {2019},
date = {2019-12-12},
journal = {ACS Energy Letters},
pages = {395-402},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
A Heuer-Jungemann, T Liedl
From DNA Tiles to Functional DNA Materials Journal Article
In: Trends in Chemistry, vol. 1, no. 9, pp. 799-814, 2019, ISSN: 2589-5974.
@article{nokey,
title = {From DNA Tiles to Functional DNA Materials},
author = {A Heuer-Jungemann and T Liedl},
url = {https://www.sciencedirect.com/science/article/pii/S258959741930190X},
doi = {https://doi.org/10.1016/j.trechm.2019.07.006},
issn = {2589-5974},
year = {2019},
date = {2019-12-01},
journal = {Trends in Chemistry},
volume = {1},
number = {9},
pages = {799-814},
abstract = {Over the past few decades, DNA has turned into one of the most widely used molecular linkers and a versatile building block for the self-assembly of DNA nanostructures. Such complexes, composed of only a few oligonucleotides (e.g., DNA tiles) or assembled from hundreds of synthetic and natural scaffolding strands (e.g., DNA origami), are being increasingly assembled into higher-order architectures such as lattices and crystals. A wide variety of assembly methods and techniques (e.g., solution-phase and substrate-assisted sticky-ended cohesion or blunt-end stacking) have emerged and are constantly being refined. This review provides a summary of the methods and building blocks for the assembly of 2D and 3D DNA lattices and crystals, and discusses some of their potential applications in materials science.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
K Hübner, M Pilo-Pais, F Selbach, T Liedl, P Tinnefeld, F D Stefani, G P Acuna
Directing Single-Molecule Emission with DNA Origami-Assembled Optical Antennas Journal Article
In: Nano Letters, vol. 19, no. 9, pp. 6629-6634, 2019, ISSN: 1530-6984.
@article{,
title = {Directing Single-Molecule Emission with DNA Origami-Assembled Optical Antennas},
author = {K H\"{u}bner and M Pilo-Pais and F Selbach and T Liedl and P Tinnefeld and F D Stefani and G P Acuna},
url = {https://doi.org/10.1021/acs.nanolett.9b02886},
doi = {10.1021/acs.nanolett.9b02886},
issn = {1530-6984},
year = {2019},
date = {2019-09-11},
urldate = {2019-09-11},
journal = {Nano Letters},
volume = {19},
number = {9},
pages = {6629-6634},
keywords = {},
pubstate = {published},
tppubtype = {article}
}