arXiv subjects

Guillermo Acuna

Publications and source records attributed to Guillermo Acuna.

5 recordsLinked to original sources

arXiv2026

Sel-assembled Rhodium Nanoantennas for Single-Protein UV SERS

Surface-enhanced Raman scattering (SERS) provides critical insights into analyte structure, dynamic processes, and intermolecular interactions at the single-molecule level. By exploiting the hotspot formation in the vicinity of plasmonic structures, SERS constitutes an established tool for fundamental biological research, particularly for early-stage disease diagnostics. In this context, the DNA Origami technique, with its high addressability, enables both the assembly of plasmonic nanostructures with nanometric accuracy, and the deterministic placement of a single analyte molecule precisely at the generated hotspot within them. To date, most DNA Origami based nanoantennas rely on gold or silver nanoparticles (NPs), whose plasmonic resonances are confined to the visible spectrum, severely limiting their use in other spectral ranges. To extend the operating range, we have recently established a robust strategy for self-assembling programmable ultraviolet (UV)-plasmonic dimer antennas using rhodium nanocubes. Herein, we leverage this tailored architecture to systematically investigate its performance for single-molecule UV-SERS. We demonstrated how biofabricated Rh-dimers can be used to detect the characteristic SERS signal of a single streptavidin molecule linked at the dimer s gap. Our results are validated through polarization dependent measurements that yield the expected signal modulation depending on the the dimer orientation only for the DNA origami with a protein at the hotspot. This work establishes a highly sensitive and polarization-tunable UV-SERS platform, laying a solid foundation for label-free optical investigation and bio-spectroscopy of individual biomolecules in the UV spectral range.

physics.app-ph↗

arXiv2025

UV-SERS monitoring of plasmons photodegradation of biomolecules on Aluminum platforms decorated with Rhodium nanoparticles

In the search for novel nanostructured materials for UV plasmonics a limited number of choices can be done. Materials such as aluminum, rhodium, gallium and few others can be used. One of the most interesting application for UV plasmonics is Surface Enhanced Raman Spectroscopy. It can be extended to this spectral range to explore spectral properties of biomolecules that have only a small cross section in the visible spectral range. We have recently reported on a functional substrates based on nanoporous aluminum decorated with rhodium nanoparticles. This system showed an interesting behavior for UV excitation at 266 nm, with an unexpected decreasing Raman intensity for increasing rhodium nanoparticles concentrations. We proposed that this effect can be due to the difficult access to the hot spots for the molecules deposited via thermal evaporation. Here we extend this study exploring the performance of the system at another UV excitation wavelengths (325 nm) reporting on experimental results obtained using a deposition process that can bring the molecules at the hot-spots in a more efficient way. Extensive spectroscopic acquisitions, combined with 3D maps, allow to shade a more clear view on the performance of this plasmonic platform. In particular, the photodegration and the potential oxidation of biomolecules driven by the hot-electron/hot-holes produced by the rhodium nanoparticles will be reported.

physics.app-ph↗

arXiv2025

Dynamics of DNA-Templated Ultrafine Silver Nanowires Formation

Recent research on silver nanowires prepared on DNA templates has focused on two fundamental applications: nano-scale circuits and sensors. Despite its broad potential, the formation kinetics of DNA-templated silver nanowires remains unclear. Here, we present an experimental demonstration of the formation of silver nanowires with a diameter of 2.2+0.4 nm at the single-molecule level through chemical reduction. We conducted equilibrium and perturbation kinetic experiments to measure force spectroscopy during the formation of Ag+ -DNA complexes and Ag-DNA complexes, using optical tweezers combined with microfluidics. The addition of AgNO3 resulted in an increase in force of 5.5-7.5 pN within 2 minutes, indicating that Ag+ compacts the DNA structure. In contrast, the addition of hydroquinone caused the force to decrease by 4-5 pN. Morphological characterization confirmed the presence of a dense structure formed by silver atoms bridging the DNA strands, and revealed conformational differences before and after metallization. We compare our experimental data with Brownian dynamics simulations using a coarse-grained double-stranded DNA (dsDNA) model that provides insights on the dependency of the force on the persistence length.

physics.app-ph↗

arXiv2024

Advances and Applications of Dynamic Surface-Enhanced Raman Spectroscopy (SERS) for Single Molecule Studies

Dynamic surface-enhanced Raman spectroscopy (SERS) is nowadays one of the most interesting applications of SERS, in particular for single molecule studies. In fact, it enables the study of real-time processes at the molecular level. This review summarizes the latest developments in dynamic SERS techniques and their applications, focusing on new instrumentation, data analysis methods, temporal resolution and sensitivity improvements, and novel substrates. We highlight the progress and applications of single-molecule dynamic SERS in monitoring chemical reactions, catalysis, biomolecular interactions, conformational dynamics, and real-time sensing and detection. We aim to provide a comprehensive review on its advancements, applications as well as its current challenges and development frontiers.

physics.app-ph↗

arXiv2024

Giant Purcell broadening and Lamb shift for DNA-assembled near-infrared quantum emitters

Controlling the light emitted by individual molecules is instrumental to a number of novel nanotechnologies ranging from super-resolution bio-imaging and molecular sensing to quantum nanophotonics. Molecular emission can be tailored by modifying the local photonic environment, for example by precisely placing a single molecule inside a plasmonic nanocavity with the help of DNA origami. Here, using this scalable approach, we show that commercial fluorophores experience giant Purcell factors and Lamb shifts, reaching values on par with those recently reported in scanning tip experiments. Engineering of plasmonic modes enables cavity-mediated fluorescence far detuned from the zero-phonon-line (ZPL) - at detunings that are up to two orders of magnitude larger than the fluorescence linewidth of the bare emitter and reach into the near-infrared. Our results evidence a regime where the emission linewidth is dominated by the excited state lifetime, as required for indistinguishable photon emission, baring relevance to the development of nanoscale, ultrafast quantum light sources and to the quest toward single-molecule cavity-QED. In the future, this approach may also allow to design efficient quantum emitters at infrared wavelengths, where standard organic sources have a reduced performance.

physics.optics↗