arXiv subjects

Emiliano Cortés

Publications and source records attributed to Emiliano Cortés.

At least 19 recordsLinked to original sources

arXiv2026

Lattice tuning of optical and mechanical interactions in gold nanodisk metasurfaces

The interaction between neighboring plasmonic nanoparticles can modify their intrinsic optical and mechanical resonances, enabling collective responses to be controlled through the geometry of their arrangement. Periodic arrays therefore provide a means of controlling both electromagnetic and mechanical interactions through a common geometrical parameter, the lattice pitch. Joint control of these two channels is particularly useful for engineering how coherent mechanical excitations couple to the substrate and are optically read out at the nanoscale. Here, we investigate the optical and mechanical response of gold nanodisk metasurface patches on silica as a function of lattice pitch using two-color pump-probe spectroscopy and numerical simulations. Optically, simulations show that varying the pitch tunes a Rayleigh anomaly across the broad localized surface plasmon resonance of the nanodisks, producing a strongly asymmetric collective optical response. Pump-probe measurements further reveal a pronounced wavelength dependence of the optical readout of coherent mechanical vibrations. Mechanically, we investigate how coupling between the nanodisks and the substrate depends on the character of the nanodisk resonances. The intrinsic nanodisk modes exhibit markedly different sensitivities to the periodic environment. One remains nearly independent of pitch, whereas another undergoes a pronounced frequency shift mediated by elastic interactions through the substrate. Numerical simulations further reveal that a third nanodisk resonance couples resonantly to a lattice-selected acoustic mode, giving rise to an avoided crossing and mode hybridization. These distinct mechanical responses are governed by how efficiently each mode couples to near-surface elastic motion in the substrate. These results demonstrate that lattice periodicity can simultaneously tune optical sensitivity and substrate-mediated mechanical coupling, providing a versatile platform for tailoring nanoscale optomechanical responses in the GHz regime.

physics.optics↗

arXiv2026

Enantioselective optical trapping and characterization of all dielectric disorder-enabled chiral particles

We trap submicroscopic silica spheres coated with randomly distributed titanium dioxide nanoparticles in optical tweezers with Laguerre-Gaussian modes and observe orbital dynamics that differ from those of achiral silica spheres. We show that the disordered nanoparticle coating generates an effective chiral geometry, giving rise to enhanced enantioselective chiral optical forces and a measurable modification of the orbital period. A theoretical model based on the Mie-Debye formalism, including optical aberrations, not only quantitatively explains the experimental results but also allows to characterize the Pasteur parameter quantifying the chiroptical response of individual composite particles. These findings constitute direct experimental evidence of chiral optical forces exerted by structured light beams on individual chiral particles and identify disorder-enabled, all-dielectric particles as a versatile material platform to tailor chiral optical forces at the nanoscale.

physics.optics↗

arXiv2026

Platinum is a Photocatalyst: Large Visible-Light Quantum Efficiency Revealed

Metal-semiconductor junctions in optoelectronic devices are commonly engineered to promote charge separation. In Pt/TiO2 Schottky junctions, Pt is typically regarded as a catalytic electron sink rather than a visible-light-active component. Here, we demonstrate that Pt nanoislands on TiO2 can generate photochemically active carriers under visible light excitation. Using quantitative scanning photoelectrochemical microscopy, we measure the wavelength-resolved external quantum efficiency (EQE) of Au and Pt nanoisland arrays on TiO2, and correlate their reactivity with their morphology and extinction spectra. Discrete 10 nm Pt nanoislands exhibit robust broadband visible light photoactivity - exceeding the photoactivity of similar-sized Au nanoislands under blue-green excitation - whereas Pt's photoactivity is strongly suppressed when the nanoislands are connected. Surprisingly, Pt exhibits an EQE-per-atom approx. 20 times higher than Au at 455 nm and approx. 2 times higher at 595 nm (at Au's optimum). We show an approximately wavelength-independent Pt internal quantum efficiency of approx. 1 percent across the visible spectral region. These findings reposition catalytic metals with strongly damped optical response in the visible as light-responsive components in metal-semiconductor hybrids, challenging the prevailing perception that they function solely as passive co-catalysts in photocatalytic systems.

cond-mat.mes-hall↗

arXiv2024

Coherent Acoustic Phonons in Plasmonic Nanoparticles: Elastic Properties and Dissipation at Low Temperatures

We studied the frequency and quality factor of mechanical plasmonic nanoresonators as a function of temperature, ranging from ambient to 4 K. Our investigation focused on individual gold nanorods and nanodisks of various sizes. We observed that oscillation frequencies increase linearly as temperature decreases until saturation is reached at cryogenic temperatures. This behavior is explained by the temperature dependence of the elastic modulus, with a Debye temperature compatible with reported bulk values for gold. To describe the behavior of the quality factor, we developed a model considering the nanostructures as anelastic solids, identifying a dissipation peak around 150 K due to a thermally activated process, likely of the Niblett-Wilks mechanism type. Importantly, our findings suggest that external dissipation factors are more critical to improving quality factors than internal friction, which can be increased by modifying the nanoresonator's environment. Our results enable the design of structures with high vibration frequencies and quality factors by effectively controlling external losses.

physics.optics↗

arXiv2024

Highly confined incident-angle-robust surface phonon polariton bound states in the continuum metasurfaces

Squeezing light into subwavelength dimensions is vital for on-chip integration of photonic technologies. One approach to overcome the diffraction limit is coupling light to material excitations, leading to polariton states. Here, we showcase how low-loss mid-infrared surface phonon polaritons enable metasurfaces supporting quasi-bound states in the continuum (qBICs) with deeply subwavelength unit cells. Utilizing 100 nm thick free-standing silicon carbide membranes, we achieve highly confined qBIC states with a unit cell volume ~ 10^4 times smaller than the diffraction limit. This results in remarkable robustness of the platform against the incident angle that is unique among qBIC systems. We also demonstrate vibrational strong coupling with a thin layer of spin-coated molecules, leveraging the small mode volume. This work introduces phononic qBICs as a novel ultra-confined nanophotonic platform, paving a way for the miniaturization of mid-infrared devices for molecular sensing and thermal radiation engineering.

physics.optics↗

arXiv2024

Focusing Surface Acoustic Waves with a Plasmonic Hypersonic Lens

Plasmonic nanoantennas have proven to be efficient transducers of electromagnetic to mechanical energy and vice versa. The sudden thermal expansion of these structures after an ultrafast optical pulsed excitation leads to the emission of hypersonic acoustic waves to the supporting substrate, which can be detected by another antenna that acts as a high-sensitive mechanical probe due to the strong modulation of its optical response. Sophisticated fabrication techniques, together with the implementation of numerical simulations, have allowed the engineering of nanostructures for the controlled directional generation and detection of high-frequency acoustic phonons at the nanoscale, with many potential applications in telecommunications, sensing, mechanical switching, and energy transport. Here, we propose and experimentally demonstrate a nanoscale acoustic lens comprised of 11 gold nanodisks whose collective oscillation gives rise to an interference pattern that results in a diffraction-limited surface acoustic beam of about 340 nm width, with an amplitude contrast of 60%. Via spatially decoupled pump-probe experiments, we were able to map the radiated acoustic energy in the proximity of the focal area, obtaining a very good agreement with the continuum elastic theory.

physics.optics↗

arXiv2024

Si Metasurface Supporting Multiple Quasi-BICs for Degenerate Four-Wave Mixing

Dielectric metasurfaces supporting quasi-bound states in the continuum (qBICs) enable high field enhancement with narrow-linewidth resonances in the visible and near-infrared ranges. The resonance emerges when distorting the meta-atom's geometry away from a symmetry-protected BIC condition and, usually, a given design can sustain one or two of these states. In this work, we introduce a silicon-on-silica metasurface that simultaneously supports up to four qBIC resonances in the near-infrared region. This is achieved by combining multiple symmetry-breaking distortions on an elliptical cylinder array. By pumping two of these resonances, the nonlinear process of degenerate four-wave mixing is experimentally realized. By comparing the nonlinear response with that of an unpatterned silicon film, the near-field enhancement inside the nanostructured dielectric is revealed. The presented results demonstrate independent geometric control of multiple qBICs and their interaction trough wave mixing processes, opening new research pathways in nanophotonics, with potential applications in information multiplexing, multi-wavelength sensing and nonlinear imaging.

physics.optics↗

arXiv2024

Tracking Surface Charge Dynamics on Single Nanoparticles

Surface charges play a fundamental role in physics and chemistry, particularly in shaping the catalytic properties of nanomaterials. Tracking nanoscale surface charge dynamics remains challenging due to the involved length and time scales. Here, we demonstrate real-time access to the nanoscale charge dynamics on dielectric nanoparticles employing reaction nanoscopy. We present a four-dimensional visualization of the non-linear charge dynamics on strong-field irradiated single SiO$_2$ nanoparticles with femtosecond-nanometer resolution and reveal how surface charges affect surface molecular bonding with quantum dynamical simulations. We performed semi-classical simulations to uncover the roles of diffusion and charge loss in the surface charge redistribution process. Understanding nanoscale surface charge dynamics and its influence on chemical bonding on a single nanoparticle level unlocks an increased ability to address global needs in renewable energy and advanced healthcare.

cond-mat.mes-hall↗

arXiv2023

Crystal Facet Effect in Plasmonic Catalysis

In the realm of plasmonic catalytic systems, much attention has been devoted to the plasmon-derived mechanisms, yet the influence of nanoparticles' crystal facets in this type of processes has been sparsely investigated. In this work, we study the plasmon-assisted electrocatalytic CO2 reduction reaction using three different shapes of plasmonic Au nanoparticles - nanocube (NC), rhombic dodecahedron (RD) and octahedron (OC) - with three different exposed facets: {100}, {110} and {111}, respectively. These particles were synthesized with similar sizes and LSPR wavelengths to reveal the role of the facet more than other contributions to the plasmon-assisted reaction. Upon plasmon excitation, Au OCs exhibited nearly a doubling in the Faradaic efficiency of CO (FE(CO)) and a remarkable threefold enhancement in the partial current density of CO (j(CO)) compared to the non-illuminated response, NCs also demonstrated an improved performance under illumination. In contrast, Au RDs showed nearly the same performance in dark or light conditions. Temperature-dependent experiments ruled out heat as the main factor in the enhanced response of Au OCs and NCs. Large-scale atomistic simulations of the nanoparticles' electronic structure and electromagnetic modeling revealed higher hot carrier abundance and electric field enhancement on Au OCs and NCs compared to RDs. Abundant hot carriers on edges facilitate molecular activation, leading to enhanced selectivity and activity. Thus, OCs with the highest edge/facet ratio exhibited the strongest enhancement in FE(CO) and j(CO) upon illumination. This observation is further supported by plasmon-assisted H2 evolution reaction experiments. Our findings highlight the dominance of low coordinated sites over facets in plasmonic catalytic processes, providing valuable insights for designing more efficient catalysts for solar fuels production.

physics.optics↗

arXiv2023

Multiplication of the orbital angular momentum of phonon polaritons via sublinear dispersion

Optical vortices (OVs) promise to greatly enhance optical information capacity via orbital angular momentum (OAM) multiplexing. The need for on-chip integration of OAM technologies has prompted research into subwavelength-confined polaritonic OVs. However, the topological order imprinted by the structure used for the transduction from free-space beams to surface polaritons is inherently fixed after fabrication. Here, we overcome this limitation via dispersion-driven topological charge multiplication. We switch the OV topological charge within a small $\sim 3 \%$ frequency range by leveraging the strong sublinear dispersion of low-loss surface phonon polaritons (SPhP) on silicon carbide membranes. Applying the Huygens principle we quantitatively evaluate the topological order of the experimental OVs detected by near-field imaging. We further explore the deuterogenic effect, which predicts the coexistence of multiple topological charges in higher-order polaritonic OVs. Our work demonstrates a viable method to manipulate the topological charge of polaritonic OVs, paving the way for the exploration of novel OAM-enabled light-matter interactions at mid-infrared frequencies.

physics.optics↗

arXiv2022

Introducing a Symmetry-Breaking Coupler into a Dielectric Metasurface Enables Robust High-Q Quasibound States in the Continuum and Efficient Nonlinear Frequency Conversion

Dielectric metasurfaces supporting quasi-bound states in the continuum (quasi-BICs) exhibit very high quality factor resonances and electric field confinement. However, accessing the high-Q end of the quasi-BIC regime usually requires marginally distorting the metasurface design from a BIC condition, pushing the needed nanoscale fabrication precision to the limit. This work introduces a novel concept for generating high-Q quasi-BICs, which strongly relaxes this requirement by incorporating a relatively large perturbative element close to high-symmetry points of an undistorted BIC metasurface, acting as a coupler to the radiation continuum. We validate this approach by adding a $\sim$100 nm diameter cylinder between two reflection-symmetry points separated by a 300 nm gap in an elliptical disk metasurface unit cell, using gallium phosphide as the dielectric. We find that high-Q resonances emerge when the cylindrical coupler is placed at any position between such symmetry points. We further explore this metasurface's second harmonic generation capability in the optical range. Displacing the coupler as much as a full diameter from a BIC condition produces record-breaking normalized conversion efficiencies >10$^{2}$ W$^{-1}$. The strategy of enclosing a disruptive element between multiple high-symmetry points in a BIC metasurface could be applied to construct robust high-Q quasi-BICs in many geometrical designs.

physics.optics↗

arXiv2021

Paired Ru-O-Mo ensemble for efficient and stable alkaline hydrogen evolution reaction

Electrocatalytic hydrogen evolution reaction (HER) in alkaline media is a promising electrochemical energy conversion strategy. Ruthenium (Ru) is an efficient catalyst with a desirable cost for HER, however, the sluggish H2O dissociation process, due to the low H2O adsorption on its surface, currently hampers the performances of this catalyst in alkaline HER. Herein, we demonstrate that the H2O adsorption improves significantly by the construction of Ru-O-Mo sites. We prepared Ru/MoO2 catalysts with Ru-O-Mo sites through a facile thermal treatment process and assessed the creation of Ru-O-Mo interfaces by transmission electron microscope (TEM) and extended X-ray absorption fine structure (EXAFS). By using Fourier-transform infrared spectroscopy (FTIR) and H2O adsorption tests, we proved Ru-O-Mo sites have tenfold stronger H2O adsorption ability than that of Ru catalyst. The catalysts with Ru-O-Mo sites exhibited a state-of-the-art overpotential of 16 mV at 10 mA cm-2 in 1 M KOH electrolyte, demonstrating a threefold reduction than the previous bests of Ru (59 mV) and commercial Pt (31 mV) catalysts. We proved the stability of these performances over 40 hours without decline. These results could open a new path for designing efficient and stable catalysts.

physics.chem-ph↗

arXiv2021

Tuning the intermediate reaction barriers by CuPd catalyst to improve the selectivity of electroreduction CO2 to C2 products

Electrochemical CO2 reduction is a promising strategy for utilization of CO2 and intermittent excess electricity. Cu is the only single-metal catalyst that can electrochemically convert CO2 to multi-carbon products. However, Cu has an undesirable selectivity and activity for C2 products, due to its insufficient amount of CO* for C-C coupling. Considering the strong CO2 adsorption and ultra-fast reaction kinetics of CO* formation on Pd, an intimate CuPd(100) interface was designed to lower the intermediate reaction barriers and then improve the efficiency of C2 products. Density functional theory (DFT) calculations showed that the CuPd(100) interface has enhanced CO2 adsorption and decreased CO2* hydrogenation energy barrier, which are beneficial for C-C coupling. The potential-determining step (PDS) barrier of CO2 to C2 products on CuPd(100) interface is 0.61 eV, which is lower than that on Cu(100) (0.72 eV). Motivated by the DFT calculation, the CuPd(100) interface catalyst was prepared by a facile chemical solution method and demonstrated by transmission electron microscope (TEM). The CO2 temperature programmed desorption (CO2-TPD) and gas sensor experiments proved the enhancements of CO2 adsorption and CO2* hydrogenation abilities on CuPd(100) interface catalyst. As a result, the obtained CuPd(100) interface catalyst exhibits a C2 Faradaic efficiency of 50.3 (+/-) 1.2% at -1.4 VRHE in 0.1 M KHCO3, which is 2.1 times higher than 23.6(+/-) 1.5% of Cu catalyst. This work provides a rational design of Cu-based electrocatalyst for multi-carbon products by fine-tuning the intermediate reaction barriers.

cond-mat.mtrl-sci↗

arXiv2021

Fermi level equilibration at the metal-molecule interface in plasmonic systems

We highlight a new metal-molecule charge transfer process by tuning the Fermi energy of plasmonic silver nanoparticles (AgNPs) in-situ. The strong adsorption of halide ions upshifts the Fermi level of AgNPs by up to ~0.3 eV in the order: Cl-<Br-<I-, favoring the spontaneous charge transfer to aligned molecular acceptor orbitals until charge neutrality across the interface is achieved. By carefully quantifying experimentally and theoretically the Fermi level upshift, we show for the first time that this effect is comparable in energy to different plasmonic effects such as the plasmoelectric effect or hot-carriers production. Moreover, by monitoring in-situ the adsorption dynamic of halide ions in different AgNP-molecule systems, we show for the first time that the catalytic role of halide ions in plasmonic nanostructures depends on the surface affinity of halide ions compared to that of the target molecule.

physics.chem-ph↗

arXiv2021

Core-Shell Bimetallic Nanoparticle Trimers for Efficient Light-to-Chemical Energy Conversion

Incorporation of catalytically active materials into plasmonic metal nanostructures can efficiently merge the reactivity and energy harvesting abilities of both types of materials for visible light photocatalysis. Here we explore the influence of electromagnetic hotspots in the ability of plasmonic core-shell colloidal structures to induce chemical transformations. For this study, we developed a synthetic strategy for the fabrication of Au nanoparticle (NP) trimers in aqueous solution through fine controlled galvanic replacement between Ag nanoprisms and Au precursors. Core-shell Au@M NP trimers with catalytically active metals (M = Pd, Pt) were subsequently synthesized using Au NP trimers as templates. Our experimental and computational results highlight the synergy of geometry and composition in plasmonic catalysts for plasmon-driven chemical reactions.

physics.chem-ph↗

arXiv2021

Challenges in Plasmonic Catalysis

The use of nanoplasmonics to control light and heat close to the thermodynamic limit enables exciting opportunities in the field of plasmonic catalysis. The decay of plasmonic excitations creates highly nonequilibrium distributions of hot carriers that can initiate or catalyze reactions through both thermal and nonthermal pathways. In this Perspective, we present the current understanding in the field of plasmonic catalysis, capturing vibrant debates in the literature, and discuss future avenues of exploration to overcome critical bottlenecks. Our Perspective spans first-principles theory and computation of correlated and far-from-equilibrium light-matter interactions, synthesis of new nanoplasmonic hybrids, and new steady-state and ultrafast spectroscopic probes of interactions in plasmonic catalysis, recognizing the key contributions of each discipline in realizing the promise of plasmonic catalysis. We conclude with our vision for fundamental and technological advances in the field of plasmon-driven chemical reactions in the coming years.

physics.optics↗

arXiv2021

Template Dissolution Interfacial Patterning of Single Colloids for Nanoelectrochemistry and Nanosensing

Deterministic positioning and assembly of colloidal nanoparticles (NPs) onto substrates is a core requirement and a promising alternative to top down lithography to create functional nanostructures and nanodevices with intriguing optical, electrical, and catalytic features. Capillary-assisted particle assembly (CAPA) has emerged as an attractive technique to this end, as it allows controlled and selective assembly of a wide variety of NPs onto predefined topographical templates using capillary forces. One critical issue with CAPA, however, lies in its final printing step, where high printing yields are possible only with the use of an adhesive polymer film. To address this problem, we have developed a template dissolution interfacial patterning (TDIP) technique to assemble and print single colloidal AuNP arrays onto various dielectric and conductive substrates in the absence of any adhesion layer, with printing yields higher than 98%. The TDIP approach grants direct access to the interface between the AuNP and the target surface, enabling the use of colloidal AuNPs as building blocks for practical applications. The versatile applicability of TDIP is demonstrated by the creation of direct electrical junctions for electro- and photoelectrochemistry and nanoparticle-on-mirror geometries for single particle molecular sensing.

cond-mat.soft↗

arXiv2021

Determination of Nanoscale Mechanical Properties of Polymers via Plasmonic Nanoantennas

Nanotechnology and the consequent emergence of miniaturized devices are driving the need to improve our understanding of the mechanical properties of a myriad of materials. Here we focus on amorphous polymeric materials and introduce a new way to determine the nanoscale mechanical response of polymeric thin films in the GHz range, using ultrafast optical means. Coupling of the films to plasmonic nanoantennas excited at their vibrational eigenfrequencies allows the extraction of the values of the mechanical moduli as well as the estimation of the glass transition temperature via time-domain measurements, here demonstrated for PMMA films. This nanoscale method can be extended to the determination of mechanical and elastic properties of a wide range of spatially strongly confined materials.

physics.optics↗