Imperial College London

ProfessorEmilianoCortes

Faculty of EngineeringDepartment of Materials

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e.cortes

 
 
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Blackett LaboratorySouth Kensington Campus

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Summary

 

Publications

Publication Type
Year
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120 results found

Lee S, Fan C, Movsesyan A, Bürger J, Wendisch FJ, de S Menezes L, Maier SA, Ren H, Liedl T, Besteiro LV, Govorov AO, Cortés Eet al., 2024, Unraveling the Chirality Transfer from Circularly Polarized Light to Single Plasmonic Nanoparticles., Angew Chem Int Ed Engl

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.

Journal article

Liu M, Wang Q, Luo T, Herran M, Cao X, Liao W, Zhu L, Li H, Stefancu A, Lu Y-R, Chan T-S, Pensa E, Ma C, Zhang S, Xiao R, Cortés Eet al., 2024, Potential Alignment in Tandem Catalysts Enhances CO2-to-C2H4 Conversion Efficiencies., J Am Chem Soc, Vol: 146, Pages: 468-475

The in-tandem catalyst holds great promise for addressing the limitation of low *CO coverage on Cu-based materials for selective C2H4 generation during CO2 electroreduction. However, the potential mismatch between the CO-formation catalyst and the favorable C-C coupling Cu catalyst represents a bottleneck in these types of electrocatalysts, resulting in low tandem efficiencies. In this study, we propose a robust solution to this problem by introducing a wide-CO generation-potential window nickel single atom catalyst (Ni SAC) supported on a Cu catalyst. The selection of Ni SAC was based on theoretical calculations, and its excellent performance was further confirmed by using in situ IR spectroscopy. The facilitated carbon dimerization in our tandem catalyst led to a ∼370 mA/cm2 partial current density of C2H4, corresponding to a faradic efficiency of ∼62%. This performance remained stable and consistent for at least ∼14 h at a high current density of 500 mA/cm2 in a flow-cell reactor, outperforming most tandem catalysts reported so far.

Journal article

Ezendam S, Gargiulo J, Sousa-Castillo A, Lee JB, Nam YS, Maier SA, Cortés Eet al., 2024, Spatial Distributions of Single-Molecule Reactivity in Plasmonic Catalysis., ACS Nano, Vol: 18, Pages: 451-460

Plasmonic catalysts have the potential to accelerate and control chemical reactions with light by exploiting localized surface plasmon resonances. However, the mechanisms governing plasmonic catalysis are not simple to decouple. Several plasmon-derived phenomena, such as electromagnetic field enhancements, temperature, or the generation of charge carriers, can affect the reactivity of the system. These effects are convoluted with the inherent (nonplasmonic) catalytic properties of the metal surface. Disentangling these coexisting effects is challenging but is the key to rationally controlling reaction pathways and enhancing reaction rates. This study utilizes super-resolution fluorescence microscopy to examine the mechanisms of plasmonic catalysis at the single-particle level. The reduction reaction of resazurin to resorufin in the presence of Au nanorods coated with a porous silica shell is investigated in situ. This allows the determination of reaction rates with a single-molecule sensitivity and subparticle resolution. By variation of the irradiation wavelength, it is possible to examine two different regimes: photoexcitation of the reactant molecules and photoexcitation of the nanoparticle's plasmon resonance. In addition, the measured spatial distribution of reactivity allows differentiation between superficial and far-field effects. Our results indicate that the reduction of resazurin can occur through more than one reaction pathway, being most efficient when the reactant is photoexcited and is in contact with the Au surface. In addition, it was found that the spatial distribution of enhancements varies, depending on the underlying mechanism. These findings contribute to the fundamental understanding of plasmonic catalysis and the rational design of future plasmonic nanocatalysts.

Journal article

Herran M, Juergensen S, Kessens M, Hoeing D, Köppen A, Sousa-Castillo A, Parak WJ, Lange H, Reich S, Schulz F, Cortés Eet al., 2023, Plasmonic bimetallic two-dimensional supercrystals for H<inf>2</inf> generation, Nature Catalysis, Vol: 6, Pages: 1205-1214

Sunlight-driven H2 generation is a central technology to tackle our impending carbon-based energy collapse. Colloidal photocatalysts consisting of plasmonic and catalytic nanoparticles are promising for H2 production at solar irradiances, but their performance is hindered by absorption and multiscattering events. Here we present a two-dimensional bimetallic catalyst by incorporating platinum nanoparticles into a well-defined supercrystal of gold nanoparticles. The bimetallic supercrystal exhibited an H2 generation rate of 139mmolgcat−1h−1 via formic acid dehydrogenation under visible light illumination and solar irradiance. This configuration makes it possible to study the interaction between the two metallic materials and the influence of this in catalysis. We observe a correlation between the intensity of the electric field in the hotspots and the boosted catalytic activity of platinum nanoparticles, while identifying a minor role of heat and gold-to-platinum charge transfer in the enhancement. Our results demonstrate the benefits of two-dimensional configurations with optimized architecture for liquid-phase photocatalysis. [Figure not available: see fulltext.].

Journal article

Boggiano HD, Ramallo JI, Nan L, Litwiller A, Cortés E, Maier SA, Grinblat G, Fuertes MC, Angelomé PC, Bragas AVet al., 2023, Optical Readout of the Mechanical Properties of Silica Mesoporous Thin Films Using Plasmonic Nanoantennas, ACS Photonics, Vol: 10, Pages: 3998-4005

In this work, we apply the recently developed frequency shift of nanoantennas (FRESA) technique to measure the Young’s modulus of thin mesoporous films at GHz frequencies as a function of porosity with local precision. The method measures changes in the mechanical oscillation frequency of optically excited plasmonic nanoantennas with modification of their surrounding medium. The values obtained range from 4 to 10 GPa for porosities extending from 35 to 4%, compatible with reports on films grown under similar conditions. We further find comparable results when using the well-established nanoindentation (NI) technique, validating the new method. By analysis of the nanoresonator’s quality factor, the measurement reveals an excellent interfacial adhesion of the films to the nanoantennas. Different from most other characterization techniques, FRESA provides elastic modulus determination at GHz frequencies, relevant for the operation of current devices. Furthermore, FRESA exhibits, in principle, no limitations in terms of film thickness, in contrast to the NI, which is strongly affected by the stiffness of the substrate for ultrathin films.

Journal article

Zhang H, Luo T, Chen Y, Liu K, Li H, Pensa E, Fu J, Lin Z, Chai L, Cortés E, Liu Met al., 2023, Frontispiz: Highly Efficient Decomposition of Perfluorocarbons for over 1000 Hours via Active Site Regeneration, Angewandte Chemie, Vol: 135, ISSN: 0044-8249

Journal article

Zhang H, Luo T, Chen Y, Liu K, Li H, Pensa E, Fu J, Lin Z, Chai L, Cortés E, Liu Met al., 2023, Highly Efficient Decomposition of Perfluorocarbons for over 1000 Hours via Active Site Regeneration, Angewandte Chemie, Vol: 135, ISSN: 0044-8249

<jats:title>Abstract</jats:title><jats:p>Tetrafluoromethane (CF<jats:sub>4</jats:sub>), the simplest perfluorocarbon (PFC), has the potential to exacerbate global warming. Catalytic hydrolysis is a viable method to degrade CF<jats:sub>4</jats:sub>, but fluorine poisoning severely restricts both the catalytic performance and catalyst lifetime. In this study, Ga is introduced to effectively assists the defluorination of poisoned Al active sites, leading to highly efficient CF<jats:sub>4</jats:sub> decomposition at 600 °C with a catalytic lifetime exceeding 1,000 hours. <jats:sup>27</jats:sup>Al and <jats:sup>71</jats:sup>Ga magic‐angle spinning nuclear magnetic resonance spectroscopy (MAS NMR) showed that the introduced Ga exists as tetracoordinated Ga sites (Ga<jats:sub>IV</jats:sub>), which readily dissociate water to form Ga−OH. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density function theory (DFT) calculations confirmed that Ga−OH assists the defluorination of poisoned Al active sites via a dehydration‐like process. As a result, the Ga/Al<jats:sub>2</jats:sub>O<jats:sub>3</jats:sub> catalyst achieved 100 % CF<jats:sub>4</jats:sub> decomposition keeping an ultra‐long catalytic lifetime and outperforming reported results. This work proposes a new approach for efficient and long‐term CF<jats:sub>4</jats:sub> decomposition by promoting the regeneration of active sites.</jats:p>

Journal article

Zhang H, Luo T, Chen Y, Liu K, Li H, Pensa E, Fu J, Lin Z, Chai L, Cortés E, Liu Met al., 2023, Frontispiece: Highly Efficient Decomposition of Perfluorocarbons for over 1000 Hours via Active Site Regeneration, Angewandte Chemie International Edition, Vol: 62, ISSN: 1433-7851

Journal article

Ben-Jaber S, Glass D, Brick T, Maier SA, Parkin IP, Cortes E, Peveler WJ, Quesada-Cabrera Ret al., 2023, Photo-induced enhanced Raman spectroscopy as a probe for photocatalytic surfaces, PHILOSOPHICAL TRANSACTIONS OF THE ROYAL SOCIETY A-MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES, Vol: 381, ISSN: 1364-503X

Journal article

Jin H, Herran M, Cortés E, Lischner Jet al., 2023, Theory of hot-carrier generation in bimetallic plasmonic catalysts, ACS Photonics, Vol: 10, Pages: 3629-3636, ISSN: 2330-4022

Bimetallic nanoreactors in which a plasmonic metal is used to funnel solar energy toward a catalytic metal have recently been studied experimentally, but a detailed theoretical understanding of these systems is lacking. Here, we present theoretical results of hot-carrier generation rates of different Au-Pd nanoarchitectures. In particular, we study spherical core-shell nanoparticles with a Au core and a Pd shell as well as antenna-reactor systems consisting of a large Au nanoparticle that acts as an antenna and a smaller Pd satellite nanoparticle separated by a gap. In addition, we investigate an antenna-reactor system in which the satellite is a core-shell nanoparticle. Hot-carrier generation rates are obtained from an atomistic quantum-mechanical modeling technique which combines a solution of Maxwell's equation with a tight-binding description of the nanoparticle electronic structure. We find that antenna-reactor systems exhibit significantly higher hot-carrier generation rates in the catalytic material than the core-shell system as a result of strong electric field enhancements associated with the gap between the antenna and the satellite. For these systems, we also study the dependence of the hot-carrier generation rate on the size of the gap, the radius of the antenna nanoparticle, and the direction of light polarization. Overall, we find a strong correlation between the calculated hot-carrier generation rates and the experimentally measured chemical activity for the different Au-Pd photocatalysts. Our insights pave the way toward a microscopic understanding of hot-carrier generation in heterogeneous nanostructures for photocatalysis and other energy-conversion applications.

Journal article

Ezendam S, Nan L, Violi IL, Maier SA, Cortes E, Baffou G, Gargiulo Jet al., 2023, Anti Stokes Thermometry of Plasmonic Nanoparticle Arrays, ADVANCED OPTICAL MATERIALS, ISSN: 2195-1071

Journal article

Zi X, Zhou Y, Zhu L, Chen Q, Tan Y, Wang X, Sayed M, Pensa E, Geioushy RA, Liu K, Fu J, Cortes E, Liu Met al., 2023, Breaking K<SUP>+</SUP> Concentration Limit on Cu Nanoneedles for Acidic Electrocatalytic CO<sub>2</sub> Reduction to Multi-Carbon Products, ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, ISSN: 1433-7851

Journal article

Zhang H, Luo T, Chen Y, Liu K, Li H, Pensa E, Fu J, Lin Z, Chai L, Cortes E, Liu Met al., 2023, Highly Efficient Decomposition of Perfluorocarbons for over 1000 Hours via Active Site Regeneration, ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, ISSN: 1433-7851

Journal article

Lin R, Chen H, Cui T, Zhang Z, Zhou Q, Nan L, Cheong W-C, Schroeck L, Ramm V, Ding Q, Liang X, Saris S, Wendisch FJ, Maier SA, Fischer RA, Zhu Y, Wang D, Cortes Eet al., 2023, Optimization of p-Type Cu<sub>2</sub>O Nanocube Photocatalysts Based on Electronic Effects, ACS CATALYSIS, Vol: 13, Pages: 11352-11361, ISSN: 2155-5435

Journal article

Gargiulo J, Herran M, Violi IL, Sousa-Castillo A, Martinez LP, Ezendam S, Barella M, Giesler H, Grzeschik R, Schluecker S, Maier SA, Stefani FD, Cortes Eet al., 2023, Impact of bimetallic interface design on heat generation in plasmonic Au/Pd nanostructures studied by single-particle thermometry, NATURE COMMUNICATIONS, Vol: 14

Journal article

Cai C, Liu K, Zhang L, Li F, Tan Y, Li P, Wang Y, Wang M, Feng Z, Motta Meira D, Qu W, Stefancu A, Li W, Li H, Fu J, Wang H, Zhang D, Cortes E, Liu Met al., 2023, Atomically Local Electric Field Induced Interface Water Reorientation for Alkaline Hydrogen Evolution Reaction, ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, Vol: 62, ISSN: 1433-7851

Journal article

Doiron B, Li Y, Bower R, Mihai A, Dal Forno S, Fearn S, Hüttenhofer L, Cortés E, Cohen LF, Alford NM, Lischner J, Petrov P, Maier SA, Oulton RFet al., 2023, Optimizing hot electron harvesting at planar metal–semiconductor interfaces with titanium oxynitride thin films, ACS Applied Materials and Interfaces, Vol: 25, Pages: 30417-30426, ISSN: 1944-8244

Understanding metal-semiconductor interfaces is critical to the advancement of photocatalysis and sub-bandgap solar energy harvesting where electrons in the metal can be excited by sub-bandgap photons and extracted into the semiconductor. In this work, we compare the electron extraction efficiency across Au/TiO2 and titanium oxynitride (TiON)/TiO2-x interfaces, where in the latter case the spontaneously forming oxide layer (TiO2-x) creates a metal-semiconductor contact. Time-resolved pump-probe spectroscopy is used to study the electron recombination rates in both cases. Unlike the nanosecond recombination lifetimes in Au/TiO2, we find a bottleneck in the electron relaxation in the TiON system, which we explain using a trap-mediated recombination model. Using this model, we investigate the tunability of the relaxation dynamics with oxygen content in the parent film. The optimized film (TiO0.5N0.5) exhibits the highest carrier extraction efficiency (NFC ≈ 2.8 × 1019 m-3), slowest trapping, and an appreciable hot electron population reaching the surface oxide (NHE ≈ 1.6 × 1018 m-3). Our results demonstrate the productive role oxygen can play in enhancing electron harvesting and prolonging electron lifetimes, providing an optimized metal-semiconductor interface using only the native oxide of titanium oxynitride.

Journal article

Vinnacombe-Willson GA, Conti Y, Stefancu A, Weiss PS, Cortes E, Scarabelli Let al., 2023, Direct Bottom-Up <i>In Situ</i> Growth: A Paradigm Shift for Studies in Wet-Chemical Synthesis of Gold Nanoparticles, CHEMICAL REVIEWS, Vol: 123, Pages: 8488-8529, ISSN: 0009-2665

Journal article

Koya AN, Romanelli M, Kuttruff J, Henriksson N, Stefancu A, Grinblat G, De Andres A, Schnur F, Vanzan M, Marsili M, Rahaman M, Viejo Rodríguez A, Tapani T, Lin H, Dana BD, Lin J, Barbillon G, Proietti Zaccaria R, Brida D, Jariwala D, Veisz L, Cortés E, Corni S, Garoli D, Maccaferri Net al., 2023, Advances in ultrafast plasmonics, Applied Physics Reviews, Vol: 10

In the past 20 years, we have reached a broad understanding of many light-driven phenomena in nanoscale systems. The temporal dynamics of the excited states are instead quite challenging to explore, and, at the same time, crucial to study for understanding the origin of fundamental physical and chemical processes. In this review, we examine the current state and prospects of ultrafast phenomena driven by plasmons both from a fundamental and applied point of view. This research area is referred to as ultrafast plasmonics and represents an outstanding playground to tailor and control fast optical and electronic processes at the nanoscale, such as ultrafast optical switching, single photon emission, and strong coupling interactions to tailor photochemical reactions. Here, we provide an overview of the field and describe the methodologies to monitor and control nanoscale phenomena with plasmons at ultrafast timescales in terms of both modeling and experimental characterization. Various directions are showcased, among others recent advances in ultrafast plasmon-driven chemistry and multi-functional plasmonics, in which charge, spin, and lattice degrees of freedom are exploited to provide active control of the optical and electronic properties of nanoscale materials. As the focus shifts to the development of practical devices, such as all-optical transistors, we also emphasize new materials and applications in ultrafast plasmonics and highlight recent development in the relativistic realm. The latter is a promising research field with potential applications in fusion research or particle and light sources providing properties such as attosecond duration.

Journal article

Berger LM, Duportal M, Menezes LDS, Cortes E, Maier SA, Tittl A, Krischer Ket al., 2023, Improved In Situ Characterization of Electrochemical Interfaces Using Metasurface-Driven Surface-Enhanced IR Absorption Spectroscopy, ADVANCED FUNCTIONAL MATERIALS, Vol: 33, ISSN: 1616-301X

Journal article

Bragas AV, Maier SA, Boggiano HD, Grinblat G, Bertc R, Menezes LDS, Cortes Eet al., 2023, Nanomechanics with plasmonic nanoantennas : ultrafast and local exchange between electromagnetic and mechanical energy, JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS, Vol: 40, Pages: 1196-1211, ISSN: 0740-3224

Journal article

Wang Q, Dai M, Li H, Lu Y-R, Chan T-S, Ma C, Liu K, Fu J, Liao W, Chen S, Pensa E, Wang Y, Zhang S, Sun Y, Cortes E, Liu Met al., 2023, Asymmetric Coordination Induces Electron Localization at Ca Sites for Robust CO<sub>2</sub> Electroreduction to CO, ADVANCED MATERIALS, Vol: 35, ISSN: 0935-9648

Journal article

Nan L, Giraldez-Martinez J, Stefancu A, Zhu L, Liu M, Govorov AO, Besteiro LV, Cortes Eet al., 2023, Investigating Plasmonic Catalysis Kinetics on Hot-Spot Engineered Nanoantennae, NANO LETTERS, Vol: 23, Pages: 2883-2889, ISSN: 1530-6984

Journal article

Long Y, He J, Zhang H, Chen Y, Liu K, Fu J, Li H, Zhu L, Lin Z, Stefancu A, Cortes E, Zhu M, Liu Met al., 2023, Highly Selective Monomethylation of Amines with CO<sub>2</sub>/H<sub>2</sub> via Ag/Al<sub>2</sub>O<sub>3</sub> as a Catalyst, CHEMISTRY-A EUROPEAN JOURNAL, Vol: 29, ISSN: 0947-6539

Journal article

Cortés E, 2023, Light-activated catalysts point the way to sustainable chemistry, Nature, Vol: 614, Pages: 230-232, ISSN: 0028-0836

Journal article

Stefancu A, Gargiulo J, Laufersky G, Auguie B, Chis V, Le Ru EC, Liu M, Leopold N, Cortes Eet al., 2023, Interface-Dependent Selectivity in Plasmon-Driven Chemical Reactions, ACS NANO, ISSN: 1936-0851

Journal article

Wang J, Ni G, Liao W, Liu K, Chen J, Liu F, Zhang Z, Jia M, Li J, Fu J, Pensa E, Jiang L, Bian Z, Cortes E, Liu Met al., 2023, Subsurface Engineering Induced Fermi Level De-pinning in Metal Oxide Semiconductors for Photoelectrochemical Water Splitting, ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, ISSN: 1433-7851

Journal article

Paredes MY, Martinez LP, Barja BC, Marchi MC, Herran M, Grinblat G, Bragas AV, Cortes E, Scarpettini AFet al., 2023, Efficient method of arsenic removal from water based on photocatalytic oxidation by a plasmonic-magnetic nanosystem, ENVIRONMENTAL SCIENCE-NANO, Vol: 10, Pages: 166-177, ISSN: 2051-8153

Journal article

Liao W, Liu K, Wang J, Stefancu A, Chen Q, Wu K, Zhou Y, Li H, Mei L, Li M, Fu J, Miyauchi M, Cortes E, Liu Met al., 2023, Boosting Nitrogen Activation<i> via</i> Ag Nanoneedle Arrays for Efficient Ammonia Synthesis, ACS NANO, Vol: 17, Pages: 411-420, ISSN: 1936-0851

Journal article

Moretti GQ, Tittl A, Cortes E, Maier SA, Bragas A, Grinblat Get al., 2022, Introducing a Symmetry-Breaking Coupler into a Dielectric Metasurface Enables Robust High-Q Quasi-BICs, ADVANCED PHOTONICS RESEARCH, Vol: 3, ISSN: 2699-9293

Journal article

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