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See detailEnhanced Optical Spectroscopy for Multiplexed DNA and Protein-Sequencing with Plasmonic Nanopores: Challenges and Prospects
Li, Wang; Zhou, Juan; Maccaferri, Nicolò UL et al

in Analytical Chemistry (2022), 94(2), 503-514

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See detailMagnetic control of particle trapping in a hybrid plasmonic nanopore
Maccaferri, Nicolò UL; Vavassori, Paolo; Garoli, Denis

in Applied Physics Letters (2021), 118

Plasmonic nanopores are extensively investigated as single molecules detectors. The main limitations in plasmonic nanopore technology are the too fast translocation velocity of the molecule through the ... [more ▼]

Plasmonic nanopores are extensively investigated as single molecules detectors. The main limitations in plasmonic nanopore technology are the too fast translocation velocity of the molecule through the pore and the consequent very short analysis times, as well as the possible instabilities due to local heating. An interesting approach to enable longer acquisition times is represented by the ability to stably trap the nanoparticles used to tag molecules close to the nanopore. Here, we theoretically investigate the performance of a magneto-plasmonic nanopore prepared with a thin layer of cobalt sandwiched between two gold layers. A nanopore is then coupled with a bifunctional (magnetic and plasmonic) core–shell nanoparticle made of magnetite (core) covered with a thin layer of gold (shell). By setting the magnetic configuration of the cobalt layer around the pore by an external magnetic field, it is possible to generate a nanoscale magnetic tweezer to trap the nanoparticle at a specific point. Considering a ∼10 nm diameter magnetite nanoparticle, we calculate a trapping force up to 28 pN, an order of magnitude above the force that can be obtained with standard optical or plasmonic trapping approaches. Moreover, the magnetic force pulls the nanoparticle in close contact with the plasmonic nanopore's wall, thus enabling the formation of a nanocavity enclosing a sub-10 nm3 confined electromagnetic field with an average field intensity enhancement up to 230 at near-infrared wavelengths. The presented hybrid magneto-plasmonic system points toward a strategy to improve nanopore-based biosensors for single-molecule detection and potentially for the analysis of various biomolecules. [less ▲]

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See detailDirectional Plasmonic Excitation by Helical Nanotips
Singh, Leeju; Maccaferri, Nicolò UL; Garoli, Denis et al

in Nanomaterials (2021), 11(5), 1333

The phenomenon of coupling between light and surface plasmon polaritons requires specific momentum matching conditions. In the case of a single scattering object on a metallic surface, such as a ... [more ▼]

The phenomenon of coupling between light and surface plasmon polaritons requires specific momentum matching conditions. In the case of a single scattering object on a metallic surface, such as a nanoparticle or a nanohole, the coupling between a broadband effect, i.e., scattering, and a discrete one, such as surface plasmon excitation, leads to Fano-like resonance lineshapes. The necessary phase matching requirements can be used to engineer the light–plasmon coupling and to achieve a directional plasmonic excitation. Here, we investigate this effect by using a chiral nanotip to excite surface plasmons with a strong spin-dependent azimuthal variation. This effect can be described by a Fano-like interference with a complex coupling factor that can be modified thanks to a symmetry breaking of the nanostructure. [less ▲]

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See detailUltrafast opto-acoustic modulation of light reflectance in metal-insulator-metal epsilon-near-zero nanocavities
Kuttruff, Joel; Krahne, Roman; De Luca, Antonio et al

in Proceedings of SPIE: The International Society for Optical Engineering (2021), 11769

We report on ultrafast opto-acoustic modulation of light reflectance in artificial epsilon-near-zero metamaterials made of two layers of Ag separated by an Al2O3 layer. By means of non-degenerate two ... [more ▼]

We report on ultrafast opto-acoustic modulation of light reflectance in artificial epsilon-near-zero metamaterials made of two layers of Ag separated by an Al2O3 layer. By means of non-degenerate two color pump-probe experiments we demonstrate an optically induced acoustic modulation of the reflectance up to 20% via generation of acoustic waves inside the cavity upon mechanical expansion of the metal due to hot electron-phonon coupling nonlinearity in the Ag layers. The presented architecture opens the pathway towards novel routes to exploit light-matter interactions for opto-acoustic modulation at GHz frequencies. Moreover, our system can be designed to work in transmission geometry and is very versatile in terms of shifting the presented properties along a broad range of wavelengths, from UV to mid-IR. Our approach, beyond light-driven information processing, might impact also opto-mechanics, light-driven phonon induced up conversion mechanisms, non-linear optical and acoustic properties of materials, energy harvesting, and heat-assisted ultrafast magneto-optical recording. [less ▲]

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See detailEnhanced second-harmonic generation by single metal–insulator multilayered nanocavities with axial symmetry resonating in the near-infrared
Zilli, Attilio; Isoniemi, Tommi; Iarossi, Marzia et al

in Proceedings of SPIE: The International Society for Optical Engineering (2021), 11770

We report efficient second-harmonic emission by single multilayer metal–dielectric nanocavities. Engineering the intrinsic interface-induced symmetry breaking by resonant optical absorption design, allows ... [more ▼]

We report efficient second-harmonic emission by single multilayer metal–dielectric nanocavities. Engineering the intrinsic interface-induced symmetry breaking by resonant optical absorption design, allows to achieve almost two orders of magnitude higher second-harmonic generation efficiency compared to gold nanostructures with the same geometry. We estimate a second-order nonlinear susceptibility of the order of 1 pm/V, which is comparable to widely used nonlinear crystals. We envision that our system, which combines the advantages of both plasmonic and dielectric materials, might enable the realization of composite nano-systems for an efficient multi-purpose manipulation of nonlinear optical processes at the nanoscale. [less ▲]

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See detailRecent advances on plasmonic nanocavities for single-molecule spectroscopy
Maccaferri, Nicolò UL; Barbillon, Grégory; Koya, Alemayehu Nana et al

in Nanoscale Advances (2021), 3

Plasmonic nanocavities are able to engineer and confine electromagnetic fields into subwavelength volumes. In the past decade, they have enabled a large set of applications, in particular for sensing ... [more ▼]

Plasmonic nanocavities are able to engineer and confine electromagnetic fields into subwavelength volumes. In the past decade, they have enabled a large set of applications, in particular for sensing, optical trapping, as well as the investigation of physical and chemical phenomena at a few or single-molecule levels. This extreme sensitivity is possible thanks to the highly confined local field intensity enhancement, which depends on the geometry of the plasmonic nanocavities. Indeed, properly designed structures providing engineered local optical fields lead to enhanced optical sensing based on different phenomena like surface enhanced Raman scattering, fluorescence, and Förster Resonant Energy Transfer. In this mini-review, we illustrate the most recent results on plasmonic nanocavities, with specific emphasis on the detection of single molecules. [less ▲]

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See detailEnhanced Nonlinear Emission from Single Multilayered Metal−Dielectric Nanocavities Resonating in the Near-Infrared
Maccaferri, Nicolò UL; Zilli, Attilio; Isoniemi, Tommi et al

in ACS Photonics (2021), 8(2), 512-520

Harmonic generation mechanisms are of great interest in nanoscience and nanotechnology, since they allow generating visible light by using near-infrared radiation, which is particularly suitable for its ... [more ▼]

Harmonic generation mechanisms are of great interest in nanoscience and nanotechnology, since they allow generating visible light by using near-infrared radiation, which is particularly suitable for its countless applications in bionanophotonics and optoelectronics. In this context, multilayer metal−dielectric nanocavities are widely used for light confinement and waveguiding at the nanoscale. They exhibit intense and localized resonances that can be conveniently tuned in the near-infrared and are therefore ideal for enhancing nonlinear effects in this spectral range. In this work, we experimentally investigate the nonlinear emission properties of multilayer metal−dielectric nanocavities. By engineering their absorption efficiency and exploiting their intrinsic interface-induced symmetry breaking, we achieve an almost 2 orders of magnitude higher second-harmonic generation efficiency compared to gold nanostructures featuring the same geometry and optical resonant behavior. In particular, while both the third-order nonlinear susceptibility and conversion efficiency are comparable with those of the Au nanoresonators, we estimate a second-order nonlinear susceptibility of the order of 1 pm/V, which is comparable with that of typical nonlinear crystals. We envision that our system, which combines the advantages of both plasmonic and dielectric materials, might enable the realization of composite and multifunctional nanosystems for the efficient manipulation of nonlinear optical processes at the nanoscale. [less ▲]

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See detailHyperbolic dispersion metasurfaces for molecular biosensing
Palermo, Giovanna; Sreekanth, Kandammathe Valiyaveedu; Maccaferri, Nicolò UL et al

in Nanophotonics (2021), 10(1), 295314

Sensor technology has become increasingly crucial in medical research and clinical diagnostics to directly detect small numbers of low-molecular-weight biomolecules relevant for lethal diseases. In recent ... [more ▼]

Sensor technology has become increasingly crucial in medical research and clinical diagnostics to directly detect small numbers of low-molecular-weight biomolecules relevant for lethal diseases. In recent years, various technologies have been developed, a number of them becoming core label-free technologies for detection of cancer biomarkers and viruses. However, to radically improve early disease diagnostics, tracking of disease progression and evaluation of treatments, today’s biosensing techniques still require a radical innovation to deliver high sensitivity, specificity, diffusion-limited transport, and accuracy for both nucleic acids and proteins. In this review, we discuss both scientific and technological aspects of hyperbolic dispersion metasurfaces for molecular biosensing. Optical metasurfaces have offered the tantalizing opportunity to engineer wavefronts while its intrinsic nanoscale patterns promote tremendous molecular interactions and selective binding. Hyperbolic dispersion metasurfaces support high-k modes that proved to be extremely sensitive to minute concentrations of ultralow-molecular-weight proteins and nucleic acids. [less ▲]

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See detailField-resolved detection of the temporal response of a single plasmonic antenna in the mid infrared
Fischer, Marco P.; Maccaferri, Nicolò UL; Gallacher, Kevin et al

in Optica (2021), 8(6), 898-903

Unveiling the spatial and temporal dynamics of a light pulse interacting with nanosized objects is of extreme importance to widen our understanding of how photons interact with matter at the nanoscale and ... [more ▼]

Unveiling the spatial and temporal dynamics of a light pulse interacting with nanosized objects is of extreme importance to widen our understanding of how photons interact with matter at the nanoscale and trigger physical and photochemical phenomena. An ideal platform to study light–matter interactions with an unprecedented spatial resolution is represented by plasmonics, which enables an extreme confinement of optical energy into sub-wavelength volumes. The ability to resolve and control the dynamics of this energy confinement on the time scale of a single optical cycle is at the ultimate frontier towards a full control of nanoscale phenomena. Here, we resolve in the time domain the linear behavior of a single germanium plasmonic antenna in the mid-infrared by measuring the complex optical field response in amplitude and phase with sub-optical-cycle precision, with the promise to extend the observation of light–matter interactions in the time domain to single quantum objects. Accessing this fundamental information opens a plethora of opportunities in a variety of research areas based on plasmon-mediated photonic processes and their coherent control, such as plasmon-enhanced chemical reactions and energy harvesting. [less ▲]

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See detailMagnetophotonics for sensing and magnetometry toward industrial applications
Rizal, Conrad; Manera, Maria Grazia; Ignatyeva, Daria O. et al

in Journal of Applied Physics (2021), 130

Magnetic nanostructures sustaining different types of optical modes have been used for magnetometry and label-free ultrasensitive refractive index probing, where the main challenge is the realization of ... [more ▼]

Magnetic nanostructures sustaining different types of optical modes have been used for magnetometry and label-free ultrasensitive refractive index probing, where the main challenge is the realization of compact devices that are able to transfer this technology from research laboratories to smart industry. This Perspective discusses the state-of-the-art and emerging trends in realizing innovative sensors containing new architectures and materials exploiting the unique ability to actively manipulate their optical properties using an externally applied magnetic field. In addition to the well-established use of propagating and localized plasmonic fields, in the so-called magnetoplasmonics, we identified a new potential of the all-dielectric platforms for sensing to overcome losses inherent to metallic components. In describing recent advances, emphasis is placed on several feasible industrial applications, trying to give our vision on the future of this promising field of research merging optics, magnetism, and nanotechnology. [less ▲]

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See detailMagneto-optical activity in nonmagnetic hyperbolic nanoparticles
Kuttruff, Joel; Gabbani, Alessio; Petrucci, Gaia et al

in Physical Review Letters (2021), 127

Active nanophotonics can be realized by controlling the optical properties of materials with external magnetic fields. Here, we explore the influence of optical anisotropy on the magneto-optical activity ... [more ▼]

Active nanophotonics can be realized by controlling the optical properties of materials with external magnetic fields. Here, we explore the influence of optical anisotropy on the magneto-optical activity in non-magnetic hyperbolic nanoparticles. We demonstrate that the magneto-optical response is driven by fundamental electric and magnetic dipole modes induced by the hyperbolic dispersion. Magnetic circular dichroism experiments confirm the theoretical predictions and reveal tunable magneto-optical activity across the visible and near infrared spectral range. [less ▲]

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See detailSpeeding up nanoscience and nanotechnology with ultrafast plasmonics
Maccaferri, Nicolò UL; Meuret, Sophie; Kornienko, Nikolay et al

in Nano Letters (2020)

Surface plasmons are collective oscillations of free electrons at the interface between a conducting material and the dielectric environment. These excitations support the formation of strongly enhanced ... [more ▼]

Surface plasmons are collective oscillations of free electrons at the interface between a conducting material and the dielectric environment. These excitations support the formation of strongly enhanced and confined electromagnetic fields. As well, they display fast dynamics lasting tens of femtoseconds and can lead to a strong nonlinear optical response at the nanoscale. Thus, they represent the perfect tool to drive and control fast optical processes, such as ultrafast optical switching, single photon emission, as well as strong coupling interactions to explore and tailor photochemical reactions. In this Virtual Issue, we gather several important papers published in Nano Letters in the past decade reporting studies on the ultrafast dynamics of surface plasmons. [less ▲]

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See detailFörster-resonance energy transfer between diffusing molecules and a functionalized plasmonic nanopore
Zambrana-Puyalto, Xavier; Ponzellini, Paolo; Maccaferri, Nicolò UL et al

in Physical Review Applied (2020), 14(5), 054065

Plasmonic nanopores are the subject of extensive investigations as a potential platform to enable efficient optical read-out in translocation experiments with biomolecules such as DNA and proteins. They ... [more ▼]

Plasmonic nanopores are the subject of extensive investigations as a potential platform to enable efficient optical read-out in translocation experiments with biomolecules such as DNA and proteins. They allow for the engineering of electromagnetic fields at the nanoscale, which are typically used to enhance the emission efficiency of fluorescent molecules. Their features make them suitable for detection strategies based on the energy transfer between translocating molecules and the nanopore itself. Here, we have carried out an optical experiment to show that a handful of diffusing dyes acting as donors can exchange energy via Fster resonance energy transfer (FRET) with a gold nanopore functionalized with dyes behaving as acceptors. The FRET pair is composed of ATTORho6G (donor) and Alexa610 (acceptor). To perform this proof-of-concept experiment, we used a gold nanopore with a diameter of 80 nm, prepared on a Si3N4 membrane. We have observed that the presence of the acceptors on the walls of the nanopore reduces the lifetime of the diffusing donors. In addition, we have observed that the presence of the acceptors reduces the fluorescence signal on the donor detection channel and increases the fluorescence signal on the acceptor detection channel. The combination of these three effects gives us enough evidence to claim that the diffusing donors exchange energy with the functionalized nanopore via FRET, despite the relatively large size of the nanopore. The FRET efficiency of the process has been found to be of the order of 30%, which is in a fairly good agreement with a theoretical value obtained using a simplified model. [less ▲]

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See detailMachine learning in nanoscience: big data at small scales
Brown, Keith A.; Brittman, Sarah; Maccaferri, Nicolò UL et al

in Nano Letters (2020), 20(1), 2-10

Recent advances in machine learning (ML) offer new tools to extract new insights from large data sets and to acquire small data sets more effectively. Researchers in nanoscience are experimenting with ... [more ▼]

Recent advances in machine learning (ML) offer new tools to extract new insights from large data sets and to acquire small data sets more effectively. Researchers in nanoscience are experimenting with these tools to tackle challenges in many fields. In addition to ML’s advancement of nanoscience, nanoscience provides the foundation for neuromorphic computing hardware to expand the implementation of ML algorithms. In this mini-review, which is not able to be comprehensive, we highlight some recent efforts to connect the ML and nanoscience communities focusing on three types of interaction: (1) using ML to analyze and extract new information from large nanoscience data sets, (2) applying ML to accelerate materials discovery, including the use of active learning to guide experimental design, and (3) the nanoscience of memristive devices to realize hardware tailored for ML. We conclude with a discussion of challenges and opportunities for future interactions between nanoscience and ML researchers. [less ▲]

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See detailUltrafast all-optical switching enabled by epsilon-near-zero-tailored absorption in metal-insulator nanocavities
Kuttruff, Joel; Garoli, Denis; Allerbeck, Jonas et al

in Communications Physics (2020), 3

Ultrafast control of light−matter interactions is fundamental in view of new technological frontiers of information processing. However, conventional optical elements are either static or feature ... [more ▼]

Ultrafast control of light−matter interactions is fundamental in view of new technological frontiers of information processing. However, conventional optical elements are either static or feature switching speeds that are extremely low with respect to the time scales at which it is possible to control light. Here, we exploit the artificial epsilon-near-zero (ENZ) modes of a metal-insulator-metal nanocavity to tailor the linear photon absorption of our system and realize a nondegenerate all-optical ultrafast modulation of the reflectance at a specific wavelength. Optical pumping of the system at its high energy ENZ mode leads to a strong redshift of the low energy mode because of the transient increase of the local dielectric function, which leads to a sub-3-ps control of the reflectance at a specific wavelength with a relative modulation depth approaching 120%. [less ▲]

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See detailPlasmon Hybridization in Compressible Metal-Insulator-Metal Nano-Cavities: an Optical Approach for Sensing Deep Sub-Wavelength Deformation
Carrara, Angelica; Maccaferri, Nicolò UL; Cerea, Andrea et al

in Advanced Optical Materials (2020), 8(18), 2000609

We present a pressure-induced deformation-sensitive device based on 2D matrices of plasmonic gold nanodisks coupled to a metal thin layer through a compressible dielectric spacer, namely a deformable ... [more ▼]

We present a pressure-induced deformation-sensitive device based on 2D matrices of plasmonic gold nanodisks coupled to a metal thin layer through a compressible dielectric spacer, namely a deformable metal-insulator-metal (MIM) nanocavity, to report deep sub-wavelength size variations (< λ/200). The system is characterized by two hybrid branches, which are resonant in the visible/near infrared spectral region. The fundamental mode, owing to the near-field interaction between the plasmonic nanostructures and the metal film, exhibits a remarkable sensitivity to the gap size, exceeding that of a planar “macroscopic” optical cavity and extending its operational domain to the sub-wavelength range, where excellent opportunities towards truly multiscale MIMs-based pressure sensors can be envisioned. Concurrently, its intrinsic plasmonic nature synergistically combines into a single platform multi-purpose functionalities, such as ultrasensitive detection, remote temperature readout etc., with practical perspectives in ultra-compact inspection tools for structural and functional information at the nanoscale. [less ▲]

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See detailElectron Energy Loss Spectroscopy of Bright and Dark Modes in Hyperbolic Metamaterial Nanostructures
Isoniemi, Tommi; Maccaferri, Nicolò UL; Ramasse, Quentin M. et al

in Advanced Optical Materials (2020), 8(13), 2000277

Layered metal/dielectric hyperbolic metamaterials (HMMs) support a wide landscape of plasmon polariton excitations. In addition to surface plasmon polaritons, coupled Bloch-like gap-plasmon polaritons ... [more ▼]

Layered metal/dielectric hyperbolic metamaterials (HMMs) support a wide landscape of plasmon polariton excitations. In addition to surface plasmon polaritons, coupled Bloch-like gap-plasmon polaritons with high modal confinement inside the multilayer are supported. Photons can excite only a subset of these polaritonic modes, typically with a limited energy and momentum range in respect to the wide set of high-K modes supported by hyperbolic dispersion media, and coupling with gratings or local excitation is necessary. Strikingly, electron energy loss spectroscopy (EELS) in a scanning transmission electron microscope allows nm-scale local excitation and mapping of the spatial field distribution of all the modes supported by a photonic or plasmonic structure, both bright and dark, and also all other inelastic interactions of the beam, including phonons and interband transitions. Herein, experimental evidence of the spatial distribution of plasmon polaritons in multilayered type II HMM nanostructures is acquired with an aloof electron beam adjacent to structures of current interest. HMM pillars are useful for their separation and adjustability of optical scattering and absorption, while HMM slot cavities can be used as waveguides with high field confinement. The nature of the modes is confirmed with corresponding simulations of EEL and optical spectra and near-field intensities. [less ▲]

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See detailTwo-state switchable plasmonic tweezers for dynamic manipulation of nano-objects
Messina, Gabriele; Zambrana-Puyalto, Xavier; Maccaferri, Nicolò UL et al

in Nanoscale (2020), 12

In this work, we present a plasmonic platform capable of trapping nano-objects in two different spatial configurations. The switch between the two trapping states, localized on the tip and on the outer ... [more ▼]

In this work, we present a plasmonic platform capable of trapping nano-objects in two different spatial configurations. The switch between the two trapping states, localized on the tip and on the outer wall of a vertical gold nanochannel, can be activated by varying the focusing position of the excitation laser along the main axis of the nanotube. We show that the switching of the trapping site is induced by changes in the distribution of the electromagnetic field and of the trapping force. The “inner” and “outer” trapping states are characterized by a static and a dynamic behavior respectively, and their stiffness is measured by analyzing the positions of the trapped specimens as a function of time. In addition, we demonstrate that the stiffness of the static state is high enough to trap particles with diameter as small as 40 nm. These results show a simple, controllable way to generate a switchable two-state trapping regime, which could be used as a model for the study of dynamic trapping or as a mechanism for the development of nanofluidic devices. [less ▲]

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See detailParticle trapping and beaming using a 3D nanotip excited with a plasmonic vortex
Liu, Kai; Maccaferri, Nicolò UL; Shen, Yuefeng et al

in Optics Letters (2020), 45(4), 823-826

Recent advances in nanotechnology have prompted the need for tools to accurately and non-invasively manipulate individual nano-objects. Among the possible strategies, optical forces have been widely used ... [more ▼]

Recent advances in nanotechnology have prompted the need for tools to accurately and non-invasively manipulate individual nano-objects. Among the possible strategies, optical forces have been widely used to enable nano-optical tweezers capable of trapping or moving a specimen with unprecedented accuracy. Here, we propose an architecture consisting of a nanotip excited with a plasmonic vortex enabling effective dynamic control of nanoparticles in three dimensions. The structure illuminated by a beam with angular momentum can generate an optical field which can be used to manipulate single dielectric nanoparticles. We demonstrate that it’s possible to stably trap or push the particle from specific points, thus enabling a new platform for nanoparticle manipulation. [less ▲]

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See detailIntracellular recording of human cardiac action potentials on market-available multielectrode array platforms
Melle, Giovanni; Bruno, Giulia; Maccaferri, Nicolò UL et al

in Frontiers in Bioengineering and Biotechnology (2020), 8

High quality attenuated intracellular action potentials from large cell networks can be recorded on multi-electrode arrays by means of 3D vertical nanopillars using electrical pulses. However,most of the ... [more ▼]

High quality attenuated intracellular action potentials from large cell networks can be recorded on multi-electrode arrays by means of 3D vertical nanopillars using electrical pulses. However,most of the techniques require complex 3D nanostructures that prevent the straightforward translation into marketable products and the wide adoption in the scientific community. Moreover, 3D nanostructures are often delicate objects that cannot sustain several harsh use/cleaning cycles. On the contrary, laser optoacoustic poration allows the recording of action potentials on planar nanoporous electrodes made of noble metals. However, these constraints of the electrode material and morphology may also hinder the full exploitation of this methodology. Here, we show that optoacoustic poration is also very effective for porating cells on a large family of MEA electrode configurations, including robust electrodes made of nanoporous titanium nitride or disordered fractal-like gold nanostructures. This enables the recording of high quality cardiac action potentials in combination with optoacoustic poration, providing thus attenuated intracellular recordings on various already commercial devices used by a significant part of the research and industrial communities. [less ▲]

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