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  • 1. Chen, S
    et al.
    Svedendahl, M
    Käll, M
    Gunnarsson, L
    Dmitriev, A
    Ultrahigh sensitivity made simple: nanoplasmonic label-free biosensing with an extremely low limit-of-detection for bacterial and cancer diagnostics.2009In: Nanotechnology, ISSN 0957-4484, E-ISSN 1361-6528, Vol. 20, no 43Article in journal (Refereed)
    Abstract [en]

    We present a simple and robust scheme for biosensing with an ultralow limit-of-detection down to several pg cm(-2) (or several tens of attomoles cm(-2)) based on optical label-free biodetection with localized surface plasmon resonances. The scheme utilizes cost-effective optical components and comprises a white light source, a properly functionalized sensor surface enclosed in a simple fluidics chip, and a spectral analyzer. The sensor surface is produced by a bottom-up nanofabrication technique with hole mask colloidal lithography. Despite its simplicity, the method is able to reliably detect protein-protein binding events at low picomolar and femtomolar concentrations, which is exemplified by the label-free detection of the extracellular adherence protein (EAP) found on the outer surface of the bacterium Staphylococcus aureus and of prostate-specific antigen (PSA), which is believed to be a prostate cancer marker. These experiments pave the way towards an ultra-sensitive yet compact biodetection platform for point-of-care diagnostics applications.

  • 2. Chen, Si
    et al.
    Svedendahl, Mikael
    Antosiewicz, Tomasz J
    Käll, Mikael
    Plasmon-enhanced enzyme-linked immunosorbent assay on large arrays of individual particles made by electron beam lithography.2013In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 7, no 10Article in journal (Refereed)
    Abstract [en]

    Ultrasensitive biosensing is one of the main driving forces behind the dynamic research field of plasmonics. We have previously demonstrated that the sensitivity of single nanoparticle plasmon spectroscopy can be greatly enhanced by enzymatic amplification of the refractive index footprint of individual protein molecules, so-called plasmon-enhanced enzyme-linked immunosorbent assay (ELISA). The technique, which is based on generation of an optically dense precipitate catalyzed by horseradish peroxidase at the metal surface, allowed for colorimetric analysis of ultralow molecular surface coverages with a limit of detection approaching the single molecule limit. However, the plasmonic response induced by a single enzyme can be expected to vary for a number of reasons, including inhomogeneous broadening of the sensing properties of individual particles, variation in electric field enhancement over the surface of a single particle and variation in size and morphology of the enzymatic precipitate. In this report, we discuss how such inhomogeneities affect the possibility to quantify the number of molecules bound to a single nanoparticle. The discussion is based on simulations and measurements of large arrays of well-separated gold nanoparticles fabricated by electron beam lithography (EBL). The new data confirms the intrinsic single-molecule sensitivity of the technique but we were not able to clearly resolve the exact number of adsorbed molecules per single particle. The results indicate that the main sources of uncertainty come from variations in sensitivity across the surface of individual particles and between different particles. There is also a considerable uncertainty in the actual precipitate morphology produced by individual enzyme molecules. Possible routes toward further improvements of the methodology are discussed.

  • 3. Chen, Si
    et al.
    Svedendahl, Mikael
    Duyne, Richard P Van
    Käll, Mikael
    Plasmon-enhanced colorimetric ELISA with single molecule sensitivity.2011In: Nano letters (Print), ISSN 1530-6984, E-ISSN 1530-6992, Vol. 11, no 4Article in journal (Refereed)
    Abstract [en]

    Robust but ultrasensitive biosensors with a capability of detecting low abundance biomarkers could revolutionize clinical diagnostics and enable early detection of cancer, neurological diseases, and infections. We utilized a combination of localized surface plasmon resonance (LSPR) refractive index sensing and the well-known enzyme-linked immunosorbent assay to develop a simple colorimetric biosensing methodology with single molecule sensitivity. The technique is based on spectral imaging of a large number of isolated gold nanoparticles. Each particle binds a variable number of horseradish peroxidase (HRP) enzyme molecules that catalyze a localized precipitation reaction at the particle surface. The enzymatic reaction dramatically amplifies the shift of the LSPR scattering maximum, λ(max), and makes it possible to detect the presence of only one or a few HRP molecules per particle.

  • 4.
    Garcia-Guirado, Jose
    et al.
    Barcelona Inst Sci & Technol, ICFO Inst Ciencies Foton, Barcelona 08860, Spain..
    Svedendahl, Mikael
    KTH, School of Engineering Sciences (SCI), Applied Physics, Quantum and Biophotonics. Barcelona Inst Sci & Technol, ICFO Inst Ciencies Foton, Barcelona 08860, Spain.
    Puigdollers, Joaquim
    Univ Politecn Cataluna, Dept Engn Elect, ES-08034 Barcelona, Spain..
    Quidantt, Romain
    Barcelona Inst Sci & Technol, ICFO Inst Ciencies Foton, Barcelona 08860, Spain.;ICREA, Barcelona 08010, Spain..
    Enantiomer-Selective Molecular Sensing Using Racemic Nanoplasmonic Arrays2018In: Nano letters (Print), ISSN 1530-6984, E-ISSN 1530-6992, Vol. 18, no 10, p. 6279-6285Article in journal (Refereed)
    Abstract [en]

    Building blocks of life show well-defined chiral symmetry which has a direct influence on their properties and role in Nature. Chiral molecules are typically characterized by optical techniques such as circular dichroism (CD) where they exhibit signatures in the ultraviolet frequency region. Plasmonic nanostructures have the potential to enhance the sensitivity of chiral detection and translate the molecular chirality to the visible spectral range. Despite recent progress, to date, it remains unclear which properties plasmonic sensors should exhibit to maximize this effect and apply it to reliable enantiomer discrimination. Here, we bring further insight into this complex problem and present a chiral plasmonic sensor composed of a racemic mixture of gammadions with no intrinsic CD, but high optical chirality and electric field enhancements in the near-fields. Owing to its unique set of properties, this configuration enables us to directly differentiate phenylalanine enantiomers in the visible frequency range.

  • 5. Hakonen, Aron
    et al.
    Rindzevicius, Tomas
    Schmidt, Michael Stenbæk
    Andersson, Per Ola
    Juhlin, Lars
    Svedendahl, Mikael
    Boisen, Anja
    Käll, Mikael
    Detection of nerve gases using surface-enhanced Raman scattering substrates with high droplet adhesion.2016In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 8, no 3Article in journal (Refereed)
    Abstract [en]

    Threats from chemical warfare agents, commonly known as nerve gases, constitute a serious security issue of increasing global concern because of surging terrorist activity worldwide. However, nerve gases are difficult to detect using current analytical tools and outside dedicated laboratories. Here we demonstrate that surface-enhanced Raman scattering (SERS) can be used for sensitive detection of femtomol quantities of two nerve gases, VX and Tabun, using a handheld Raman device and SERS substrates consisting of flexible gold-covered Si nanopillars. The substrate surface exhibits high droplet adhesion and nanopillar clustering due to elasto-capillary forces, resulting in enrichment of target molecules in plasmonic hot-spots with high Raman enhancement. The results may pave the way for strategic life-saving SERS detection of chemical warfare agents in the field.

  • 6. Hakonen, Aron
    et al.
    Svedendahl, Mikael
    Ogier, Robin
    Yang, Zhong-Jian
    Lodewijks, Kristof
    Verre, Ruggero
    Shegai, Timur
    Andersson, Per Ola
    Käll, Mikael
    Dimer-on-mirror SERS substrates with attogram sensitivity fabricated by colloidal lithography.2015In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 7, no 21Article in journal (Refereed)
    Abstract [en]

    Nanoplasmonic substrates with optimized field-enhancement properties are a key component in the continued development of surface-enhanced Raman scattering (SERS) molecular analysis but are challenging to produce inexpensively in large scale. We used a facile and cost-effective bottom-up technique, colloidal hole-mask lithography, to produce macroscopic dimer-on-mirror gold nanostructures. The optimized structures exhibit excellent SERS performance, as exemplified by detection of 2.5 and 50 attograms of BPE, a common SERS probe, using Raman microscopy and a simple handheld device, respectively. The corresponding Raman enhancement factor is of the order 10(11), which compares favourably to previously reported record performance values.

  • 7. Ogier, Robin
    et al.
    Fang, Yurui
    Käll, Mikael
    Svedendahl, Mikael
    Chalmers University of Technology, Sweden.
    Near-Complete Photon Spin Selectivity in a Metasurface of Anisotropic Plasmonic Antennas2015In: Physical Review X, ISSN 2160-3308, E-ISSN 2160-3308, Vol. 5, no 4, article id 041019Article in journal (Refereed)
    Abstract [en]

    Simple chiroptically active metamaterials are difficult to realize in practice but could pave the way for a range of important applications, such as sensitive optical biosensors, asymmetric catalysis, and novel polarization manipulation devices. We show that a metasurface based on a random arrangement of anisotropic but aligned gold nanoparticles can exhibit an almost perfect selectivity towards incident photon spin for evanescent excitation with visible to near-infrared light. The experimentally attained reflection contrast between left- and right-handed circularly polarized light peaks at similar to 90%, in excellent agreement with analytical theory. These results are important for the development of future photonic and plasmonic polarization-based technologies.

  • 8. Ogier, Robin
    et al.
    Shao, Lei
    Svedendahl, Mikael
    Chalmers University of Technology, Sweden.
    Käll, Mikael
    Continuous-Gradient Plasmonic Nanostructures Fabricated by Evaporation on a Partially Exposed Rotating Substrate.2016In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 28, no 23, p. 4658-4664Article in journal (Refereed)
    Abstract [en]

    A continuous-gradient approach of material evaporation is employed to fabricate nanostructures with varying geometric parameters, such as thickness, lateral positioning, and orientation on a single substrate. The method developed for mask lithography allows continuous tuning of the physical properties of a sample. The technique is highly valuable in simplifying the overall optimization process for constructing metasurfaces.

  • 9. Ogier, Robin
    et al.
    Shao, Lei
    Svedendahl, Mikael
    Käll, Mikael
    Metasurfaces: Continuous-Gradient Plasmonic Nanostructures Fabricated by Evaporation on a Partially Exposed Rotating Substrate (Adv. Mater. 23/2016).2016In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 28, no 23Article in journal (Refereed)
    Abstract [en]

    A continuous-gradient approach of material evaporation is employed by L. Shao, M. Käll, and co-workers to fabricate nanostructures with varying geometric parameters such as thickness, lateral positioning, and orientation on a single substrate. This method for mask lithography, described on page 4658, allows continuous tuning of the physical properties of a sample. The technique is highly valuable in simplifying the overall optimization process for constructing metasurfaces.

  • 10.
    Svedendahl, Mikael
    et al.
    Chalmers University of Technology, Sweden.
    Chen, Si
    Dmitriev, Alexandre
    Käll, Mikael
    Refractometric sensing using propagating versus localized surface plasmons: a direct comparison2009In: Nano letters (Print), ISSN 1530-6984, E-ISSN 1530-6992, Vol. 9, no 12, p. 4428-4433Article in journal (Refereed)
    Abstract [en]

    We present a direct experimental comparison between the refractive index sensing capabilities of localized surface plasmon resonances (LSPRs) in gold nanodisks and propagating surface plasmon resonances (SPRs) on 50 nm gold films. The comparison is made using identical experimental conditions, and for the same resonance wavelength, lambda(SP) congruent with 700 nm. Biosensing experiments with biotin-avidin coupling reveal that the two sensing platforms have very similar performance, despite a superior bulk refractive index sensing figure of merit for the SPR sensor. The results demonstrate that LSPR sensing based on simple transmission or reflection measurements is a highly competitive technique compared to the traditional SPR sensor.

  • 11.
    Svedendahl, Mikael
    et al.
    Chalmers University of Technology, Sweden.
    Johansson, Peter
    Käll, Mikael
    Complete light annihilation in an ultrathin layer of gold nanoparticles.2013In: Nano letters (Print), ISSN 1530-6984, E-ISSN 1530-6992, Vol. 13, no 7, p. 3053-3058Article in journal (Refereed)
    Abstract [en]

    We experimentally demonstrate that an incident light beam can be completely annihilated in a single layer of randomly distributed, widely spaced gold nanoparticle antennas. Under certain conditions, each antenna dissipates more than 10 times the number of photons that enter its geometric cross-sectional area. The underlying physics can be understood in terms of a critical coupling to localized plasmons in the nanoparticles or, equivalently, in terms of destructive optical Fano interference and so-called coherent absorption.

  • 12.
    Svedendahl, Mikael
    et al.
    Chalmers University of Technology, Sweden.
    Käll, Mikael
    Fano interference between localized plasmons and interface reflections2012In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 6, no 8, p. 7533-7539Article in journal (Refereed)
    Abstract [en]

    Layers of subwavelength metal nanostructures that support localized surface plasmon resonances are of broad interest in applied nanotechnology, for example, in optical sensor development and solar energy harvesting devices. We measured specular reflection spectra as a function of incidence angle for two-dimensional layers of gold nanodisks on glass and found highly asymmetric line-shapes and a spectral red-shift of up to 0.2 eV, or 10% of the plasmon resonance energy, as the angle changed from normal toward grazing incidence. This dramatic angular dispersion is the result of a tunable Fano interference between the spectrally narrow plasmon emission and a "white" continuum caused by the interface reflection. The data are found to be in excellent agreement with predictions based on a theory for Fresnel reflection coefficients of an interface with subwavelength inclusions. The theory can also be used to derive analytical expressions for the Fano parameters.

  • 13.
    Svedendahl, Mikael
    et al.
    Chalmers University of Technology, Sweden.
    Verre, Ruggero
    Käll, Mikael
    Refractometric biosensing based on optical phase flips in sparse and short-range-ordered nanoplasmonic layers2014In: Light: Science & Applications, ISSN 2095-5545, E-ISSN 2047-7538, ISSN ´, Vol. 3, article id e220Article in journal (Refereed)
    Abstract [en]

    Noble metal nanoparticles support localized surface plasmon resonances (LSPRs) that are extremely sensitive to the local dielectric properties of the environment within distances up to 10-100[emsp14]nm from the metal surface. The significant overlap between the sensing volume of the nanoparticles and the size of biological macromolecules has made LSPR biosensing a key field for the application of plasmonics. Recent advancements in evaluating plasmonic refractometric sensors have suggested that the phase detection of light can surpass the sensitivity of standard intensity-based detection techniques. Here, we experimentally confirm that the phase of light can be used to precisely track local refractive index changes induced by biomolecular reactions, even for dilute and layers of short-range-ordered plasmonic nanoparticles. In particular, we demonstrate that the sensitivity can be enhanced by tuning in to a zero reflection condition, in which an abrupt phase flip of the reflected light is achieved. Using a cost-effective interference fringe tracking technique, we demonstrate that phase measurements yield an approximately one order of magnitude larger relative shift compared with traditional LSPR measurements for the model system of NeutrAvidin binding to biotinylated nanodisks.

  • 14. Verre, R
    et al.
    Maccaferri, N
    Fleischer, K
    Svedendahl, Mikael
    Chalmers University of Technology, Sweden.
    Odebo Länk, N.
    Dmitriev, A.
    Vavassori, P.
    Shvets, I. V.
    Käll, M.
    Polarization conversion-based molecular sensing using anisotropic plasmonic metasurfaces2016In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 8, no 20, p. 10576-10581Article in journal (Refereed)
    Abstract [en]

    Anisotropic media induce changes in the polarization state of transmitted and reflected light. Here we combine this effect with the refractive index sensitivity typical of plasmonic nanoparticles to experimentally demonstrate self-referenced single wavelength refractometric sensing based on polarization conversion. We fabricated anisotropic plasmonic metasurfaces composed of gold dimers and, as a proof of principle, measured the changes in the rotation of light polarization induced by biomolecular adsorption with a surface sensitivity of 0.2 ng cm(-2). We demonstrate the possibility of miniaturized sensing and we show that experimental results can be reproduced by analytical theory. Various ways to increase the sensitivity and applicability of the sensing scheme are discussed.

  • 15. Verre, R.
    et al.
    Svedendahl, Mikael
    Chalmers University of Technology, Sweden.
    Odebo Länk, N.
    Yang, Z. J.
    Zengin, G.
    Antosiewicz, T. J.
    Käll, M.
    Directional Light Extinction and Emission in a Metasurface of Tilted Plasmonic Nanopillars.2016In: Nano letters (Print), ISSN 1530-6984, E-ISSN 1530-6992, Vol. 16, no 1, p. 98-104Article in journal (Refereed)
    Abstract [en]

    Plasmonic optical antennas and metamaterials with an ability to boost light-matter interactions for particular incidence or emission angles could find widespread use in solar harvesting, biophotonics, and in improving photon source performance at optical frequencies. However, directional plasmonic structures have generally large footprints or require complicated geometries and costly nanofabrication technologies. Here, we present a directional metasurface realized by breaking the out-of-plane symmetry of its individual elements: tilted subwavelength plasmonic gold nanopillars. Directionality is caused by the complex charge oscillation induced in each individual nanopillar, which essentially acts as a tilted dipole above a dielectric interface. The metasurface is homogeneous over a macroscopic area and it is fabricated by a combination of facile colloidal lithography and off-normal metal deposition. Fluorescence excitation and emission from dye molecules deposited on the metasurface is enhanced in specific directions determined by the tilt angle of the nanopillars. We envisage that these directional metasurfaces can be used as cost-effective substrates for surface-enhanced spectroscopies and a variety of nanophotonic applications.

  • 16. Verre, Ruggero
    et al.
    Antosiewicz, Tomasz .
    Svedendahl, Mikael
    Chalmers University of Technology, Sweden.
    Lodewijks, Kristof
    Shegai, Timur
    Käll, Mikael
    Quasi-isotropic surface plasmon polariton generation through near-field coupling to a penrose pattern of silver nanoparticles2014In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 8, no 9, p. 9286-9294Article in journal (Refereed)
    Abstract [en]

    Quasicrystals are structures that possess long-range order without being periodic. We investigate the unique characteristics of a photonic quasicrystal that consists of plasmonic Ag nanodisks arranged in a Penrose pattern. The quasicrystal scatters light in a complex but spectacular diffraction pattern that can be directly imaged in the back focal plane of an optical microscope, allowing us to assess the excitation efficiency of the various diffraction modes. Furthermore, surface plasmon polaritons can be launched almost isotropically through near-field grating coupling when the quasicrystal is positioned close to a homogeneous silver surface. We characterize the dispersion relation of the different excited plasmon modes by reflection measurements and simulations. It is demonstrated that the quasicrystal in-coupling efficiency is strongly enhanced compared to a nanoparticle array with the same particle density but only short-range lateral order. We envision that the system can be useful for a number of advanced light harvesting and optoelectronic applications.

  • 17. Virk, Mudassar
    et al.
    Xiong, Kunli
    Svedendahl, Mikael
    Chalmers University of Technology, Sweden.
    Käll, Mikael
    Dahlin, Andreas B.
    A thermal plasmonic sensor platform: resistive heating of nanohole arrays.2014In: Nano letters (Print), ISSN 1530-6984, E-ISSN 1530-6992, Vol. 14, no 6, p. 3544-3549Article in journal (Refereed)
    Abstract [en]

    We have created a simple and efficient thermal plasmonic sensor platform by letting a DC current heat plasmonic nanohole arrays. The sensor can be used to determine thermodynamic parameters in addition to monitoring molecular reactions in real-time. As an application example, we use the thermal sensor to determine the kinetics and activation energy for desorption of thiol monolayers on gold. Further, the temperature of the metal can be measured optically by the spectral shift of the bonding surface plasmon mode (0.015 nm/K). We show that this resonance shift is caused by thermal lattice expansion, which reduces the plasma frequency of the metal. The sensor is also used to determine the thin film thermal expansion coefficient through a theoretical model for the expected resonance shift.

  • 18. Wersäll, Martin
    et al.
    Verre, Ruggero
    Svedendahl, Mikael
    Chalmers University of Technology, Sweden.
    Johansson, Peter
    Käll, Mikael
    Shegai, Timur
    Directional Nanoplasmonic Antennas for Self-Referenced Refractometric Molecular Analysis2014In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 118, no 36, p. 21075-21080Article in journal (Refereed)
    Abstract [en]

    Localized surface-plasmon resonance (LSPR) sensors are typically based on tracing resonance peak shifts that precisely follow changes in the local refractive index. Such measurements usually require a spectrometer, a stable light source, and an accurate LSPR position tracing technique. As a simple but efficient alternative, we investigated a self-referenced single-wavelength sensing scheme based on angle-dependent and highly directional radiation patterns originating from a monolayer of asymmetric gold nanodimers. We found that one could easily trace a model biotinneutravidin recognition reaction as well as minute bulk refractive index changes, by measuring the intensity ratio between the light scattered in two different directions with respect to the dimers. The refractometric resolution of the methodology was estimated to be on the order of Delta n approximate to 10(-5) RIU. These results may be particularly useful for label-free biosensing applications that require a combination of simple and cost-effective optical readout with a reasonable sensitivity.

  • 19. Yavas, O.
    et al.
    Svedendahl, Mikael
    KTH, School of Engineering Sciences (SCI), Applied Physics. ICFO - Institut de Ciències Fotòniques, Barcelona Institute of Science and Technology, Castelldefels Barcelona, 08860, Spain.
    Quidant, R.
    Unravelling the Role of Electric and Magnetic Dipoles in Biosensing with Si Nanoresonators2019In: ACS Nano, ISSN 1936-0851, E-ISSN 1936-086X, Vol. 13, no 4, p. 4582-4588Article in journal (Refereed)
    Abstract [en]

    High refractive index dielectric nanoresonators are attracting much attention due to their ability to control both electric and magnetic components of light. Due to the combination of confined modes with reduced absorption losses, they have recently been proposed as an alternative to nanoplasmonic biosensors. In this context, we study the use of semirandom silicon nanocylinder arrays, fabricated with simple and scalable colloidal lithography for the efficient and reliable detection of biomolecules in biological samples. Interestingly, electric and magnetic dipole resonances are associated with two different transduction mechanisms: extinction decrease and resonance red shift. By contrasting both observables, we identify clear advantages in tracking changes in the extinction magnitude. Our data demonstrate that, despite its simplicity, the proposed platform is able to detect prostate-specific antigen in human serum with limits of detection meeting clinical needs.

  • 20. Yavas, Ozlem
    et al.
    Svedendahl, Mikael
    Barcelona Institute of Science and Technology, Spain.
    Dobosz, Paulina
    Sanz, Vanesa
    Quidant, Romain
    On-a-chip Biosensing Based on All-Dielectric Nanoresonators2017In: Nano letters (Print), ISSN 1530-6984, E-ISSN 1530-6992, Vol. 17, no 7, p. 4421-4426Article in journal (Refereed)
    Abstract [en]

    Nanophotonics has become a key enabling technology in biomedicine with great promises in early diagnosis and less invasive therapies. In this context, the unique capability of plasmonic noble metal nanoparticles to concentrate light on the nanometer scale has widely contributed to biosensing and enhanced spectroscopy. Recently, high-refractive index dielectric nanostructures featuring low loss resonances have been proposed as a promising alternative to nanoplasmonics, potentially offering better sensing performances along with full compatibility with the microelectronics industry. In this letter we report the fitst demonstration of biosensing with silicon nanoresonators integrated in state-of-the-art microfluidics. Our lab-on-a-chip platform enables detecting Prostate Specific Antigen (PSA) cancer marker in human serum with a sensitivity that meefs clinical needs. These performances are directly compared with its plasmonic counterpart based on gold nanorods. Our work opens new opportunities in the development of future point-of-care devices toward a more personalized healthcare.

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