Role of Symmetry Breaking in Observing Strong Molecule-Cavity Coupling Using Dielectric Microspheres

This is the final version. Available from the American Chemical Society via the DOI in this record. The emergence of dielectric open optical cavities has opened a new research avenue in nanophotonics. In particular, dielectric microspheres support a rich set of cavity modes with varying spectral characteristics, making them an ideal platform to study molecule-cavity interactions. The symmetry of the structure plays a critical role in the outcoupling of these modes and, hence, the perceived molecule-cavity coupling strength. Here, we experimentally and theoretically study molecule-cavity coupling mediated by the Mie scattering modes of a dielectric microsphere placed on a glass substrate and excited with far-field illumination, from which we collect scattering signatures both in the air and glass sides. Glass-side collection reveals clear signatures of strong molecule-cavity coupling (coupling strength 2g = 74 meV), in contrast to the air-side scattering signal. Rigorous electromagnetic modeling allows us to understand molecule-cavity coupling and unravel the role played by the spatial mode profile in the observed coupling strength.European Research Council (ERC)European Research Council (ERC)Spanish MICINNSpanish MICINNCatalan CERCA ProgramFundaciós Cellex and Mir-Pui

Intrinsic Plasmon-Phonon Interactions in Highly Doped Graphene: A Near-Field Imaging Study.

Author's accepted versionFinal version available from ACS via the DOI in this recordAs a two-dimensional semimetal, graphene offers clear advantages for plasmonic applications over conventional metals, such as stronger optical field confinement, in situ tunability, and relatively low intrinsic losses. However, the operational frequencies at which plasmons can be excited in graphene are limited by the Fermi energy EF, which in practice can be controlled electrostatically only up to a few tenths of an electronvolt. Higher Fermi energies open the door to novel plasmonic devices with unprecedented capabilities, particularly at mid-infrared and shorter-wave infrared frequencies. In addition, this grants us a better understanding of the interaction physics of intrinsic graphene phonons with graphene plasmons. Here, we present FeCl3-intercalated graphene as a new plasmonic material with high stability under environmental conditions and carrier concentrations corresponding to EF > 1 eV. Near-field imaging of this highly doped form of graphene allows us to characterize plasmons, including their corresponding lifetimes, over a broad frequency range. For bilayer graphene, in contrast to the monolayer system, a phonon-induced dipole moment results in increased plasmon damping around the intrinsic phonon frequency. Strong coupling between intrinsic graphene phonons and plasmons is found, supported by ab initio calculations of the coupling strength, which are in good agreement with the experimental data.FJGA and PA-G acknowledge support from the Spanish Ministry of Economy and Competitiveness through the national programs MAT2014-59096-P and FIS2014-60195-JIN, respectively. MFC and SR acknowledge support from EPSRC (Grant no. EP/J000396/1, 281 EP/K017160/1, EP/K010050/1, EPG036101/1, EP/M001024/1, EPM- 002438/1), from Royal Society International Exchanges Scheme 2012/R3 and 2013/R2 and from European Commission (FP7-ICT-2013-613024-GRASP). SD, DNB and MF acknowledge support of ONR N00014-15-1-2671. DNB is the Moore Investigator in Quantum Materials funded by the Gordon and Betty Moore Foundation’s EPiQS Initiative through Grant GBMF4533

Risk of upper gastrointestinal bleeding and perforation associated with low-dose aspirin as plain and enteric-coated formulations

BACKGROUND: The use of low-dose aspirin has been reported to be associated with an increased risk of upper gastrointestinal complications (UGIC). The coating of aspirin has been proposed as an approach to reduce such a risk. To test this hypothesis, we carried out a population based case-control study. METHODS: We identified incident cases of UGIC (bleeding or perforation) aged 40 to 79 years between April 1993 to October 1998 registered in the General Practice Research Database. Controls were selected randomly from the source population. Adjusted estimates of relative risk (RR) associated with current use of aspirin as compared to non use were computed using unconditional logistic regression. RESULTS: We identified 2,105 cases of UGIC and selected 11,500 controls. Among them, 287 (13.6%) cases and 837 (7.3%) controls were exposed to aspirin, resulting in an adjusted RR of 2.0 (1.7-2.3). No clear dose-effect was found within the range of 75-300 mg. The RR associated with enteric-coated formulations (2.3, 1.6-3.2) was similar to the one of plain aspirin (1.9, 1.6-2.3), and no difference was observed depending on the site. The first two months of treatment was the period of greater risk (RR= 4.5, 2.9-7.1). The concomitant use of aspirin with high-dose NSAIDs greatly increased the risk of UGIC (13.3, 8.5-20.9) while no interaction was apparent with low-medium doses (2.2, 1.0-4.6). CONCLUSIONS: Low-dose aspirin increases by twofold the risk of UGIC in the general population and its coating does not modify the effect. Concomitant use of low-dose aspirin and NSAIDs at high doses put patients at a specially high risk of UGIC

Extraordinary absorption of sound in porous lamella-crystals

We present the design of a structured material supporting complete absorption of sound with a broadband response and functional for any direction of incident radiation. The structure which is fabricated out of porous lamellas is arranged into a low-density crystal and backed by a reflecting support. Experimental measurements show that strong all-angle sound absorption with almost zero reflectance takes place for a frequency range exceeding two octaves. We demonstrate that lowering the crystal filling fraction increases the wave interaction time and is responsible for the enhancement of intrinsic material dissipation, making the system more absorptive with less material.The work was supported by the Spanish Ministry of Science and Innovation and European Union FEDER through project FIS2011-29734-C02-01. J.C. gratefully acknowledges financial support from the Danish Council for Independent Research and a Sapere Aude grant (12-134776). V. R. G. gratefully acknowledges financial support from the ''Contratos Post-Doctorales Campus Excelencia Internacional'' UPV CEI-01-11.Christensen, J.; Romero García, V.; Picó Vila, R.; Cebrecos Ruiz, A.; Garcia De Abajo, FJ.; Mortensen, NA.; Willatzen, M.... (2014). Extraordinary absorption of sound in porous lamella-crystals. Scientific Reports. 4(4674). https://doi.org/10.1038/srep04674S44674Mei, J. et al. Dark acoustic metamaterials as super absorbers for low-frequency sound. Nat. Commun. 3, 756 (2012).Leroy, V., Strybulevych, A., Scanlon, M. G. & Page, J. Transmission of ultrasound through a single layer of bubbles. Eur. Phys. J. E 29, 123 (2009).Leroy, V., Bretagne, A., Fink, M. H. W., Tabeling, P. & Tourin, A. Design and characterization of bubble phononic crystals. Appl. Phys. Lett. 95, 171904 (2009).Thomas, E. L. Applied physics: Bubbly but quiet. Nature 462, 990 (2009).Romero-García, V., Sánchez-Pérez, J. V. & Garcia-Raffi, L. M. Tunable wideband bandstop acoustic filter based on two-dimensional multiphysical phenomena periodic systems. J. Appl. Phys. 110, 014904 (2011).Garcia-Chocano, V. M., Cabrera, S. & Sanchez-Dehesa, J. Broadband sound absorption by lattices of microperforated cylindrical shells. Appl. Phys. Lett. 101, 184101 (2012).Kushwaha, M. S., Halevi, P., Dobrzynski, L. & Djafari-Rouhani, B. Acoustic band structure of periodic elastic composites. Phys. Rev. Lett. 71, 2022 (1993).Vasseur, J. O. et al. Experimental and Theoretical Evidence for the Existence of Absolute Acoustic Band Gaps in Two-Dimensional Solid Phononic Crystals. Phys. Rev. Lett. 86, 3012 (2001).Liu, Z. et al. Locally Resonant Sonic Materials. Science 289, 1734 (2000).Christensen, J., Martin-Moreno, L. & Garcia-Vidal, F. J. All-angle blockage of sound by an acoustic double-fishnet metamaterial. Appl. Phys. Lett. 97, 134106 (2010).Botten, L. C., Craig, M. S., McPhedran, R. C., Adams, J. L. & Andrewartha, J. R. The finitely conducting lamellar diffraction grating. Optica Acta 28, 1087 (1981).McPhedran, R. C., Botten, L. C., Craif, M. S., Neviere, M. & Maystre, D. Lossy lamellar gratings in the quasistatic limit. Optica Acta 29, 289 (1982).Kravets, V. G., Schedin, F. & Grigorenko, A. N. Plasmonic blackbody: Almost complete absorption of light in nanostructured metallic coatings. Phys. Rev. B 78, 205405 (2008).Sondergaard, T. et al. Plasmonic black gold by adiabatic nanofocusing and absorption of light in ultra-sharp convex grooves. Nat. Commun. 3, 969 (2012).Clapham, P. B. & Hurtley, M. C. Reduction of Lens Reflexion by the Moth Eye Principle. Nature Vol. 244, 281 (1973).Garcia-Vidal, F. J., Pitarke, J. M. & Pendry, J. B. Effective Medium Theory of the Optical Properties of Aligned Carbon Nanotubes. Phys. Rev. Lett. 78, 4289 (1997).Yang, Z., Ci, L., Bur, J. A., Lin, S. & Ajayan, P. M. Experimental Observation of an Extremely Dark Material Made By a Low-Density Nanotube Array. Nano Lett. 8, 446 (2008).Garcia-Vidal, F. J. Metamaterials: Towards the dark side. Nat. Photonics 2, 215 (2008).Mizunoa, K. et al. A black body absorber from vertically aligned single-walled carbon nanotubes. Proc. Natl. Acad. Sci. USA 106, 6044 (2009).Lidorkis, E. & Ferrari, A. C. Photonics with Multiwall Carbon Nanotube Arrays. ACS Nano 3, 1238 (2009).Beenakker, C. W. J. & Brouwer, P. W. Distribution of the reflection eigenvalues of a weakly absorbing chaotic cavity. Physica E 9, 463 (2001).Lafarge, D., Lemarinier, P., Allard, J. F. & Tarnow, V. Dynamic compressibility of air in porous structures at audible frequencies. J. Acoust. Soc. Am. 102, 1995 (1997), With the macroscopic parameters: ϕ = 0.94, α∞ = 1, σ = 20000 Nm−4s and Λ = Λ′ = 0.41 μm.García de Abajo, F. J. Colloquium: Light scattering by particle and hole arrays. Rev. Mod. Phys. 79, 1267–1290 (2007)

Broadband metamaterial for nonresonant matching of acoustic waves

Unity transmittance at an interface between bulk media is quite common for polarized electromagnetic waves incident at the Brewster angle, but it is rarely observed for sound waves at any angle of incidence. In the following, we theoretically and experimentally demonstrate an acoustic metamaterial possessing a Brewster-like angle that is completely transparent to sound waves over an ultra-broadband frequency range with >100% bandwidth. The metamaterial, consisting of a hard metal with subwavelength apertures, provides a surface impedance matching mechanism that can be arbitrarily tailored to specific media. The nonresonant nature of the impedance matching effectively decouples the front and back surfaces of the metamaterial allowing one to independently tailor the acoustic impedance at each interface. On the contrary, traditional methods for acoustic impedance matching, for example in medical imaging, rely on resonant tunneling through a thin antireflection layer, which is inherently narrowband and angle specific

Maximal Spontaneous Photon Emission and Energy Loss from Free Electrons

Free electron radiation such as Cerenkov, Smith--Purcell, and transition radiation can be greatly affected by structured optical environments, as has been demonstrated in a variety of polaritonic, photonic-crystal, and metamaterial systems. However, the amount of radiation that can ultimately be extracted from free electrons near an arbitrary material structure has remained elusive. Here we derive a fundamental upper limit to the spontaneous photon emission and energy loss of free electrons, regardless of geometry, which illuminates the effects of material properties and electron velocities. We obtain experimental evidence for our theory with quantitative measurements of Smith--Purcell radiation. Our framework allows us to make two predictions. One is a new regime of radiation operation---at subwavelength separations, slower (nonrelativistic) electrons can achieve stronger radiation than fast (relativistic) electrons. The second is a divergence of the emission probability in the limit of lossless materials. We further reveal that such divergences can be approached by coupling free electrons to photonic bound states in the continuum (BICs). Our findings suggest that compact and efficient free-electron radiation sources from microwaves to the soft X-ray regime may be achievable without requiring ultrahigh accelerating voltages.Comment: 7 pages, 4 figure

Metal nanoparticles for microscopy and spectroscopy

Metal nanoparticles interact strongly with light due to a resonant response of their free electrons. These ‘plasmon’ resonances appear as very strong extinction and scattering for particular wavelengths, and result in high enhancements of the local field compared to the incident electric field. In this chapter we introduce the reader to the optical properties of single plasmon particles as well as finite clusters and periodic lattices, and discuss several applications

Quantum surface-response of metals revealed by acoustic graphene plasmons

A quantitative understanding of the electromagnetic response of materials is essential for the precise engineering of maximal, versatile, and controllable light-matter interactions. Material surfaces, in particular, are prominent platforms for enhancing electromagnetic interactions and for tailoring chemical processes. However, at the deep nanoscale, the electromagnetic response of electron systems is significantly impacted by quantum surface-response at material interfaces, which is challenging to probe using standard optical techniques. Here, we show how ultraconfined acoustic graphene plasmons in graphene-dielectric-metal structures can be used to probe the quantum surface-response functions of nearby metals, here encoded through the so-called Feibelman d-parameters. Based on our theoretical formalism, we introduce a concrete proposal for experimentally inferring the low-frequency quantum response of metals from quantum shifts of the acoustic graphene plasmons dispersion, and demonstrate that the high field confinement of acoustic graphene plasmons can resolve intrinsically quantum mechanical electronic length-scales with subnanometer resolution. Our findings reveal a promising scheme to probe the quantum response of metals, and further suggest the utilization of acoustic graphene plasmons as plasmon rulers with angstrom-scale accuracy. Knowledge of the quantum response of materials is essential for designing light-matter interactions at the nanoscale. Here, the authors report a theory for understanding the impact of metallic quantum response on acoustic graphene plasmons and how such response could be inferred from measurements.N.A.M. is a VILLUM Investigator supported by VILLUM FONDEN (Grant No. 16498) and Independent Research Fund Denmark (Grant No. 7026-00117B). The Center for Nano Optics is financially supported by the University of Southern Denmark (SDU 2020 funding). The Center for Nanostructured Graphene (CNG) is sponsored by the Danish National Research Foundation (Project No. DNRF103). This work was partly supported by the Army Research Office through the Institute for Soldier Nanotechnologies under Contract No. W911NF-18-2-0048. N.M.R.P. acknowledges support from the European Commission through the project "Graphene-Driven Revolutions in ICT and Beyond" (No. 881603, Core 3), COMPETE 2020, PORTUGAL 2020, FEDER and the Portuguese Foundation for Science and Technology (FCT) through project POCI-01-0145-FEDER028114 and through the framework of the Strategic Financing UID/FIS/04650/2019. F.H. L.K. acknowledges financial support from the Government of Catalonia through the SGR grant and from the Spanish Ministry of Economy and Competitiveness (MINECO) through the Severo Ochoa Programme for Centres of Excellence in R&D (SEV-20150522), support by Fundacio Cellex Barcelona, Generalitat de Catalunya through the CERCA program, and the MINECO grants Plan Nacional (FIS2016-81044-P) and the Agency for Management of University and Research Grants (AGAUR) 2017 SGR 1656. Furthermore, the research leading to these results has received funding from the European Union's Horizon 2020 program under the Graphene Flagship Grant Agreements No. 785219 (Core 2) and no. 881603 (Core 3), and the Quantum Flagship Grant No. 820378. This work was also supported by the ERC TOPONANOP (Grant No. 726001)

Absorption Enhancement in Peridinin–Chlorophyll–Protein Light-Harvesting Complexes Coupled to Semicontinuous Silver Film

We report on experimental and theoretical studies of plasmon-induced effects in a hybrid nanostructure composed of light-harvesting complexes and metallic nanoparticles in the form of semicontinuous silver film. The results of continuous-wave and time-resolved spectroscopy indicate that absorption of the light-harvesting complexes is strongly enhanced upon coupling with the metallic film spaced by 25 nm of a dielectric silica layer. This conclusion is corroborated by modeling, which confirms the morphology of the silver island film

Perfect imaging, epsilon-near zero phenomena and waveguiding in the scope of nonlocal effects.

7 pags, 4 figsPlasmons in metals can oscillate on a sub-wavelength length scale and this large-k response constitutes an inherent prerequisite for fascinating effects such as perfect imaging and intriguing wave phenomena associated with the epsilon-near-zero (ENZ) regime. While there is no upper cut-off within the local-response approximation (LRA) of the plasma polarization, nonlocal dynamics suppress response beyond ω/v F, where v F is the Fermi velocity of the electron gas. Nonlocal response has previously been found to pose limitations to field-enhancement phenomena. Accounting for nonlocal hydrodynamic response, we show that perfect imaging is surprisingly only marginally affected by nonlocal properties of a metal slab, even for a deep subwavelength case and an extremely thin film. Similarly, for the ENZ response we find no indications of nonlocal response jeopardizing the basic behaviors anticipated from the LRA. Finally, our study of waveguiding of gap plasmons even shows a positive nonlocal influence on the propagation length. © 2013 Macmillan Publishers Limited. All rights reserved.C. D. acknowledges a FPU fellowship by the Spanish Ministerio de Educación. J. C. gratefully acknowledges financial support from the Danish Council for Independent Research and a Sapere Aude grant (12-134776). The Center for Nanostructured Graphene is sponsored by the Danish National Research Foundation, Project DNRF58