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We investigate the potential of surface plasmon polaritons at noble metal interfaces for surface-enhanced chiroptical sensing of dilute chiral drug solutions. The high quality factor of surface plasmon resonances in both Otto and Kretschmann configurations enables the enhancement of circular dichroism differenatial absorption thanks to the large near-field intensity of such plasmonic excitations. Furthermore, the subwavelength confinement of surface plasmon polaritons is key to attain chiroptical sensitivity to small amounts of drug volumes placed around $\simeq 100$ nm by the metal surface. Our calculations focus on reparixin, a pharmaceutical molecule currently used in clinical studies for patients with community-acquired pneumonia, including COVID-19 and acute respiratory distress syndrome. Considering realistic dilute solutions of reparixin dissolved in water with concentration $\leq 5$ mg$/$ml, we find a circular-dichroism differential absorption enhancement factor of the order $\simeq 20$ and chirality-induced polarization distortion upon surface plasmon polariton excitation.

High-index dielectric subwavelength structures and metasurfaces are capable of enhancing light-matter interaction by orders of magnitude via geometry-dependent optical resonances. This enhancement, however, comes with a fundamental limitation of a narrow spectral range of operation in the vicinity of one or few resonant frequencies. Here we tackle this limitation and introduce an innovative and practical approach to achieve spectrally tunable enhancement of light-matter interaction with resonant metasurfaces. We design and fabricate {\it resonance-gradient metasurfaces} with varying geometrical parameters that translate into resonant frequencies dependence on one of the coordinates of the metasurface. The metasurfaces are composed of bone-like nanoresonators which are made of germanium, and they support high-$Q$ optical resonances in the mid-IR spectral range. We apply this general concept to observe the resonant enhancement of the $3^{\text{rd}}$ and $5^{\text{th}}$ harmonics generated from the gradient metasurfaces being used in conjunction with a tunable excitation laser to provide a wide spectral coverage of resonantly-enhanced tunable generation of multiple optical harmonics., Comment: Main text: 17 pages and 5 figures. Supplementary Information: 5 pages and 2 figures. Conference presentation link: https://doi.org/10.1364/CLEO_FS.2023.FTh4D.7

Most present-day resonant systems, throughout physics and engineering, are characterized by a strict time-reversal symmetry between the rates of energy coupled in and out of the system, which leads to a trade-off between how long a wave can be stored in the system and the system bandwidth. Any attempt to reduce the losses of the resonant system, and hence store a (mechanical, acoustic, electronic, optical, atomic, or of any other nature) wave for more time, will inevitably also reduce the bandwidth of the system. Until recently, this time-bandwidth limit has been considered fundamental, arising from basic Fourier reciprocity. A recent theory suggested that it might in fact be overcome by breaking Lorentz reciprocity in the resonant system, reinvigorated a debate about whether (or not) this was indeed the case. Here, we report an experimental realization of a cavity where, inducing nonreciprocity by breaking the time invariance, we do overcome the fundamental time-bandwidth limit of ordinary resonant systems by a factor of 30, in full agreement with accompanying numerical simulations. We show that, although in practice experimental constraints limit our scheme, the time bandwidth product can be arbitrarily large, simply dictated by the finesse of the cavity. Our experimental realization uses a simple macroscopic, time-variant, fiber-optic cavity, where we break Lorentz reciprocity by non-adiabatically opening the cavity, injecting a pulse of large bandwidth, and then closing the cavity, storing the pulse which can be released on-demand at a later time. Our results open the path for designing resonant systems, ubiquitous in physics and engineering, that can simultaneously be broadband (i.e., ultrafast) and possessing long storage times, thereby unleashing fundamentally new functionalities in wave physics and wave-matter interactions.

Interactions between localized plasmons in proximal nanostructures is a well-studied phenomenon. Here we explore plasmon plasmon interactions in connected extended systems. Such systems can now be easily produced using graphene. Specifically we employ the finite element method to study such interactions in graphene nanoribbon arrays with a periodically modulated electrochemical potential or number of layers. We find a rich variation in the resulting plasmonic resonances depending on the dimensions and the electrochemical potentials (doping) of the nanoribbon segments and the involvement of transverse and longitudinal plasmon interactions. Unlike predictions based of the well-known "orbital hybridization model", the energies of the resulting hybrid plasmonic resonances of the extended system can lie between the energies of the plasmons of the individual components. The results demonstrate the wide range tunability of the graphene plasmons and can help to design structures with desired spectra, which can be used to enhance optical fields in the infrared region of the electromagnetic spectrum., Comment: 20 pages, 6 figures, 5 supplementary figures

Infrared spectroscopy is the technique of choice for chemical identification of biomolecules through their vibrational fingerprints. However, infrared light interacts poorly with nanometric size molecules. Here, we exploit the unique electro-optical properties of graphene to demonstrate a high-sensitivity tunable plasmonic biosensor for chemically-specific label-free detection of protein monolayers. The plasmon resonance of nanostructured graphene is dynamically tuned to selectively probe the protein at different frequencies and extract its complex refractive index. Additionally, the extreme spatial light confinement in graphene, up to two orders of magnitude higher than in metals, produces an unprecedentedly high overlap with nanometric biomolecules, enabling superior sensitivity in the detection of their refractive index and vibrational fingerprints. The combination of tunable spectral selectivity and enhanced sensitivity of graphene opens exciting prospects for biosensing., Comment: Supplementary Information included. 14 pages, 6 figures

The functionalities of a wide range of optical and opto-electronic devices are based on resonance effects and active tuning of the amplitude and wavelength response is often essential. Plasmonic nanostructures are an efficient way to create optical resonances, a prominent example is the extraordinary optical transmission (EOT) through arrays of nanoholes patterned in a metallic film. Tuning of resonances by heating, applying electrical or optical signals has proven to be more elusive, due to the lack of materials that can induce modulation over a broad spectral range and/or at high speeds. Here we show that nanopatterned metals combined with phase change materials (PCMs) can overcome this limitation due to the large change in optical constants which can be induced thermally or on an ultrafast timescale. We demonstrate resonance wavelength shifts as large as 385 nm - an order of magnitude higher than previously reported - by combining properly designed Au EOT nanostructures with Ge2Sb2Te5 (GST). Moreover, we show, through pump probe measurements, repeatable and reversible, large amplitude modulations in the resonances, especially at telecommunication wavelengths, over ps time scales and at powers far below those needed to produce a permanent phase transition. Our findings open a pathway to the design of hybrid metal PCM nanostructures with ultrafast and widely tuneable resonance responses, which hold potential impact on active nanophotonic devices such as tuneable optical filters, smart windows, biosensors and reconfigurable memories.

We report on the mid-infrared nonlinear photothermal spectrum of the neat liquid crystal 4-Octyl-4'-Cyanobiphenyl (8CB) using a tunable Quantum Cascade Laser (QCL). The nonequilibrium steady state characterized by the nonlinear photothermal infrared response undergoes a supercritical pitchfork bifurcation. The bifurcation, observed in heterodyne two-color pump-probe detection, leads to ultrasharp nonlinear infrared spectra similar to those reported in the visible region. A systematic study of the peak splitting as function of absorbed infrared power shows the bifurcation has a critical exponent of 0.5. The surprising observation of an apparently universal critical exponent in a nonequilibrium state is explained using a simple model reminiscent of mean field theory. Apart from the intrinsic interest for nonequilibrium studies, nonlinear photothermal methods lead to a dramatic narrowing of spectral lines, giving rise to a potential new contrast mechanism for the rapidly emerging new field of mid-infrared microspectroscopy using QCLs., Comment: 15 pages, 5 figures, preprint

We measure the lasing dynamics of single and coupled photonic crystal nanocavity array lasers fabricated in the indium gallium arsenide phosphide material system. Under short optical excitation, single cavity lasers produce pulses as fast as 11 ps (FWHM), while coupled cavity lasers show significantly longer lasing duration which is not explained by a simple rate equations model. A Finite Difference Time Domain simulation including carrier gain and diffusion suggests that asynchronous lasing across the nanocavity array extends the laser's pulse duration., Comment: 4 pages, 4 figures

We describe an efficient surface-passivated photonic crystal nanocavity laser, demonstrating room-temperature operation with 3-ps total pulse duration (detector response limited) and low-temperature operation with ultra-low-threshold near 9uW., Comment: 6 pages, 3 figures

The efficiency and operating range of a photonic crystal laser is improved by passivating the InGaAs quantum well (QW) gain medium and GaAs membrane using an (NH4)S treatment. The passivated laser shows a four-fold reduction in nonradiative surface recombination rate, resulting in a four-fold reduction in lasing threshold. A three-level carrier dynamics model explains the results and shows that lasing threshold is as much determined by surface recombination losses as by the cavity quality factor (Q). Surface passivation therefore appears crucial in operating such lasers under practical conditions., Comment: 3 pages, 2 figures

We have experimentally studied polarization properties of the two-dimensional coupled photonic crystal microcavity arrays, and observed a strong polarization dependence of the transmission and reflection of light from the structures - the effects that can be employed in building miniaturized polarizing optical components. Moreover, by combining these properties with a strong sensitivity of the coupled bands on the surrounding refractive index, we have demonstrated a detection of small refractive index changes in the environment, which is useful for construction of bio-chemical sensors., Comment: 8 pages text and 4 figures on 4 pages. Submitted for publication on 07/14/04

We present the design and fabrication of photonic crystal structures exhibiting electromagnetic bands that are flattened in all crystal directions, i.e., whose frequency variation with wavevector is minimized. Such bands can be used to reduce group velocity of light propagating in arbitrary crystal direction, which is of importance for construction of miniaturized tunable optical delay components, low-threshold photonic crystal lasers, and study of nonlinear optics phenomena., Comment: 8 pages text and 3 figures on 3 pages. Published on Appl. Phys. Lett. 2004

We recently proposed two-dimensional coupled photonic crystal microcavity arrays as a route to achieve a slow-group velocity of light (flat band) in all crystal directions. In this paper we present the first experimental demonstration of such structures with a measured group velocity below 0.008c and discuss the feasibility of applications such as low-threshold photonic crystal lasers with increased output powers, optical delay components and sensors., Comment: 8 pages text and 3 figures on 3 pages. Submitted for publication on 06/19/04