In this paper we theoretically show that the Raman scattering by a core-shell micron or submicron particle with epsilon-near-zero metamaterial shell and silica spherical or cylindrical core can combine useful features of cavity-enhanced and surface-enhanced Raman scattering. The cavity resonance together with the plasmon resonance lead to the giant enhancement of the field inside the metashell which is performed as a layer of silver or gold nanoparticles and is penetrable for molecules to be detected. This approach results in the significant increase of both effective volume in which molecules are affected by enhanced electric field and Raman gain averaged over this volume.
A tri-layer metamaterial perfect absorber of light, consisting of (Al/ZnS/Al) films with the top aluminium layer patterned as an array of circular disk nanoantennas, is investigated for resonantly enhancing Raman scattering from C-60 fullerene molecules deposited on the metamaterial. The metamaterial is designed to have resonant bands due to plasmonic and electromagnetic resonances at the Raman pump frequency (725 nm) as well as Stokes emission bands. The Raman scattering from C60 on the metamaterial with resonantly matched bands is measured to be enhanced by an order of magnitude more than fr…
We demonstrate that the metamaterial perfect absorber behaves as a meta-cavity bounded between a resonant metasurface and a metallic thin-film reflector. The perfect absorption is achieved by the Fabry-Perot cavity resonance via multiple reflections between the "quasi-open" boundary of resonator and the "closed" boundary of reflector. The characteristic features including angle independence, ultra-thin thickness and strong field localization can be well explained by this model. With this model, metamaterial perfect absorber can be redefined as a meta-cavity exhibiting high Q-factor, strong fie…
We propose a scheme to realize a lossless propagation of linear and nonlinear Airy surface polaritons (SPs) via active Raman gain (ARG). The system we suggest is a planar interface superposed by a negative index metamaterial (NIMM) and a dielectric, where three-level quantum emitters are doped. By using the ARG from the quantum emitters and the destructive interference effect between the electric and magnetic responses from the NIMM, we show that not only the Ohmic loss of the NIMM but also the light absorption of the quantum emitters can be completely eliminated. As a result, non-diffractive …
Cavity array metamaterials (CAMs), composed of optical microcavities in a lattice coupled via tight-binding interactions, represent a novel architecture for engineering metamaterials. Since the size of the CAMs' constituent elements are commensurate with the operating wavelength of the device, it cannot directly utilise classical transformation optics in the same way as traditional metamaterials. By directly transforming the internal geometry of the system, and locally tuning the permittivity between cavities, we provide an alternative framework suitable for tight-binding implementations of me…
Dynamic dipolar toroidal response is demonstrated by an optical plasmonic metamaterial composed of double disks. This response with a hotspot of localized E-field concentration is a well-behaved toroidal cavity mode that exhibits a large Purcell factor due to its deep-subwavelength mode volume. All-optical Hall effect (photovoltaic) due to this optical toroidal moment is demonstrated numerically, in mimicking the magnetoelectric effect in multiferroic systems. The result shows a promising avenue to explore various optical phenomena associated with this intriguing dynamic toroidal moment.
We theoretically investigate coupling interaction between molecule excitons and whispering gallery modes (WGMs) that approaches the limit of single exciton strong coupling in hyperbolic metamaterial (HMM) cavity, composed of a dielectric core wrapped by several stacks of alternative layers of metal and dielectric. We demonstrate that associated with the excitation of the whispering gallery mode, the electric fields with resonance wavelengths that are much larger than the cavity size can be highly localized within a dielectric layer, leading to extremely small mode volumes. By using temporal co…
Localized cavity resonances due to nanostructures at material surfaces can greatly enhance radiative heat transfer (RHT) between two closely placed bodies owing to stretching of cavity states in momentum space beyond light line. Based on such understanding, we numerically demonstrate the possibility of ultra-broadband super-Planckian RHT between two plates patterned with trapezoidal-shaped hyperbolic metamaterial (HMM) arrays. The phenomenon is rooted not only in HMM's high effective index for creating sub-wavelength resonators, but also its extremely anisotropic isofrequency contour. The two …
We propose a new class of resonant electromagnetic structures, and study their response to free-space illumination. The structures consist of partial cylindrical shells that have cloaking material properties proposed by Pendry et al. These metamaterial shells have apertures that allow the propagation of incident irradiation into an interior resonant cavity. We use full wave time-harmonic analysis to study the field distribution inside the cavity, and show that an analogue of Whispering Gallery Modes (WGMs) can be efficiently excited via free-space illumination.
We fabricate a fiber coupled ultrahigh-Q resonator from a μdroplet per se; and experimentally measure stimulated Raman emission showing itself at a 160μW threshold. We observe Raman-laser lines that agree with their related calculated molecular-vibrations, as well as with a control-group experiment that uses a Raman-spectrometer. Yet, unlike spectrometers where emission is spontaneous and less directional, our droplet emitter is stimulated, single-mode-fiber coupled, resonantly enhanced with Q of 250 million, confined to a 23 um3 mode volume and has 7 orders of magnitude higher power.
We demonstrate efficient generation of a Raman-type optical frequency comb by employing adiabatic Raman excitation in an enhancement cavity. A broad frequency comb spanning over 130 THz is realized with an excitation power reduction exceeding three orders of magnitude compared with a single-pass configuration.
Raman spectroscopy reveals chemically specific information and provides label-free insight into the molecular world. However, the signals are intrinsically weak and call for enhancement techniques. Here, we demonstrate Purcell enhancement of Raman scattering in a tunable high-finesse microcavity, and utilize it for molecular diagnostics by combined Raman and absorption imaging. Studying individual single-wall carbon nanotubes, we identify crucial structural parameters such as nanotube radius, electronic structure and extinction cross-section. We observe a 320-times enhanced Raman scattering sp…
We study a generalized notion of two-mode squeezing for the Stokes and anti-Stokes fields in a model of a cavity Raman laser, which leads to a significant reduction in decoherence or quantum noise. The model comprises a loss-less cavity with classical pump, unsaturated medium and arbitrary homogeneous broadening and dispersion. Allowing for arbitrary linear combinations of the two modes in the definition of quadrature variables, we find that there always exists a combination of the two output modes which exhibits quadrature squeezing with noise reduction below the vacuum level. The number of n…
We analyze the effects of noise and parameter deviations in a bichromatic Raman type white light cavity, with potential applications in precision measurements such as gravitational wave detection. The results show that the dispersion variation induced by parameter deviation can be controlled within $10^{-4}$. The laser phase noise decreases the dispersion magnitude while the amplitude noise increases it. Although we can always adjust the parameters to satisfy the white light condition, both noises make the cavity transmission curve uneven.
A simple metamaterial absorber suitable for fabrication over large areas associated with a Fano like resonance is proposed. The proposed designed of the metamaterial absorber consists of photoresist disk arrays on a silicon substrate followed by the deposition of a tri layer of Au, ZnS and Au on the top of the structure. Due to the tri layer, there is a formation of a cavity between the substrate and gold layer on the top of photoresist disk and a waveguide in the ZnS layer in between the gold layers on the substrate and the ZnS layer itself. The Fano like resonance arises due to the interfere…
We demonstrate the dynamics of stimulated Raman scattering in designed high-Q/Vm silicon photonic band gap nanocavities through the coupled-mode theory framework towards optically-pumped silicon lasing. The interplay of other chi(3) effects such as two-photon absorption and optical Kerr, related free-carrier dynamics, thermal effects, as well as linear losses such as cavity radiation and linear material absorption are included and investigated numerically. Our results clarify the relative contributions and evolution of the mechanisms, and demonstrate the lasing and shutdown thresholds. Our stu…
In this thesis various plasmonic materials, such as hyperbolic metamaterial nanohole arrays and Au-coated free standing nanoassembly supporting nanopores, are investigated with the aim to perform optical sensing of DNA molecules with Surface-Enhanced Raman Spectroscopy in flow-through configuration.
We show that topological frequency band structures emerge in two-dimensional electromagnetic lattices of metamaterial components without the application of an external magnetic field. The topological nature of the band structure manifests itself by the occurrence of exceptional points in the band structure or by the emergence of one-way guided modes. Based on an EM network with nearly flat frequency bands of nontrivial topology, we propose a coupled-cavity lattice made of superconducting transmission lines and cavity QED components which is described by the Janes-Cummings-Hubbard model and can…
We demonstrate cavity-enhanced Raman emission from a single atomic defect in a solid. Our platform is a single silicon-vacancy center in diamond coupled with a monolithic diamond photonic crystal cavity. The cavity enables an unprecedented frequency tuning range of the Raman emission (100 GHz) that significantly exceeds the spectral inhomogeneity of silicon-vacancy centers in diamond nanostructures. We also show that the cavity selectively suppresses the phonon-induced spontaneous emission that degrades the efficiency of Raman photon generation. Our results pave the way towards photon-mediated…
We estimate the dominating frequencies contributing to the Casimir energy in a cavity of metamaterials mimicking de Sitter space, by solving the eigenvalue problem of Maxwell equations. It turns out the dominating frequencies are the inverse of the size of the cavity, and the degeneracy of these frequencies also explains our previous result on the unusually large Casimir energy. Our result suggests that carrying out the experiment in laboratory is possible theoretically.
The radiation dynamics of optical emitters can be manipulated by properly designed material structures providing high local density of photonic states, a phenomenon often referred to as the Purcell effect. Plasmonic nanorod metamaterials with hyperbolic dispersion of electromagnetic modes are believed to deliver a significant Purcell enhancement with both broadband and non-resonant nature. Here, we have investigated finite-size cavities formed by nanorod metamaterials and shown that the main mechanism of the Purcell effect in these hyperbolic resonators originates from the cavity hyperbolic mo…
The efficiency of the frequency conversion process at the heart of Raman heterodyne spectroscopy was improved by nearly four orders of magnitude by resonant enhancement of both the pump and signal optical fields. Our results using an erbium doped Y$_2$SiO$_5$ crystal at temperatures near 4K suggest that such an approach is promising for the quantum conversion of microwave to optical photons.
Temporal cavity solitons (CS) are optical pulses that can persist in passive resonators, and they play a key role in the generation of coherent microresonator frequency combs. In resonators made of amorphous materials, such as fused silica, they can exhibit a spectral red-shift due to stimulated Raman scattering. Here we show that this Raman-induced self-frequency-shift imposes a fundamental limit on the duration and bandwidth of temporal CSs. Specifically, we theoretically predict that stimulated Raman scattering introduces a previously unidentified Hopf bifurcation that leads to destabilizat…
We investigate the use of coherent optical fields as a means of dynamically controlling the resonant behaviour of a variety of composite metamaterials, wherein the metamaterial structures are embedded in a dispersive dielectric medium. Control and switching is implemented by coherently driving the resonant permittivity of the embedding medium by applied optical radiation. The effect of embedding Split ring resonators (SRR) in a frequency- dispersive medium with Lorentz-like dispersion or with dispersion engineered by electromagnetic induced transparency (EIT), is manifested in the splitting of…
Anisotropic and inhomogeneous metamaterial shells are studied in order to exploit all their resonant mode richness. These multilayer structures are based on a cylindrical distribution of radially dependent constitutive parameters including an inner void cavity. Shell, cavity and whispering gallery modes are characterized, and special attention is paid to the latter ones. The whispering gallery modes are created at the boundary layers of the shell with the background and energy localization is produced with highly radiative characteristics. These low-Q resonant states have frequencies that are …
We experimentally study the relaxation oscillations and amplitude stability properties of an optical laser operating deep into the bad-cavity regime using a laser-cooled $^{87}$Rb Raman laser. By combining measurements of the laser light field with nondemolition measurements of the atomic populations, we infer the response of the gain medium represented by a collective atomic Bloch vector. The results are qualitatively explained with a simple model. Measurements and theory are extended to include the effect of intermediate repumping states on the closed-loop stability of the oscillator and the…
We study a critically coupled cavity doped with resonant atoms with metamaterial slabs as mirrors. We show how resonant atom-cavity interaction can lead to a splitting of the critical coupling dip. The results are explained in terms of the frequency and lifetime splitting of the coupled system.
Herein we report experimental evidence of directional SERS from molecules situated inside a single nanowire-nanoparticle junction cavity. The emission was confined to a narrow range of wavevectors perpendicular to the axis of the cavity. In addition to this, the molecules excite multiple guided modes of the nanowire which were imaged using leakage radiation Fourier microscopy. We further characterize the emission wavevectors as a function of output polarization. The excited guided modes of the wire show interesting polarization signatures. All the results were corroborated using finite element…
Ultrafast atomic vibrations mediate heat transport, serve as fingerprints for chemical bonds and drive phase transitions in condensed matter systems. Light pulses shorter than the atomic oscillation period can not only probe, but even stimulate and control collective excitations. In general, such interactions are performed with free-propagating pulses. Here, we demonstrate intra-cavity excitation and time-domain sampling of coherent optical phonons inside an active laser oscillator. Employing real-time spectral interferometry, we reveal that Terahertz beats of Raman-active optical phonons can …
The Raman gain of a probe light in a three-state $Λ$-scheme placed into a defect of a one-dimensional photonic crystal is studied theoretically. We show that there exists a pump intensity range, where the transmission and reflection spectra of the probe field exhibit \textit{simultaneously} occurring narrow peaks (resonances) whose position is determined by the Raman resonance. Transmission and reflection coefficients can be larger than unity at pump intensities of order tens of $μ$W/cm$^{2}$. When the pump intensity is outside this region, the peak in the transmission spectrum turns into a na…
The evolution versus pump power of the spectrum of a singly resonant optical parametric oscillator based on an MgO-doped periodically poled stoichiometric lithium tantalate crystal is observed. The onset of cascade Raman lasing due to stimulated Raman scattering in the nonlinear crystal is analyzed. Spurious frequency doubling and sum-frequency generation phenomena are observed and understood. A strong reduction of the intracavity Raman scattering is obtained by a careful adjustment of the cavity losses.
In the development of high efficiency and high gradient RF-accelerators, RF waveguides and cavities have been designed with Photonic Band Gap (PBG) and fishnet- metamaterial structures. The designed structures are comprised of a periodically corrugated channel sandwiched between two photonic crystal slabs with alternating high to low dielectric constants and a multi-cell cavity-resonator designed with fishnet-metamaterial apertures. The structural designs of our interest are intended to only allow an operating-mode or -band within a narrow frequency range to propagate. The simulation analysis …
Continuous Wave (CW) Terahertz spectroscopy enabled by photomixing is a promising high precision spectroscopic tool for the examination of a wide variety of samples including biological, chemical, and solid state. However, often it would be of interest to examine isolated samples free from bulk effects that broaden spectral features. In this form samples with low concentrations of absorbers have a reduced cross section making coupling to an external driving field a challenge. By utilising THz metamaterials one can borrow the concepts of surface enhanced Raman spectroscopy to confine and concen…
We numerically study the mechanisms of frequency comb generation in the mid-infrared spectral region from cw pumped silicon microring resonators. Coherent soliton comb generation may be obtained even for a pump with zero linear cavity detuning, through suitable control of the effective lifetime of free-carriers from multiphoton absorption, which introduces a nonlinear cavity detuning via free-carrier dispersion. Conditions for optimal octave spanning Raman comb generation are also described.
Signature of Magnon-Raman Phonon-Polariton Condensation in a Cavity via Transverse Pumping
Birla Institute of Technology and Science, Pilani-Dubai Campus（比拉理工学院，皮拉尼-迪拜校区）；Birla Institute of Technology and Science, Pilani, Hyderabad Campus（比拉理工学院，海德拉巴校区）
The conventional explanation of plasmon-enhanced Raman scattering attributes the enhancement to the antenna effect focusing the electromagnetic field into sub-wavelength volumes. Here we introduce a new model that additionally accounts for the dynamical and coherent nature of the plasmon-molecule interaction and thereby reveals an enhancement mechanism not contemplated before: dynamical backaction amplification of molecular vibrations. We first map the problem onto the canonical model of cavity optomechanics, in which the molecular vibration and the plasmon are \textit{parametrically coupled}.…
We develop a concept for a waveguide that exploits spatial control of nonlinear surface-polaritonic waves. Our scheme includes an optical cavity with four-level $\text{N}$-type atoms in a lossless dielectric placed above a negative-index metamaterial layer. We propose exciting a polaritonic Akhmediev breather at a certain position of the interface between the atomic medium and the metamaterial by modifying laser-field intensities and detunings. Furthermore, we propose generating position-dependent polaritonic frequency combs by engineering widths of the electromagnetically induced transparency…
We present fabrication and optical characterization of micro-cavities made of multilayer graphene (MLG) cantilevers clamped by metallic electrodes and suspended over Si/Si02 substrate. Graphene cantilevers act as a semi-transparent mirrors closing an air-wedge optical cavity. This simple geometry implements a standing-wave optical resonator along with a mechanical one. Equal thickness interference fringes are observed in both Raman and Rayleigh backscattered signals with interfringe given by their specific wavelength.Chromatic dispersion within the cavity makes possible spatial modulation of g…
We observe toroidal response from a planar metamaterial comprised of asymmetric split ring resonators (ASRRs). It is showed that a toroidal-molecule can be constructed through rational arrangement of planar ASRRs as meta-atoms via manipulating structural symmetry of the meta-atoms. Field maps clearly indicate that the toroidal resonance paves new electromagnetic confinement style in a subwavelength scale. Planar scheme of manipulating the coupling among the ASRRs may stimulate research in optical region involving toroidal multipoles. Toroidal geometry together with the Fano resonance made high…
Multimode hollow microcavities in three-dimensional (3D) photonic crystals (PhCs) are designed for achieving enhanced coherent anti-Stokes Raman scattering, which requires a cavity to have three high quality-factor (Q) modes with equally spaced resonant frequencies. Cavities in 3D PhCs allows more flexibility in design and tuning than their 2D slab counterparts, since radiation loss that degrades Q can be suppressed by the 3D photonic band gap. We first tune all the mode frequencies simultaneously by changing the material and geometry of the cavity based on perturbation theory. Spectral spacin…
Simultaneously enhanced reflectance and transmittance greater than 35 dB are demonstrated for the lasing spaser (or spasing) behavior in an active fishnet metamaterial. In mimicking a lasing cavity, an equivalent active slab with Lorentz dispersion for the index of refraction is established to model the spasing metamaterial through the Fabry-Perot effect. Numerical and theoretical results show good agreement in the equal enhancement of reflectance and transmittance, as well as the non-monotonic dependence of the spasing intensity on the gain coefficient. In addition, directed emission of the s…
Molecular optomechanics stems from the description of Raman scattering in the presence of an optical resonator using a cavity optomechanics formalism. We extend the molecular optomechanics formalism to the case of hybrid dielectric-plasmonic resonators, with multiple optical resonances and with both free-space and waveguide addressing. We demonstrate how the Raman enhancement is the product of a pump enhancement and a modified LDOS, that simply depend on the complex response functions of the hybrid system. The Fano lineshapes that result from hybridization of a broadband and narrowband modes a…
Presented here are studies of the impact of excitation angle on surface enhanced Raman and luminescence spectroscopy of dye immobilised on a plasmon active nanocavity array support. Results show that both Raman and luminescence intensities depend on the angle of incidence consistent with the presence of cavity supported plasmon modes. Dependence of scattering or emission intensity with excitation angle occurs over the window of observation.
The temperature dependence of the asymmetry between Stokes and anti-Stokes Raman scattering can be exploited for self-calibrating, optically-based thermometry. In the context of cavity optomechanics, we observe the cavity-enhanced scattering of light interacting with the standing-wave drumhead modes of a silicon nitride membrane mechanical resonator. The ratio of the amplitude of Stokes to anti-Stokes scattered light is used to measure temperatures of optically-cooled mechanical modes down to the level of a few vibrational quanta. We demonstrate that the Raman-ratio technique is able to measur…
A possibility to greatly enhance frequency-conversion efficiency of stimulated Raman scattering is shown by making use of extraordinary properties of three-wave mixing of ordinary and backward waves. Such processes are commonly attributed to negative-index plasmonic metamaterials. This work demonstrates the possibility to replace such metamaterials that are very challenging to engineer by readily available crystals which support elastic waves with contra-directed phase and group velocities. The main goal of this work is to investigate specific properties of indicated nonlinear optical process …
We propose a gravimeter based on a matter-wave resonant cavity loaded with a Bose-Einstein condensate and closed with a sequence of periodic Raman pulses. The gravimeter sensitivity increases quickly with the number of cycles experienced by the condensate inside the cavity. The matter wave is refocused thanks to a spherical wave-front of the Raman pulses. This provides a transverse confinement of the condensate which is discussed in terms of a stability analysis. We develop the analogy of this device with a resonator in momentum space for matter waves.
