Enhancement Of Spontaneous Emission Research Articles

Non-resonant enhancement of spontaneous emission of HITC dye in metal-insulator-metal waveguides

We have experimentally studied the non-resonant enhancement of spontaneous emission of HITC laser dye in metal-insulator-metal (MIM) waveguides (also referred to as Fabry–Perot cavities). We have found that in the cavities, whose size was too small to support a fundamental or any higher order resonance, the emission decay rate increased, by nearly an order of magnitude, with reduction of the cavity size. At the same time, the emission intensity increased when the cavity size was reduced from ∼200 to ∼30 nm and dropped sharply when the cavity was smaller than ∼30 nm. This emission enhancement, consistent with the perpendicular orientation of the emitting dipole with respect to the mirrors, is in a good agreement with the theoretical predictions known from the literature.

Microcavity-Mediated Spectrally Tunable Amplification of Absorption in Plasmonic Nanoantennas.

Nanoantenna-microcavity hybrid systems offer unique platforms for the study and manipulation of light at the nanoscale, since their constituents have either low mode volume or long photon storage time. A nearby dielectric optical cavity can modify the photonic environment surrounding a plasmonic nanoantenna, presenting opportunities to sculpt its spectral response. However, matching the polar opposites for enhanced light-matter interactions remains challenging, as the antenna can be rendered transparent by the cavity through destructive Fano interferences. In this work, we tackle this issue by offering a new plasmonic-photonic interaction framework. By coupling to a photonic crystal guided resonance, a gold nanostar delivers 1 order of magnitude amplified absorption, and the ultrasharp Lorentzian-line-shaped hybrid resonance is continuously tunable over a broad spectral range by scanning of the incidence angle. Our intuitive coupled mode model reveals that a distinct optical pathway highlighting the cavity-mediated activation of nanoantennas is key for absorption enhancement. Moreover, we show that the line width of the enhancementcan be widely tunable, and that the maximum power transferred to the antennas is attained under critical coupling. The cooperative hybrid system opens up new opportunities to boost a wealth of applications including ultrasensitive molecular spectroscopy, plasmonic hot carrier chemistry, thermoplasmonic, spontaneous emission enhancement, nanolasers, and many more.

Revealing Temperature-Dependent Absorption and Emission Enhancement Factors in Plasmon Coupled Semiconductor Heterostructures

Localized surface plasmon resonances can increase the quantum efficiency of photon emitters through both absorption and spontaneous emission enhancement effects. Despite extensive studies, experimental results that clearly distinguish the two plasmonic enhancement effects are rarely available. Here, we present clear spectral signatures of the plasmonic enhancement effects on the absorption (excitation) and spontaneous emission (Purcell factor) by analyzing the temperature-dependent photoluminescence (PL) properties of an InGaAs/GaAs single quantum well (QW) coupled to colloidal gold nanorods (AuNRs) at different GaAs capping layer thicknesses (d). We find that when the emitting InGaAs layer is close to the AuNRs (d = 5 nm), the plasmonic enhancement effect on the QW PL is dominated by the Purcell factor, which significantly increases the external quantum efficiency of the QW that otherwise barely emits. When d is increased to 10 nm, the temperature dependence of the PL enhancement factor (F) reflects absorption enhancement in the capping layer followed by carrier diffusion and capture by the well. First, F increases with temperature and then decreases following the temperature dependence of the carrier diffusion coefficient in GaAs. By factoring out the contribution of the captured carriers to F, it is shown that carrier transfer to the well reaches saturation with increasing incident laser power. In addition to providing insight into the plasmonic enhancement mechanism, the results presented in this work suggest that colloidal plasmonic nanoparticles can be used as simple probes for understanding carrier transport phenomena in arbitrary semiconductor heterostructures.

Strain-Tunable Single-Photon Source Based on a Quantum Dot–Micropillar System

Scalable quantum photonic architectures demand highly efficient, high-purity single-photon sources, which can be frequency matched via external tuning. We demonstrate a single-photon source based on an InAs quantum dot embedded in a micropillar resonator, which is frequency tunable via externally-applied stress. Our platform combines the advantages of a Bragg micropillar cavity and the piezo-strain-tuning technique enabling single photon spontaneous emission enhancement via the Purcell effect and quantum dot (QD) with tunable wavelength. Our optomechanical platform has been implemented by integration of semiconductor-based QD-micropillars on a piezoelectric substrate. The fabricated device exhibits spontaneous emission enhancement with a Purcell factor of 4.4$\pm$0.7 and allows for a pure triggered single-photon generation with $g^{(2)}(0)$ < 0.07 under resonant excitation. A quantum dot emission energy tuning range of 0.75 meV for 27 kV/cm applied to the piezo substrate has been achieved. Our results pave the way towards the scalable implementation of single-photon quantum photonic technologies using optoelectronic devices.

Improving Upconversion Efficiency Based on Cross-Patterned Upconversion Material Slot Waveguides on a Silicon Layer.

Upconversion (UC) materials can be used to harvest near-infrared (NIR) light and convert it into visible light. Although this improves optical device operating spectral range and efficiency, e.g., solar cells, typical UC material conversion efficiency is too low for practical devices. We propose a cross-patterned slot waveguide constructed from UC material embedded in a high index semiconductor layer to improve UC. Since the slot waveguide mode is induced in the low index UC slot, NIR absorption (~970 nm) increased 25-fold compared with film structures. Furthermore, the spontaneous emission enhancement rate at 660 nm increased 9.6-fold compared to the reference film due to resonance excited in the UC slot (Purcell effect). Thus, the proposed UC slot array structure improved UC efficiency 240-fold considering absorption and emission enhancements. This double resonance UC improvement can be applied to practical optical devices.

Phonon Polaritonics in Two-Dimensional Materials.

Extreme confinement of electromagnetic energy by phonon polaritons holds the promise of strong and new forms of control over the dynamics of matter. To bring such control to the atomic-scale limit, it is important to consider phonon polaritons in two-dimensional (2D) systems. Recent studies have pointed out that in 2D, splitting between longitudinal and transverse optical (LO and TO) phonons is absent at the Γ point, even for polar materials. Does this lack of LO-TO splitting imply the absence of a phonon polariton in polar monolayers? To answer this, we connect the microscopic phonon properties with the macroscopic electromagnetic response. Specifically, we derive a first-principles expression for the conductivity of a polar monolayer specified by the wave-vector-dependent LO and TO phonon dispersions. In the long-wavelength (local) limit, we find a universal form for the conductivity in terms of the LO phonon frequency at the Γ point, its lifetime, and the group velocity of the LO phonon. Our analysis reveals that the phonon polariton of 2D is simply the LO phonon of the 2D system. For the specific example of hexagonal boron nitride (hBN), we estimate the confinement and propagation losses of the LO phonons, finding that high confinement and reasonable propagation quality factors coincide in regions that may be difficult to detect with current near-field optical microscopy techniques. Finally, we study the interaction of external emitters with 2D hBN nanostructures, finding an extreme enhancement of spontaneous emission due to coupling with localized 2D phonon polaritons and the possibility of multimode strong and ultrastrong coupling between an external emitter and hBN phonons. This may lead to the design of new hybrid states of electrons and phonons based on strong coupling.

Definition of polaritonic fluctuations in natural hyperbolic media

The discovery of photonic hyperbolic dispersion surfaces in certain van der Waals bonded solids, such as hexagonal boron nitride and bismuth selenide (a topological insulator), offers intriguing possibilities for creating strongly modified light-matter interactions. However, open problems exist in quantifying electromagnetic field fluctuations in these media, complicating typical approaches for modeling photonic characteristics. Here, we address this issue by linking the identifying traits of hyperbolic response to a coupling between longitudinal and transverse fields that can not occur in isotropic media. This description allows us to calculate the influence of hyperbolic response on electromagnetic fluctuations without explicitly imposing a characteristic size (model of nonlocality), leading to formally bounded expressions so long as material absorption is included. We then apply this framework to two exemplary areas: the optical sum rule for modified spontaneous emission enhancement in a general uniaxial medium, and thermal electromagnetic field fluctuations in hexagonal boron nitride and bismuth selenide. We find that while the sum rule is satisfied, it does not constrain the enhancement of light-matter interactions in either case. We also show that both hexagonal boron nitride and bismuth selenide possess broad spectral regions where the magnitude of electromagnetic field fluctuations are over 120 times larger, and over 800 times larger along specific angular directions, than they are in vacuum.

Fundamental Limits to Near-Field Optical Response over Any Bandwidth

We develop an analytical framework to derive upper bounds to light--matter interactions in the optical near field, where applications ranging from spontaneous-emission amplification to greater-than-blackbody heat transfer show transformative potential. Our framework connects the classic complex-analytic properties of causal fields with newly developed energy-conservation principles, resulting in a new class of power--bandwidth limits. These limits demonstrate the possibility of orders-of-magnitude enhancement in near-field optical response with the right combination of material and geometry. At specific frequency and bandwidth combinations, the bounds can be closely approached by canonical plasmonic geometries, with the opportunity for new designs to emerge away from those frequency ranges. Embedded in the bounds is a material "figure of merit," which determines the maximum response of any material (metal/dielectric, bulk/2D, etc.), for any frequency and bandwidth. Our bounds on local density of states (LDOS) represent maximal spontaneous-emission enhancements, our bounds on cross density of states (CDOS) limit electromagnetic-field correlations, and our bounds on radiative heat transfer (RHT) represent the first such analytical rule, revealing fundamental limits relative to the classical Stefan--Boltzmann law.

Engineered metallic nanostructures for dye fluorescence enhancement: Experiment and simulation

The author reports spectroscopic characterization, and simulation of metallic nanoantennas consisting of arrays of Au nanostructures for enhancement of dye fluorescence. The molecular dye fluorescence was significantly enhanced by near-field interaction between plasmons excited from the Au nanostructures and the molecule. The resulting fluorescence enhancement caused by the near-field enhancement was attributed to plasmon resonances and correlated to the extinction of the metal nanostructure. The author also performed numerical calculations of the Purcell enhancement factors, simulating the spontaneous emission enhancement of a dipole emitter positioned near the nanostructure, and these are in good agreement with the measured fluorescence enhancement.

Chaos synchronization of coupled nano-quantum cascade lasers with negative optoelectronic feedback

In this paper, a theoretical investigation of chaos synchronization in two nano-quantum cascade lasers with delayed negative optoelectronic feedback is presented. Since the spontaneous emission effect is an important factor in a microcavity the rate equations model has been reconsidered to include the Purcell spontaneous emission enhancement factor F and the spontaneous emission factor. It is found that the synchronization takes place under suitable system parameters. The results indicate that the coupling strength, the delay time in the transmitter, and the transmission time between the two lasers have significant effects on the synchronization quality while the stage number and the delay time in receiver have poor effects on the synchronization quality. Also, when the system is a closed-loop or open-loop, synchronization with poor dynamics occurs when the spontaneous emission factor is small while the synchronization happens in the open-loop system only when the spontaneous emission factor is large. Furthermore, when the system is a closed-loop, synchronization occurs when Purcell factor is large while the synchronization happens to the open-loop system of any values for the spontaneous emission factor and Purcell factor.

Manipulation of Magnetic Dipole Emission from Eu3+ with Mie-Resonant Dielectric Metasurfaces.

Mie-resonant high-index dielectric nanoparticles and metasurfaces have been suggested as a viable platform for enhancing both electric and magnetic dipole transitions of fluorescent emitters. While the enhancement of the electric dipole transitions by such dielectric nanoparticles has been demonstrated experimentally, the case of magnetic-dipole transitions remains largely unexplored. Here, we study the enhancement of spontaneous emission of Eu3+ ions, featuring both electric and magnetic-dominated dipole transitions, by dielectric metasurfaces composed of Mie-resonant silicon nanocylinders. By coating the metasurfaces with a layer of an Eu3+ doped polymer, we observe an enhancement of the Eu3+ emission associated with the electric (at 610 nm) and magnetic-dominated (at 590 nm) dipole transitions. The enhancement factor depends systematically on the spectral proximity of the atomic transitions to the Mie resonances as well as their multipolar order, both controlled by the nanocylinder size. Importantly, the branching ratio of emission via the electric or magnetic transition channel can be modified by carefully designing the metasurface, where the magnetic dipole transition is enhanced more than the electric transition for cylinders with radii of about 130 nm. We confirm our observations by numerical simulations based on the reciprocity principle. Our results open new opportunities for bright nanoscale light sources based on magnetic transitions.

Nonlinear Atom-Plasmon Interactions Enabled by Nanostructured Graphene.

Electrically tunable graphene plasmons are anticipated to enable strong light-matter interactions with resonant quantum emitters. However, plasmon resonances in graphene are typically limited to infrared frequencies, below those of optical excitations in robust quantum light sources and many biologically interesting molecules. Here we propose to utilize near fields generated by the plasmon-assisted nonlinear optical response of nanostructured graphene to resonantly couple with proximal quantum emitters operating in the near infrared. We show that the nonlinear near field produced by a graphene nanodisk can strongly excite and coherently control quantum states in two- and three-level atomic systems when the third harmonic of its plasmon resonance is tuned to a particular electronic transition. In the present scheme, emitter and plasmon resonances are nondegenerate, circumventing strong enhancement of spontaneous emission. We envision potential applications for the proposed nonlinear plasmonic coupling scheme in sensing and temporal quantum control.

Enhancement of spontaneous emission probability in a disordered media

Was provided statistical analysis of Purcell effect dependence on emission frequency and emitter position in disordered structure. Fact that the presence of disorder in one-dimensional photonic crystals could lead to a modification of spontaneous emission rate in the frequency region corresponding to a photonic band gap (PBG) was demonstrated. Was shown, that amount of disorder regulates the two different regimes of the Purcell effect. In case of weak disorder Purcell enhancement of spontaneous emission occurs at PBG edges, and in case of strong disorder at PBG centre.

Spontaneous emission enhancement in planar metal-organic structures

We provide an experimental investigation of a Purcell enhancement in a silver-organic periodic structure with an organic material CBP (4,4′-Bis(N-carbazolyl)-1,1′-biphenyl). Were fabricated two structures using a thermal evaporation technique with a different thickness ratio between layers. A rate of a fluorescence intensity decay of the periodic structures was experimentally measured in a near ultraviolet region. We show experimentally, that the rate of CBP molecule fluorescence decay increasing. A maximum registered value of the Purcell factor is close to 10.

Extreme terahertz electric-field enhancement in high-Q photonic crystal slab cavity with nanoholes.

A one-dimensional photonic-crystal (PC) cavity with nanoholes is proposed for extreme enhancement of terahertz (THz) electric fields using the electromagnetic (EM) boundary conditions. Both slot (for the perpendicular component of the electric displacement field) and anti-slot (for the parallel component of the electric field) effects contribute to the considerable field enhancement. The EM energy density can be enhanced by a factor of (εh/εl)2 in the high-refractive-index material, where εh and εl are the permittivities of the high- and low-refractive-index materials, respectively. Correspondingly, the mode volume can be reduced by a factor of 288, compared with a conventional THz PC cavity, and is three orders of magnitude smaller than the diffraction limitation. Further, the proposed THz cavity design also supports modes with high quality factors (Q) > 104, which induces strong Purcell enhancement by a factor exceeding 106. Our THz cavity design is feasible and attractive for experimental demonstrations, because the semiconductor layer in which the EM is maximized can naturally be filled with quantum-engineered active materials. Thus, the proposed design can possibly be used to develop room-temperature coherent THz radiation sources.

Optimization of Nanopatterned Multilayer Hyperbolic Metamaterials for Spontaneous Light Emission Enhancement

Light emission processes can be modified through the Purcell effect near a metallic surface. Such effect relies on the matching between spontaneous emission spectra and surface plasmon resonances, and the latter is typically limited by the existing metal properties. Nanopatterned multilayer hyperbolic metamaterials (HMMs) with engineerable material property are promising in enhancing spontaneous emission rates at desired frequencies with improved far‐field radiative power. In this work, the authors study the optimization process for spontaneous emission enhancement by using nanopatterned HMMs. By theoretically investigating the Purcell effect on HMMs compared with traditional metals, the authors choose better material combinations for stronger Purcell enhancement. Different decay channels in the HMM are analyzed against the emitter distance and their wavelengths. Systematic optimization of achieving large emission intensity is demonstrated by comparing performance of nanopatterned HMMs with different geometry parameters. The promise in achieving light emission with both high decay rates and brightness has various potential applications including light‐emitting devices, single‐molecule detection, and surface‐enhanced Raman scattering.

Experimental Study of Spontaneous-Emission Enhancement in Tamm Plasmon Structures with an Organic Active Region

Spontaneous-emission enhancement in a Tamm plasmon microcavity with an active region with organic material 4.4'-bis(N-carbazolyl)-1.1'-biphenyl (CBP) is theoretically and experimentally studied. The microcavity consisted of a Bragg reflector made of silicon oxide and tantalum oxide, over which CBP and silver layers are applied. The dependences of the Purcell modal factor on the emission direction and frequency, as well as the Purcell factor spectrum are calculated. The emission and fluorescence decay spectra in time are measured in the ultraviolet range. It is found that the probability of spontaneous emission increases and the maximum Purcell factor reaches three at frequencies corresponding to eigenmodes of the Tamm plasmon.

Different regimes of the Purcell effect in disordered photonic crystals

We demonstrate that disorder in photonic crystals could lead to pronounced modification of spontaneous emission rate in the frequency region corresponding to the photonic band gap (PBG). Depending on the amount of disorder, two different regimes of the Purcell effect occurs. We provide statistical analysis of Purcell coefficient on the frequency of the emitter and its position within the sample. For the moderate disorder, an enhancement of spontaneous emission occurs at the edge of PBG due to the modification of properties of the edge state. This effect is responsible for recently observed mirrorless lasing in photonic crystals at the edge of PBG. When the level of disorder increases, the spontaneous emission rate enhances within the PBG due to the appearance of the high quality factor states. This effect is likely responsible for a superlinear dependence of emissions on pumping observed in synthetic opals.

Superconducting metamaterials for waveguide quantum electrodynamics

Embedding tunable quantum emitters in a photonic bandgap structure enables control of dissipative and dispersive interactions between emitters and their photonic bath. Operation in the transmission band, outside the gap, allows for studying waveguide quantum electrodynamics in the slow-light regime. Alternatively, tuning the emitter into the bandgap results in finite-range emitter–emitter interactions via bound photonic states. Here, we couple a transmon qubit to a superconducting metamaterial with a deep sub-wavelength lattice constant (λ/60). The metamaterial is formed by periodically loading a transmission line with compact, low-loss, low-disorder lumped-element microwave resonators. Tuning the qubit frequency in the vicinity of a band-edge with a group index of ng = 450, we observe an anomalous Lamb shift of −28 MHz accompanied by a 24-fold enhancement in the qubit lifetime. In addition, we demonstrate selective enhancement and inhibition of spontaneous emission of different transmon transitions, which provide simultaneous access to short-lived radiatively damped and long-lived metastable qubit states.

Hyperbolic metamaterial resonator–antenna scheme for large, broadband emission enhancement and single-photon collection

We model the broadband enhancement of single-photon emission from color centres in silicon carbide nanocrystals coupled to a planar hyperbolic metamaterial, HMM resonator. The design is based on positioning the single photon emitters within the HMM resonator, made of a dielectric index-matched with silicon-carbide material. The broadband response results from the successive resonance peaks of the lossy Fabry Perot structure modes arising within the high-index HMM cavity. To capture this broadband enhancement in the single photon emitters spontaneous emission, we placed a simple gold based cylindrical antenna on top of the HMM resonator. We analyzed the performance of this HMM coupled antenna structure in terms of the Purcell enhancement, quantum efficiency, collection efficiency and overall collected photon rate. For perpendicular dipole orientation relative to the interface, the HMM coupled antenna resonator leads to a significantly large spontaneous emission enhancement with Purcell factor of the order of 250 along with a very high average total collected photon rate, CPR of about 30 over a broad emission spectrum, 700 nm to 1000 nm. The peak CPR increases to about 80 at 900 nm, corresponding to the emission of silicon-carbide quantum emitters. This is a state of the art improvement considering the previous computational designs have reported a maximum average CPR of 25 across the nitrogen-vacancy centre emission spectrum, 600 nm to 800 nm with the highest value being about 40 at 650 nm.