Emitter Lifetime Research Articles

Total pressure in thermionic orificed hollow cathodes: Controlling mechanisms and their relative importance

A statistical analysis is conducted to identify which physically relevant non-dimensional parameters influence the total (neutral, ion, and electron) static pressure inside thermionic orificed hollow cathodes. It is critical to uncover and order the importance of the physical mechanisms that affect the pressure inside hollow cathodes because it influences the plasma attachment length, the electron temperature, and the sheath potential. These plasma parameters, in turn, affect the emitter lifetime. A principal component analysis of total pressure data obtained from the literature reveals that four non-dimensional variables can account for most of the variation in the total-to-magnetic pressure ratio over five orders of magnitude. The relevant variables are identified with a backward stepwise selection process and an exhaustive grid search and include, by order of importance: the gasdynamic-to-magnetic pressure ratio, the ratio of the mass flow rate to the discharge current, the orifice-to-insert diameter ratio, and the orifice Reynolds number. It is also shown, using various models and regression analyses, that empirical, Poiseuille, or isentropic flow models should not be used for predictive cathode design work. The data-driven study suggests that, while viscous effects may be important, the variation in those effects between cathodes is negligible compared to the effects of the modification of the gas constant due to the plasma, the transitional flow, the flux of heavy species on the orifice plate, and the Lorentz force.

Purcell effect of nitrogen-vacancy centers in nanodiamond coupled to propagating and localized surface plasmons revealed by photon-correlation cathodoluminescence

We measured the second-order correlation function of the cathodoluminescence intensity and investigated the Purcell effect by comparing the lifetimes of quantum emitters with and without metal structure. The increase in the electromagnetic local density of state due to the coupling of a quantum emitter with a plasmonic structure causes a shortening of the emitter lifetime, which is called the Purcell effect. Since the plasmon-enhanced electric field is confined well below the wavelength of light, the quantum emitter lifetime is changed in the nanoscale range. In this study, we combined cathodoluminescence in scanning (transmission) electron microscopy with Hanbury Brown-Twiss interferometry to measure the Purcell effect with nanometer and nanosecond resolutions. We used nitrogen-vacancy centers contained in nanodiamonds as quantum emitters and compared their lifetime in different environments: on a thin SiO2 membrane, on a thick flat silver film, and embedded in a silver film. The lifetime reductions of nitrogen-vacancy centers were clearly observed in the samples with silver. We evaluated the lifetime by analytical calculation and numerical simulations and revealed the Purcell effects of emitters coupled to propagating and localized surface plasmons. This is the first experimental result showing the Purcell effect due to the coupling between nitrogen-vacancy centers in nanodiamonds and surface plasmon polaritons with nanometer resolution.

Dual Intramolecular Electron Transfer for In Situ Coreactant‐Embedded Electrochemiluminescence Microimaging of Membrane Protein

AbstractThe demand for transporting coreactant to emitter and short lifetime of the radicals in electrochemiluminescence (ECL) emission inhibit greatly its application in cytosensing and microscopic imaging. Herein we designed a dual intramolecular electron transfer strategy and tertiary amine conjugated polymer dots (TEA‐Pdots) to develop a coreactant‐embedded ECL mechanism and microimaging system. The TEA‐Pdots could produce ECL emission at +1.2 V without need of coreactant in test solution. The superstructure and intramolecular electron transfer led to unprecedented ECL strength, which was 132 and 45 times stronger than those from the mixture of Pdots with TEA at equivalent and 62.5 times higher amounts, respectively. The ECL efficiency was even higher than that of typical [Ru(bpy)3]2+ system. Therefore, this strategy and coreactant‐embedded ECL system could be used for in situ ECL microimaging of membrane protein on single living cells without additional permeable treatment for transporting coreactant. The feasibility and validity were demonstrated by evaluating the specific protein expression on cell surface. This work opens new avenues for ECL applications in single cell analysis and dynamic study of biological events.

Dual Intramolecular Electron Transfer for In Situ Coreactant-Embedded Electrochemiluminescence Microimaging of Membrane Protein.

The demand for transporting coreactant to emitter and short lifetime of the radicals in electrochemiluminescence (ECL) emission inhibit greatly its application in cytosensing and microscopic imaging. Herein we designed a dual intramolecular electron transfer strategy and tertiary amine conjugated polymer dots (TEA-Pdots) to develop a coreactant-embedded ECL mechanism and microimaging system. The TEA-Pdots could produce ECL emission at +1.2 V without need of coreactant in test solution. The superstructure and intramolecular electron transfer led to unprecedented ECL strength, which was 132 and 45 times stronger than those from the mixture of Pdots with TEA at equivalent and 62.5 times higher amounts, respectively. The ECL efficiency was even higher than that of typical [Ru(bpy)3 ]2+ system. Therefore, this strategy and coreactant-embedded ECL system could be used for in situ ECL microimaging of membrane protein on single living cells without additional permeable treatment for transporting coreactant. The feasibility and validity were demonstrated by evaluating the specific protein expression on cell surface. This work opens new avenues for ECL applications in single cell analysis and dynamic study of biological events.

Few-photon transport in Fano-resonance waveguide geometries

We present a theoretical study of Fano interference effects in few-photon transport. Under appropriate conditions, a local defect in an optical waveguide induces a highly asymmetric transmission lineshape, characteristic of Fano interference. For a two-level emitter placed adjacent to such a defect, here modeled as a partially transmitting element, we find an analytical expression for the full time evolution of single-photon wavepackets and the emitter excitation probability. We show how the partially transmitting element affects the emitter lifetime and shifts the spectral position of the effective system resonances. Using input-output formalism, we determine the single and two-photon $ S $-matrices for both a two-level emitter and a cavity-emitter system coupled to a waveguide with a partially transmitting element. We show how the Fano interference effect can be exploited for the implementation of a Hong-Ou-Mandel switch in analogy with a tunable linear or nonlinear beam splitter.

Achieving high-performance phosphorescent organic light-emitting diodes using thermally activated delayed fluorescence with low concentration

We fabricated phosphorescent organic light-emitting diodes (PhOLEDs) using thermally activated delayed fluorescence (TADF) material 10,10′-(4,4′-sulfonylbis(4,1-phenylene)) bis(9,9-dimethyl-9,10-dihydroacridine) (DMAC-DPS) with low concentration, which showed better performance compared with 1,3-bis(carbazole-9-yl) benzene (mCP) based devices. When the concentration of DMAC-DPS was 1wt%, the driving voltage of the device was only 3.3 V at 1 000 cd/m2, and the efficiency and lifetime of the device were effectively improved compared with those of mCP based devices. The result indicated that DMAC-DPS could effectively improve the performance of phosphorescent devices. We believe that the better device performance can be attributed to the optimization of the energy transfer process in the emitter layer and lifetime of triplet excitons by DMAC-DPS. The study may provide a simple and effective strategy to achieve high-performance OLEDs.

Light-Forbidden Transitions in Plasmon-Emitter Interactions beyond the Weak Coupling Regime

We investigate the impact of light-forbidden exciton transitions in plasmon-emitter interactions beyond the weak coupling regime. We consider a V-type quantum emitter, with dipolar and quadrupolar excited states, placed at the subnanometric gap of a particle-on-a-mirror metallic cavity. We present a fully analytical description of the near-field population dynamics and far-field scattering spectrum of the hybrid system. Our approach enables us to reveal two realistic system configurations in which the dipole-inactive exciton alters significantly and in completely opposite ways the Purcell enhancement and Rabi splitting phenomenology, effectively enlarging or reducing the emitter lifetime and generating or removing spectral features in the cavity cross section.

Plasmonic enhancement of electroluminescence

Here plasmonic effect specifically on electroluminescence (EL) is studied in terms of radiative and nonradiative decay rates for a dipole near a metal spherical nanoparticle (NP). Contribution from scattering is taken into account and is shown to play a decisive role in EL enhancement owing to pronounced size-dependent radiative decay enhancement and weak size effect on non-radiative counterpart. Unlike photoluminescence where local incident field factor mainly determines the enhancement possibility and level, EL enhancement is only possible by means of quantum yield rise, EL enhancement being feasible only for an intrinsic quantum yield Q0 < 1. The resulting plasmonic effect is independent of intrinsic emitter lifetime but is exclusively defined by the value of Q0, emission spectrum, NP diameter and emitter-metal spacing. For 0.1< Q0 < 0.25, Ag nanoparticles are shown to enhance LED/OLED intensity by several times over the whole visible whereas Au particles feature lower effect within the red-orange range only. Independently of positive effect on quantum yield, metal nanoparticles embedded in an electroluminescent device will improve its efficiency at high currents owing to enhanced overall recombination rate which will diminish manifestation of Auger processes. The latter are believed to be responsible for the known undesirable efficiency droop in semiconductor commercial quantum well based LEDs at higher current. For the same reason plasmonics can diminish quantum dot photodegradation from Auger process induced non-radiative recombination and photoionization thus opening a way to avoid negative Auger effects in emerging colloidal semiconductor LEDs.

Improving the Radiative Efficiency of InGaN Quantum Dots via an Open Top Cavity

A self-aligned, highly tolerant “open top” cavity design is proposed and shown to enhance the spontaneous emission of InGaN quantum dots. Compared to the “closed top” counterpart, removing the metal cap, creating an “open top” cavity, enhances both the emission intensity and recombination rate. The localized surface plasmon resonance of the Ag “open top” cavity was matched to the InGaN quantum dots’ emission wavelength, resulting in an observed final emitter lifetime of 132 ps. The proposed cavity structure exhibits high cavity antenna quantum efficiency, can be self-aligned to the quantum dot, and has good tolerance to quantum dot emission wavelength, polarization, and processing variations.

Purcell effect at the percolation transition

We investigate the spontaneous emission rate of a two-level quantum emitter next to a composite medium made of randomly distributed metallic inclusions embedded in a dielectric host matrix. In the near-field, the Purcell factor can be enhanced by two-orders of magnitude relative to the case of an homogeneous metallic medium, and reaches its maximum precisely at the insulator-metal transition. By unveiling the role of the decay pathways on the emitter's lifetime, we demonstrate that, close to the percolation threshold, the radiation emission process is dictated by electromagnetic absorption in the heterogeneous medium. We show that our findings are robust against change in material properties, shape of inclusions, and apply for different effective medium theories as well as for a wide range of transition frequencies.

Field evaporation behaviour for carbon nanotube thin-film

In recent years, the carbon nanotube (CNT) emitters used for ion sources or gas sensors have been investigated, and the progress of several approaches such as field ionization and field desorption sources has been reported. However, a major concern for these applications is possible loss of CNTs caused by field evaporation, which can shorten the lifetimes of CNT-based emitters used for high electric field ion sources. So in CNT-based field emitter technology, emitter lifetime and degradation will be key parameters to be controlled. However, up to now only very few investigations in this direction have been conducted. The reason for this might lie in the fact that one often considers that the threshold value of field evaporation for a kind of material ( 40 V/nm) is much higher than the field of ionization or desorption ( 10 V/nm) according to the metal material characteristics (such as the threshold values of field evaporation for tungsten and molybdenum are 54 V/nm and 45 V/nm, respectively). In this work, the carbon nanotube thin-film (the density of CNTs is about 2.5108/cm2) is fabricated by screen-printing method, and the field evaporation behavior of CNT thin-film is studied experimentally in an ultrahigh vacuum system typically operating at a pressure of lower than 10-9 Torr after a 4-hour bake-out at ~200℃. Unlike the vertically aligned CNT array having higher electric field around the edge of the array because of the shielding effect, the printed CNT thin-film has more uniform distribution of electric field and is very easy to relize the mass production. The results show that the prepared CNT thin-film has quite obvious field evaporation behavior (some contaminants have deposited on the surface of grid after field evaporation, and energy-dispersive X-ray spectroscopy elemental mapping result of the grid indicates that the contaminants consist mainly of carbon elements), with turn-on field in a range of 10.0-12.6 V/nm, ion current could reach up to hundreds of pA. Meanwhile, the results with scanning electron microscope analysis and field electron emission measurement indicate that the CNT distribution turns into more non-uniform distribution after field evaporation; even some CNTs are directly dragged away from the substrate by the strong field. The field evaporation of CNT thin-film also leads to field electron emission onset voltage increasing from 240 V to 300 V, field enhancement factor decreasing from 8300 to 4200, and threshold field of field evaporation rising from 10.0 V/nm to 12.6 V/nm. However, the repeatability of sample treated by the field evaporation brings about an improvement to a certain extent. It could be understood in this way: upon applying a positive voltage, the most protruding parts, which have the strongest emissive capability, are evaporated first, which leads to the declined field enhancement factor; the parts of CNTs which have relatively weak emissive capability are not evaporated. So the uniformity of electric field is improved through reducing the difference in field enhancement factor rather than surface morphology between carbon nanotubes. The field evaporation of CNT thin-film is also a process which improves the uniformity of electric field. Therefore, the stability and repeatability of the field electron emission for carbon nanotube thin-film are improved naturally.

Active magneto-optical control of spontaneous emission in graphene

We investigate the spontaneous emission rate of a two-level quantum emitter near a graphene-coated substrate under the influence of an external magnetic field or strain induced pseudo-magnetic field. We demonstrate that the application of the magnetic field can substantially increase or decrease the decay rate. We show that a suppression as large as 99$\%$ in the Purcell factor is achieved even for moderate magnetic fields. The emitter's lifetime is a discontinuous function of $|{\bf B}|$, which is a direct consequence of the occurrence of discrete Landau levels in graphene. We demonstrate that, in the near-field regime, the magnetic field enables an unprecedented control of the decay pathways into which the photon/polariton can be emitted. Our findings strongly suggest that a magnetic field could act as an efficient agent for on-demand, active control of light-matter interactions in graphene at the quantum level.

Deterministic coupling of a single silicon-vacancy color center to a photonic crystal cavity in diamond.

Deterministic coupling of single solid-state emitters to nanocavities is the key for integrated quantum information devices. We here fabricate a photonic crystal cavity around a preselected single silicon-vacancy color center in diamond and demonstrate modification of the emitters internal population dynamics and radiative quantum efficiency. The controlled, room-temperature cavity coupling gives rise to a resonant Purcell enhancement of the zero-phonon transition by a factor of 19, coming along with a 2.5-fold reduction of the emitter's lifetime.

Scanning Single Quantum Emitter Fluorescence Lifetime Imaging: Quantitative Analysis of the Local Density of Photonic States

Their intrinsic properties render single quantum systems as ideal tools for quantum enhanced sensing and microscopy. As an additional benefit, their size is typically on an atomic scale that enables sensing with very high spatial resolution. Here, we report on utilizing a single nitrogen vacancy center in nanodiamond for performing three-dimensional scanning-probe fluorescence lifetime imaging microscopy. By measuring changes of the single emitter's lifetime, information on the local density of optical states is acquired at the nanoscale. Three-dimensional ab initio discontinuous Galerkin time-domain simulations are used in order to verify the results and to obtain additional insights. This combination of experiment and simulations to gather quantitative information on the local density of optical states is of direct relevance for the understanding of fundamental quantum optical processes as well as for the engineering of novel photonic and plasmonic devices.

A Reduced-Order Model for Thermionic Hollow Cathodes

A reduced-order numerical model describing the plasma in an orificed hollow cathode is presented as a quick tool for the design of thermionic cathodes. A time-independent, volume-averaged model is developed to determine plasma properties, wall temperatures, and cathode lifetime without requiring experimental data as input. A system of particle and energy balance equations is numerically solved without invoking a Saha-type equilibrium under the hypothesis of a direct-impact ionization process. Further, a lumped-parameter thermal model is coupled with the plasma model to estimate the temperature profile along the cathode axis and the emitter lifetime. The obtained results capture most of the characteristic features of this class of hollow cathodes as compared with the available experimental data. In addition, the model gives insight into the most important power deposition processes affecting the emitter and orifice regions. The effect of the geometry on both plasma parameters and cathode performance is discussed to suggest design guidelines for the development of state-of-the-art hollow cathodes.

Exciton and Polaron Quenching in Doping‐Free Phosphorescent Organic Light‐Emitting Diodes from a Pt(II)‐Based Fast Phosphor

AbstractBy introducing a neat Pt(II)‐based phosphor with a remarkably short decay lifetime, a simplified doping‐free phosphorescent organic light‐emitting diode (OLED) with a forward viewing external quantum efficiency (EQE) and power efficiency of 20.3 ± 0.5% and 63.0 ± 0.4 lm W−1, respectively, is demonstrated. A quantitative analysis of how triplet‐triplet annihilation (TTA) and triplet‐polaron annihilation (TPA) affect the device EQE roll‐off at high current densities is performed. The contributions from loss of charge balance associated with charge leakage and field‐induced exciton dissociation are found negligible. The rate constants kTTA and kTPA are determined by time‐resolved photoluminescence experiments of a thin film and an electrically‐driven unipolar device, respectively. Using the parameters extracted experimentally, the EQE is modeled versus electric current characteristics of the OLEDs by taking both TTA and TPA into account. Based on this model, the impacts of the emitter lifetime, quenching rate constants, and exciton formation zone upon device efficiency are analyzed. It is found that the short lifetime of the neat emitter is key for the reduction of triplet quenching.

Improved chopping of a lithium beam for plasma edge diagnostic at ASDEX Upgrade

The lithium beam diagnostic at ASDEX Upgrade routinely delivers electron density profiles in the plasma edge by lithium beam impact excitation spectroscopy. An accurate background subtraction requires a periodically chopped lithium beam. A new, improved chopping system was developed and installed. It involves a voltage modulation for the extractor electrode and the beam deflection plates. The modulation of the extractor electrode reduces the unused portion of lithium ions and improves the stability of the beam with respect to its position. Furthermore, the data indicate an extended emitter lifetime. The extractor chopping was also found to be insensitive to sparks. The deflection chopping experiments demonstrated beam chopping in the kilohertz range. The significantly higher modulation frequency of the deflection chopping improves background subtraction of fast transient events. It allows a more accurate density measurements in the scrape off layer during impurity injections and edge localized modes.

Scanning Emitter Lifetime Imaging Microscopy for Spontaneous Emission Control

We report an experimental technique to map and exploit the local density of optical states of arbitrary planar nanophotonic structures. The method relies on positioning a spontaneous emitter attached to a scanning probe deterministically and reversibly with respect to its photonic environment while measuring its lifetime. We demonstrate the method by imaging the enhancement of the local density of optical states around metal nanowires. By nanopositioning, the decay rate of a pointlike source of fluorescence can be reversibly and repeatedly changed by a factor of 2 by coupling it to the guided plasmonic mode of the wire.

The role of energy transfer in bioluminescence quenching by xanthene dyes

The paper reports the experimental results of bioluminescence quenching in the coupled enzyme system NADH:FMN-oxidoreductase-luciferase in the presence of xanthene dyes (fluorescein, eosin Y, erythrosin B) featured by the rate constants of intersystem crossing. From the spectral data and with the help of kinetic model the rate constants of energy transfer from emitter to dye were determined (2.9 × 10 12–6.5 × 10 13 M −1 s −1) and the emitter lifetime was estimated (1.2–2.7 ns). The calculated rate constants of energy transfer in a series of xanthene molecules are higher than the diffusion-controlled constants. The rate constants of energy transfer correlate with the probability of intersystem crossing of a dye. The combined analysis of emitter fluorescence quenching and acceptor fluorescence enhancement indicates that the significant bioluminescence intensity decrease in the presence of xanthene dyes is determined by both the quenching processes via the energy transfer and the inhibition of bioluminescent reaction.

Single photon nonlinear optics on photonic crystal chips

The promise of quantum information processing is driving developments in several different physical implementations. Photons are attractive as carriers of quantum information because they can travel long distances without losing their information through interactions with their environment. However, their passive nature can be a problem in applications such as the construction of logic gates, where it is necessary for two or more photons to interact. This interaction requires a nonlinear optical medium. Particularly strong nonlinearities are achieved when photons drive an emitter near its resonance frequency, and this nonlinearity is even greater if the photon is confined near the emitter in an optical cavity. We work with single semiconductor quantum dots (QDs) coupled to photonic crystal nanocavities. Recently, we showed that such a system enables an optical nonlinearity1 at the single-photon level: the cavity transmission spectrum changes dramatically when the power nears one intracavity photon number 〈ncav〉 per cavity lifetime (see Figure 1). The transmission spectrum obtained in the cross-polarized configuration shown in Figure 1(a) changes as plotted in Figure 1(b) when 〈ncav〉 increases from nearly zero to 〈ncav〉 ∼ 5. This nonlinearity relies on saturation of the QD, which occurs when the photon flux reaches roughly one photon per emitter lifetime. This single-photon-level nonlinearity has many promising applications. One application of particular interest in quantum information processing concerns the realization of large phase shifts on a signal beam conditioned on the intensity of a control beam. Using a homodyne setup, we measured the phase of the transmission through the cavity near the QD resonance frequency.2 As the probe power increases to 〈ncav〉 ∼ 3 and the QD saturates, we found that the phase of the transmitted beam changes by up to 0.24π . In applications such as quantum Figure 1. Resonant probing of the quantum dot (QD)-cavity system. (a) The cavity is probed by a vertically (V) polarized laser beam. The transmission of the cavity is detected in the orthogonal polarization (H) in order to reduce direct scattering from the incident beam. We model the quantum dot as an excited (e) and ground state (g) which is coupled to the cavity mode by a rate g. (b) The transmission spectrum shows the vacuum Rabi splitting due to the strongly coupled QD. The splitting disappears as the QD is saturated at an intracavity photon number 〈ncav〉 near unity. (c) The phase of the signal beam changes by up to 0.16π when the control beam intensity is raised to an incident power of 1μW, corresponding to 〈ncav〉 ≈ 1.