Nonradiative Contributions Research Articles

Strong signature of one-loop self-energy in polarization resolved nonlinear Compton scattering

The polarization dynamics of electrons including multiple nonlinear Compton scattering during the interaction of a circularly polarized ultraintense laser pulse with a counterpropagating ultrarelativistic electron beam is investigated. While electron polarization emerges mostly due to spin-flips at photon emissions, there is a nonradiative contribution to the polarization which stems from the one-loop QED radiative corrections to the self-energy, which admits of a simple physical model. We put forward a method to single out the nonradiative contribution to the polarization, employing the reflection regime of the interaction when the radiation reaction is significant. The polarization of electrons that penetrate in the forward direction through a colliding laser is shown to be dominated by the loop effect, while the reflected electrons are mostly polarized by spin-flips at photon emissions. We confirm this effect by quantum Monte Carlo simulations considering the helicity transfer from the laser field to the electrons, taking into account the opposite sign of the polarizations induced by the nonradiative loop effect and radiative spin-flip. Our Monte Carlo simulations show a polarization signal as high as $\ensuremath{\gtrsim}10%$ from the nonradiative effect, amenable for experimental detection with current technology.

Effect of the effective refractive index on the radiative decay rate in nanoparticle thin films.

In this work, we theoretically and experimentally study the influence of the optical environment on the radiative decay rate of rare-earth transitions in luminescent nanoparticles forming a thin film. We use electric dipole sources in finite-difference time-domain simulations to analyze the effect of modifying the effective refractive index of transparent layers made of phosphor nanocrystals doped with rare earth cations, and propose a correction to previously reported analytical models for calculating the radiative decay rate. Our predictions are tested against an experimental realization of such luminescent films, in which we manage to vary the effective refractive index in a gradual and controllable manner. Our model accurately accounts for the measurements attained, allows us to discriminate the radiative and non-radiative contributions to the time-resolved photoluminescence, and provides a way to rationally tune the spontaneous decay rate and hence the photoluminescence quantum yield in an ensemble of luminescent nanoparticles.

Radiative Contributions Dominate Plasmon Broadening for Post-Transition Metals in the Ultraviolet

We use classical electrodynamics calculations to investigate the plasmonic properties of the post-transition metals Al, Bi, Ga, In, and Sn, which are active in the ultraviolet, focusing in particular on the material- and resonance-dependent origins of plasmon broadening. Analytic Mie theory, the modified-long wavelength approximation, and the quasistatic dipole approximation together show that radiative processes dominate plasmon dephasing and damping in small (5–25 nm radius) Al, Bi, Ga, In, and Sn spheres. For Al, Ga, In, and Sn, the radiative contribution (∼0.5–2 eV) to the plasmon linewidth is more than 100-fold greater than the nonradiative contribution (0.001–0.02 eV) derived from the bulk dielectric function. This is significantly different than what is observed for Ag spheres, where nonradiative contributions (∼0.1 eV) are the primary source of broadening up to a radius of 25 nm. Overall, these data suggest that the plasmonic properties, dephasing, and lifetimes for Al, Ga, In, and Sn—and to a lesser extent Bi—spheres are qualitatively similar. To develop a more general understanding of the relationship between plasmon energy and linewidth, we use a model for ideal free-electron Drude metals. It is seen that the linewidth increases at higher energies even for lossless Drude metals, suggesting that the increased broadening observed in UV-active metals is a generalizable observation. These data have important implications for the use of these metals for ultraviolet plasmonics. The increased importance of radiative damping for post-transition metals could influence the ability to harvest photons, generate hot carriers, and enhance spectroscopy in the ultraviolet while providing new opportunities for manipulating high-energy photons.

A Halomanganates(II) with P,P'-Diprotonated Bis(2-Diphenylphosphinophenyl)ether: Wavelength-Excitation Dependence of the Quantum Yield and Role of the Non-Covalent Interactions.

A [H2DPEphos][MnX4] [X = Br, Cl] tetrahalomanganates(II) with P,P’-diprotonated bis[2-(diphenylphosphino)phenyl]ether cation has been designed and investigated in photophysics and EPR terms. The complexes exhibit a green luminescence resulted from the Mn(II) d–d transitions (4T1→6A1) with the wavelength-excitation dependence of the quantum yield. The solid [H2DPEphos][MnBr4] complex exhibits a bright green phosphorescence (λmax = 515 nm) with the high luminescence quantum yield depending on the excitation energy whereas the solid [H2DPEphos][MnCl4] complex exhibits a very weak phosphorescence (λmax = 523 nm). The unexpected shorter luminescence lifetime for the [H2DPEphos][MnCl4] than for the [H2DPEphos][MnBr4] at 300 K can be a result of the higher non-radiative relaxation contribution. On the one hand, the non-covalent PH…X(Mn) interactions quench the manganese(II) luminescence. On the other hand, the PH…X(Mn) interactions are a pathway of the excitation transfer from [H2DPEphos]2+ to [MnX4]2−.

Non-radiative luminescence decay with self-trapped hole migration in strontium titanate: Interplay between optical and transport properties

A novel model for the non-radiative decay of self-trapped excitons (STEs) in the advanced functional oxide SrTiO3 is proposed and supported by experimental observations. The study is based on the initial ionoluminescence stage for STE emission at 2.5 eV, and its dependence on temperature and electronic excitation rate under energetic heavy-ion irradiation. For all temperatures, this initial stage reaches rapidly a quasi-steady level, and then decreases as induced-structural damage increases. The quasi-steady luminescence exhibits a linear dependence on the excitation rate, suggesting a constant efficiency for STEs formation. An activation energy of 55 meV, essentially independent of the incident ion mass and energy of projectile-ion, is deduced from an Arrhenius-type relationship with irradiation temperature. This energy is in good agreement with experimental values, measured for non-radiative STE decay under ns-laser pulse excitation, and reasonably consistent with density functional theory calculations for migration of self-trapped holes (STHs) described by a small-polaron adiabatic hopping model. A new mechanism dealing with a non-radiative contribution to the STE transition is discussed, consisting of STH migration through thermally-activated hopping and annihilation with the STE-electron. Luminescence kinetics from the chromium intrinsic impurity strongly supports this model, being consistent with the annihilation of Cr3+ centers through recombination with migrating STHs.

Radiative p_{perp }-broadening of fast partons in an expanding quark\u2013gluon plasma

We study contribution of radiative processes to p_{perp }-broadening of fast partons in an expanding quark–gluon plasma. It is shown that the radiative correction to langle p_{perp }^2rangle for the QGP produced in AA-collisions at RHIC and LHC may be negative, and comparable in absolute value with the non-radiative contribution. We have found that the QGP expansion enhances the radiative suppression of p_perp -broadening as compared to the static medium.

Radiative Contribution to p⊥ Broadening of Fast Partons in a Quark–Gluon Plasma

The contribution of radiative processes to the p⊥ broadening of fast partons in a quark–gluon plasma is investigated. Calculations are performed beyond the soft gluon approximation. It is shown that the radiative correction to 〈$$p_{ \bot }^{2}$$〉 in conditions of collision of heavy ions at RHIC and LHC is negative and can be comparable in absolute value with the nonradiative contribution. This prediction differs radically from the essentially positive contribution of radiative processes to the p⊥ broadening, which was predicted earlier in the literature.

Periodic Green functions for 2D magneto-electric quadrupolar arrays: explicitly satisfying the optical theorem

We present all the periodic Green function dyadics that enter a description of a 2D array of emitters at the level that includes the electric dipole, magnetic dipole and electric quadrupole moment of each emitter. We find a concise analytic form for the radiative contributions to the periodic Green function dyadics that give rise to radiation reaction fields, and so our description of the scattered light explicitly satisfies the optical theorem; we give the non-radiative contributions that do not affect energy balance in the form of rapidly converging series. Finally, we present an approximation scheme for evaluating periodic Green function dyadics at long wavelengths that rigorously respects energy conservation. The scheme extends the range of validity of the usual static approximation by the inclusion of a simple dynamic correction.

Understanding Variations in Circularly Polarized Photoluminescence in Monolayer Transition Metal Dichalcogenides.

Monolayer transition metal dichalcogenides are promising materials for valleytronic operations. They exhibit two inequivalent valleys in the Brillouin zone, and the valley populations can be directly controlled and determined using circularly polarized optical excitation and emission. The photoluminescence polarization reflects the ratio of the two valley populations. A wide range of values for the degree of circularly polarized emission, Pcirc, has been reported for monolayer WS2, although the reasons for the disparity are unclear. Here, we optically populate one valley and measure Pcirc to explore the valley population dynamics at room temperature in a large number of monolayer WS2 samples synthesized via chemical vapor deposition. Under resonant excitation, Pcirc ranges from 2 to 32%, and we observe a pronounced inverse relationship between photoluminescence (PL) intensity and Pcirc. High-quality samples exhibiting strong PL and long exciton relaxation time exhibit a low degree of valley polarization, and vice versa. This behavior is also demonstrated in monolayer WSe2 samples and transferred WS2, indicating that this correlation may be more generally observed and account for the wide variations reported for Pcirc. Time-resolved PL provides insight into the role of radiative and nonradiative contributions to the observed polarization. Short nonradiative lifetimes result in a higher measured polarization by limiting opportunity for depolarizing scattering events.

Engineering the Losses and Beam Divergence in Arrays of Patch Antenna Microcavities for Terahertz Sources

We perform a comprehensive study on the emission from finite arrays of patch antenna microcavities designed for the terahertz range by using a finite element method. The emission properties including quality factors, far-field pattern, and photon extraction efficiency are investigated for etched and non-etched structures as a function of the number of resonators, the dielectric layer thickness, and period of the array. In addition, the simulations are achieved for lossy and perfect metals and dielectric layers, allowing to extract the radiative and non-radiative contributions to the total quality factors of the arrays. Our study shows that this structure can be optimized to obtain low beam divergence (FWHM 50% while keeping a strongly localized mode. These results show that the use of these microcavities would lead to efficient terahertz emitters with a low divergence vertical emission and engineered losses.

Absolute measurement of effective radiative-efficiency in GaAs grown with molecular-beam-epitaxy

In this work, we have decoupled the radiative and nonradiative contributions to recombination by developing analytical models to fit observed non-monoexponential photoluminescence decay and bulk-lifetime temperature-dependence, which has enabled absolute measurement of the effective radiative efficiency and characterization of the dominant defect in lightly doped GaAs samples grown using molecular-beam-epitaxy. The measured effective radiative efficiency values under low level injection conditions range from (88.9 ± 0.1)% and (81.2 ± 0.1)% at 77 K to (0.028 ± 0.001)% and (0.034 ± 0.001)% at 700 K, with 300 K values of (17.3 ± 0.1)% and (10.5 ± 0.1)% in the p-type and n-type samples, respectively. A common defect-signature is observed in the temperature-dependence of the nonradiative lifetime in samples of both doping types, and our measured parameters are consistent with characteristics previously measured for the EL2 defect using deep-level transient spectroscopy.

High temperature stabilization of Y2Sn2O7:Eu luminescent nanoparticles – A facile synthesis

In the present work Y2Sn2O7:Eu nanoparticles dispersed in Y2O3 matrix (Y2Sn2O7:Eu–Y2O3) have been synthesized with a view to improve the luminescence properties of Eu in Y2Sn2O7 host. These nanoparticles are found to retain their nanocrystalline nature even at elevated temperature as high as 1300°C. Luminescence from the sample has been compared with bulk and nano-size dimensions particle of neat Y2Sn2O7:Eu and Y2O3:Eu. Quantum efficiency of luminescence from Y2Sn2O7:Eu–Y2O3 samples have been found to be around 88% and is much higher than bulk and nanoparticles of Y2Sn2O7:Eu and Y2O3:Eu. This improved luminescence has been attributed to removal of surface effect by Y2O3 matrix and deterioration in the non-radiative contributions. Thus present studies provide an easy method to synthesize Y2Sn2O7:Eu nanoparticles which could avoid aggregation and bulk phase formation even at 1300°C.

Eu3+ ions imminence impact on its photoluminescence in Y2O3 host

A systematic photoluminescence study on 2% Eu-doped Y2O3 particles has been carried out. It is observed that 1300°C annealed samples show higher non-radiative contributions, poor lifetime and quantum efficiency in comparison to the samples annealed at lower temperatures (700°C and 900°C), even though the structural symmetry and emission profile remains almost unaffected by the increasing annealing temperature. Based on empirical exploration it has been established that annealing at 1300°C, reduces the average distance between Eu ions to ~6.7Å on. Odd behavior of 1300°C heated Y2O3:Eu sample has been attributed to the decreased interatomic separation i.e. increased proximity and associated increase in interaction between Eu ions. The inferences has been further supported by luminescence investigation of Y2O3 sampled co-doped with Yb–Er.

Radiative Cooling: Principles, Progress, and Potentials.

The recent progress on radiative cooling reveals its potential for applications in highly efficient passive cooling. This approach utilizes the maximized emission of infrared thermal radiation through the atmospheric window for releasing heat and minimized absorption of incoming atmospheric radiation. These simultaneous processes can lead to a device temperature substantially below the ambient temperature. Although the application of radiative cooling for nighttime cooling was demonstrated a few decades ago, significant cooling under direct sunlight has been achieved only recently, indicating its potential as a practical passive cooler during the day. In this article, the basic principles of radiative cooling and its performance characteristics for nonradiative contributions, solar radiation, and atmospheric conditions are discussed. The recent advancements over the traditional approaches and their material and structural characteristics are outlined. The key characteristics of the thermal radiators and solar reflectors of the current state‐of‐the‐art radiative coolers are evaluated and their benchmarks are remarked for the peak cooling ability. The scopes for further improvements on radiative cooling efficiency for optimized device characteristics are also theoretically estimated.

Carrier dynamics analysis for efficiency droop in GaN-based light-emitting diodes with different defect densities using time-resolved electroluminescence

We developed a direct experimental approach for investigating the correlation between efficiency droop and recombination rate variation under current injection conditions by using time-resolved electroluminescence (EL) technique. We applied this approach to understand the droop phenomenon of GaN-based light-emitting diodes grown on patterned sapphire substrates (LED-on-PAT) and planar sapphire substrates (LED-on-PLA). Because of lower dislocation density and current leakage in LED-on-PAT compared to LED-on-PLA, it was found that the effective carrier density injected into quantum wells (QWs) in LED-on-PAT was higher than that of the LED-on-PLA under the same current injection conditions, based on the analysis of spectral broadening of EL spectra with varying current injection and photoluminescence experiments under resonant and non-resonant excitation conditions. The efficiency droop in LED-on-PAT was found to be much more severe than that of LED-on-PLA, despite the higher overall quantum efficiency of LED-on-PAT. From the time-resolved EL analysis, we could separate radiative and non-radiative recombination contributions and directly observe (i) the decrease and saturation of radiative recombination time and (ii) the increase and following decrease in behavior of non-radiative recombination time with increasing current injection level, showing a strong correlation between efficiency droop and recombination rate variation.

Metric perturbations produced by eccentric equatorial orbits around a Kerr black hole

We present the first numerical calculation of the (local) metric perturbation produced by a small compact object moving on an eccentric equatorial geodesic around a Kerr black hole, accurate to first order in the mass ratio. The procedure starts by first solving the Teukolsky equation to obtain the Weyl scalar $\psi_4$ using semi-analytical methods. The metric perturbation is then reconstructed from $\psi_4$ in an (outgoing) radiation gauge, adding the appropriate non-radiative contributions arising from the shifts in mass and angular momentum of the spacetime. As a demonstration we calculate the generalized redshift $U$ as a function of the orbital frequencies $\Omega_r$ and $\Omega_\phi$ to linear order in the mass ratio, a gauge invariant measure of the conservative corrections to the orbit due to self-interactions. In Schwarzschild, the results surpass the existing result in the literature in accuracy, and we find new estimates for some of the unknown 4PN and 5PN terms in the post-Newtonian expansion of $U$. In Kerr, we provide completely novel values of $U$ for eccentric equatorial orbits. Calculation of the full self-force will appear in a forthcoming paper.

Non-radiative recombination in Ge1−ySny light emitting diodes: The role of strain relaxation in tuned heterostructure designs

This paper describes the properties of Ge1−ySny light emitting diodes with a broad range of Sn concentrations (y = 0.0–0.11). The devices are grown upon Si(100) platforms using ultra-low temperature deposition of highly reactive Ge and Sn hydrides. The device fabrication adopts two new photodiode designs which lead to optimized performance and enables a systematic study of the effects of strain relaxation on emission efficiency. In contrast with n-Ge/i-Ge1−ySny/p-Ge analogs, which in most cases contain two defected interfaces, our designs include a p-layer with composition Ge1−zSnz chosen to be z < y to facilitate light extraction, but with z close enough to y to guarantee no strain relaxation at the i/p interface. In addition, a Ge1−xSnx alloy is also used for the n layer, with compositions in the 0 ≤ x ≤ y range, so that defected and non-defected n/i interfaces can be studied. The electroluminescence spectra vs the Sn content y in the intrinsic layer of the diodes exhibit a monotonic shift in the emission wavelength from 1550 nm to 2500 nm. On the other hand, the emission intensities show a complex dependence that cannot be explained solely on the basis of Sn concentrations. Detailed theoretical modeling of these intensities makes it possible to extract recombination lifetimes that are found to be more than three times longer in samples in which strain relaxation has not occurred at the n-i interface, demonstrating the existence of a large non-radiative contribution from the relaxation defects. This finding is particularly significant for direct gap diodes with y > 0.09, for which it is practically impossible to avoid strain relaxation in n-Ge/i-Ge1−ySny/p-Ge analogs. The new designs introduced here open the door to the fabrication of highly efficient electrically pumped systems for applications in future generations of integrated photonics.

Mapping the Radiative and the Apparent Nonradiative Local Density of States in the Near Field of a Metallic Nanoantenna

We present a novel method to extract the various contributions to the photonic local density of states from near-field fluorescence maps. The approach is based on the simultaneous mapping of the fluorescence intensity and decay rate, and on the rigorous application of the reciprocity theorem. It allows us to separate the contributions of the radiative and the apparent non-radiative local density of states to the change in the decay rate. The apparent non-radiative contribution accounts for losses due to radiation out of the detection solid angle and to absorption in the environment. Data analysis relies on a new analytical calculation, and does not require the use of numerical simulations. One of the most relevant applications of the method is the characterization of nanostructures aimed at maximizing the number of photons emitted in the detection solid angle, which is a crucial issue in modern nanophotonics.

Thermal hyperconductivity: Radiative energy transport in hyperbolic media

We develop a theoretical description of radiative thermal conductivity in hyperbolic metamaterials. We demonstrate a dramatic enhancement of the radiative thermal transport due to the super-singularity of the photonic density of states in hyperbolic media, leading to the radiative heat conductivity which can be comparable to the non-radiative contribution.

Collective eigenstates of emission in an N-entity heterostructure and the evaluation of its Green tensors and self-energy components

Optical emission from emitters strongly interacting among themselves and also with other polarizable matter in close proximity has been approximated by emission from independent emitters. This is primarily due to our inability to evaluate the self-energy matrices and radiative properties of the collective eigenstates of emitters in heterogeneous ensembles. A method to evaluate self-energy matrices that is not limited by the geometry and material composition is presented to understand and exploit such collective excitations. Numerical evaluations using this method are used to highlight the significant differences between independent and the collective modes of emission in nanoscale heterostructures. A set of N Lorentz emitters and other polarizable entities is used to represent the coupled system of a generalized geometry in a volume integral approach. Closed form relations between the Green tensors of entity pairs in free space and their correspondents in a heterostructure are derived concisely. This is made possible for general geometries because the global matrices consisting of all free-space Green dyads are subject to conservation laws. The self-energy matrix can then be assembled using the evaluated Green tensors of the heterostructure, but a decomposition of its components into their radiative and nonradiative decay contributions is nontrivial. The relations to compute the observables of the eigenstates (such as quantum efficiency, power/energy of emission, radiative and nonradiative decay rates) are presented. A note on extension of this method to collective excitations, which also includes strong interactions with a surface in the near-field, is added.