Dipole Emission Research Articles

Carbon-Related Quantum Emitter in Hexagonal Boron Nitride with Homogeneous Energy and 3-Fold Polarization.

Most hexagonal boron nitride (hBN) single-photon emitters (SPEs) studied to date suffer from variable emission energy and unpredictable polarization, two crucial obstacles to their application in quantum technologies. Here, we report an SPE in hBN with an energy of 2.2444 ± 0.0013 eV created via carbon implantation that exhibits a small inhomogeneity of the emission energy. Polarization-resolved measurements reveal aligned absorption and emission dipole orientations with a 3-fold distribution, which follows the crystal symmetry. Photoluminescence excitation (PLE) spectroscopy results show the predictability of polarization is associated with a reproducible PLE band, in contrast with the non-reproducible bands found in previous hBN SPE species. Photon correlation measurements are consistent with a three-level model with weak coupling to a shelving state. Our ab initio excited-state calculations shed light on the atomic origin of this SPE defect, which consists of a pair of substitutional carbon atoms located at boron and nitrogen sites separated by a hexagonal unit cell.

Robust valley quantum coherence in synthetic 3R-phase MoS2: A material for future valley based devices

Two-dimensional layered transition metal dichalcogenides (TMDCs) offer the ideal platform to optically initialize the qubits utilizing the superposition of valley polarized photons. However, in the commonly available 2H phase TMDCs, thickness sensitive crystal inversion symmetry demands the precise control over the number of layers, which makes the study of valley physics challenging. On the other hand, 3R-polymorphic phase TMDCs are non-centrosymmetric irrespective of the number of layers and therefore retain valley degree of freedom for all the thicknesses. Here, using polarization resolved photoluminescence measurements under linearly polarized excitations, we demonstrate the coherent superposition of the valley photons (known as valley coherence) in synthetic 3R-phase MoS2 with different numbers of layers ranging from 3 layers to 11 layers. With near-resonant excitation (633 nm for AX0), the degree of linear polarization (a measure of the valley coherence) is observed up to 70% at 80 K measurement temperatures and is found to be layer thickness independent. Robust valley coherence is attributed to the high optical quality and the 3R crystal symmetry of the MoS2. Using angle resolved polarization dependent measurements, it is established that the net dipolar emission aligns with the polarization orientations of the incident laser, which signifies the valley coherence to be independent of the crystal orientation. This study paves the way toward using 3R-phase MoS2 as a key material for the development of future quantum technologies utilizing valley polarized photons.

GW190425: Pan-STARRS and ATLAS coverage of the skymap and limits on optical emission associated with FRB 20190425A

ABSTRACT GW190425 is the second of two binary neutron star (BNS) merger events to be significantly detected by the Laser Interferometer Gravitational Wave (GW) Observatory (LIGO), Virgo and the Kamioka Gravitational Wave (KAGRA) detector network. With a detection only in LIGO Livingston, the skymap containing the source was large and no plausible electromagnetic counterpart was found in real-time searching in 2019. Here, we summarize Asteroid Terrestrial-Impact Last Alert System (ATLAS) and Panoramic Survey Telescope and Rapid Response System (Pan-STARRS) wide-field optical coverage of the skymap beginning within 1 and 3 h, respectively, of the GW190425 merger time. More recently, a potential coincidence between GW190425 and a fast radio burst FRB 20190425A has been suggested, given their spatial and temporal coincidences. The smaller sky localization area of FRB 20190425A and its dispersion measure led to the identification of a likely host galaxy, UGC 10667 at a distance of 141 ± 10 Mpc. Our optical imaging covered the galaxy 6.0 h after GW190425 was detected and 3.5 h after the FRB 20190425A. No optical emission was detected and further imaging at +1.2 and +13.2 d also revealed no emission. If the FRB 20190425A and GW190425 association were real, we highlight our limits on kilonova emission from a BNS merger in UGC 10667. The model for producing FRB 20190425A from a BNS merger involves a supramassive magnetized neutron star spinning down by dipole emission on the time-scale of hours. We show that magnetar-enhanced kilonova emission is ruled out by optical upper limits. The lack of detected optical emission from a kilonova in UGC 10667 disfavours, but does not disprove, the FRB–GW link for this source.

Design of external microtextures for efficient light outcoupling in OLEDs with different preferential orientation of emission dipoles

Design of external microtextures for efficient light outcoupling in OLEDs with different preferential orientation of emission dipoles

Highly Tunable Dielectric Nano Antenna Consisting Chain of Silicon Particles by Dipole Emitter

Highly Tunable Dielectric Nano Antenna Consisting Chain of Silicon Particles by Dipole Emitter

Optical characterization of a single molecule complete spatial orientation using intra-molecular triplet-triplet absorption.

Progress in single molecule fluorescence experiments have enabled an in-depth characterization of fluorophores, ranging from their photophysical rates to the orientation of their emission dipole moments in three dimensions. However, one crucial spatial information remains elusive: the molecule orientation relative to its emission dipole moment. One can retrieve the latter only by the use of another non-colinear transition dipole moment. We experimentally demonstrate the optical retrieval of this information for single terrylene (Tr) molecules in a 30 nm thin para-terphenyl matrix. We show, through second-order correlation measurements at varying excitation power and polarization, that Tr molecules experience an optically induced deshelving of their triplet states, mediated by two orthogonal intra-molecular triplet-triplet absorption dipole moments. We take advantage of these two transition dipole moments to retrieve the full orientation of the Tr molecule, employing a 3-level scheme for the molecule photophysics and analytical calculations for the exciting electric field distribution. This modelling approach enables us to accurately describe both varying power and polarization measurements, giving access to the molecule's photophysical rates and to its complete orientation in three dimensions. This includes the orientation of the singlet emission dipole moment in the laboratory frame, and the orientation of the molecule plane with respect to the singlet emission dipole moment.

Investigation of unidirectional coupling of dipole emitters in valley photonic heterostructure waveguides.

Photonic heterostructure has recently become a promising platform to study topological photonics with the introduction of mode width degree of freedom (DOF). However, there is still a lack of comprehensive analysis on the coupling of dipole emitters in photonic heterostructures, which constrains the development of on-chip quantum optics based on chiral dipole sources. We systematically analyze the unidirectional coupling mechanism between dipole emitters and valley photonic heterostructure waveguides (VPHWs). With the eigenmode calculations and full-wave simulations, the Stokes parameters are obtained to compare the coupling performance of two types of valley-interface VPHWs. Simulation results show that compared to the zigzag interface with inversion symmetry, the strategy of bearded interface with glide symmetry is easier to realize high-efficiency coupling. By adjusting the position and chirality of dipole emitters in VPHWs, the transmission of light reverses with guided modes coupled to different directions. Furthermore, a topological beam modulator is realized based on VPHWs, which maintains the robustness to large-area potential barriers and sharp corners. Our work supplies a powerful guide for chiral light-matter interaction, which is expected to be applied to increasingly compact and efficient on-chip optical platforms in the future.

Color Routing of the Emission from Magnetic and Electric Dipole Transitions of Eu3+ by Broken-Symmetry TiO2 Metasurfaces.

Manipulation of magnetic dipole emission with resonant photonic nanostructures is of great interest for both fundamental research and applications. However, obtaining selective control over the emission properties of magnetic dipole transitions is challenging, as they usually occur within a manifold of spectrally close emission lines associated with different spin states of the involved electronic levels. Here we demonstrate spectrally selective directional tailoring of magnetic dipole emission using designed photonic nanostructures featuring a high quality factor. Specifically, we employ a hybrid nanoscale optical system consisting of a Eu3+ compound coupled to a designed broken-symmetry TiO2 metasurface to demonstrate directional color routing of the compound's emission through its distinct electric and magnetic-dominated electronic transition channels. Using low numerical aperture collection optics, we achieve a fluorescence signal enhancement of up to 33.13 for the magnetic-dominated dipole transition at 590 nm when it spectrally overlaps with a spectrally narrow resonance of the metasurface. This makes the, usually weak, magnetic dipole transition the most intense spectral line in our recorded fluorescence spectra. By studying the directional emission properties for the coupled system using Fourier imaging and time-resolved fluorescence measurements, we demonstrate that the high-quality-factor modes in the metasurface enable free-space light routing, where forward-directed emission is established for the magnetic-dominated dipole transition, whereas the light emitted via the electric dipole transition is mainly directed sideways. Our results underpin the importance of magnetic light-matter interactions as an additional degree of freedom in photonic and optoelectronic systems. Moreover, they facilitate the development of spectrometer-free and highly integrated nanophotonic imaging, sensing, and probing devices.

Elucidating The Horizontal Orientation Mechanism of Emissive Transition Dipole Moment in A Series of Stick‐Like Delayed Fluorescent Emitters for Ultra‐High‐Efficiency OLEDs

AbstractThe horizontal orientation of the emissive transition dipole moment (TDM) of emissive molecules is a crucial factor in improving the efficiency of organic light‐emitting diodes (OLEDs). However, the mechanism of this horizontal orientation remains unclear. Herein, to elucidate the horizontal orientation mechanism of the TDM of the molecules in thermally activated delayed fluorescent (TADF) emitters, the relationship between the horizontal orientation ratio (Θ) of the TDM and the key parameters of stick‐like TADF emitters dispersed in carbazole‐based host materials is systematically and quantitatively investigated. The introduction of functional groups containing weak CH/n (n = O, N) hydrogen bonds into the host material is found to significantly increase the Θ values up to 30%. The physical parameters of the dispersed emitter exhibit a strong relationship with the Θ values, with the following influence order: glass transition temperature (Tg) ≥ total surface area of the largest π‐plane and the corresponding parallel π‐plane > molecular weight > aspect ratio > permanent dipole moment. The Tg value of the host material is another key parameter determining the Θ values. By using a P=O‐based host material, namely mCP2PO, a high PLQY of 97%, a high Θ value of 88%, and a sky‐blue OLED with an EQE of 37.6% are simultaneously realized.

Highly luminescent ultra-thin films with rare earth for plasmonic applications

Amphiphilic complexes with luminescent rare earth metal ions suitable for Lanmuir-Blodgett (LB) deposition have been synthesized. LB monolayers with closely packed Eu complexes deposited directly on silver demonstrate significant far-field emission in contrast to the theoretical predictions of full quenching. Angular radiation and polarization patterns of the electric and magnetic dipole emission of Eu3+ point to a high excitation efficiency of surface plasmon polaritons. Different luminescent behavior of closely packed emitters in comparison to diluted systems is tentatively attributed to the collective state of emitters in LB layers formed via near-field coupling with surface plasmons.

Emission Dipole and Pressure‐Driven Tunability of Second Harmonic Generation in vdWs Ferroelectric NbOI2

Abstract2D in‐plane ferroelectric NbOI2 exhibits strong second harmonic generation (SHG) and ultrahigh effective susceptibility. To push forward their applications in nonlinear photonics and optoelectronics, it is highly desirable to understand the emission dipole orientation and tunability of SHG, which is not achieved. Here, by integrating tight focusing from parabolic mirror with back focal plane (BFP) imaging technique, for the first time it is demonstrated that SHG emission of NbOI2 presents purely in‐plane dipole orientation in consistent with numerical simulations, suggesting the in‐plane components of the SHG susceptibility tensor in NbOI2 dominate the emission. Moreover, with the aid of ab‐initio calculations, it is found that the hydrostatic pressure can dramatically change the structure and resultant SHG intensity of NbOI2. Explicitly, SHG intensity endures a slight increase due to the distortion of octahedral at low pressure pressure, and then monotonously decreases due to the improvement of structural symmetry with further increasing pressure, and drastically quenching resulting from the ferroelectric to paraelectric phase transition. This work unambiguously demonstrates the dipole emission behavior of SHG and the relationship between structural evolution and SHG intensity, which provides an avenue for tunable nonlinear optics and optoelectronics.

Expanded multiple-resonance structure for highly efficient narrowband deep-blue organic light-emitting diodes

Excellent color purity and high external quantum efficiency (EQE) are major requirements in the development of deep-blue organic light-emitting diodes (OLEDs). To achieve this, multiple-resonance (MR)–thermally activated delayed fluorescence (TADF) emitters have been considered as promising options. Herein, we suggest a novel expanded MR design strategy to fabricate deep-blue MR–TADF emitters derived from a fused indolo[3,2,1-jk]carbazole framework. The expanded MR structure managed a triplet excited state for the accelerated spin–vibronic coupling-assisted reverse intersystem crossing and increased the emission dipole orientation while maintaining the high efficiency and deep-blue emission color. The rigid and planar structure of the MR core yielded a small full-width at half-maximum (FWHM; less than 16 nm), high photoluminescence quantum yield (over 97%), and high horizontal emitting dipole orientation (over 90%), and facilitated a second-order spin–vibronic coupling-assisted triplet-to-singlet spin crossover. The fabricated MR–TADF OLEDs recorded a high EQE of 24.3% and FWHM of 21 nm at a CIEy of 0.044, thereby satisfying the BT.2020 blue standard. Additionally, further optimized device architecture provided an EQE of 26.8%.

Tuning the Photoluminescence Anisotropy of Semiconductor Nanocrystals.

Semiconductor nanocrystals are promising optoelectronic materials. Understanding their anisotropic photoluminescence is fundamental for developing quantum-dot-based devices such as light-emitting diodes, solar cells, and polarized single-photon sources. In this study, we experimentally and theoretically investigate the photoluminescence anisotropy of CdSe semiconductor nanocrystals with various shapes, including plates, rods, and spheres, with either wurtzite or zincblende structures. We use defocused wide-field microscopy to visualize the emission dipole orientation and find that spheres, rods, and plates exhibit the optical properties of 2D, 1D, and 2D emission dipoles, respectively. We rationalize the seemingly counterintuitive observation that despite having similar aspect ratios (width/length), rods and long nanoplatelets exhibit different defocused emission patterns by considering valence band structures calculated using multiband effective mass theory and the dielectric effect. The principles are extended to provide general relationships that can be used to tune the emission dipole orientation for different materials, crystalline structures, and shapes.

Control of light emission of quantum emitters coupled to silicon nanoantenna using cylindrical vector beams

Light emission of europium (Eu3+) ions placed in the vicinity of optically resonant nanoantennas is usually controlled by tailoring the local density of photon states (LDOS). We show that the polarization and shape of the excitation beam can also be used to manipulate light emission, as azimuthally or radially polarized cylindrical vector beam offers to spatially shape the electric and magnetic fields, in addition to the effect of silicon nanorings (Si-NRs) used as nanoantennas. The photoluminescence (PL) mappings of the Eu3+ transitions and the Si phonon mappings are strongly dependent of both the excitation beam and the Si-NR dimensions. The experimental results of Raman scattering and photoluminescence are confirmed by numerical simulations of the near-field intensity in the Si nanoantenna and in the Eu3+-doped film, respectively. The branching ratios obtained from the experimental PL maps also reveal a redistribution of the electric and magnetic emission channels. Our results show that it could be possible to spatially control both electric and magnetic dipolar emission of Eu3+ ions by switching the laser beam polarization, hence the near field at the excitation wavelength, and the electric and magnetic LDOS at the emission wavelength. This paves the way for optimized geometries taking advantage of both excitation and emission processes.

Selective Enhancement of Crystal‐Field‐Split Narrow f‐f Emission Lines of Europium Ions by Electric and Magnetic Purcell Effect of Mie Resonant Silicon Nanosphere

AbstractNarrow‐band Purcell enhancement for electric and magnetic dipole emitters by high‐order Mie resonances up to the magnetic and electric octupole modes of a silicon nanosphere antenna is experimentally demonstrated. Eu3+ complexes are attached on the surface of a silicon nanosphere 160 to 316 nm in diameter, and the photoluminescence and scattering properties are investigated. It is shown that the branching ratio of the 5D0→7Fj (j = 0–4) f‐f transitions of Eu3+ is controlled in a wide range by tuning the resonance wavelength of a silicon nanosphere by the size. Because of the high‐quality factor resonances, not only a specific 5D0→7Fj transition, but also a specific Stark sublevel transition whose spectral separation is 3–9 nm can be selectively enhanced by precisely controlling the size of a silicon nanosphere with the accuracy of ≈2 nm.

A long-period radio transient active for three decades.

Several long-period radio transients have recently been discovered, with strongly polarized coherent radio pulses appearing on timescales between tens to thousands of seconds1,2. In some cases, the radio pulses have been interpreted as coming from rotating neutron stars with extremely strong magnetic fields, known as magnetars; the origin of other, occasionally periodic and less-well-sampled radio transients is still debated3. Coherent periodic radio emission is usually explained by rotating dipolar magnetic fields and pair-production mechanisms, but such models do not easily predict radio emission from such slowly rotating neutron stars and maintain it for extended times. On the other hand, highly magnetic isolated white dwarfs would be expected to have long spin periodicities, but periodic coherent radio emission has not yet been directly detected from these sources. Here we report observations of a long-period (21 min) radio transient, which we have labelled GPM J1839-10. The pulses vary in brightness by two orders of magnitude, last between 30 and 300 s and have quasiperiodic substructure. The observations prompted a search of radio archives and we found that the source has been repeating since at least 1988. The archival data enabled constraint of the period derivative to <3.6 × 10-13 s s-1, which is at the very limit of any classical theoretical model that predicts dipolar radio emission from an isolated neutron star.

Engineering the Macrocyclic Donor Structures towards Deep-Blue Thermally Activated Delayed Fluorescence Emitters.

Deep-blue thermally activated delayed fluorescence (TADF) molecules present promising potential in organic light-emitting diodes (OLEDs), especially for display applications. Here, an efficient molecular engineering approach to modifying the donor or acceptor features of the D-π-A-configured TADF molecules for deep-blue emission is reported. By introducing oxygen and sulfone as a bridge unit onto the macrocyclic donor, two emitters, c-ON-MeTRZ and c-NS-MeTRZ, are synthesized and characterized, respectively. The reduced donor strength of c-ON-MeTRZ and c-NS-MeTRZ as compared to that of the model molecule c-NN-MeTRZ leads to blue-shifted emissions with high photoluminescence quantum yields (PLQYs) and retains TADF characters, while the new emitter c-NN-MePym with the most blue-shifted emission only exhibits a pure fluorescent nature because of the electron-accepting feature of pyrimidine that is insufficient for inducing the TADF property. In the presence of macrocyclic donors, these new emitters show high horizontal dipole ratios (Θ// = 85-89%), which are beneficial for improving the light out-coupling efficiency. Deep-blue TADF OLEDs incorporating c-ON-MeTRZ as an emitter doped in the mCPCN host achieves a high maximum external quantum efficiency (EQEmax) of 30.2% together with 1931 Commission Internationale de I'Eclairage (CIE) coordinates of (0.14, 0.13), while the counter device employing c-NS-MeTRZ as a dopant gives EQEmax of 15.4% and CIE coordinates of (0.14, 0.09). The EQEmax of c-ON-MeTRZ- and c-NS-MeTRZ-based devices can be significantly improved to 34.4 and 29.3%, respectively, with a polar host DPEPO, which stabilizes the charge transfer (CT) S1 state to give lower ΔEST for improving the reverse intersystem crossing process. The efficient TADF character, high PLQYs, and high anisotropic emission dipole ratios work together to render the superior electroluminescence (EL) efficiencies. Based on the detailed characterizations of physical properties, theoretical analyses, and comprehensive study on the corresponding devices, a clear structure-property-performance relationship has been successfully established to verify the effective molecular design strategy of modulating the macrocyclic donor characters for efficient deep-blue TADF emitters.

Strong Purcell effect of magnetic quasi-BICs in the dielectric metasurface

The ultra-strong light field trapped in micro- and nanostructures, and derived from optical bound states in the continuums (BICs), provides a new platform for the facilitation of light–matter interactions. In this work, the spontaneous emission enhancement of quantum emitters using magnetic quasi-BICs metasurfaces is numerically studied. It is found that ultrahigh Purcell factor (PF) () can be easily achieved when the asymmetry parameter decreases. In theory, infinite PF may emerge due to the infinite Q-factor at the BICs. In addition, the PF exhibits a strong dependence on the polarization direction of dipole emitter and the local field distribution in the metasurface. Finally, the photoluminescence enhancement for different perturbation parameters is calculated to confirm strong Purcell effect in the quasi-BICs metasurface. These results show that the magnetic dipole BICs mode holds an enormous potential in manipulating spontaneous emission.

A tip-enhanced quantum emitter with integrated TiO2 slot waveguides in the optical regime

We study the coupling between a nanoscopic dielectric slot waveguide and a metallic-tip-enhanced dipole quantum emitter and search for optimal emission and guiding of photons along a titanium dioxide photonic waveguide. Finite element calculations are used to characterize the mode properties of the waveguide over a range of parameters and predict the efficiency of emission guidance along the waveguide. We show how the effective quantum yield is dependent on the waveguide parameters as well as the dipole position and orientation and show that the integrated system can reach a maximum quantum yield of more than 30% along each direction of the waveguide. By placing the dipole emitter near the apex of a silver nanotip situated above or inside the slot waveguide to increase the overall emission rate, we also enable the capability of controlling the emitter–waveguide​ coupling in situ. We numerically compute the excitation and radiation fields and find that despite a reduction in the quantum yield, a 35-fold increase in the overall emission rate can be obtained due to very large field enhancement factors of up to 4000 at the location of the dipole. By using alternative materials for the tip, this tip-enhanced-waveguide approach has the potential of further increasing the guided photon emission rate. With the possibility of controlling emitter–waveguide coupling in situ, this tip-enhanced emitter configuration provides an alternative approach for the realization of an efficient single-photon source.

Numerical Studies of Back Reaction Effects in an Analog Model of Cosmological Preheating.

We theoretically propose an atomic Bose-Einstein condensate as an analog model of backreaction effects during the preheating stage of the early Universe. In particular, we address the out-of-equilibrium dynamics where the initially excited inflaton field decays by parametrically exciting the matter fields. We consider a two-dimensional, ring-shaped BEC under a tight transverse confinement whose transverse breathing mode and the Goldstone and dipole excitation branches simulate the inflaton and quantum matter fields, respectively. A strong excitation of the breathing mode leads to an exponentially growing emission of dipole and Goldstone excitations via parametric pair creation: Our numerical simulations of the BEC dynamics show how the associated backreaction effect results not only in an effective friction of the breathing mode, but also in a quick loss of longitudinal spatial coherence of the initially in-phase excitations. Implications of this result on the validity of the usual semiclassical description of backreaction are finally discussed.