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At least 271 records · Page 15

Mitigation of birefringence in cavity-based quantum networks using frequency-encoded photons

Atom-cavity systems offer unique advantages for building large-scale distributed quantum computers by providing strong atom-photon coupling while allowing for high-fidelity local operations of atomic qubits. However, in prevalent schemes where the photonic state is encoded in polarization, cavity birefringence introduces an energy splitting of the cavity eigenmodes and alters the polarization states, thus limiting the fidelity of remote entanglement generation. To address this challenge, we propose a scheme that encodes the photonic qubit in the frequency degree-of-freedom. The scheme relies on resonant coupling of multiple transverse cavity modes to different atomic transitions that are well-separated in frequency. We numerically investigate the temporal properties of the photonic wavepacket, two-photon interference visibility, and atom-atom entanglement fidelity under various cavity polarization-mode splittings and find that our scheme is less affected by cavity birefringence. Finally, we propose practical implementations in two trapped ion systems, using the fine structure splitting in the metastable D state of 40 Ca + , and the hyperfine splitting in the ground state of 225 Ra + . Furthermore, our study presents an alternative approach for cavity-based quantum networks that is less sensitive to birefringent effects, and is applicable to a variety of atomic and solid-state emitter-cavity interfaces.

Cavity quantum electrodynamics↗

Enhanced Emission from Bright Excitons in Asymmetrically Strained Colloidal CdSe/Cd x Zn 1– x Se Quantum Dots

Colloidal CdSe quantum dots (QDs) designed with a high degree of asymmetric internal strain have recently been shown to host a number of desirable optical properties including subthermal room-temperature line widths, suppressed spectral diffusion, and high photoluminescence (PL) quantum yields. It remains an open question, however, whether they are well-suited for applications requiring emission of identical single photons. Here we measure the low-temperature PL dynamics and the polarization-resolved fluorescence line narrowing spectra from ensembles of these strained QDs. Our spectroscopy reveals the radiative recombination rates of bright and dark excitons, the relaxation rate between the two, and the energy spectra of the quantized acoustic phonons in the QDs that can contribute to relaxation processes. In comparison to conventional colloidal CdSe/ZnS core/shell QDs, we find that in asymmetrically strained CdSe QDs over six times more light is emitted directly by the bright exciton. Furthermore, these results are therefore encouraging for the prospects of chemically synthesized colloidal QDs as emitters of single indistinguishable photons.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Achieving extreme light confinement in low-index dielectric resonators through quasi-bound states in the continuum

Obtaining large field enhancement in low-refractive-index dielectric materials is highly relevant to many photonic and quantum optics applications. However, confining light in these materials is challenging, owing to light leakage through coupling to continuum modes in the surrounding environment. Here, we investigate the possibility of achieving high quality factors in low-index dielectric resonators through the bound states in the continuum (BIC). Our simulations demonstrate that destructive interference between leaky modes can be achieved by tuning the geometrical parameters of the resonator arrays, leading to the emergence of quasi-BIC in resonators that have a small index contrast to the underlying substrates. The resultant large field enhancement gives rise to giant quality factors and Purcell effects. By introducing vertical mirror symmetry, the quasi-BIC can be tuned into an ideal BIC. In addition, the quasi-BIC can modify the emission patterns of the coupled emitters, rendering highly directional and focused far-field emission. These findings may provide a path for the practical implementation of photonic and quantum devices based on low-index dielectric materials.

42 ENGINEERING↗

Room‐Temperature Phosphorescent Platinum(II) Alkynyls with Microsecond Lifetimes Bearing a Strong‐Field Pincer Ligand

Abstract The use of organometallic triplet emitters in organic light emitting diodes (OLEDs) is motivated by the premise of efficient intersystem crossing leading to unit internal quantum efficiencies. However, since most devices are based on solid‐state components, an inherent limitation to square‐planar platinum(II) phosphors is their tendency toward aggregation‐based quenching. Here, a new class of emissive, four‐coordinate Pt II species based on the bisimidazolyl carbazolide (BIMCA) ligand is introduced, which displays highly efficient, long‐lived solid‐state phosphorescence at room temperature. A set of four BIMCAPt phenyl acetylides were synthesized that emit in the green ( λ max =507–540 nm) with >60 % quantum yield and millisecond lifetimes. The structures of the resulting species reveal a non‐planar structure imposed by steric clashes between BIMCA and the iodo or alkynyl co‐ligand. Ground‐state and photophysical characterization are presented. Density functional theory calculations indicate that the BIMCA ligand dominates the frontier orbitals along with the first Franck–Condon singlet and triplet excited states.

Liska, Tadeas↗

Experimental 3-dimensional tracking of the dynamics of a single electron in the Fermilab Integrable Optics Test Accelerator (IOTA)

We present the results of experimental studies on the transverse and longitudinal dynamics of a single electron in the IOTA storage ring. IOTA is a flexible machine dedicated to beam physics experiments with electrons and protons. A method was developed to reliably inject and circulate a controlled number of electrons in the ring. A key beam diagnostic system is the set of sensitive high-resolution digital cameras for the detection of synchrotron light emitted by the electrons. With 60–130 electrons in the machine, we measured beam lifetime and derived an absolute calibration of the optical system. At exposure times of 0.5 s, the cameras were sensitive to individual electrons. Camera images were used to reconstruct the time evolution of oscillation amplitudes of a single electron in all 3 degrees of freedom. The evolution of amplitudes directly showed the interplay between synchrotron-radiation damping, quantum excitations, and scattering with the residual gas. From the distribution of measured single-electron oscillation amplitudes, we deduced transverse emittances, momentum spread, damping times, and beam energy. Estimates of residual-gas density and composition were calculated from the measured distributions of vertical scattering angles. Combining scattering and lifetime data, we also provide an estimate of the aperture of the ring. To our knowledge, this is the first time that the dynamics of a single electron are tracked in all three dimensions with digital cameras in a storage ring.

43 PARTICLE ACCELERATORS↗

Ab initio evaluation of the electronic and optical properties of V B C B defect in wurtzite boron nitride as promising single-photon emitter

Single-photon emitters (SPEs) in the near-infrared (NIR) range with sharp and intense zero-phonon lines (ZPLs) of emission are critical for quantum communications. Certain local defects in wide-bandgap semiconductors create isolated occupied and unoccupied states within the bandgap of the host semiconductor and thus exhibit sharp ZPLs of emission. We designed and studied a defect in the wurtzite boron nitride as a potential SPE. It consists of a boron vacancy and a carbon atom substituting another boron atom (V B C B defect). The density of states is obtained within the GW method to identify favorable local defect states that may dominate optical transitions. The dielectric function and oscillator strength of the V B C B defect are obtained using the Bethe-Salpeter equation method to identify the optical excitations of the V B C B defect, from which we conclude that the defect could be a source of NIR emission with a narrow bright ZPL peak, thus an efficient SPE.

36 MATERIALS SCIENCE↗

On-demand directional microwave photon emission using waveguide quantum electrodynamics

Routing quantum information between non-local computational nodes is a foundation for extensible networks of quantum processors. Quantum information transfer between arbitrary nodes is generally mediated either by photons that propagate between them or by resonantly coupling nearby nodes. The utility is determined by the type of emitter, propagation channel and receiver. Conventional approaches involving propagating microwave photons have limited fidelity due to photon loss and are often unidirectional, whereas architectures that use direct resonant coupling are bidirectional in principle but can generally accommodate only a few local nodes. Here we demonstrate high-fidelity, on-demand, directional, microwave photon emission. We do this using an artificial molecule comprising two superconducting qubits strongly coupled to a bidirectional waveguide, effectively creating a chiral microwave waveguide. Quantum interference between the photon emission pathways from the molecule generates single photons that selectively propagate in a chosen direction. This circuit will also be capable of photon absorption, making it suitable for building interconnects within extensible quantum networks.

42 ENGINEERING↗

Super-resolution Imaging of Plasmonic Near-Fields: Overcoming Emitter Mislocalizations

Plasmonic nano-objects have shown great potential in enhancing applications like biological/chemical sensing, light harvesting and energy transfer, and optical/quantum computing. Therefore, an extensive effort has been vested in optimizing plasmonic systems and exploiting their field enhancement properties. Super-resolution imaging with quantum dots (QDs) is a promising method to probe plasmonic near-fields but is hindered by the distortion of the QD radiation pattern. Here, we investigate the interaction between QDs and “L-shaped” gold nanoantennas and demonstrate both theoretically and experimentally that this strong interaction can induce polarization-dependent modifications to the apparent QD emission intensity, polarization, and localization. Based on FDTD simulations and polarization-modulated single-molecule microscopy, we show that the displacement of the emitter’s localization is due to the position-dependent interference between the emitter and the induced dipole, and can be up to 100 nm. Our results help pave a pathway for higher precision plasmonic near-field mapping and its underlying applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-efficiency solar thermophotovoltaic system using a nanostructure-based selective emitter

Herein, we present the design, fabrication, optimization, and experimental results of a high-efficiency planar solar thermophotovoltaic (STPV) system utilizing a micro-textured absorber and a nanostructure multilayer metal-dielectric coated selective emitter fabricated on a tungsten (W) substrate. Light absorptance of more than 90% was achieved at visible and near-infrared wavelengths using the microtextured absorbing surface. The nanostructure selective emitter consists of two thin-film optical coatings of silicon nitride (Si3N4) and a layer of W in between to increase the surface emissivity in spectral regimes matching the quantum efficiency of the thermophotovoltaic (TPV) cells. Gallium antimonide (GaSb)-based TPV cells are used in our STPV design. The experiment was conducted at different operating temperatures using a high-power continuous wave laser diode stack as a simulated source of concentrated incident radiation. Our experimental setup measured a maximum electrical output power density of 1.71 W/cm 2 at 1676 K STPV temperature, and the overall power conversion efficiency of 8.4% after normalizing the output power density to the emitter area. This is the highest STPV system efficiency reported so far for any experimental STPV device. The incident optical laser power on the absorber side was 131 W. This is equivalent to a solar concentration factor of ~2100, which is within the practical limit and readily achievable with Fresnel lens setup.

14 SOLAR ENERGY↗

Arrays of Si vacancies in 4 H -SiC produced by focused Li ion beam implantation

Point defects in SiC are an attractive platform for quantum information and sensing applications because they provide relatively long spin coherence times, optical spin initialization, and spin-dependent fluorescence readout in a fabrication-friendly semiconductor. The ability to precisely place these defects at the optimal location in a host material with nano-scale accuracy is desirable for integration of these quantum systems with traditional electronic and photonic structures. Here, we demonstrate the precise spatial patterning of arrays of silicon vacancy (${V}_{Si}$) emitters in an epitaxial 4H -SiC (0001) layer through mask-less focused ion beam implantation of Li + . We characterize these arrays with high-resolution scanning confocal fluorescence microscopy on the Si-face, observing sharp emission lines primarily coming from the ${V1}^{{\prime}}$ zero-phonon line (ZPL). The implantation dose is varied over 3 orders of magnitude, leading to ${V}_{Si}$ densities from a few per implantation spot to thousands per spot, with a linear dependence between ZPL emission and implantation dose. Optically-detected magnetic resonance (ODMR) is also performed, confirming the presence of V2 ${V}_{Si}$. Our investigation reveals scalable and reproducible defect generation.

36 MATERIALS SCIENCE↗

Thermal emittance and lifetime of alkali-antimonide photocathodes grown on GaAs and molybdenum substrates evaluated in a –300 kV dc photogun

In this work, Cs x K y Sb photocathodes grown on GaAs and molybdenum substrates were evaluated using a –300 kV dc high voltage photogun and diagnostic beam line. Photocathodes grown on GaAs substrates, with varying antimony layer thickness (estimated range from <20 nm to >1 um), yielded similar thermal emittance per rms laser spot size values (~0.4 mmmrad=mm) but very different operating lifetime. Similar thermal emittance was obtained for a photocathode grown on a molybdenum substrate but with markedly improved lifetime. For this photocathode, no decay in quantum efficiency was measured at 4.5 mA average current and with peak current 0.55 A at the photocathode.

43 PARTICLE ACCELERATORS↗

Machine learning framework for quantum sampling of highly constrained, continuous optimization problems

In recent years, there is growing interest in using quantum computers for solving combinatorial optimization problems. In this work, we developed a generic, machine learning-based framework for mapping continuous-space inverse design problems into surrogate quadratic unconstrained binary optimization (QUBO) problems by employing a binary variational autoencoder and a factorization machine. The factorization machine is trained as a low-dimensional, binary surrogate model for the continuous design space and sampled using various QUBO samplers. Using the D-Wave Advantage hybrid sampler and simulated annealing, we demonstrate that by repeated resampling and retraining of the factorization machine, our framework finds designs that exhibit figures of merit exceeding those of its training set. We showcase the framework’s performance on two inverse design problems by optimizing (i) thermal emitter topologies for thermophotovoltaic applications and (ii) diffractive meta-gratings for highly efficient beam steering. This technique can be further scaled to leverage future developments in quantum optimization to solve advanced inverse design problems for science and engineering applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

2D Semiconductor Nanosheets Supported on Colloidal Quantum Cubes

Two-dimensional (2D) colloidal nanocrystals bridge the physics of epitaxial quantum wells with the synthetic scalability of solution-processed nanomaterials, making them an attractive platform for future LEDs, lasers, and photodetectors. However, their strongly anisotropic 2D morphology complicates the formation of close-packed films required for electrically interfaced devices. Here, we address this limitation by introducing semiconductor quantum cubes (QCs) in which 2D CdSe nanosheets are conformally grown on six faces of CdS cubic scaffolds. This architecture preserves excitonic physics of quasi-2D nanosheets while leveraging the mechanical rigidity and self-assembly of nanocubes, enabling close-packed films with improved electronic coupling and electrical conductivity. By extending CdS/CdSe QCs into a CdS/CdSe/CdS core/shell/shell structure, we realize 2D quantum wells that exhibit unusual multiexciton behavior. In particular, CdS/CdSe/CdS QCs show repulsive exciton–exciton interactions, which decouple CdSe facets into quasi-independent emitters. This leads to the suppressed Auger recombination, long multiexciton lifetimes, and broadband optical gain. The demonstrated combination of unusual multiexciton photophysics and favorable film self-assembly characteristics in QCs presents opportunities for solution-processed optoelectronic devices.

perovskites↗

Thermally Activated Delayed Fluorescence Sensitization for Highly Efficient Blue Fluorescent Emitters

Hyperfluorescence is emerging as a powerful strategy to develop optoelectronic devices with high-color purity and enhanced stability. It requires appropriate integration of a sensitizer displaying efficient thermally activated delayed fluorescence (TADF) and an emitter displaying strong, narrow-band fluorescence. Here, through a joint computational and experimental approach, we provide an unprecedented, end-to-end systems level description of the electronic and optical processes that take place in a hyperfluorescent emissive layer composed of a TADF sensitizer, bis(2,5-di(9H-carbazol-9-yl)phenyl)-1,3,4-oxadiazole (4CzDPO), and a fluorescent emitter, 2,5,8,11-tetra-tert-butylperylene (TBPe). We combine the photophysical properties measurement of the emissive layer with the computational determination of the electronic properties, film morphology, and excitation transfer phenomena. The Förster resonance energy transfer rates from 4CzDPO to TBPe are on the order of 1011 s–1, considerably higher than the radiative and non-radiative recombination rates for 4CzDPO. These features ensure nearly complete energy transfer to TBPe, leading to a five-fold increase in the photoluminescence quantum yields in the 4CzDPO:TBPe system in comparison to neat films of 4CzDPO. Furthermore, our approach highlights the factors that can provide efficient energy transfer from TADF molecules to fluorescent emitters, suppress energy transfer among TADF molecules, and avoid the need for a host material within the emissive layer.

36 MATERIALS SCIENCE↗

The Path to Enlightenment: Progress and Opportunities in High Efficiency Halide Perovskite Light-Emitting Devices

Besides the flourishment in photovoltaics, halide perovskites hold great promise to compete with leading contenders among solution-processed emitters, such as organics and semiconductor colloidal nanocrystals, in the field of light emission. Halide perovskites exhibit outstanding optoelectronic properties, including high photoluminescence quantum yields, facile bandgap tunability, narrow emission line widths, and respectable carrier mobilities, promoting them to thrive in versatile light-emitting applications such as light-emitting diodes, lasers, X-ray scintillators, and circularly polarized light sources. Herein, we discuss the underlying physics of light emission in state-of-the-art perovskite light-emitting devices and focus on promising strategies for further improvement of device performance.

42 ENGINEERING↗

Roadmap on perovskite light-emitting diodes

Abstract In recent years, the field of metal-halide perovskite emitters has rapidly emerged as a new community in solid-state lighting. Their exceptional optoelectronic properties have contributed to the rapid rise in external quantum efficiencies (EQEs) in perovskite light-emitting diodes (PeLEDs) from <1% (in 2014) to over 30% (in 2023) across a wide range of wavelengths. However, several challenges still hinder their commercialization, including the relatively low EQEs of blue/white devices, limited EQEs in large-area devices, poor device stability, as well as the toxicity of the easily accessible lead components and the solvents used in the synthesis and processing of PeLEDs. This roadmap addresses the current and future challenges in PeLEDs across fundamental and applied research areas, by sharing the community’s perspectives. This work will provide the field with practical guidelines to advance PeLED development and facilitate more rapid commercialization.

14 SOLAR ENERGY↗

High-efficiency stretchable light-emitting polymers from thermally activated delayed fluorescence

Stretchable light-emitting materials are the key components for realizing skin-like displays and optical biostimulation. All the stretchable emitters reported to date, to the best of our knowledge, have been based on electroluminescent polymers that only harness singlet excitons, limiting their theoretical quantum yield to 25%. Here we present a design concept for imparting stretchability onto electroluminescent polymers that can harness all the excitons through thermally activated delayed fluorescence, thereby reaching a near-unity theoretical quantum yield. We show that our design strategy of inserting flexible, linear units into a polymer backbone can substantially increase the mechanical stretchability without affecting the underlying electroluminescent processes. As a result, our synthesized polymer achieves a stretchability of 125%, with an external quantum efficiency of 10%. Additionally, we demonstrate a fully stretchable organic light-emitting diode, confirming that the proposed stretchable thermally activated delayed fluorescence polymers provide a path towards simultaneously achieving desirable electroluminescent and mechanical characteristics, including high efficiency, brightness, switching speed and stretchability as well as low driving voltage.

36 MATERIALS SCIENCE↗

Tuning colour centres at a twisted hexagonal boron nitride interface

The colour centre platform holds promise for quantum technologies, and hexagonal boron nitride has attracted attention due to the high brightness and stability, optically addressable spin states and wide wavelength coverage discovered in its emitters. However, its application is hindered by the typically random defect distribution and complex mesoscopic environment. In this study, employing cathodoluminescence, we demonstrate on-demand activation and control of colour centre emission at the twisted interface of two hexagonal boron nitride flakes. Further, we show that colour centre emission brightness can be enhanced by two orders of magnitude by tuning the twist angle. Additionally, by applying an external voltage, nearly 100% brightness modulation is achieved. Our ab initio GW and GW plus Bethe–Salpeter equation calculations suggest that the emission is correlated to nitrogen vacancies and that a twist-induced moiré potential facilitates electron–hole recombination. This mechanism is further exploited to draw nanoscale colour centre patterns using electron beams.

36 MATERIALS SCIENCE↗