Emission Quantum Research Articles

Spin angular momentum-encoded single-photon emitters in a chiral nanoparticle-coupled WSe2 monolayer.

Spin angular momentum (SAM)-encoded single-photon emitters, also known as circularly polarized single photons, are basic building blocks for the advancement of chiral quantum optics and cryptography. Despite substantial efforts such as coupling quantum emitters to grating-like optical metasurfaces and applying intense magnetic fields, it remains challenging to generate circularly polarized single photons from a subwavelength-scale nanostructure in the absence of a magnetic field. Here, we demonstrate single-photon emitters encoded with SAM in a strained WSe2 monolayer coupled with chiral plasmonic gold nanoparticles. Single-photon emissions were observed at the nanoparticle position, exhibiting photon antibunching behavior with a g(2)(0) value of ~0.3 and circular polarization properties with a slight preference for left-circular polarization. Specifically, the measured Stokes parameters confirmed strong circular polarization characteristics, in contrast to emitters coupled with achiral gold nanocubes. Therefore, this work provides potential insights to make SAM-encoded single-photon emitters and understand the interaction of plasmonic dipoles and single photons, facilitating the development of chiral quantum optics.

Breakdown of steady-state superradiance in extended driven atomic arrays

Recent advances in generating well controlled dense arrangements of individual atoms in free space have generated interest in understanding how the extended nature of these systems influences superradiance phenomena. Here, we provide an in-depth analysis on how space-dependent light shifts and decay rates induced by dipole-dipole interactions modify the steady-state properties of coherently driven arrays of quantum emitters. We characterize the steady-state phase diagram, with particular focus on the radiative properties in the steady state. Interestingly, we find that diverging from the well-established Dicke paradigm of equal all-to-all interactions significantly modifies the emission properties. In particular, the prominent quadratic scaling of the radiated light intensity with particle number in the steady state—a hallmark of steady-state Dicke superradiance—is entirely suppressed, resulting in only linear scaling with particle number. We show that this breakdown of steady-state superradiance occurs due to the emergence of additional dissipation channels that populate not only superradiant states but also subradiant ones. The additional contribution of subradiant dark states in the dynamics leads to a divergence in the time scales needed to achieve steady states. Building on this, we further show that measurements taken at finite times for extended atom ensembles reveal properties closely mirroring the idealized Dicke scenario. Published by the American Physical Society 2024

Wideband and low-spurious optical waveform generator for optically addressable quantum systems manipulation and control

Optical manipulation of quantum systems requires stable laser sources able to produce complex waveforms over a large frequency range. In the visible region, such waveforms can be generated using an acousto-optic modulator driven by an arbitrary waveform generator, but these suffer from a limited tuning range typically of a few tens of MHz. Visible-range electro-optic modulators are an alternative option offering a larger modulation bandwidth, however they have limited output power which drastically restricts the scalability of quantum applications. There is currently no architecture able to perform phase-stabilized waveforms over several GHz in the visible or near infrared region while providing sufficient optical power for quantum applications. Here we propose and develop a modulation and frequency conversion set-up able to deliver optical waveforms over a large frequency range, with a high spurious extinction ratio, scalable to the entire visible/near infrared region with high optical power. The optical waveforms are first generated at telecom wavelength and then converted to the emitter wavelength through a sum frequency generation process. By adapting the pump laser frequency, the optical waveforms can be tuned to interact with a broad range of optical quantum emitters or qubits such as alkali atoms, trapped ions, rare earth ions, or fluorescent defects in solid-state matrices. Using this architecture, we were able to detect and study a single erbium ion in a nanoparticle. We also generated high bandwidth signals at 606 nm, which would enable frequency multiplexing of on-demand read-out Pr3+:Y2SiO5 quantum memories.

Super-resolved snapshot hyperspectral imaging of solid-state quantum emitters for high-throughput integrated quantum technologies

Super-resolved snapshot hyperspectral imaging of solid-state quantum emitters for high-throughput integrated quantum technologies

Transient Study of Photoluminescence in Nanowaveguides Doped with Quantum Emitters and Metallic Nanoparticles.

We have studied the time-dependent optical properties of nanowaveguides containing an ensemble of noninteracting quantum emitters and interaction metallic nanoparticles. We have developed a theory for transient photoluminescence (PL) and exciton population density using the density matrix method. In our theory, we have included the effect of the dipole-dipole interaction (DDI) between metallic nanoparticles along with the effect of the surface plasmon polaritons (SPPs) created by metallic nanoparticles. We compared our theory with the transient PL experiments of nanohybrids fabricated from CdSe/ZnS quantum dots and an Ag nanorod array. A good agreement between theory and PL experiment is found. We have also examined the transient behavior of the photoluminescence in the presence of the DDI and SPP couplings. It is observed that the number of transient PL oscillations increases as the DDI coupling increases. The width of the transient peaks also increases as the amount of the DDI coupling increases. Finally, we predicted that the peaks of the transient PL oscillation split from one peak to two peaks as the intensity of the DDI coupling reaches the strong coupling limit. The strong coupling limit is defined when the DDI coupling is larger than the PL decay rates. This finding can be used to fabricate nano switches by using one peak as the OFF position and two peaks as the ON position. The above findings also suggest the transient plasmonic properties of nanowaveguides can be controlled by the SPP and DDI couplings. These findings have potential applications in the development of transient nanoscale plasmonic devices such as nano detectors and optical nano switches.

Crystal structure, Hirshfeld surface analysis and photophysical properties of disubstituted 4,4′-(benzo[c][1,2,5]thiadiazole-4,7-diyl)dianiline

Two independent molecules of the crystal structure of the title compound C18H14N4S were found to occupy the asymmetric unit of the space group. The flanking 4-anilines were not coplanar with the central benzothiadiazole. In the crystal, two unique types of hydrogen bonds were found: i) one set between two NH2 of two molecules in the asymmetric unit and ii) another set between hydrogen atoms of the second aniline NH2 and the nitrogen atom of benzothiadiazole. The two-dimensional fingerprint plots along with the Hirshfeld surface confirmed the most important contributions for the crystal packing were C···H, H···H and N···H interactions. The compound was also solvatochromic with both its emission wavelength and quantum yield contingent on the solvent polarity. The fluorophore had a reversible oxidation. This was used to induce both a reversible color change from yellow to blue and emission off/on with an applied potential.

Engineering the Impact of Phonon Dephasing on the Coherence of a WSe_{2} Single-Photon Source via Cavity Quantum Electrodynamics.

Emitter dephasing is one of the key issues in the performance of solid-state single-photon sources. Among the various sources of dephasing, acoustic phonons play a central role in adding decoherence to the single-photon emission. Here, we demonstrate that it is possible to tune and engineer the coherence of photons emitted from a single WSe_{2} monolayer quantum dot via selectively coupling it to a spectral cavity resonance. We utilize an open cavity to demonstrate spectral enhancement, leveling, and suppression of the highly asymmetric phonon sideband, finding excellent agreement with a microscopic description of the exciton-phonon dephasing in a truly two-dimensional system. Moreover, the impact of cavity tuning on the dephasing is directly assessed via optical interferometry, which points out the capability to utilize light-matter coupling to steer and design dephasing and coherence of quantum emitters in atomically thin crystals.

Chirality-assisted enhancement of tripartite entanglement in waveguide QED

We study the generation and control of genuine tripartite entanglement among quantum emitters (QEs) that are side-coupled to one-dimensional spin-momentum locked (or chiral) waveguides. By applying the machinery of Fock state master equations along with the recently proposed concurrence fill measure of tripartite entanglement [S. Xie and J. H. Eberly, Phys. Rev. Lett. 127, 040403 (2021)], we analyze how three-photon Gaussian wavepackets can distribute entanglement among two and three QEs. We show that with a five times larger waveguide decay rate in the right direction as compared to the left direction, the maximum value of tripartite entanglement can be elevated by 35%\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$35\\%$$\\end{document} as compared to the symmetric scenario where both left, and right direction decay rates are equal. Additionally, chirality can maintain the tripartite entanglement for longer than the corresponding symmetric decay rate. Finally, we study the influence of detunings and spontaneous emission on the resulting entanglement. We envision quantum networking and long-distance quantum communication as two main areas of applications of this work.

Highly Efficient and Thermally Durable Luminescence of 1D Eu3+ Coordination Polymers with Arsenic Bridging Ligands.

In this work, bisarsine oxides were evaluated as novel bridging ligands, aiming to develop practical and efficient luminescent lanthanide coordination polymers. We have synthesized one-dimensional (1D) Eu3+ coordination polymers that incorporate bisarsine oxide bridging ligands and hexafluoroacetylacetonate anions. These polymers exhibited a denser packing of chains compared to analogous polymers bridged with bisphosphine oxides. The coordination polymers demonstrated exceptional thermal stability and substantial emission quantum yields. Additionally, the bisarsine oxides induced a pronounced polarization effect, facilitating a sensitive electric dipole transition that yields considerably narrow band red emission. Remarkably, the Eu3+ coordination polymers with bisarsine oxides maintained intense emission even at 550 K. A distinctive feature of these polymers is their heating-induced emission enhancement observed when the temperature was increased from 300 K to 400 K.

Tetrazolate-based neutral Cu(I) complex for efficient and short-lived blue thermally activated delayed fluorescence

Endowing thermally activated delayed fluorescence (TADF) emitters simultaneously with high emission quantum yields and short radiative lifetimes is of fundamental significance in optoelectronic field. In this contribution, two neutral tetrahedral Cu(I) complexes (1 and 2) have been developed, which realize blue-TADF with photoluminescent quantum yield of up to 85 % due to the high structural rigidity. Meanwhile, short TADF lifetimes (<10 μs) of the Cu(I) complexes suggest that the synergistic effects of small ΔE(S1-T1) gap and relatively large SOC value introduced by the copper ion could facilitate fast reverse ISC processes compared to the typical organic-TADF materials.

Enhancing crystal integrity and structural rigidity of CsPbBr3 nanoplatelets to achieve a narrow color-saturated blue emission

Quantum-confined CsPbBr3 perovskites are promising blue emitters for ultra-high-definition displays, but their soft lattice caused by highly ionic nature has a limited stability. Here, we endow CsPbBr3 nanoplatelets (NPLs) with atomic crystal-like structural rigidity through proper surface engineering, by using strongly bound N-dodecylbenzene sulfonic acid (DBSA). A stable, rigid crystal structure, as well as uniform, orderly-arranged surface of these NPLs is achieved by optimizing intermediate reaction stage, by switching from molecular clusters to mono-octahedra, while interaction with DBSA resulted in formation of a CsxO monolayer shell capping the NPL surface. As a result, both structural and optical stability of the CsPbBr3 NPLs is enhanced by strong covalent bonding of DBSA, which inhibits undesired phase transitions and decomposition of the perovskite phase potentially caused by ligand desorption. Moreover, rather small amount of DBSA ligands at the NPL surface results in a short inter-NPL spacing in their closely-packed films, which facilitates efficient charge injection and transport. Blue photoluminescence of the produced CsPbBr3 NPLs is bright (nearly unity emission quantum yield) and peaks at 457 nm with an extremely narrow bandwidth of 3.7 nm at 80 K, while the bandwidth of the electroluminescence (peaked at 460 nm) also reaches a record-narrow value of 15 nm at room temperature. This value corresponds to the CIE coordinates of (0.141, 0.062), which meets Rec. 2020 standards for ultra-high-definition displays.

Individual Tuning of Directional Emission and Luminance of a Quantum Emitter in a Composite Plasmonic Antenna

High directional emission and high radiative quantum efficiency are strongly needed when moving a single optical nano-emitter (such as a quantum dot) into the practical realm. However, a typical optical nano-emitter struggles to meet the requirements above, which limits its practical applications in next-generation nano-photonic devices such as single-photon sources. Here, to achieve these features simultaneously, we propose and theoretically investigate a composite plasmonic antenna consisting of a hemispherical solid immersion lens (SIL) and a bowtie plasmonic nano-antenna, wherein a high directional emission of 10° and 2.5 × 103 of Purcell factor have both been enabled. Moreover, we find that directionality and the Purcell factor can be manipulated independently in our antenna, which provides a novel platform for the optimization of single-photon sources.

Computational Investigations of the Detailed Mechanism of Reverse Intersystem Crossing in Inverted Singlet-Triplet Gap Molecules.

Inverted singlet-triplet gap (INVEST) materials have promising photophysical properties for optoelectronic applications due to an inversion of their lowest singlet (S1) and triplet (T1) excited states. This results in an exothermic reverse intersystem crossing (rISC) process that potentially enhances triplet harvesting, compared to thermally activated delayed fluorescence (TADF) emitters with endothermic rISCs. However, the processes and phenomena that facilitate conversion between excited states for INVEST materials are underexplored. We investigate the complex potential energy surfaces (PESs) of the excited states of three heavily studied azaphenalene INVEST compounds, namely, cyclazine, pentazine, and heptazine using two state-of-the-art computational methodologies, namely, RMS-CASPT2 and SCS-ADC(2) methods. Our findings suggest that ISC and rISC processes take place directly between the S1 and T1 electronic states in all three compounds through a minimum-energy crossing point (MECP) with an activation energy barrier between 0.11 to 0.58 eV above the S1 state for ISC and between 0.06 and 0.36 eV above the T1 state for rISC. We predict that higher-lying triplet states are not populated, since the crossing point structures to these states are not energetically accessible. Furthermore, the conical intersection (CI) between the ground and S1 states is high in energy for all compounds (between 0.4 to 2.0 eV) which makes nonradiative decay back to the ground state a relatively slow process. We demonstrate that the spin-orbit coupling (SOC) driving the S1-T1 conversion is enhanced by vibronic coupling with higher-lying singlet and triplet states possessing vibrational modes of proper symmetry. We also rationalize that the experimentally observed anti-Kasha emission of cyclazine is due to the energetically inaccessible CI between the bright S2 and the dark S1 states, hindering internal conversion. Finally, we show that SCS-ADC(2) is able to qualitatively reproduce excited state features, but consistently overpredict relative energies of excited state structural minima compared to RMS-CASPT2. The identification of these excited state features elaborates design rules for new INVEST emitters with improved emission quantum yields.

Microwave analogy of Förster resonance energy transfer and effect of finite antenna length

The near-field interaction between quantum emitters, governed by Förster resonance energy transfer (FRET), plays a pivotal role in nanoscale energy transfer mechanisms. However, FRET measurements in the optical regime are challenging as they require nanoscale control of the position and orientation of the emitters. To overcome these challenges, microwave measurements were proposed for enhanced spatial resolution and precise orientation control. However, unlike in optical systems for which the dipole can be taken to be infinitesimal in size, the finite size of microwave antennas can affect energy transfer measurements, especially at short distances. This highlights the necessity to consider the finite antenna length to obtain accurate results. In this study, we advance the understanding of dipole–dipole energy transfer in the microwave regime by developing an analytical model that explicitly considers finite antennas. Unlike previous works, our model calculates the mutual impedance of finite-length thin-wire dipole antennas without assuming a uniform current distribution. We validate our analytical model through experiments investigating energy transfer between antennas placed adjacent to a perfect electric conductor mirror. This allows us to provide clear guidelines for designing microwave experiments, distinguishing conditions where finite-size effects can be neglected and where they must be taken into account. Our study not only contributes to the fundamental physics of energy transfer but also opens avenues for microwave antenna impedance-based measurements to complement optical FRET experiments and quantitatively explore dipole–dipole energy transfer in a wider range of conditions.

Suppressing Self‐Oxidation of Eu2+ in Li2CaSiO4 for Full‐Spectrum Lighting and Accurate Temperature Sensing

AbstractEu2+‐doped phosphors have attracted the great attention of researchers in the past decade. However, Eu2+ dopant in inorganic hosts often suffers from the self‐oxidation effect, therefore causing the attenuated emission intensity and quantum efficiency. In this regard, developing Eu2+ doped phosphors with the prohibited self‐oxidation effect of Eu2+ and increased thermal stability is urgently required. Herein, an innovative cyan‐light emitting Li2CaSiO4:Eu2+/Eu3+, Lu3+ (LCSO) phosphor is designed. Both experimental results and theoretical calculations demonstrate that adding Lu3+ restricts the self‐oxidation of Eu2+ into Eu3+, thus improving the emission of Eu2+. Meanwhile, the Lu3+ introduction brings out excellent thermal stability. Finally, an efficient WLED with a color temperature (CCT) of 4573 K and a high color rendering index (Ra) of 84.2 is obtained using the as‐prepared phosphor due to the perfect compensation of the cyan light. As the introduction of Lu3+ improves the stability of Eu2+, a much greater difference in PL decay rate between Eu2+ and Eu3+ in LCSO is reached, thereby improving their sensitivity in temperature sensing. The strategy of Lu3+ introduction for prohibiting the self‐oxidation of Eu2+ for efficient and stable Eu2+ emission may stimulate some new ideas in designing high‐performance phosphors for more diverse applications.

Asymmetric-absorption-induced spectral redshift in a monolithic III-nitride on-chip system

Integrating optoelectronic devices with various functions into a monolithic chip is a popular research frontier. The top-down integration scheme on silicon-based III-nitride wafers has unique advantages. A monolithic III-nitride on-chip system with lighting source, electrical absorption modulator, waveguide and photodetector with the same structure were designed and fabricated to discover the asymmetry of photon emission and absorption in quantum well diode. The characteristics of the chip were characterized in detail and three different spectral redshifts were observed in the experiment. Results revealed that the asymmetric absorption causes spectral redshift in a quantum well diode, and self-absorption is a fundamental and universal phenomenon in quantum wells. This work provides an important reference for future III-nitride optoelectronic integration.

Enhanced photoluminescence emission intensity and stability of deep blue-emissive (Et3NH)PbBr3 perovskite nanocrystals by using metal-organic frameworks

The primary obstacle faced by researchers in the field of luminescent metal-halide perovskites is their inherent instability, prompting a shift in focus towards enhancing the stability of perovskite nanocrystals (PNCs). One of the promising approaches to address this challenge involves the utilization of metal-organic frameworks (MOFs) to fabricate PNCs@MOF composites. The present study reports a facile and low-cost colloidal strategy to prepare (Et3NH)PbBr3 PNCs followed by their encapsulation within UiO-67 to enhance their photoluminescence (PL) emission stability. The PNCs and modified UiO-67 were prepared separately via simple and efficient ligand-assisted reprecipitation (LARP) and hydrothermal methods, respectively. After modification of the UiO-67, the pore sizes experienced a substantial increase from 1.90 to 28.84 nm which significantly facilitated the localization of PNCs within the porous matrix. Under a full survey of experimental conditions, the resulting (Et3NH)PbBr3@UiO-67 composite exhibited a bright deep-blue emission at around 410 nm with an emission quantum yield of 52 %. The emission durability of the fabricated PNCs@MOF composites was assessed against temperature and long-time of storage, confirming the superior advantages of MOF even at elevated temperatures of up to 100 °C. The stable and luminous deep-blue emission displayed by the PNCs@MOF composites in this investigation, offers a promising advancement in materials development for optoelectronic applications.

Single-Photon Emission from Point Defects in Hexagonal Boron Nitride Induced by Plasma Treatment.

Solid-state quantum emitters are gaining significant attention for many quantum information applications. Hexagonal boron nitride (h-BN) is an emerging host material for generating bright, stable, and tunable single-photon emission with narrow line widths at room temperature. In this work, we present a facile and efficient approach to generate high-density single-photon emitters (SPEs) in mechanically exfoliated h-BN through H- or Ar-plasma treatment followed by high-temperature annealing in air. It is notable that the postannealing is essential to suppress the fluorescence background in photoluminescence spectra and enhance emitter stability. These quantum emitters exhibit excellent optical properties, including high purity, brightness, stability, polarization degree, monochromaticity, and saturation intensity. The effects of process parameters on the quality of quantum emitters were systematic investigated. We find that there exists an optimal plasma power and h-BN thickness to achieve a high SPE density. This work offers a practical avenue for generating SPEs in h-BN and holds promise for future research and applications in quantum photonics.

Spatial photoluminescence and lifetime mappings of quasi-2D perovskites coupled with a dielectric metasurface.

Light-matter interaction between quantum emitters and optical cavities plays a vital role in fundamental quantum photonics and the development of optoelectronics. Resonant metasurfaces are proven to be an efficient platform for tailoring the spontaneous emission (SE) of the emitters. In this work, we study the interplay between quasi-2D perovskites and dielectric TiO2 metasurfaces. The metasurface, functioning as an open cavity, enhances electric fields near its plane, thereby influencing the emissions of the perovskite. This is verified through angle-resolved photoluminescence (PL) studies. We also conducted reflectivity measurements and numerical simulations to validate the coupling between the quasi-2D perovskites and photonic modes. Notably, our work introduces a spatial mapping approach to study Purcell enhancement. Using fluorescence lifetime imaging microscopy (FLIM), we directly link the PL and lifetimes of the quasi-2D perovskites in spatial distribution when positioned on the metasurface. This correlation provides unprecedented insights into emitter distribution and emitter-resonator interactions. The methodology opens a new (to the best of our knowledge) approach for studies in quantum optics, optoelectronics, and medical imaging by enabling spatial mapping of both PL intensity and lifetime, differentiating between uncoupled quantum emitters and those coupled with different types of resonators.

Band gap engineering and controlling transport properties of single photons in periodic and disordered Jaynes–Cummings arrays

We theoretically study the single-photon transport properties in periodic and position-disordered Jaynes–Cummings (or JC) arrays of waveguide-coupled microtoroidal ring resonators, each interacting with a single two-level quantum emitter. Employing the real-space formalism of quantum optics, we focus on various parameter regimes of cavity quantum electrodynamics (cQED) to gain better control of single-photon propagation in such a many-body quantum optical setting. As for some of the key findings, we observe that the periodic setting leads to the formation of the band structure in the photon transmission spectra, which is most evident in the strong coupling regime of cQED. However, under resonant conditions with no losses, the application of Bloch’s theorem indicates that the width of forbidden gaps can be altered by tuning the emitter-cavity coupling to small values. Moreover, in the disordered case, we find that the single-photon transmission curves show the disappearance of band formation. However, spectral features originating from cQED interactions observed for the single atom-cavity problem remain robust against weak-disordered conditions. The results of this work may find application in the study of quantum many-body effects in the optical domain as well as in different areas of quantum computation and quantum networking.