Light-emitting Quantum Research Articles

Internal Electric Field Manipulates Exciton-Phonon Couplings in Single Lead Halide Perovskite Nanocrystals.

Lead halide perovskite nanocrystals (NCs) have attracted much attention as materials for light-emitting diodes and quantum light sources. A deep understanding of exciton-phonon couplings is essential for obtaining a narrow emission line, weak phonon-sideband photoluminescence (PL), and a long exciton coherence time, which are especially useful for high-color-purity quantum-light-source applications. Here, we report the PL spectra of single CsPbBr3 NCs at 5.5 K as a function of the applied electric field. The exciton peak energy shows an asymmetric parabolic shift for positive and negative biases, implying the presence of a spontaneously generated internal electric field in the NCs when no field is applied. Both the internal electric field and exciton-phonon couplings become larger in smaller NCs, and they have a positive correlation with each other. Our findings show that the exciton-phonon couplings can be manipulated with an electric field, which dominates the PL properties of perovskite NCs.

Measurement of inkjet droplet speed using interference fringe by diffracted light

Inkjet printers are key technologies in manufacturing organic light-emitting diodes and quantum dot light-emitting diode panels, but precise measurement and control of inkjet droplets remains challenging. The international standard, IEC 62899-302-1, uses shadow image-based measurement with high magnification microscopes to observe picoliter-sized droplets. However, high magnification lens results in a shallow depth of field or narrow optimal measurement area, causing the blurring image if the droplet does not pass through the optimal measurement area. To solve this, we propose using the interference image-based measurement with interference fringe patterns by inkjet droplets as a tool to measure the flight speed of droplets. The interference fringe patterns can be obtained simply passing the droplet through within the light beam path, providing approximately 1000× wider measurement area compared to the shadow image-based measurement, making it practical to use in the industry. The flight speed of droplets analyzed with the interference image-based measurement at various frequencies and amplitudes of the inkjet driving voltage were compared with the shadow image-based measurement. The interference image-based measurement showed a coefficient of variation of less than 3%, showing higher repeatability than the shadow image-based measurements.

Characterization of quantum dot-like emitters in programmable arrays of nanowrinkles of 1L-WSe2

When combined with nanostructured substrates, two-dimensional semiconductors can be engineered with strain to tailor light–matter interactions on the nanoscale. Recently, room-temperature nanoscale exciton localization with controllable wrinkling in 1L-WSe2 was achieved using arrays of gold nanocones. Here, the characterization of quantum dot-like states and single-photon emitters in the 1L-WSe2/nanocone system is reported. The nanocones induce a wide range of strains, and as a result, a diverse ensemble of narrowband, potential single-photon emitters is observed. The distribution of emitter energies reveals that most reside in two spectrally isolated bands, leaving a less populated intermediate band that is spectrally isolated from the ensembles. The spectral isolation is advantageous for high-purity quantum light emitters, and anti-bunched emission from one of these states is confirmed up to 25 K. Although the spatial distribution of strain is expected to influence the orientation of the transition dipoles of the emitters, multimodal emission polarization anisotropy and atomic force microscopy reveal that the macroscopic orientation of the wrinkles is not a good predictor of dipole orientation. Finally, the emission is found to change with thermal cycling from 4 to 290 K and back to 4 K, highlighting the need to control factors such as temperature-induced strain to enhance the robustness of this quantum emitter platform. The initial characterization here shows that controlled nanowrinkles of 1L-WSe2 generate quantum light in addition to uncovering potential challenges that need to be addressed for their adoption into quantum photonic technologies.

Application of quantum dot light-emitting diode harvest by quantum dot solar cells

Recent progress in photovoltaic (PV) cell usage has been hindered due to a shortage of suitable materials that emit adequate wavelengths of light energy and convert it to electricity. Quantum dot light-emitting diodes (QLEDs) and quantum dot solar cells (QDSCs) have been identified as promising artificial light sources and PV cell types to nicely fit into this solution, not only complying with that but also being controllable, flexible, portable, and lightweight. The purpose of this study is to provide a review of the application of how QLEDs can be collected for QDSCs. First, we introduce QLEDs as artificial light sources, briefly outline their mechanics and benefits, and compare them to other light sources for QDSC harvesting. Then, we summarize the mechanisms that occur when a QDSC absorbs a photon from a QLED, as well as how these energy flow pathways influence artificial light energy harvest. Finally, we explore the optoelectronic properties of lead sulphide (PbS) and lead selenide (PbSe) as appropriate quantum dots (QDs) materials for current applications in QDSC and QLED technologies. We anticipate that the literature will be comprehensive and relevant to the scientific community interested in creating artificial light energy harvesting and thus researching the most recent alternative method of getting healthy energy.

Narrowband Quantum Light Emission from Oxygen-Related Color Centers in Hexagonal Boron Nitride

Narrowband Quantum Light Emission from Oxygen-Related Color Centers in Hexagonal Boron Nitride

Inducing Circularly Polarized Single-Photon Emission via Chiral-Induced Spin Selectivity.

One of the central aims of the field of spintronics is the control of individual electron spins to effectively manage the transmission of quantized data. One well-known mechanism for controlling electronic spin transport is the chiral-induced spin-selectivity (CISS) effect in which a helical nanostructure imparts a preferential spin orientation on the electronic transport. One potential application of the CISS effect is as a transduction pathway between electronic spin and circularly polarized light within nonreciprocal photonic devices. In this work, we identify and quantify the degree of chiral-induced spin-selective electronic transport in helical polyaniline films using magnetoconductive atomic force microscopy (mcAFM). We then induce circularly polarized quantum light emission from CdSe/CdS core/shell quantum dots placed on these films, demonstrating a degree of circular polarization of up to ∼21%. Utilizing time-resolved photoluminescence microscopy, we measure the radiative lifetime difference associated with left- and right-handed circular polarizations of single emitters. These lifetime differences, in combination with Kelvin probe mapping of the variation of surface potential with magnetization of the substrate, help establish an energy level diagram describing the spin-dependent transport pathways that enable the circularly polarized photoluminescence.

Size Dependence of Trion and Biexciton Binding Energies in Lead Halide Perovskite Nanocrystals.

Lead halide perovskite nanocrystals (NCs) have attracted much attention as light-source materials for light-emitting diodes, lasers, and quantum light emitters. The luminescence properties of perovskite NCs and the performance of NC-based light-source devices depend on trion and biexciton dynamics. Here, we examined the size dependence of trion and biexciton binding energies by conducting low-temperature single-dot spectroscopy on three different perovskite NCs: CsPbBr3, CsPbI3, and FAPbBr3. While the photoluminescence spectral widths of the all-inorganic CsPbBr3 and CsPbI3 NCs were narrow, compared with those of the organic-inorganic hybrid FAPbBr3 NCs, the binding energies of trions and biexcitons of all three samples showed similar size dependences, independent of the A-site cation and halogen. The effective-mass approximation calculations implied the importance of dynamical dielectric screening on the formation of trions and biexcitons.

Driving multicolor lignin-based carbon quantum dots into selective metal-ion recognition and photocatalytic antibiotic decomposition

Achieving a waste-treats-pollutant vision, rationally designed lignin valorization that encompasses a shining story of multicolor carbon dots is proposed to promote selective metal-ion sensing and photocatalytic antibiotic removal.

Optical activation of praseodymium ions implanted in gallium nitride after ultra-high pressure annealing

Lanthanide (Ln)-implanted gallium nitride (GaN) semiconductors have a variety of potential applications as light-emitting devices and quantum light sources, but their optical properties are not well understood. In this study, we investigate the room temperature optical properties of praseodymium (Pr) ion implanted single-crystal GaN and their changes upon ultrahigh pressure annealing (UHPA) up to 1480 °C. Photoluminescence (PL) spectra, luminescence transition lifetime, and excitation cross section of the implanted Pr ions are analyzed. In addition, the recovery of implantation-induced damage and the thermal diffusion of implanted Pr ions by UHPA are investigated by X-ray diffraction, Raman spectroscopy, and secondary ion mass spectrometry. The results show that the implantation damage is recovered by annealing at temperatures above 1200 °C, but Pr ions thermally diffuse to the surface as the annealing temperature increases. The annealing temperature at which a maximum PL intensity is obtained increases with increasing the implantation dose. However, the PL intensity decreases in all cases after annealing at 1480 °C, indicating that a quenching factor is dominant in this temperature range.

Manipulating Interlayer Excitons for Near-Infrared Quantum Light Generation.

Interlayer excitons (IXs) formed at the interface of van der Waals materials possess various novel properties. In parallel development, strain engineering has emerged as an effective means for creating 2D quantum emitters. Exploring the intersection of these two exciting areas, we use MoS2/WSe2 heterostructure as a model system and demonstrate how strain, defects, and layering can be utilized to create defect-bound IXs capable of bright, robust, and tunable quantum light emission in the technologically important near-infrared spectral range. Our work presents defect-bound IXs as a promising platform for pushing the performance of 2D quantum emitters beyond their current limitations.

Efficient sky-blue perovskite light-emitting diodes enabled by buried guanidine passivation

The light-emitting efficiencies of blue perovskite light-emitting diodes (PeLEDs) based on quasi-two-dimensional (quasi-2D) halide perovskite emissive layers still lag behind in comparison to their green and red counterparts. The buried interfaces strongly affect the properties of upper solution-processed quasi-2D halide perovskites and the resultant PeLEDs. Herein, it is proposed to passivate the defects of blue quasi-2D perovskites at the buried interfaces by modifying the poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) hole-transport layer (HTL) with 4-guanidinobutyric acid (GBA). The GBA-modified PEDOT:PSS can help to passivate the defects of blue quasi-2D perovskites at the buried interfaces through the interaction between the amine groups of GBA and lead ions and enhance the ratios of halide ions and 4-fluorophenylethylammonium bromide to lead ions. Owing to the reduced halogen vacancies and the passivated defects at the buried interfaces, the blue quasi-2D perovskites prepared on the GBA-modified PEDOT:PSS HTL lead to an increased photoluminescence quantum yield (PLQY) of 60.8 %. The corresponding sky blue PeLEDs achieve a maximum light-emitting quantum efficiency of 9.41 % with an emission peak at 488 nm. This work contributes to enhancing the light-emitting performance of blue PeLEDs through the buried interface passivation point of view.

Synthesis and Biological Toxicity Evaluation of Red Light-Emitting Carbon Quantum Dots

This study delineates the successful fabrication of red light-emitting carbon quantum dots (R-CQDs), approximately 3.5 nm in size, via hydrothermal methods. These carbon quantum dots (CQDs) display distinctive fluorescence properties, particularly a laser-dependency. The infrared and Raman spectra were subjected to a thorough investigation, revealing the presence of hydroxyl, amino, and carboxyl groups on the surface of the CQDs. Experimental findings indicate a significant correlation between the antibacterial effect of R-CQDs on E. coli and Yeast and their concentration. Subsequent research suggests that this antibacterial activity primarily stems from the CQDs’ disruption of cell membrane integrity, leading to the leakage of intracellular substances and consequently inhibiting the growth of these two microorganisms. The study also reveals that R-CQDs can trigger chromosomal aberrations in the root tip cells of broad beans and induce micronuclei formation. The frequency of micronuclei is directly proportional to the CQDs dosage, and an extended treatment duration results in an increased micronucleus rate. This suggests potential damage to the genetic material of broad beans by CQDs, which could adversely affect their growth and development. The study further identifies a significant impact of R-CQDs on the height of rice seedlings, causing a substantial reduction. Moreover, it was found that CQDs can infiltrate the rice body and instigate oxidative stress responses.

(Invited) Proximity Induced Chiral Quantum Light Generation in Strain-Engineered WSe2/NiPS3 Heterostructures

Quantum light emitters (QEs) capable of generating single photons of well-defined circular polarization could enable non-reciprocal single photon devices and deterministic spin-photon interfaces critical for realizing complex quantum networks. To date, emission of such chiral quantum light has been achieved via the application of intense external magnetic fields electrical/optical injection of spin polarized carriers/excitons, or coupling with complex photonic/meta-structures. Here we report free-space generation of highly chiral single photons from QEs created via nanoindentation of monolayer WSe2 - NiPS3 heterostructures at zero external magnetic field. These QEs emit in the 760-800 nm range with a degree of circular polarization and single photon purity as high as 0.89 and 80% respectively, independent of pump laser polarization. Scanning diamond nitrogen vacancy microscopy and temperature dependent magneto-photoluminescence studies reveal that the chiral quantum light emission arises from magnetic proximity interactions between localized excitons in the WSe2 monolayer and the out-of-plane magnetization of defects in antiferromagnetic (AFM) order of NiPS3, both of which are co-localized by the strain field associated with the nanoscale indentations.

(Invited) On-the-Fly Non-Adiabatic Dynamics Simulations of Single-Walled Carbon Nanotubes with Covalent Defects

Single-walled carbon nanotubes (SWCNTs) with covalent surface defects have been explored recently due to their promise for use in single-photon telecommunication emission and in spintronic applications. The dynamical evolution of excitons (the primary electronic excitations) in these systems has only been loosely explored using atomistic modeling due to the size-limitations of these large systems. We present computational modeling of non-radiative relaxation on a variety of SWCNT chiralities with single-defect functionalization schemes. Our modeling uses a trajectory surface hopping algorithm accounting for excitonic effects with a configuration interaction approach. We find a strong chirality and defect-composition dependence on the population relaxation (50 – 500 fs) between the nanotube band-gap excitation and the defect-associated, single-photon-emitting state, giving insight into the dynamic trapping nature of these localized excitonic states. Engineering fast population decay into the quasi-two-level sub-system with weak coupling to higher-energy states increases the effectiveness and controllability of these quantum light emitters.

Proximity-induced chiral quantum light generation in strain-engineered WSe2/NiPS3 heterostructures.

Quantum light emitters capable of generating single photons with circular polarization and non-classical statistics could enable non-reciprocal single-photon devices and deterministic spin-photon interfaces for quantum networks. To date, the emission of such chiral quantum light relies on the application of intense external magnetic fields, electrical/optical injection of spin-polarized carriers/excitons or coupling with complex photonic metastructures. Here we report the creation of free-space chiral quantum light emitters via the nanoindentation of monolayer WSe2/NiPS3 heterostructures at zero external magnetic field. These quantum light emitters emit with a high degree of circular polarization (0.89) and single-photon purity (95%), independent of pump laser polarization. Scanning diamond nitrogen-vacancy microscopy and temperature-dependent magneto-photoluminescence studies reveal that the chiral quantum light emission arises from magnetic proximity interactions between localized excitons in the WSe2 monolayer and the out-of-plane magnetization of defects in the antiferromagnetic order of NiPS3, both of which are co-localized by strain fields associated with the nanoscale indentations.

Two Biexciton Types Coexisting in Coupled Quantum Dot Molecules.

Coupled colloidal quantum dot molecules (CQDMs) are an emerging class of nanomaterials, manifesting two coupled emission centers and thus introducing additional degrees of freedom for designing quantum-dot-based technologies. The properties of multiply excited states in these CQDMs are crucial to their performance as quantum light emitters, but they cannot be fully resolved by existing spectroscopic techniques. Here we study the characteristics of biexcitonic species, which represent a rich landscape of different configurations essentially categorized as either segregated or localized biexciton states. To this end, we introduce an extension of Heralded Spectroscopy to resolve the different biexciton species in the prototypical CdSe/CdS CQDM system. By comparing CQDMs with single quantum dots and with nonfused quantum dot pairs, we uncover the coexistence and interplay of two distinct biexciton species: A fast-decaying, strongly interacting biexciton species, analogous to biexcitons in single quantum dots, and a long-lived, weakly interacting species corresponding to two nearly independent excitons. The two biexciton types are consistent with numerical simulations, assigning the strongly interacting species to two excitons localized at one side of the quantum dot molecule and the weakly interacting species to excitons segregated to the two quantum dot molecule sides. This deeper understanding of multiply excited states in coupled quantum dot molecules can support the rational design of tunable single- or multiple-photon quantum emitters.

One-Pot Synthesis of All-Inorganic CsPbClBr2 Blue Perovskite Quantum Dots via Stoichiometric Precursor.

The synthesis of perovskite-based blue light-emitting particles is valuable for several applications as the excellent optical properties and performances of the constituting materials associated with multi-exciton generation can be exploited. However, the preparation of perovskite precursors requires high temperatures, resulting in a complex manufacturing process. This paper proposes a one-pot method to synthesize CsPbClBr2 blue light-emitting quantum dots (QDs). In the case of nonstoichiometric precursor synthesis, the CsPbClBr2 QDs coexisted with additional products. The solvent for synthesizing mixed perovskite nanoparticles (containing chloride) was selected by mixing dimethylformamide (DMF) and/or dimethyl sulfoxide (DMSO) in different ratios. When only DMF was used with the stoichiometric CsBr and PbX2 (X = Cl, Br) ratio, the quantum yield was 70.55%, and superior optical properties were achieved. Moreover, no discoloration was observed for 400 h, and a high photoluminescence intensity was maintained. When deionized water was added to form a double layer with hexane, the luminescence was maintained for 15 days. In other words, the perovskite did not easily decompose even when in contact with water, which suppressed the release of Pb2+, which are heavy metal atoms in the structure. Overall, the proposed one-pot method for all-inorganic-based perovskite QDs provides a platform for synthesizing superior blue light-emitting materials.

Design Rules for Obtaining Narrow Luminescence from Semiconductors Made in Solution.

Solution-processed semiconductors are in demand for present and next-generation optoelectronic technologies ranging from displays to quantum light sources because of their scalability and ease of integration into devices with diverse form factors. One of the central requirements for semiconductors used in these applications is a narrow photoluminescence (PL) line width. Narrow emission line widths are needed to ensure both color and single-photon purity, raising the question of what design rules are needed to obtain narrow emission from semiconductors made in solution. In this review, we first examine the requirements for colloidal emitters for a variety of applications including light-emitting diodes, photodetectors, lasers, and quantum information science. Next, we will delve into the sources of spectral broadening, including "homogeneous" broadening from dynamical broadening mechanisms in single-particle spectra, heterogeneous broadening from static structural differences in ensemble spectra, and spectral diffusion. Then, we compare the current state of the art in terms of emission line width for a variety of colloidal materials including II-VI quantum dots (QDs) and nanoplatelets, III-V QDs, alloyed QDs, metal-halide perovskites including nanocrystals and 2D structures, doped nanocrystals, and, finally, as a point of comparison, organic molecules. We end with some conclusions and connections, including an outline of promising paths forward.

Localization-enhanced moiré exciton in twisted transition metal dichalcogenide heterotrilayer superlattices

The stacking of twisted two-dimensional (2D) layered materials has led to the creation of moiré superlattices, which have become a new platform for the study of quantum optics. The strong coupling of moiré superlattices can result in flat minibands that boost electronic interactions and generate interesting strongly correlated states, including unconventional superconductivity, Mott insulating states, and moiré excitons. However, the impact of adjusting and localizing moiré excitons in Van der Waals heterostructures has yet to be explored experimentally. Here, we present experimental evidence of the localization-enhanced moiré excitons in the twisted WSe2/WS2/WSe2 heterotrilayer with type-II band alignments. At low temperatures, we observed multiple excitons splitting in the twisted WSe2/WS2/WSe2 heterotrilayer, which is manifested as multiple sharp emission lines, in stark contrast to the moiré excitonic behavior of the twisted WSe2/WS2 heterobilayer (which has a linewidth 4 times wider). This is due to the enhancement of the two moiré potentials in the twisted heterotrilayer, enabling highly localized moiré excitons at the interface. The confinement effect of moiré potential on moiré excitons is further demonstrated by changes in temperature, laser power, and valley polarization. Our findings offer a new approach for localizing moiré excitons in twist-angle heterostructures, which has the potential for the development of coherent quantum light emitters.

Optically Active Telecom Defects in MoTe2 Fewlayers at Room Temperature.

The optical and electrical properties of semiconductors are strongly affected by defect states. The defects in molybdenum ditelluride (MoTe2) show the potential for quantum light emission at optical fiber communication bands. However, the observation of defect-related light emission is still limited to cryogenic temperatures. In this work, we demonstrate the deep defect states in MoTe2 fewlayers produced via a standard van der Waal material transfer method with a heating process, which enables light emission in the telecommunication O-band. The optical measurements show evidence of localized excitons and strong interaction among defects. Furthermore, the optical emission of defects depends on the thickness of the host materials. Our findings offer a new route for tailoring the optical properties of two-dimensional materials in optoelectronic applications.