Charge Carrier Injection Research Articles

Modulation of Charge Transport Layer for Perovskite Light-Emitting Diodes.

Perovskite light-emitting diodes (Pero-LEDs) have garnered significant attention due to their exceptional emission characteristics, including narrow full width at half maximum, high color purity, and tunable emission colors. Recent efficiency and operational stability advancements have positioned Pero-LEDs as a promising next-generation display technology. Extensive research and review articles on the compositional engineering and defect passivation of perovskite layers have substantially contributed to the development of multi-color and high-efficiency Pero-LEDs. However, the crucial aspect of charge transport layer (CTL) modulation in Pero-LEDs remains relatively underexplored. CTL modulation not only impacts the charge carrier transport efficiency and injection balance but also plays a critical role in passivating the perovskite surface, blocking ion migration, enhancing perovskite crystallinity, and improving light extraction efficiency. Therefore, optimizing CTLs is pivotal for further enhancing Pero-LED performance. Herein, this review discusses the roles of CTLs in Pero-LEDs and categorizes both reported and potential CTL materials. Then, various CTL optimization strategies are presented, alongside an analysis of the selection criteria for CTLs in high-performance Pero-LEDs. Finally, a summary and outlook on the potential of CTL modulation to further advance Pero-LED performances are provided.

Polarized and Directional Electroluminescence from Organic Light‐Emitting Devices by Using a Bifunctional Meta‐Electrode

AbstractOrganic light‐emitting devices (OLEDs) with polarized and directional emission are highly desired for their promising applications in optical imaging, optical communication, and immersive visual technologies. Existing implementation methods based on free space bulk optical elements suffer from significant power loss, limiting their practical applications. Here, a bifunctional meta‐electrode is proposed by integrating a metasurface consisting of Ag periodic corrugations onto the indium tin oxide (ITO) anode to simultaneously realize the functions of charge carrier injection and photon management in the OLEDs. Highly polarized and directional light emission is demonstrated while maintaining a high device efficiency using the meta‐electrode. The electroluminescence with a polarization extinction ratio of 5 is achieved by judiciously engineering the polarization‐dependent Purcell factor of the resonant cavity constructed by the meta‐electrode. Meanwhile, the directional light emission with a divergence angle of 10° can be obtained by the efficient out‐coupling of surface plasmon‐polariton mode. The light beam can be collimated in one direction by using 1D nanogratings and in two directions by using 2D nanopillars, respectively.

Organic‐Inorganic Hybrid Cuprous‐Based Metal Halides with Unique Two‐Dimensional Crystal Structure for White Light‐Emitting Diodes

AbstractTernary cuprous (Cu+)‐based metal halides, represented by cesium copper iodide (e.g., CsCu2I3 and Cs3Cu2I5), are garnering increasing interest for light‐emitting applications owing to their intrinsically high photoluminescence quantum yield and direct band gap. Toward electrically driven light‐emitting diodes (LEDs), it is highly desirable for the light emitters to have a high structural dimensionality as it may favor efficient electrical injection. However, unlike lead‐based halide perovskites whose light‐emitting units can be facilely arranged in three‐dimensional (3D) ways, to date, nearly all ternary Cu+‐based metal halides crystallize into 0D or 1D networks of Cu−X (X=Cl, Br, I) polyhedra, whereas 3D and even 2D structures remain mostly uncharted. Here, by employing a fluorinated organic cation, we report a new kind of ternary Cu+‐based metal halides, (DFPD)CuX2 (DFPD+=4,4‐difluoropiperidinium), which exhibits unique 2D layered crystal structure. Theoretical calculations reveal a highly dispersive conduction band of (DFPD)CuBr2, which is beneficial for charge carrier injection. It is also of particular significance to find that the 2D (DFPD)CuBr2 crystals show appealing properties, including improved ambient stability and an efficient warm white‐light emission, making it a promising candidate for single‐component lighting and display applications.

Enhanced performance of ambient-air processed CsPbBr3 perovskite light-emitting electrochemical cells via synergistic incorporation of dual additives

Metal halide perovskite light-emitting electrochemical cells (MHP-LECs) are promising due to their facile solution processability and exceptional optoelectrical properties. However, commercialization is hindered by poor thin-film coverage and the need for glovebox processing. This study addresses these issues by incorporating poly(ethylene oxide) (PEO) and potassium hexafluorophosphate (KPF6) into cesium lead bromide perovskite (CsPbBr3) emitting layers (EML), processed under ambient-air conditions. These perovskite composite thin films were spin-coated on a preheated substrate, and the device structure was ITO/PEDOT:PSS/EML/Al. Notably, the MHP-LEC based on CsPbBr3:PEO:KPF6 (100:65:0.2, weight ratio) exhibited pure-green emission with a peak at 524 nm and a narrow full width at half-maximum of 27 nm. Compared to a reference device (CsPbBr3:PEO (100:65, weight ratio)), the new device showed 1.5-, 4-, and 5-fold improvements in current density, electroluminescence (EL) intensity, and lifetime, respectively. These enhancements are attributed to reduced non-radiative current leakage, improved film surface coverage and passivation, and balanced charge carrier injection and transportation. This study offers a straightforward approach for processing CsPbBr3 thin films under ambient-air conditions, enhancing the EL performance of MHP-LECs.

Electron Transport over 2D Molecular Materials and Assemblies.

ConspectusTwo-dimensional (2D) molecular materials, in which the major interactions are confined in 2D planes with contrasted force fields acting in between the planes, have been key electronic functional materials since the past decade. Even without referring to the functionals of graphene-based systems, 2D electronic conjugated systems are expected to show extrawide dynamic ranges in electronic density of states (DOS) tuning, effective electron mass, electron mobility, and conductivity. A major advantage of 2D electronic systems is their compatibility with the ubiquitous electronic devices designed using planar structures, such as transistors and memories, which is associated with the utility of 2D active materials. The mobility of electrons in 2D systems is the key to their utility, and various conjugated molecular and 2D materials have been designed to optimize the mobility. This Account begins with an introduction for mobility assessment: using noncontact time-resolved microwave conductivity (TRMC) measurements as a technique to probe differential conductivity upon transient charge carrier injection into the materials. Electronic transport over 2D electronic materials such as graphenes, covalent organic frameworks (COFs), and metal-organic frameworks (MOFs) is discussed with a special emphasis on molecular building blocks, fine-tuning conducting species and linkages, topology of the framework, and controlling molecular doping. The superiority of β-ketoenamine-linked COF over imine-linked COF films in charge transport and dominant in-plane charge carrier mobility over out-of-plane mobility is also illustrated. Systematic molecular engineering of the building blocks of β-ketoenamine-linked COFs with varying degrees of donor-acceptor (D-A) conjugation, torsional angles, and reaction conditions resulted in the modulation of the efficiency of charge carrier generation/transport as well as exciton migration. The advantages of 2D systems are finally discussed in terms of the mobility interplaying with spatial arrangements of molecules as well as the substantial role of intermolecular interactions in stabilizing their condensed phases. The strong correlation between the dispersion of mobility and hierarchical intermolecular interactions sheds light on the way to overcome structural fluctuation on the optimization of charge transport in molecular electronic materials. The point of singularity in the dispersion at an intermolecular distance of d ∼ 0.3 nm is deduced from the overall mobility assessment in condensed phases of conjugated molecules, suggesting key roles of intermolecular electronic coupling: the new concept of electronic conjugation. Exceptional electronic coupling with relatively high charge carrier mobility was also observed, particularly in 2D spatial arrangements of chiral molecules in contrast to 3D analogues, where the reduction of gravitational density of the molecular condensates was impacting DOS: the Wallach's rule. 2D electronic systems are strong candidates for the violation of the long-lasting Wallach's rule in terms of DOS.

Synthesis, Photoluminescence, and Electroluminescence of Phosphorescent Dipyrido[3,2-a;2'3'-c]phenazine-Platinum(II) Complexes Bearing Hole-Transporting Acetylide Ligands.

In this study, novel phosphorescent dipyrido[3,2-a;2'3'-c]phenazine (dppz)-platinum(II)-phenylacetylide complexes were developed to fabricate non-doped organic light-emitting diodes (OLED) by solution-processing. To facilitate the charge carrier injection into the emitting layer (EML), 3,6-di-tert-butylcarbazole-functinalized phenylacetylides were employed. As for the dppz ligand, 9,9-dihexylfluoren-2-yl and 4-hexylthiophen-2-yl side-arms were introduced to the 2,7-positions, which led to reddish orange and red photoluminescence (PL), respectively, in solution and film states (PL wavelength: ca. 600 and ca. 625 nm, respectively). The carbazole-appended phenylacetylide ligands hardly affected the emission color, although unsubstituted phenylacetylides gave rise to aggregate- or excimer-based near-infrared PL with a low quantum yield. Two types of non-doped OLEDs were fabricated: single-layer and multilayer devices. In both devices, the organic layers were fabricated by spin-coating, and the EML consisted of a neat film of the corresponding platinum(II) complex. Therein, electroluminescence spectra corresponding to those of PL were observed. The single-layer devices exhibited low device efficiencies due to a deteriorated charge carrier balance. The multilayer devices possessed hole- and electron-transporting layers on the anode and cathode sides of the EML, respectively. Owing to an improved charge carrier balance, the multilayer devices exhibited higher device performance, affording considerably improved values of luminance and external quantum efficiency.

Optimizing Energy Storage Performance in Polymer Dielectrics through Dual Strategies: Constructing “Peaked” Barrieras and Enhancing Carrier Scattering

AbstractDielectric capacitors play a pivotal role in the advancement of electric power systems and emerging energy technologies. However, the deterioration of dielectric performance in energy storage materials at elevated temperatures represents a significant challenge. In this study, organic electron‐scattering agents into polyetherimide (PEI) are introduced, creating a “peaked barrier” to impede charge carrier transport. By doping PEI with an ultralow volume fraction (0.8%) of the organic molecule filler 4‐(dimethylamino)phenylboronic acid (4‐NB), the electron‐repelling nature of 4‐NB is leveraged in order to regulate charge carrier injection and transport in a synergistic manner. Consequently, the discharged energy density of the PEI composite material increases to 7.93 J cm−3 (720 kV mm−1) at 30 °C. At 150 °C, the discharged energy density increases to 5.21 J cm−3 (580 kV mm−1). In both cases, the charge and discharge efficiencies are maintained at 90%. It is noteworthy that the prepared PEI composite material also exhibits excellent charge dissipation characteristics, maintaining stable charge and discharge efficiency even after 50 000 charge–discharge cycles. In summary, the study's design concept systematically optimizes the processes of charge carrier injection, transport, and dissipation. This approach offers a novel perspective for the development of dielectrics that are suitable for long‐term energy storage.

(Invited) Probing Charge Carrier-Induced Changes in the Complex Dielectric Function in Carbon Nanotube Dispersions

The injection of charge carriers into pi-conjugated semiconductors, whether by electrochemical injection or chemical charge transfer, is a powerful approach to tune their electrical conductivity. Recently, the concept of dielectric catastrophe, where the charge carrier density is sufficiently large to significantly alter the intrinsic dielectric properties, has been demonstrated at high doping levels in organic semiconductor thin films. The observed increase in the dielectric constant leads to reduced coulombic interactions between charge carriers and the associated counterions, promoting enhanced free carrier generation and transport.Here, we employ a combination of steady state optical spectroscopy, quantitative 19F NMR studies, and microwave dielectric loss spectroscopy to probe charge carrier density and transport in doped single-walled carbon nanotube dispersions. We demonstrate that a similar dielectric catastrophe phenomenon can be observed even in isolated single-walled carbon nanotubes dispersed in a low dielectric constant solvent AND, perhaps more surprisingly, at carrier densities less than one carrier per nanotube. The precise details of the observed changes in complex dielectric function are dependent on the chemical structure of the charge-transfer dopant, with a near-instantaneous increase in the dielectric constant and electrical conductivity observed for low carrier densities using bulky benzyloxy-substituted icosahedral dodecaborane cluster dopants, DDBs. We attribute the observations to weak coulombic interactions between the injected charge carrier and the dopant counterion, along with the large polarizability afforded by the unique physicochemical properties of single-walled carbon nanotubes. If time permits, we will show results from recent studies where we extend this approach to the doping of other nanocarbons.

(Invited) Enabling Bio-Realistic Artificial Intelligence Hardware with Neuromorphic Nanoelectronics

The exponentially improving performance of digital computers has recently slowed due to the speed and power consumption issues resulting from the von Neumann bottleneck. In contrast, neuromorphic computing aims to circumvent these limitations by spatially co-locating logic and memory in a manner analogous to biological neuronal networks [1]. Beyond reducing power consumption, neuromorphic devices provide efficient architectures for image recognition, machine learning, and artificial intelligence [2]. This talk will explore how low-dimensional nanoelectronic materials enable gate-tunable neuromorphic devices [3]. For example, by utilizing self-aligned, atomically thin heterojunctions, dual-gated Gaussian transistors have been realized, which show tunable anti-ambipolarity for artificial neurons, competitive learning, spiking circuits, and mixed-kernel support vector machines [4,5]. In addition, field-driven defect motion in polycrystalline monolayer MoS2 enables gate-tunable memristive phenomena that serve as the basis of hybrid memristor/transistor devices (i.e., ‘memtransistors’) that concurrently provide logic and data storage functions [6]. The planar geometry of memtransistors further allows multiple contacts and dual gating that mimic the behavior of biological systems such as heterosynaptic responses [7]. Moreover, control over polycrystalline grain structure enhances the tunability of potentiation and depression, which enables unsupervised continuous learning in spiking neural networks [8]. Finally, the moiré potential in asymmetric twisted bilayer graphene/hexagonal boron nitride heterostructures gives rise to robust electronic ratchet states. The resulting hysteretic, non-volatile injection of charge carriers enables room-temperature operation of moiré synaptic transistors with diverse bio-realistic neuromorphic functionalities and efficient compute-in-memory designs for low-power artificial intelligence and machine learning hardware [9].[1] V. K. Sangwan, et al., Matter, 5, 4133 (2022).[2] V. K. Sangwan, et al., Nature Nanotechnology, 15, 517 (2020).[3] M. E. Beck, et al., ACS Nano, 14, 6498 (2020).[4] M. E. Beck, et al., Nature Communications, 11, 1565 (2020).[5] X. Yan, et al., Nature Electronics, DOI: 10.1038/s41928-023-01042-7 (2023).[6] X. Yan, et al., Advanced Materials, 34, 2108025 (2022).[7] H.-S. Lee, et al., Advanced Functional Materials, 30, 2003683 (2020).[8] J. Yuan, et al., Nano Letters, 21, 6432 (2021).[9] X. Yan, et al., Nature, DOI: 10.1038/s41586-023-06791-1 (2023).

Solid Solution Behavior of High Performance BiOBrxI1-X Photoanodes Probed Using Solid-State NMR, XRD and Optical Spectroscopy

Bismuth oxyhalides (BIOX) are a family of solution-synthesizable 2D layered semiconductors constituted of earth-abundant elements namely bismuth, oxygen and the halogens. BIOX based thin films and heterojunctions are the subject of immense scientific interest due to their impressive performance in photocatalytic and photoelectrochemical devices. Solid solutions of Br/I bismuth oxyhalides exhibit continuously tunable absorption and emission spectra similar to that observed in mixed halide MAPbClxBryI3-x-y perovskites and mixed anion III-V GaAsxP1-x semiconductors. The excited state decay showed two components for all the mixed halide BiOX semiconductors with a dominant short-lived component in the nanosecond range and a weaker longer-lived component of ~100 ns. The average photoluminescence (PL) lifetime varied from 5.4 ns in bare BiOI to 1.49 ns in bare BiOBr with intermediate compositions exhibiting monotonically increasing average PL lifetimes with increasing iodine content. Using a combination of characterization techniques such as solid-state nuclear magnetic resonance (ssNMR), x-ray diffraction (XRD), x-ray photoelectron spectroscopy (XPS) and optical spectroscopy, we demonstrate the formation of atomic level solid solutions in Br/I bismuth oxyhalides. Through refinement of the lattice parameters using powder XRD and complementary atomic-level 209Bi SSNMR spectroscopy, we found that Vegard's law was obeyed by the BIOBrxI1-x solid solutions. By varying the Br:I ratio, it is also possible to tune the electronic band gap as well as the energy levels corresponding to the conduction band minimum (ECB, min) and the valence band maximum (EVB, max), thus allowing control over the thermodynamic driving force available to drive chemical reactions using photogenerated or electrically injected charge carriers. Suppression of the longitudinal optical phonon in solid solutions of Br/I bismuth oxyhalides is suggestive of lower phonon scattering of charge carriers and improved electronic transport. A synergistic enhancement of more than 1 order of magnitude in the photoelectrochemical water-splitting performance was obtained for the optimized solid solution (BiOBr0.67I0.33) under AM 1.5G 1 sun illumination. Our results pave the way for a one pot synthesis protocol to form BiOX thin films, powders and colloidal suspensions with deterministic control over the stoichiometry.

The Rise of Xene Hybrids.

Xenes, mono-elemental atomic sheets, exhibit Dirac/Dirac-like quantum behavior. When interfaced with other 2D materials such as boron nitride, transition metal dichalcogenides, and metal carbides/nitrides/carbonitrides, it enables them with unique physicochemical properties, including structural stability, desirable bandgap, efficient charge carrier injection, flexibility/breaking stress, thermal conductivity, chemical reactivity, catalytic efficiency, molecular adsorption, and wettability. For example, BN acts as an anti-oxidative shield, MoS2 injects electrons upon laser excitation, and MXene provides mechanical flexibility. Beyond precise compositional modulations, stacking sequences, and inter-layer coupling controlled by parameters, achieving scalability and reproducibility in hybridization is crucial for implementing these quantum materials in consumer applications. However, realizing the full potential of these hybrid materials faces challenges such as air gaps, uneven interfaces, and the formation of defects and functional groups. Advanced synthesis techniques, a deep understanding of quantum behaviors, precise control over interfacial interactions, and awareness of cross-correlations among these factors are essential. Xene-based hybrids show immense promise for groundbreaking applications in quantum computing, flexible electronics, energy storage, and catalysis. In this timely perspective, recent discoveries of novel Xenes and their hybrids are highlighted, emphasizing correlations among synthetic parameters, structure, properties, and applications. It is anticipated that these insights will revolutionize diverse industries and technologies.

Small sized of anion doping effect on semiconducting single-walled carbon nanotube network for field-effect transistors

Carbon nanotubes have shown great promise for high-performance, large-area, solution processable field-effect transistors due to their exceptional charge transport properties. In this study, we utilize the spin-coating method to form networks from selectively sorted semiconducting single-walled carbon nanotubes (s-SWNTs), aiming for scalable electronic device fabrication. The one-dimensional nature of s-SWNTs, however, introduces significant roughness and charge trap sites, hindering charge transport due to the van der Waals gap (∼0.32 nm) between nanotubes. Addressing this, we explored the effects of anion doping on the spin-coated s-SWNT random network, with a focus on the influence of the small size of halogen anions (0.13–0.22 nm) on these electronic properties. Raman and ultraviolet–visible–near-infrared optical spectroscopy results indicate that smaller anions significantly enhance doping effects through strong non-covalent anion–π interactions, improving charge transport and carrier injection efficiency in s-SWNTs, especially for n-type operation. This improvement is inversely proportional to the size of the halogen anions, with the smallest anion (fluorine) effectively transitioning the electrical characteristics of the s-SWNT network from ambipolar to n-type by reducing both junction and contact resistances through anion doping, based on anion–π interaction.

Organic-Inorganic Hybrid Cuprous-Based Metal Halides with Unique Two-Dimensional Crystal Structure for White Light-Emitting Diodes.

Ternary cuprous (Cu+)-based metal halides, represented by cesium copper iodide (e.g., CsCu2I3 and Cs3Cu2I5), are garnering increasing interest for light-emitting applications owing to their intrinsically high photoluminescence quantum yield and direct band gap. Toward electrically driven light-emitting diodes (LEDs), it is highly desirable for the light emitters to have a high structural dimensionality as it may favor efficient electrical injection. However, unlike lead-based halide perovskites whose light-emitting units can be facilely arranged in three-dimensional (3D) ways, to date, nearly all ternary Cu+-based metal halides crystallize into 0D or 1D networks of Cu-X (X=Cl, Br, I) polyhedra, whereas 3D and even 2D structures remain mostly uncharted. Here, by employing a fluorinated organic cation, we report a new kind of ternary Cu+-based metal halides, (DFPD)CuX2 (DFPD+=4,4-difluoropiperidinium), which exhibits unique 2D layered crystal structure. Theoretical calculations reveal a highly dispersive conduction band of (DFPD)CuBr2, which is beneficial for charge carrier injection. It is also of particular significance to find that the 2D (DFPD)CuBr2 crystals show appealing properties, including improved ambient stability and an efficient warm white-light emission, making it a promising candidate for single-component lighting and display applications.

Reducing the Metal-Graphene Contact Resistance through Laser-Induced Defects.

Graphene has been extensively studied for a variety of electronic and optoelectronic applications. The reported contact resistance between metal and graphene, or rather its specific contact resistance (R C), ranges from a few tens of Ω μm up to a few kΩ μm. Manufacturable solutions for defining ohmic contacts to graphene remain a subject of research. Here, we report a scalable method based on laser irradiation of graphene to reduce the R C in nickel-contacted devices. A laser with a wavelength of l = 532 nm is used to induce defects at the contact regions, which are monitored in situ using micro-Raman spectroscopy. Physical damage is observed using ex situ atomic force and scanning electron microscopy. The transfer length method (TLM) is used to extract R C from back-gated graphene devices with and without laser treatment under ambient and vacuum conditions. A significant reduction in R C is observed in devices where the contacts are laser irradiated, which scales with the laser power. The lowest R C of about 250 Ω μm is obtained for the devices irradiated with a laser power of 20 mW, compared to 900 Ω μm for the untreated devices. The reduction is attributed to an increase in defect density, which leads to the formation of crystallite edges and in-plane dangling bonds that enhance the injection of charge carriers from the metal into the graphene. Our work suggests laser irradiation as a scalable technology for R C reduction in graphene and potentially other two-dimensional materials.

Diode Equation for Sandwich-Type Thin-Film Photovoltaic Devices Limited by Bimolecular Recombination

Analytical diode models that relate the current to key material parameters are invaluable for understanding the device physics in photovoltaic (PV) devices. However, a diode model that accurately describes the current in thin-film PVs based on low-mobility semiconductors (including organic solar cells) limited by bimolecular recombination has been lacking. Previous models neglect effects of injected charge carriers, which are the predominant source for bimolecular recombination in thin-film PV systems with Ohmic contacts. In this work, we derive a unified diode equation for thin-film PVs based on undoped semiconductors limited by bimolecular recombination. Based on a regional approximation approach, we derive an analytical model for the current accounting for the interplay between charge-carrier extraction, injection, and bimolecular recombination. The analytical model is validated by numerical simulations and tested experimentally on organic solar cells. Our findings provide key insights into the mechanisms driving and limiting charge collection, and ultimately the power-conversion efficiency, in low-mobility PV devices. The presented framework is material agnostic and generally applicable to sandwich-type thin-film PV devices, including photodiodes and indoor light-harvesting cells. Published by the American Physical Society 2024

Evaluating Fluorinated-Aniline Units with Functionalized Spiro[Fluorene-9,9'-Xanthene] as Hole-Transporting Materials in Perovskite Solar Cells and Light-Emitting Diodes.

In the field of perovskite optoelectronics, developing hole-transporting materials (HTMs) on the spiro[fluorene-9,9'-xanthene] (SFX) platform is one of the current research focuses. The SFX inherits the merits of spirobifluorene in terms of the configuration and property, but it is more easily derivatized and regulated by virtue of its binary structure. In this work, we design and synthesize four isomeric SFX-based HTMs, namely m-SFX-mF, p-SFX-mF, m-SFX-oF, and p-SFX-oF, through varying the positions of fluorination on the peripheral aniline units and their substitutions on the SFX core, and the optoelectronic performance of the resulting HTMs is evaluated in both perovskite solar cells (PSCs) and light-emitting diodes (PeLEDs) by the vacuum thermal evaporating hole-transporting layers (HTLs). The HTM p-SFX-oF exhibits an improved power conversion efficiency of 15.21% in an inverted PSC using CH3NH3PbI3 as an absorber, benefiting from the deep HOMO level and good HTL/perovskite interface contact. Meanwhile, the HTM m-SFX-mF provides a maximum external quantum efficiency of 3.15% in CsPb(Br/Cl)3-based PeLEDs, which is attributed to its perched HOMO level and shrunken band-gap for facilitating charge carrier injection and then exciton combination. Through elucidating the synergistic position effect of fluorination on aniline units and their substitutions on the SFX core, this work lays the foundation for developing low-cost and efficient HTMs in the future.

Single-crystalline hole-transporting layers for efficient and stable organic light-emitting devices

Efficient charge-carrier injection and transport in organic light-emitting devices (OLEDs) are essential to simultaneously achieving their high efficiency and long-term stability. However, the charge-transporting layers (CTLs) deposited by various vapor or solution processes are usually in amorphous forms, and their low charge-carrier mobilities, defect-induced high trap densities and inhomogeneous thickness with rough surface morphologies have been obstacles towards high-performance devices. Here, organic single-crystalline (SC) films were employed as the hole-transporting layers (HTLs) instead of the conventional amorphous films to fabricate highly efficient and stable OLEDs. The high-mobility and ultrasmooth morphology of the SC-HTLs facilitate superior interfacial characteristics of both HTL/electrode and HTL/emissive layer interfaces, resulting in a high Haacke’s figure of merit (FoM) of the ultrathin top electrode and low series-resistance joule-heat loss ratio of the SC-OLEDs. Moreover, the thick and compact SC-HTL can function as a barrier layer against moisture and oxygen permeation. As a result, the SC-OLEDs show much improved efficiency and stability compared to the OLEDs based on amorphous or polycrystalline HTLs, suggesting a new strategy to developing advanced OLEDs with high efficiency and high stability.

Controlling the frequencies of photons emitted by a single quantum dot in a one-dimensional photonic crystal

Subject of study. A single InAs quantum dot in a one-dimensional photonic crystal based on GaAs is examined. Aim of study. The aim of this study is to develop a method for controlling photon emission frequencies from a single quantum dot within a one-dimensional photonic crystal based on changes in the electromagnetic mass of an electron in the photonic crystal medium. Method. The proposed approach leverages the effect of changing the electromagnetic mass of an electron in the photonic crystal medium, manifesting as corrections to electron energy levels depending on the optical density of the medium. To control this density, the injection of free charge carriers and the quadratic electro-optic Kerr effect are proposed. Main results. The feasibility of in situ control of photon emission frequencies from a quantum dot was demonstrated using quantum transitions between the p- and s-states of a hydrogen-like InAs quantum dot situated in the air voids of a one-dimensional GaAs photonic crystal. This control is achieved through the effect of changing the electromagnetic mass of an electron, as well as tuning the refractive index of the photonic crystal via free charge carrier injection and the electro-optic Kerr effect. Calculations indicate that the photon energy control range available in experiments is limited to several tens of microelectronvolts, restricting practical applicability, and the observed displacement effect is smaller than experimentally recorded values. However, the energy level displacement, influenced by the quantum electrodynamic effect under investigation, exhibits a quadratic dependence on the refractive index of the material forming the photonic crystal. Consequently, the method is expected to scale significantly with increasing optical density. Such photonic crystals could be constructed using metamaterials with a high refractive index. Practical significance. The findings of this study, centered on developing a method for controlling photon emission frequencies from a single quantum dot in a one-dimensional photonic crystal, lay the groundwork for photon-emitter interfaces. These interfaces will incorporate key quantum functionalities, including photonic qubits, single-photon light sources, and nonlinear quantum photon-photon gates.

Highly enhanced Quantum dot light-emitting diode performance by controlling energy resonance in inorganic insertion layers

Quantum-dot light-emitting diodes (QLED) have become a research trend in the field of new displays due to their low cost, wide color gamut, narrow bandwidth, and characteristics that enable production through the solution-gel method. However, the electrical performance of QLED is consistently constrained by energy losses and imbalanced charge carrier injection. This motivates our focus on exciton recombination and energy losses within the quantum-dot layer to enhance the electrical efficiency of QLED. In this work, we introduce a method using a CdZnS quantum dot (B-QD) interlayer to modulate energy transfer and charge carrier transport in QLED devices employing CdSe quantum dot (G-QD) as the emissive layer. By strategically incorporating a B-QD layer between the G-QD and HTL/ETL, we facilitate energy transfer due to the overlap between the excitation wavelength of B-QD and the absorption wavelength of G-QDs. This leads to enhanced energy injection in QLED devices, resulting in a high current efficiency of 39.54 Cd/A and a peak brightness of 522,272 cd/m2 for efficient QLED. The corresponding external quantum efficiency (EQE) is greatly improved from 5.62 % to 9.4 %. Our work provides a straightforward and effective approach to modulate exciton recombination and energy injection and further can be applicable to other photo-electronics devices.

Toward Gigahertz Photodetection with Transition Metal Dichalcogenides.

ConspectusTransition metal dichalcogenides (TMDCs) exhibit favorable properties for optical communication in the gigahertz (GHz) regime, such as large mobilities, high extinction coefficients, cheap fabrication, and silicon compatibility. While impressive improvements in their sensitivity have been realized over the past decade, the bandwidths of these devices have been mostly limited to a few megahertz. We argue that this shortcoming originates in the relatively large RC constants of TMDC-based photodetectors, which suffer from high surface defect densities, inefficient charge carrier injection at the electrode/TMDC interface, and long charging times. However, we show in a series of papers that rather simple adjustments in the device architecture afford TMDC-based photodetectors with bandwidths of several hundreds of megahertz. We rationalize the success of these adjustments in terms of the specific physical-chemical properties of TMDCs, namely their anisotropic in-plane/out-of-plane carrier behavior, large optical absorption, and chalcogenide-dependent surface chemistry. Just one surprisingly simple yet effective pathway to fast TMDC photodetection is the reduction of the photoresistance by using light-focusing optics, which enables bandwidths of 0.23 GHz with an energy consumption of only 27 fJ/bit.By reflecting on the ultrafast intrinsic photoresponse times of a few picoseconds in TMDC heterostructures, we motivate the application of more demanding chemical strategies to exploit such ultrafast intrinsic properties for true GHz operation in real devices. A key aspect in this regard is the management of surface defects, which we discuss in terms of its dependence on the layer thickness, its tunability by molecular adlayers, and the prospects of replacing thermally evaporated metal contacts by laser-printed electrodes fabricated with inks of metalloid clusters. We highlight the benefits of combining TMDCs with graphene to heterostructures that exhibit the ultrafast photoresponse and large spectral range of Dirac materials with the low dark currents and high responsivities of semiconductors. We introduce the bulk photovoltaic effect in TMDC-based materials with broken inversion symmetry as well as a combination of TMDCs with plasmonic nanostructures as means for increasing the bandwidth and responsivity simultaneously. Finally, we describe the prospects of embedding TMDC photodetectors into optical cavities with the objective of tuning the lifetime of the photoexcited state and increasing the carrier mobility in the photoactive layer.The findings and concepts detailed in this Account demonstrate that GHz photodetection with TMDCs is feasible, and we hope that these bright prospects for their application as next-generation optoelectronic materials motivate more chemists and material scientists to actively pursue the development of the more complicated material combinations outlined here.