Suppression Of Auger Recombination Research Articles

Research on the assessment of technical methods to suppress auger recombination

Human demand for fossil fuels has reached a very high level. However, fossil energy stocks are limited and, more importantly, their impact on the environment is increasing. The exploration of clean energy is particularly important. Among all the clean energy sources, solar energy is a very promising and important alternative to fossil fuels. And one of the primary reasons for the failure of solar photovoltaic cells to achieve rapid development is the generation of Auger composite. In order to provide support to solve this problem or facilitate the follow-up of researchers, this paper summarizes several effective methods such as Interfacial Engineering and Gradient Alloying to solve the Auger recombination problem in multi-exciton photovoltaic cells through reading and comparing a large number of relevant authoritative literature. The two methods mentioned above suppress Auger recombination by applying a new type of MXene (Nb2CTX-MXene) to the interface of SnO2 layers to pssivate the interfacial defects and promote charge transport and to generate InAs/CdSe core/shell QDs, overcoating InAs QDs with a lattice-matched CdSe shell. Comparing a large number of pieces of literature, it is found that the above two methods have guiding effects in improving the efficiency of photovoltaic cells.

Green Light from Red-Emitting Nanocrystals: Broadband, Low-Threshold Lasing from Colloidal Quantum Shells in Optical Nanocavities.

Spherical semiconductor nanoplatelets, known as quantum shells (QSs), have captured significant interest for their strong suppression of Auger recombination, which leads to long multiexciton lifetimes and wide optical gain bandwidth. Yet, the realization of benefits associated with the multiexciton lasing regime using a suitably designed photonic cavity remains elusive. Here, we demonstrate broadly tunable lasing from close-packed films of CdS/CdSe/CdS QSs deposited over nanopillar arrays on Si substrates. Wide spectral tuning of the stimulated emission in QSs with a fixed bandgap value was achieved by engaging single exciton (λX ∼ 634 nm), biexciton (λBX ∼ 627 nm), and multiple exciton (λMX ∼ 615-565 nm) transitions. The ensemble-averaged gain threshold of <N> ∼ 2.6 electron-hole pairs per QS particle and the low photonic cavity fluence threshold of ∼4 μJ/cm2 were attributed to Auger suppression. The tuning of the lasing emission closely aligns with our model predictions achieved by varying the array period while preserving mode confinement and quality (Q) factors. These results mark a notable step toward the development of colloidal nanocrystal lasers.

Long-Lived and Bright Biexcitons in Quantum Dots with Parabolic Band Potentials.

Multiple exciton physics in semiconductor nanocrystals play an important role in optoelectronic devices. This work investigates radially alloyed CdZnSe/CdS nanocrystals with suppressed Auger recombination due to the spatial separation of carriers, which also underpins their performance in optical gain and scintillation experiments. Due to suppressed Auger recombination, the biexciton lifetime is greater than 10 ns, much longer than most nanocrystals. The samples show optical gain, amplified spontaneous emission, and lasing at thresholds <2 excitons per particle. They also show broad gain bandwidth (>500 meV) encompassing 4 amplified spontaneous emission bands. Similarly enabled by slowed multiple exciton relaxation, the samples display strong performance in scintillating films under X-ray illumination. The CdZnSe/CdS samples have fast radioluminescence rise (<80 ps) and decay times (<5 ns), light yields up to 6700 photons·MeV-1, and the demonstrated capacity for incorporation into large area films for scintillation imaging.

Correction: Tian et al. Fluorescence Resonance Energy Transfer Properties and Auger Recombination Suppression in Supraparticles Self-Assembled from Colloidal Quantum Dots. Inorganics 2023, 11, 218

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Highly Efficient Van Der Waals Heterojunction on Graphdiyne toward the High-Performance Photodetector.

Graphdiyne (GDY), a new 2D material, has recently proven excellent performance in photodetector applications due toits direct bandgap and high mobility. Different from the zero-gap of graphene, these preeminent properties made GDY emerge as a rising star for solving the bottleneck of graphene-based inefficient heterojunction. Herein, a highly effective graphdiyne/molybdenum (GDY/MoS2 ) type-II heterojunction in a charge separation is reported toward a high-performance photodetector. Characterized by robust electron repulsion of alkyne-rich skeleton, the GDY based junction facilitates the effective electron-hole pairs separation and transfer. This results in significant suppression of Auger recombination up to six times at the GDY/MoS2 interface compared with the pristine materials owing to an ultrafast hot hole transfer from MoS2 to GDY. GDY/MoS2 device demonstrates notable photovoltaic behavior with a short-circuit current of -1.3 × 10-5 A and a large open-circuit voltage of 0.23V under visible irradiation. As a positive-charge-attracting magnet, under illumination, alkyne-rich framework induces positive photogating effect on the neighboring MoS2 , further enhancing photocurrent. Consequently, the device exhibits broadband detection (453-1064nm) with a maximum responsivity of 78.5 A W-1 and a high speed of 50 µs. Results open up a new promising strategy using GDY toward effective junction for future optoelectronic applications.

Fluorescence Resonance Energy Transfer Properties and Auger Recombination Suppression in Supraparticles Self-Assembled from Colloidal Quantum Dots

Colloid quantum dots (CQDs) are recognized as an ideal material for applications in next-generation optoelectronic devices, owing to their unique structures, outstanding optical properties, and low-cost preparation processes. However, monodisperse CQDs cannot meet the requirements of stability and collective properties for device applications. Therefore, it is urgent to build stable 3D multiparticle systems with collective physical and optical properties, which is still a great challenge for nanoscience. Herein, we developed a modified microemulsion template method to synthesize quantum dot supraparticles (QD-SPs) with regular shapes and a high packing density, which is an excellent research platform for ultrafast optical properties of composite systems. The redshift of the steady-state fluorescence spectra of QD-SPs compared to CQD solutions indicates that fluorescence resonance energy transfer (FRET) occurred between the CQDs. Moreover, we investigated the dynamic processes of energy transfer in QD-SPs by time-resolved ultrafast fluorescence spectroscopy. The dynamic redshift and lifetime changes of the spectra further verified the existence of rapid energy transfer between CQDs with different exciton energies. In addition, compared with CQD solutions, the steady-state fluorescence lifetime of SPs increased and the fluorescence intensity decreased slowly with increasing temperature, which indicates that the SP structure suppressed the Auger recombination of CQDs. Our results provide a practical approach to enhance the coupling and luminescence stability of CQDs, which may enable new physical phenomena and improve the performance of optoelectronic devices.

Electrically driven amplified spontaneous emission from colloidal quantum dots

Colloidal quantum dots (QDs) are attractive materials for realizing solution-processable laser diodes that could benefit from size-controlled emission wavelengths, low optical-gain thresholds and ease of integration with photonic and electronic circuits1–7. However, the implementation of such devices has been hampered by fast Auger recombination of gain-active multicarrier states1,8, poor stability of QD films at high current densities9,10 and the difficulty to obtain net optical gain in a complex device stack wherein a thin electroluminescent QD layer is combined with optically lossy charge-conducting layers11–13. Here we resolve these challenges and achieve amplified spontaneous emission (ASE) from electrically pumped colloidal QDs. The developed devices use compact, continuously graded QDs with suppressed Auger recombination incorporated into a pulsed, high-current-density charge-injection structure supplemented by a low-loss photonic waveguide. These colloidal QD ASE diodes exhibit strong, broadband optical gain and demonstrate bright edge emission with instantaneous power of up to 170 μW.

Simultaneous Dual‐Color Amplified Spontaneous Emission and Lasing from Colloidal Quantum Well Gain Media in their Own Layered Waveguide and Cavity

AbstractMicro/nanoscale semiconductor multicolor lasers offer great potential for enhanced‐performance photonic circuits. Colloidal quantum wells (CQWs) are excellent candidates as active materials for these platforms owing to their superior properties including suppressed Auger recombination and large absorption cross‐section. In this work, multicolor optical gain and lasing from the heterostructures of CQWs as the gain media in their own all‐solution processed optical cavity are proposed and demonstrated for the first time. Here, using a simple waveguide slab consisting of the thin films of green‐emitting CdSeS/Cd0.1Zn0.9S core/hot‐injection‐shell grown CQWs and red‐emitting CdSe/CdS@CdZnS core/crown@shell CQWs, a transparent low refractive index colloidal spacing layer of silica nanoparticles (NPs) is devised that critically suppresses otherwise detrimental nonradiative energy transfer between the green and red‐emitting CQWs. This multilayer configuration is key to enabling simultaneous amplified spontaneous emission behavior in two colors with low threshold levels. This layered architecture is further adapted to a whispering‐gallery‐mode cavity by fabricating a microdisk pattern directly out of these CQWs‐NPs‐CQWs colloids. The resulting device exhibits dual‐color multimode lasing both at 569 and 648 nm at the same time. This unique multicolor lasing layered architecture holds great promise for on‐chip photonic applications such as dual‐color biological imaging.

An efficient green-emitting quantum dot with near-unity quantum yield and suppressed Auger recombination for high-performance light-emitting diodes

Near 100% photoluminescence quantum yield (PL QY) is the first target for designing luminescent quantum dots (QDs). Here, an alloyed QD with a core/shell structure of Cd0.194Zn0.806Se0.406S0.594/ZnS is synthesized and characterized by the feature of large core size (about 10 nm) and thin shell (around three ZnS monolayers). It exhibits an efficient green emission with the PL QY of 99.8% and ultra-fast radiative transition rate (kr) of 4.16 × 107 s−1. It demonstrates that the excited state will be rapidly decayed to its ground state through a radiative channel and less vulnerable to non-radiative processes. Under a high pump intensity (254.65 μJ cm−2), the Cd0.194Zn0.806Se0.406S0.594/ZnS QD still owns a long biexciton decay lifetime (τxx) of 1.05 ns and high biexciton QYxx of 25.1%, corresponding to a suppressed non-radiative Auger recombination. The Cd0.194Zn0.806Se0.406S0.594/ZnS QD based light-emitting diode exhibits a peak external quantum efficiency of 20.1% and brightness of over 105 cd m−2 at 5.2 V. We believe that the Cd0.194Zn0.806Se0.406S0.594/ZnS QD not only provides a near-unity QY but also ensures its QD based light-emitting diode (QLED) with an excellent performance, which could be an excellent QD material for QLED applications.

Single particle level dynamics of photoactivation and suppression of Auger recombination in aqueous Cu-doped CdS quantum dots.

Cu-doped CdS quantum dots (QDs) have been synthesized in water using 3-mercaptopropionic acid (3-MPA) as the capping agent. They exhibit intense photoluminescence and excellent color tunability, unlike most of the QDs synthesized/dispersed in water so far. Complete characterization of these aqueous doped CdS QDs has been performed for the first time, along with a single particle level elucidation of their exciton dynamics using fluorescence correlation spectroscopy. Photoactivation via dim/dark to bright particle conversion is observed at higher excitation powers. Dispersive blinking kinetics in undoped QDs reflects the involvement of a broad distribution of trap states. A lesser extent of dispersity is observed for doped QDs, in which hole-capture by Cu-defect states predominates. Excitation fluence dependence of the blinking rate highlights the role of Auger recombination in undoped QDs, which is suppressed significantly upon doping, due to disruption of the electron-hole correlation.

Suppressed Auger recombination and enhanced emission of InP/ZnSe/ZnS quantum dots through inner shell manipulation.

Understanding the influence of the inner shell on fluorescence blinking and exciton dynamics is essential to promote the optical performances of InP-based quantum dots (QDs). Here, the fluorescence blinking, exciton dynamics, second-order correlation function g2(τ), and ultrafast carrier dynamics of InP/ZnSe/ZnS QDs regulated by the inner ZnSe shell thickness varying from 2 to 7 monolayers (MLs) were systematically investigated. With an inner ZnSe shell thickness of 5 MLs, the photoluminescence quantum yield (PL QY) can reach 98% due to the suppressed blinking and increased probability of multiphoton emission. The exciton dynamics of InP/ZnSe/ZnS QDs with different inner shells indicates that two decay components of neural excitons and charged trions are competitive to affect the photon emission behavior. The probability density distributions of the ON and OFF state duration in the blinking traces demonstrate an effective manipulation of the inner ZnSe shell in the non-radiative processes via defect passivation. Accordingly, the radiative recombination dominates the exciton deactivation and the non-radiative Auger recombination rate is remarkably reduced, leading to a QY close to unity and a high PL stability for InP/ZnSe/ZnS QDs with 5 MLs of the ZnSe shell. These results provide insights into the photophysical mechanism of InP-based QDs and are significant for developing novel semiconductor PL core/shell QDs.

Suppressing Auger Recombination of Perovskite Quantum Dots for Efficient Pure-Blue-Light-Emitting Diodes

It is a big challenge to achieve pure-blue (≤470 nm) perovskite light-emitting diodes (PeLEDs) with high efficiency and stability. Here, we report pure-blue (electroluminescence at 469 nm) PeLEDs with a full width at half-maximum of 21 nm, high external quantum efficiency of 10.3%, luminance of 12 060 cd m–2, and continuous operation half-life of 25 h, representing the state-of-the-art performance. This design is based on strongly quantum confined CsPbBr3 quantum dots (QDs) with suppression of Auger recombination, which was enabled by inorganic ligands, replacing initial organic ligands on the QDs. The inorganic ligand acts as a “capacitor” to alleviate the charge accumulation and reduce the exciton binding energy of the QDs, which suppresses the Auger recombination, resulting in much lower efficiency roll-off of PeLEDs. Thus, the devices maintain high efficiency (>10%) at high luminance (>2000 cd m–2), which is of considerable significance for the display application.

Balancing the Number of Quantum Wells in HgCdTe/CdHgTe Heterostructures for Mid-Infrared Lasing.

HgCdTe-based heterostructures with quantum wells (QWs) are a promising material for semiconductor lasers in the atmospheric transparency window (3-5 μm) thanks to the possibility of suppressing Auger recombination due to the no-parabolic law of carrier dispersion. In this work, we analyze the thresholds of stimulated emission (SE) under optical pumping from heterostructures with a different number of QWs in the active region of the structure. Total losses in structures are determined from the comparison of thresholds for the different number of QWs in the active region. It is shown that, thanks to the increased modal gain, a higher number of QWs results in lower threshold pumping intensity and, consequently, higher temperature of SE. These results indicate that improvements to the modal gain can result in a moderate uplift in the temperature of SE from mid-infrared HgCdTe-based heterostructures. On the other hand, at a high enough QW count threshold, the intensity no longer depends on the number of the QWs and is determined by the transparency concentration of a single QW.

Colloidal Quantum Dot Infrared Lasers Featuring Sub-Single-Exciton Threshold and Very High Gain.

The use of colloidal quantum dots (CQDs) as a gain medium in infrared laser devices has been underpinned by the need for high pumping intensities, very short gain lifetimes, and low gain coefficients. Here, PbS/PbSSe core/alloyed-shell CQDs are employed as an infrared gain medium that results in highly suppressed Auger recombination with a lifetime of 485ps, lowering the amplified spontaneous emission (ASE) threshold down to 300µJcm-2 , and showing a record high net modal gain coefficient of 2180cm-1 . By doping these engineered core/shell CQDs up to nearly filling the first excited state, a significant reduction of optical gain threshold is demonstrated, measured by transient absorption, to an average-exciton population-per-dot 〈Nth 〉g of 0.45due to bleaching of the ground state absorption. This in turn have led to a fivefold reduction in ASE threshold at 〈Nth 〉ASE =0.70excitons-per-dot, associated with a gain lifetime of 280ps. Finally, these heterostructured QDs are used to achieve near-infrared lasing at 1670nm at a pump fluences corresponding to sub-single-exciton-per-dot threshold (〈Nth 〉Las =0.87). This work brings infrared CQD lasing thresholds on par to their visible counterparts, and paves the way toward solution-processed infrared laser diodes.

High-Efficiency Pure-Red Perovskite Quantum-Dot Light-Emitting Diodes

It is still challenging to achieve high-efficiency pure-red (620-650 nm wavelength) perovskite light-emitting diodes (PeLEDs). Herein, we report pure-red PeLEDs with Commission Internationale de l'Eclairage coordinates (0.703, 0.297) meeting the Rec. 2020, an external quantum efficiency of 20.8%, and a luminance of 3775 cd/m2. This design is based on the strong quantum confinement CsPbI3 quantum dots (QDs) capped by composite ligands of 3-phenyl-1-propylamine and tetrabutylammonium iodide. This strategy stabilized the structure of the strong-confined QDs and reduced the influence of the electric field-induced Stark effect on the PeLEDs. Furthermore, the exciton binding energy of the QDs was decreased by the composited ligands to suppress Auger recombination within the devices. Additionally, the valence-band maximum of the QDs was lifted to match the hole-transport layer, thus balancing charge injection in the PeLEDs. Our device also demonstrated a stable electroluminescence spectrum and a lifetime of 5.6 times longer than the control device.

Pushing the Emission Envelope for Full-Color Realization of Colloidal Semiconductor Core/Shell Nanoplatelets

Colloidal semiconductor nanoplatelets (NPLs) have been known to exhibit favorable optical characteristics, such as a narrow emission bandwidth, giant oscillator strength, suppressed Auger recombination, and polarized emission, which can merit their use in light-emitting diodes and lasing devices. However, to date, NPLs have shown a relatively limited range of emission energy because of their thickness-dependent discrete band gap and restricted choice of chemical composition (mostly CdSe-based), impeding the realization of R, G, and B full-color display based on NPLs. CdSe-based core/shell NPLs can only cover the emission range from yellowish green (∼550 nm) to red (∼620 nm). In this study, we synthesize CdZnSe/ZnS core/shell NPLs with significantly enhanced spectral tunability over a broad spectral range (425–570 nm). Particularly, to overcome the difficulty in the synthesis of composition-controlled CdZnSe NPLs, we carried out a Cd-to-Zn direct cation exchange reaction on CdSe/ZnS core/shell NPLs using ZnI2 and an oleylamine (or trioctylphosphine oxide) ligand, which allows for the composition change in NPL emitting core while maintaining the original shape of NPLs. With the control of the reaction temperature and time as well as the ligands, the exchange reaction enables us to demonstrate an unprecedentedly wide emission range and spectral tunability of NPLs with the emission wavelength reaching 425 nm. Furthermore, as the core alloying proceeds, NPLs maintain excellent color purity and exhibit linearly polarized emission. Our light-emitting devices using the cation-exchanged CdZnSe/ZnS NPLs hinted at the possibility of using the NPLs in full-color display applications. Based on the elemental mapping analysis and experimental results, we proposed the temperature-dependent cation exchange reaction process in core/shell NPLs.

(Keynote) Colloidal Quantum Shells: An Emerging Class of 2D Semiconductors

Low-dimensional colloidal semiconductors are inexpensive to process and offer a broad spectrum of attractive quantum-mechanical properties. The notorious problem of these nanostructures lies in their limited performance under high energetic loads, when more than one exciton per particle is created. Multiple excitons undergo fast Auger recombination, causing efficiently roll-off in energy-intensive applications, including high-brightness LEDs, X-ray scintillators, and solar cells. This presentation will discuss an emerging type of low-dimensional semiconductors, known as colloidal quantum shells that allow avoiding such multi-exciton (MX) energy losses. The geometry of quantum shells benefits from the spatial separation of multiple excitons, which leads to extraordinary improvements to MX lifetimes and MX quantum yield. We will compare quantum shells with other nanoscale geometries in three categories: Auger suppression, multi-exciton level structure, and solution-processed film conductivity, highlighting the potential benefits quantum shells can contribute to various applications. Theoretical analysis discussing the role of the quantum shell geometry in suppressing Auger recombination will also be presented.

(Invited) Quantum Well Architecture to Realize High Optical Gain Lasing Media

Photonic applications of semiconductor quantum dots (QDs) had significant drawbacks due to their ultrafast Auger decay of multiple excitons. These nonradiative processes have hindered the performance of electroluminescent and lasing devices. The emergence of the colloidal quantum well (QW) architecture where semiconductor quantum shell with an inverted QD geometry has led to suppressed Auger recombination. Ultra long biexciton lifetime (>10 ns) and large biexciton quantum yields has been achieved through spatial separation promoted by the QW geometry. Moreover, architecture induced exciton-exciton repulsions have led to the splitting of exciton and biexciton optical transitions which resulted in the single exciton gain mode along with the biexciton gain mode. High biexciton lifetime and the longest reported single exciton gain lifetime (>6 ns) has rendered this geometry a worthy candidate for the development of optically and electrically pumped gain media

Superior External Quantum Efficiency of LEDs via Quasi-2D Perovskite Crystals Implanted with Phenethylammonium Acetate.

The multiple quantum well structure of a quasi-two-dimensional (quasi-2D) perovskite leads to nonradiative Auger recombination (AR). This is due to high local carrier density in recombination centers, although the radiative recombination is improved by efficient energy transfer. In this study, we suppress the AR by introducing phenethylammonium acetate (PEAAc) into the quasi-2D PEA2Csn-1PbnBr3n+1 perovskite. The recombination centers of n ≥ 4 phases can be promoted because the COO- preferentially coordinates with Pb2+, inhibiting the fast formation of n = 1, 2, 3 phases with phenethylammonium anion (PEA+). Thus, the AR is suppressed due to the lower density of local charge carriers. To balance the AR suppression and decreasing binding energy in promoting the n ≥ 4 phases, the PEAAc:PEABr molar ratios are adjusted. At the optimal molar ratio, perovskite light-emitting diodes (PeLEDs) with a maximum luminescence of ∼29942 cd m-2 and a maximum external quantum efficiency of ∼20.2% are achieved. These results confirm the most efficient PeLEDs based on PEA2Csn-1PbnBr3n+1 without passivation. Moreover, the efficiency roll off is significantly mitigated with a high threshold of over 3.51 mA/cm2. This study develops high-efficiency PeLEDs with a low efficiency rolloff.

Efficient generation of emissive many-body correlations in copper-doped colloidal quantum wells

Colloidal quantum wells (CQWs) provide an appealing platform to achieve emissive many-body correlations for novel optoelectronic devices, given that they act as hosts for strong carrier Coulomb interactions and present suppressed Auger recombination. However, the demonstrated high-order excitonic emission in CQWs requires ultrafast pumping with high excitation levels and can only be spectrally resolved at the single-particle level under cryogenic conditions. Here, through systematic investigation using static power-dependent emission spectroscopy and transient carrier dynamics, we show that Cu-doped CdSe CQWs exhibit continuous-wave-pumped high-order excitonic emission at room temperature with a large binding energy of ∼64 meV. We attribute this unique behavior to dopant excitons in which the ultralong lifetime and the highly localized wavefunction facilitate the formation of many-body correlations. The spectrally resolved high-order excitonic emission generated at power levels compatible with solar irradiation and electrical injection might pave the way for novel solution-processed solid-state devices. • Continuous-wave-pumped high-order excitonic emission at room temperature is shown • The excitation level is compatible with solar irradiation and electrical injection • 64 meV binding energy enables spectrally resolved high-order excitonic emission Yu et al. demonstrate continuous-wave-pumped high-order excitonic emission at room temperature in Cu-doped CdSe colloidal quantum wells. The properties of dopant excitons enable an ultra-low excitation level compatible with solar irradiation or electrical injection and a binding energy of ∼64 meV, which makes the high-order excitonic emission spectrally resolvable at room temperature.