Solution-processed Quantum Research Articles

Solution-processed quantum dot short-wavelength infrared photodetectors via integrating 2D MXenes into electron transport layer

Solution-processed quantum dots (QDs) have attracted intensive attention in short-wavelength infrared (SWIR) photodetectors due to their excellent optical properties and tunable size-dependent bandgap. However, the intrinsic defects of the widely used ZnO electron-transport layer (ETL) and the inappropriate band alignment at the interface between the ETL and photoactive QDs inevitably impact the optoelectronic performance of the photodetector. Herein, a high-performance self-powered SWIR photodetector is developed by using 2D Ti3C2 MXenes to passivate the defects of ZnO ETL and to tailor the band alignment at the interface of the ETL/photoactive layer through interface engineering. As a result, the SWIR photodetectors demonstrate the ultra-high light-to-dark current (Ilight/Idark) ratio of ∼ 105 and the low dark current density of 8.33 × 10-4 mA/cm2, and the high specific detectivity (D*) of 1.99 × 1011 Jones at 0 V. By the systematic characterizations, it is proofed that 2D MXene can efficiently passivate defects in ZnO and optimize the alignment of energy levels between the ETL and photoactive layer, which will suppress the recombination of electrons and holes and eventually promote photogenerated carrier transfer at the interface and thus improve device performance. This work revealed that the high-performance solution-processed QD based SWIR photodetector enabled by interface engineering will promote the development of optoelectronic devices in the future.

Linearly Polarized Broadband Emission and Multiwavelength Lasing in Solution-Processed Quantum Dots.

A miniature laser with linear polarization is a long sought-after component of photonic integrated circuits. In particular, for multiwavelength polarization lasers, it supports simultaneous access to multiple, widely varying laser wavelengths in a small spatial region, which is of great significance for advancing applications such as optical computing, optical storage, and optical sensing. However, there is a trade-off between the size of small-scale lasers and laser performance, and multiwavelength co-gain of laser media and multicavity micromachining in the process of laser miniaturization remain as significant challenges. Herein, room-temperature linearly polarized multiwavelength lasers in the visible and near-infrared wavelength ranges are demonstrated, by fabricating random cavities scattered with silica in an Er-doped Cs2Ag0.4Na0.6In0.98Bi0.02Cl6 double-perovskite quantum dots gain membrane. By regulating the local symmetry and enabling effective energy transfer in nanocrystals, multiwavelength lasers with ultralow thresholds are achieved at room temperature. The maximum degree of polarization reaches 0.89. With their advantages in terms of miniaturization, ultralow power consumption, and adaptability for integration, these lasers offer a prospective light source for future photonic integrated circuits aimed at high-capacity optical applications.

Photothermal Synergic Cross-Linking Hole Transport Layer for Highly Efficient RGB QLEDs.

Developing an insoluble cross-linkable hole transport layer (HTL) plays an important role for solution-processed quantum dots light-emitting diodes (QLEDs) to fabricate a multilayer device with separated quantum dots layers and HTLs. In this work, a facile photothermal synergic cross-linking strategy is simultaneous annealing and UV irradiation to form the high-quality cross-linked film as the HTL without any photoinitiator, which efficiently reduces the cross-linking temperature to the low temperature of 130 °C and enhances the hole mobility of the 3-vinyl-9-{4-[4-(3-vinylcarbazol-9-yl)phenyl]phenyl}carbazole (CBP-V) thin films. The obtained high-quality cross-linked CBP-V films exhibited smooth morphology, excellent solvent resistance, and high mobility. Moreover, the high-performance red, green, and blue (RGB) QLEDs are successfully fabricated by using the photothermal synergic cross-linked HTLs, which achieved the maximum external quantum efficiency of 25.69, 24.42, and 16.51%, respectively. This work presents a strategy of using the photothermal synergic cross-linked HTLs for fabrication of high-performance QLEDs and advancing their related device applications.

Direct Optical Patterning of MoO3 Nanoparticles and Their Application as a Hole Injection Layer for Solution-Processed Quantum Dot Light-Emitting Diodes

Direct Optical Patterning of MoO₃ Nanoparticles and Their Application as a Hole Injection Layer for Solution-Processed Quantum Dot Light-Emitting Diodes

Simulation and design of dual-wavelength all-optical semiconductor optical amplifier with solution-processed quantum dots

All-optical semiconductor optical amplifiers (SOAs) present a cost-effective and highly efficient solution for long-distance WDM networks. In this study, the investigation of a dual-wavelength all-optical SOA incorporating two distinct sizes of solution-processed InAs/AlAs core/shell quantum dots (QDs), operating at 1.31 and 1.55 μm wavelengths, both simultaneously and individually, has been proposed. To comprehensively evaluate the optical performance of our proposed dual-wavelength all-optical SOA, the modified coupled rate equations governing carriers dynamics and the optical photon propagation equations have been solved numerically while taking into account both homogeneous and inhomogeneous broadening, as well as fluorescence or förster resonance energy transfer (FRET) effects. This computational approach provides valuable insights into the optical behavior of dual-wavelength all-optical SOA. In our proposed structure, cost-effective solution-based methods for implementing QDs of varying sizes offer flexibility to adjust QD size across a broad range, from as small as 0.1 nm to meet specific requirements. This adjustment is made with meticulous consideration of appropriate synthesis techniques.

Record high external quantum efficiency of 20% achieved in fully solution-processed quantum dot light-emitting diodes based on hole-conductive metal oxides

Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) has been widely used as a hole injection material in quantum dot (QD) light-emitting diodes (QLEDs). However, it degrades the organic materials and electrodes in QLEDs due to its strong hydroscopicity and acidity. Although hole-conductive metal oxides have a great potential to solve this disadvantage, it is still a challenge to achieve efficient and stable QLEDs by using these solution-processed metal oxides. Herein, the state-of-the-art QLEDs fabricated by using hole-conductive MoOx QDs are achieved. The α-phase MoOx QDs exhibit a monodispersed size distribution with clear and regular crystal lattices, corresponding to high-quality nanocrystals. Meanwhile, the MoOx film owns an excellent transmittance, suitable valence band, good morphology and impressive hole-conductivity, demonstrating that the MoOx film could be used as a hole injection layer in QLEDs. Moreover, the rigid and flexible red QLEDs made by MoOx exhibit peak external quantum efficiencies of over 20%, representing a new record for the hole-conductive metal oxide based QLEDs. Most importantly, the MoOx QDs afford their QLEDs with a longer T95 lifetime than these devices made by PEDOT:PSS. As a result, we believe that the MoOx QDs could be used as efficient and stable hole injection materials used in QLEDs.

Gallium Sulfide Quantum Dots with Zinc Sulfide and Alumina Shells Showing Efficient Deep Blue Emission.

Solution-processed quantum dot (QD) based blue emitters are of paramount importance in the field of optoelectronics. Despite large research efforts, examples of efficient deep blue/near UV-emitting QDs remain rare due to lack of luminescent wide band gap materials and high defect densities in the existing ones. Here, we introduce a novel type of QDs based on heavy metal free gallium sulfide (Ga2 S3 ) and their core/shell heterostructures Ga2 S3 /ZnS as well as Ga2 S3 /ZnS/Al2 O3 . The photoluminescence (PL) properties of core Ga2 S3 QDs exhibit various decay pathways due to intrinsic defects, resulting in a broad overall PL spectrum. We show that the overgrowth of the Ga2 S3 core QDs with a ZnS shell results in the suppression of the intrinsic defect-mediated states leading to efficient deep-blue emission at 400 nm. Passivation of the core/shell structure with amorphous alumina yields a further enhancement of the PL quantum yield approaching 50 % and leads to an excellent optical and colloidal stability. Finally, we develop a strategy for the aqueous phase transfer of the obtained QDs retaining 80 % of the initial fluorescence intensity.

Ultrafast Cascade Charge Transfer in Multibandgap Colloidal Quantum Dot Solids Enables Threshold Reduction for Optical Gain and Stimulated Emission.

Achieving low-threshold infrared stimulated emission in solution-processed quantum dots is critical to enable real-life applications including photonic integrated circuits (PICs), LIDAR application, and optical telecommunication. However, realization of low threshold infrared gain is fundamentally challenging due to high degeneracy of the first emissive state (e.g., 8-fold) and fast Auger recombination. In this Letter, we demonstrate ultra-low-threshold infrared stimulated emission with an onset of 110 μJ cm-2 employing cascade charge transfer (CT) in Pb-chalcogenide colloidal quantum dot (CQD) solids. In doing so, we investigate this idea in two different architectures including a mixture of multiband gap CQDs and a layer-by-layer (LBL) configuration. Using transient absorption spectroscopy, we show ultrafast cascade CT from large band gap PbS CQD to small band gap PbS/PbSSe core/shell CQDs in LBL (∼2 ps) and mixture (∼9 ps) configurations. These results indicate the feasibility of using cascade CT as an efficient method to reduce the optical gain threshold in CQD solid films.

Low-Temperature Cross-Linkable Hole Transport Materials for Solution-Processed Quantum Dot and Organic Light-Emitting Diodes with High Efficiency and Color Purity.

Cross-linkable hole transport materials (HTMs) are ideal for improving the performance of solution-processed quantum dot light-emitting diodes (QLEDs) and phosphorescent light-emitting diodes (OLEDs). However, previously developed cross-linkable HTMs possessed poor hole transport properties, high cross-linking temperatures, and long curing times. To achieve efficient cross-linkable HTMs with high mobility, low cross-linking temperature, and short curing time, we designed and synthesized a series of low-temperature cross-linkable HTMs comprising dibenzofuran (DBF) and 4-divinyltriphenylamine (TPA) segments for highly efficient solution-processed QLEDs and OLEDs. The introduction of divinyl-functionalized TPA in various positions of the DBF core remarkably affected their chemical, physical, and electrochemical properties. In particular, cross-linked 4-(dibenzo[b,d]furan-3-yl)-N,N-bis(4-vinylphenyl)aniline (3-CDTPA) exhibited a deep highest occupied molecular orbital energy level (5.50 eV), high hole mobility (2.44 × 10-4 cm2 V-1 s-1), low cross-linking temperature (150 °C), and short curing time (30 min). Furthermore, a green QLED with 3-CDTPA as the hole transport layer (HTL) exhibited a notable maximum external quantum efficiency (EQEmax) of 18.59% with a remarkable maximum current efficiency (CEmax) of 78.48 cd A-1. In addition, solution-processed green OLEDs with 3-CDTPA showed excellent device performance with an EQEmax of 15.61%, a CEmax of 52.51 cd A-1, and outstanding CIE(x, y) color coordinates of (0.29, 0.61). This is one of the highest reported EQEs and CEs with high color purity for green solution-processed QLEDs and OLEDs using a divinyl-functionalized cross-linked HTM as the HTL. We believe that this study provides a new strategy for designing and synthesizing practical cross-linakable HTMs with enhanced performance for highly efficient solution-processed QLEDs and OLEDs.

Inverted Solution-Processed Quantum Dot Light-Emitting Devices with Wide Band Gap Quantum Dot Interlayers.

Despite its benefits for facilitating device fabrication, utilization of a polymeric hole transport layer (HTL) in inverted quantum dots (QDs) light-emitting devices (IQLEDs) often leads to poor device performance. In this work, we find that the poor performance arises primarily from electron leakage, inefficient charge injection, and significant exciton quenching at the HTL interface in the inverted architecture and not due to solvent damage effects as is widely believed. We also find that using a layer of wider band gap QDs as an interlayer (IL) in between the HTL and the main QDs' emission material layer (EML) can facilitate hole injection, suppress electron leakage, and reduce exciton quenching, effectively mitigating the poor interface effects and resulting in high electroluminescence performance. Using an IL in IQLEDs with a solution-processed poly(9,9-dioctylfluorene-alt-N-(4-sec-butylphenyl)-diphenylamine) (TFB), HTL improves the efficiency by 2.85× (from 3 to 8.56%) and prolongs the lifetime by 9.4× (from 1266 to 11,950 h at 100 cd/m2), which, to the best of our knowledge, is the longest lifetime for an R-IQLED with a solution-coated HTL. Measurements on single-carrier devices reveal that while electron injection becomes easier as the band gap of the QDs decreases, hole injection surprisingly becomes more difficult, indicating that EMLs of QLEDs are more electron-rich in the case of red devices and more hole-rich in the case of blue devices. Ultraviolet photoelectron spectroscopy measurements verify that blue QDs have a shallower valence band energy than their red counterparts, corroborating these conclusions. The findings in this work, therefore, provide not only a simple approach for achieving high performance in IQLEDs with solution-coated HTLs but also novel insights into charge injection and its dependence on QDs' band gap as well as into different HTL interface properties of the inverted versus upright architecture.

Broadband Tunable Optical Gain from Ecofriendly Semiconductor Quantum Dots with Near-Half-Exciton Threshold.

Optical gain in solution-processable quantum dots (QDs) has attracted intense interest toward next-generation optoelectronics; however, the development of optical gain in heavy-metal-free QDs remains challenging. Herein, we reveal that the ZnSe1-xTex-based QDs show excellent optical gain covering the violet to near-red regime. A new gain mechanism is established in the alloy QDs, which promotes a theoretically threshold-less optical gain thanks to the ultrafast carrier localization and suppression of ground-state absorption by the Te-derived isoelectronic state. Further, we disclose that the hot-carrier trapping represents the main culprit to exacerbate the gain performance. With the increase of Te-to-Se ratio, a sub-band-gap photoinduced absorption (PA) appears and extinguishes the optical gain. To overcome this issue, we modulate the inner ZnSe shell thickness, and the gain is recovered by reducing the overlap between the gain and PA regions in the Te-rich QDs. Our finding represents a significant step toward sustainable QD-based optoelectronics.

Vertical Architecture Solution-Processed Quantum Dot Photodetectors with Amorphous Selenium Hole Transport Layer

Colloidal quantum dots (CQDs) provide wide spectral tunability and high absorption coefficients owing to quantum confinement and large oscillator strengths, which along with solution processability, allow a facile, low-cost, and room-temperature deposition technique for the fabrication of photonic devices. However, many solution-processed CQD photodetector devices demonstrate low specific-detectivity and slow temporal response. To achieve improved photodetector characteristics, limiting carrier recombination and enhancing photogenerated carrier separation are crucial. In this study, we develop and present an alternate vertical-stack photodetector wherein we use a solution-processed quantum dot photoconversion layer coupled to an amorphous selenium (a-Se) wide-bandgap charge transport layer that is capable of exhibiting single-carrier hole impact ionization and is compatible with active-matrix readout circuitry. This a-Se chalcogenide transport layer enables the fabrication of high-performance and reliable solution-processed quantum dot photodetectors, with enhanced charge extraction capabilities, high specific detectivity (D* ∼ 0.5–5 × 1012 Jones), fast 3 dB electrical bandwidth (3 dB BW ∼ 22 MHz), low dark current density (JD ∼ 5–10 pA/cm2), low noise current (in ∼ 20–25 fW/Hz1/2), and high linear dynamic range (LDR ∼ 130–150 dB) across the measured visible electromagnetic spectrum (∼405–656 nm).

High-speed and high-contrast two-channel all-optical modulator based on solution-processed CdSe/ZnS quantum dots

Recently, all-optical modulators are potentially the most promising candidate to achieve high-bit rate modulation in high-speed all-optical communication technologies and signal processing. In this study, a two-channel all-optical modulator based on a solution-processed quantum dot structure is introduced for two sizes of quantum dots to operate at two wavelengths of MIR spectra (3 µm and 5 µm). To perform numerical and theoretical analysis and evaluate the optical behavior of the proposed all-optical modulator, the coupled rate and propagation equations have been solved by considering homogeneous and inhomogeneous broadening effects. The modulation depth at the 50 GHz frequency and 3 mW probe power is attained, about 94% for channel-1 with the wavelength of 559 nm at 300 Wcm−2 pump power density as well as approximately 83.5% for channel-2 with the wavelength of 619 nm at 500 Wcm−2 pump power density. The introduced two-channel all-optical modulator can operate simultaneously at two wavelengths during the modulation process in which information could be transmitted through both signals from the control light. This approach can present the practical device as a high-contrast and high-speed two-channel all-optical modulator with a high modulation depth in numerous applications such as thermal imaging in night vision cameras, wavelength de-multiplexing, signal processing, free-space communication.

Solution-processed quantum dot SnO2 as an interfacial electron transporter for stable fully-air-fabricated metal-free perovskite solar cells

Perovskite solar cells could strongly compete with the silicon solar cells in the market soon as illustrated in recent studies. In this work, promising and stable metal-free perovskite solar cells (PSCs) has been successfully fabricated using an inorganic SnO2/Quantum dot SnO2 (QD-SnO2) double layer as an efficient electron transport layer via a low-temperature solution process. The fully-air fabricated PSCs in the form of FTO/SnO2/QD-SnO2/CH3NH3PbI3/Carbon were tested at different annealed QD-SnO2 between 300 and 500 °C. The as-prepared QD-SnO2 and the fabricated devices are characterized by various techniques, including XRD, XPS, HR-TEM, FE-SEM, UV–vis–NIR spectroscopy, PL, and solar simulator. The prepared QD-SnO2 at 300 °C has shown well-ordered nanoparticles of 5.6 nm in diameter with superior carrier density (1.5 × 1015 cm−3) and highest carrier mobility (64.1 cm2·V-1·s−1), accelerating the carriers separation process within the cell. The best devices demonstrated a maximum power conversion efficiency (PCE) of 11.7%, VOC 0.81 V, JSC 19.5 mA·cm−2, and FF 74%. The presence of an interfacial layer of QD-SnO2 over the blocking SnO2 upsurges the band gaps alignment and accelerates the carriers extraction rate affecting the performance of the fabricated perovskite devices. Moreover, the optimized fabricated devices revealed a shelf stability-life of four months in humid air (40%–50%) with >83% of its initial PCE. This simple synthetic approach can develop the opportunities to transfer the cell from the lab to the market, which will be compatible with large-scale production.

Low-Cost Solution-Processed MoS2 Quantum Dots-Based Deep UV Photodetector for Monitoring Disinfection

Deep UV radiation is commonly used as a disinfectant with an appropriate dose for better efficacy. However, continuous monitoring of UV radiation is required to have appropriate dose exposure for proper disinfection. This article reports a low-cost solution-processed fabrication method of the UV photodetector (PD) with a device geometry of Al/MoS <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> quantum dots (QDs)/Al on Si/SiO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> substrate, which is sensitive to deep UV radiations ~275 nm, commonly used for water and surfaces disinfection technologies. Colloidal MoS <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> QDs with an average size of 1.99 nm have been synthesized by an inexpensive hydrothermal method. The surface ligand of MoS <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> QDs has been replaced by a shorter ligand 1, 2-ethanedithiol (EDT) to reduce dot-to-dot distance. The fabricated device shows high responsivity (21.62 mA/W), external quantum efficiency (EQE) (9.74%), and detectivity ( <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$3.57\times 10$ </tex-math></inline-formula> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">10</sup> Jones) under the deep UV irradiation of ~275 nm. The PD has a good photoresponse speed of rise and decay times of 173 and 92 ms, respectively.

Solution-Processed Red, Green, and Blue Quantum Rod Light-Emitting Diodes.

Solution-processed semiconductor nanocrystals are evolving as potential candidates for future display and lighting applications owing to their size-tunable emission, ultrasaturated colors, and compatibility with large-area flexible substrates. Among them, quantum rods (QRs) are emerging materials for optoelectronic applications, offering polarized emission, high light outcoupling efficiency, color purity, and better stability in solid films. However, synthesizing QRs covering the full visible wavelength region has been a big challenge, particularly in the blue range. Herein, we report for the first time the synthesis of red CdSe/CdS, green CdSe/ZnxCd1-xS/ZnS, and blue CdSe/ZnxCd1-xS/ZnS QRs and their application in red, green, and blue QR-based light-emitting diodes (QR-LEDs). We have improved the charge injection balance into the QRs through embedding a poly(methyl methacrylate) (PMMA) layer between the emissive and electron transport layers. The thin PMMA electron-blocking layer (EBL) suppresses the excessive electron flux and thus promotes charge injection balance and pushes the recombination zone back to the QR layer, resulting in 1.35×, 1.2×, and 1.7× peak external quantum efficiency improvement for red, green, and blue QR-LEDs, respectively. The efficiency roll-off of green and blue QR-LEDs with an EBL is less than 50% at maximum current density. The proposed red, green, and blue QR-LEDs open up an avenue toward further improving the light source efficiency and stability focusing on real device applications.

Boosting the performance of solution-processed quantum dots light-emitting diodes by a hybrid emissive layer via doping small molecule hole transport materials into quantum dots

Solution-processed colloidal quantum dot light-emitting diodes (QLED) have attracted many attentions with significant progress in recent years. However, QLED devices still face some challenges. The energy barrier between Cd-base quantum dots (QDs) and commonly used hole transport materials is larger than that between QDs and electron transport materials, which leads to the imbalance of carriers in the light emitting layer (EML) and the low performance of QLED devices. Herein, we report a simple strategy to improve the device performance by doping small molecule transport material 4,4′-cyclohexylidenebis[N,N-bis(p-tolyl)aniline] (TAPC) into red CdSe/ZnS QDs. The optimized red QLED devices with TAPC-doped emissive layer at a ratio of 3.2 wt% achieve 20.0 cd/A of maximum current efficiency, 16.6 lm/W of power efficiency and 15.7% of external quantum efficiency, which is 30%, 58% and 33% higher than the control device. The improved performance of devices can be ascribed to the increase of hole current density, decrease of leakage electrons and more balanced quantity of carriers in EML. This work put forward a viewpoint to improve the performance of QLED devices via doping high hole mobility materials into emission layer. • Small molecule hole transport material TAPC is doped into red CdSe/ZnS QDs to enhance the device performance. • The EML solution consists of QD octane solution and TAPC o-xylene solution. • The introduction of TAPC leads to the reduction of leakage electrons and the improvement of hole density.

Fast-response, high-stability, and high-efficiency full-color quantum dot light-emitting diodes with charge storage layer

Recently, solution-processed quantum dot light-emitting diodes (QLEDs) have emerged as a promising candidate for next-generation lighting and display devices. However, when given a constant voltage or current, the QLEDs need a certain working time to reach their maximum brightness. Such positive aging challenge, dramatically reducing the response speed of the device and causing a luminescence delay, is urgent to be investigated and resolved. In the current work, we introduce a charge-storage layer architecture by inserting copper(I) thiocyanate (CuSCN) between the organic hole-injection layer and hole-transport layer. The extracted holes will be released during the next electrical signal stimulation to increase the efficiency of charge transport. As a result, the response speed of the QLEDs is improved by an order of magnitude. In addition, by inserting an inorganic CuSCN layer, the efficiency, lifetime, and environmental stability of red/green/blue full-color QLEDs are enhanced simultaneously. Moreover, this work provides a generic strategy for the fabrication of fast-response and high-efficiency full-color QLEDs without luminescence delay, which plays a critical role in the practical industrialization of QLEDs.

Selective Energy Contacts and Multi-Wavelength Solution-Processed Quantum Dot Infrared Photodetector

In this work, a three-channel infrared photodetector with three independent related electric signals as a single optoelectronic chip has been introduced. The proposed structure has been implemented by exploiting an array of PbSe/ZnSe quantum dots and the PbSe/ZnS selective energy contacts considering solution-processed nanotechnology. The electron transport system has been designed to allow the transmission of electrons stimulated by three wavelengths simultaneously from different paths to the corresponding output. The high efficiency, simplicity and fabrication ease, cost-effectiveness, and high tunability of the photodetector have been accomplished as a consequence of solution-process technology. Moreover, the dark current has been significantly declined as a consequence of resonance tunneling in the proposed selective energy contacts. Last but not least, our proposed multi-wavelength ( λ <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">1</sub> =2.9 μm, λ <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> =2.25 μm, λ <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> =1.75 μm) infrared photodetector has been promising candidates for a wideband spectrum analyzer or multi-wavelength infrared camera.

Quantitative Electrochemical Control over Optical Gain in Quantum-Dot Solids.

Solution-processed quantum dot (QD) lasers are one of the holy grails of nanoscience. They are not yet commercialized because the lasing threshold is too high: one needs >1 exciton per QD, which is difficult to achieve because of fast nonradiative Auger recombination. The threshold can, however, be reduced by electronic doping of the QDs, which decreases the absorption near the band-edge, such that the stimulated emission (SE) can easily outcompete absorption. Here, we show that by electrochemically doping films of CdSe/CdS/ZnS QDs, we achieve quantitative control over the gain threshold. We obtain stable and reversible doping of more than two electrons per QD. We quantify the gain threshold and the charge carrier dynamics using ultrafast spectroelectrochemistry and achieve quantitative agreement between experiments and theory, including a vanishingly low gain threshold for doubly doped QDs. Over a range of wavelengths with appreciable gain coefficients, the gain thresholds reach record-low values of ∼1 × 10–5 excitons per QD. These results demonstrate a high level of control over the gain threshold in doped QD solids, opening a new route for the creation of cheap, solution-processable, low-threshold QD lasers.