PbS quantum dots (QDs) are promising materials for short-wave infrared (SWIR) photodetectors due to their tunable bandgap and broad spectral absorption. This study explores the impact of trioctylphosphine (TOP)-mediated surface reconstruction on PbS QDs, revealing that the TOP treatment enhances QD surface morphology, reduces trap states, and improves QD stacking behavior in solid films. Notably, a diode-type photodetector based on TOP-treated QDs exhibits a significantly enhanced specific detectivity (D*) of 2.07 x 10(11) Jones at 1290 nm, which is 50 times higher than that of devices using conventional QDs. It also shows a marked reduction in dark current density to 237 nA cm(-2) at -0.5 V. Furthermore, the TOP-QD photodetector demonstrates improved storage stability under non-encapsulated conditions, underscoring the effectiveness of TOP-mediated surface reconstruction in enhancing both performance and reliability. This work offers valuable insights into the surface engineering of PbS QDs and presents a pathway for the development of high-performance, solution-processed SWIR imaging systems and environmental monitoring technologies.
This study proposes a bilayer interface engineering strategy that significantly enhances device performance in inverted PbS quantum dot photodetectors through the incorporation of an ultrathin LiF layer and a conventional C60 layer. The LiF/C60 bilayer structure effectively passivates surface traps, improves film flatness, and ensures favorable energy level alignment and efficient electron extraction. Experimental results demonstrate that devices employing this strategy exhibit nearly an order of magnitude reduction in dark current, an increase in external quantum efficiency from 15.45% to 28.90%, and a specific detectivity exceeding 8.47 & times; 10(11) Jones-representing a more than sixfold improvement compared to unmodified devices.
Comprehensive Summary Despite recent breakthroughs in organic solar cell (OSC) efficiency, the trade‐off between broadening spectral response and minimizing non‐radiative energy loss remains a critical bottleneck. While ternary strategies and sequential deposition (SqP) each offer unique benefits, their single‐dimensional optimization often fails to balance efficient photon harvesting with ideal vertical phase separation. Herein, we report a multi‐dimensional synergistic regulation strategy by incorporating polymer acceptor PYF‐T‐ o into the SqP‐processed PM6/eC9 system, where PYF‐T‐ o establishes a cascade energy‐level alignment and forms an alloy‐like acceptor phase with eC9. This unique microstructure broadens spectral absorption, lowers the donor/acceptor surface energy difference, accelerates crystallization kinetics (reducing nucleation time by 60 ms), and refines phase separation. Consequently, the ternary devices exhibit balanced carrier mobilities, ultrafast charge extraction (0.197 μs), and prolonged carrier lifetime (4.54 μs), effectively suppressing trap‐assisted recombination. The energetic disorder is reduced to 23.43 meV, minimizing non‐radiative voltage loss from 0.218 eV to 0.205 eV. By utilizing a 2PACz self‐assembled monolayer, the optimized device achieves a high power conversion efficiency of 20.23% and demonstrates enhanced photostability with the T 80 lifetime extended from 117 h to 260 h. This work establishes a robust paradigm for synchronously reducing energy loss and enhancing device performance via multi‐dimensional synergistic regulation.
Short-wave infrared colloidal quantum dot photodetectors are promising for low-cost, solution-processable infrared imaging, but their performance and reproducibility are limited by the trade-off between efficient hole extraction and leakage-current suppression. Here, we report a P3HT/PTB7-Th hybrid polymer hole-transport layer that simultaneously regulates molecular packing and film morphology in PbS quantum-dot photodetectors. GIWAXS and AFM reveal that polymer blending induces tighter, preferentially out-of-plane π–π stacking while suppressing excessive crystallization and surface roughness, consistent with more favorable hole extraction and reduced defect-related leakage. The optimized devices exhibit reduced dark current, suppressed noise, enhanced external quantum efficiency, a specific detectivity of up to 7.36 × 1012 Jones, a demonstrated linear dynamic range of at least 80 dB, and fast rise/fall times of 2.45/10.31 μs. Statistical measurements confirm improved device-to-device uniformity compared with single-polymer hole-transport layers. A monolithically integrated 12 × 12 photodetector array further demonstrates SWIR imaging under 1310 nm illumination without post-processing, while pixel-level statistics indicate reduced electrical variation in the optimized hybrid array. This work highlights molecular-packing engineering of hybrid polymer interlayers as an effective strategy for scalable and reproducible quantum-dot infrared optoelectronics.
Precisely controlling reaction pathway is vital for selective oxidation chemistry but remains challenging due to the complexity of oxidant-catalyst interactions, especially during activation of peracetic acid (PAA) that offers greater structural flexibility than inorganic oxidants. While various catalyst engineering approaches are available to strengthen PAA nonradical catalysis, they fail to fundamental suppress radicals generation. Here, we propose an interlayer confinement strategy to deterministically reprogram the PAA activation pathway toward singlet oxygen (1O2) generation. By stabilizing atomically dispersed cobalt sites within a KOH-compressed interlayer space of montmorillonite (MT) nano-galleries (CoSAC-KMT), a deck-effect-induced confined microenvironment is constructed to fundamentally alters the PAA-catalyst interaction. Such confinement suppresses radical-dominated channels and redirects PAA activation route to nearly exclusive 1O2 generation. Mechanistic and theoretical analyses reveal that reduced interlayer spacing reshapes the local PAA adsorption configuration and energy landscape to facilitate 1O2 formation. Such a confinement regulation strategy can also be extended to peroxymonosulfate (PMS) activation for efficient pathway modulation, indicating it may serve as a transferable principle to guide Fenton-like catalyst design. With 1O2-dominated pathway, the CoSAC-KMT/PAA system demonstrated superior environmental robustness and long-term stability for real water treatment.
Colloidal PbS quantum dots (QDs) are promising for short-wave infrared (SWIR) photodetection and imaging but intrinsically suffer from surface defects and poor stacking configuration in solids. Here, we employ 1-octanethiol (OT) mixing with bis(trimethylsilyl) sulfide (TMS) as double sulfur sources to dynamically regulate PbS QD growth and surface passivation. By optimizing the OT/TMS ratio, the resulting QDs exhibit improved monodispersity, reduced surface defects, and prolonged carrier lifetimes. Grazing-incidence small-angle X-ray scattering (GISAXS) reveals that OT drives QDs toward octahedral-like morphologies and orders body-centered cubic superlattices, distinct from the truncated octahedral and face-centered cubic structures of control QDs. Such morphology with less (100) facet regulation reduces the trap density and enhances inter-dot electronic coupling after ligand exchange. Devices based on the OT-QDs demonstrate suppressed dark current, higher external quantum efficiency (59.1% at 1308 nm), and improved specific detectivity reaching 8.34 & times; 1011 Jones.
Colloidal quantum dots (CQDs) have emerged as a promising material platform for short-wave infrared (SWIR) detection and imaging, demonstrating significant potential for applications in information sensing, biomedical imaging, industrial inspection, and consumer electronics. Compared to conventional infrared semiconductors, such as InGaAs and InSb, CQDs exhibit unique advantages, including tunable bandgap, solution-processability, abundant raw materials, and compatibility with scalable manufacturing, enabling substantial cost reduction and ease of integration with existing electronic platforms. This review systematically summarizes recent advances in high-performance CQD-based SWIR photodetectors and imaging systems. Firstly, representative CQD materials covering IV-VI, II-VI, and III-V semiconductor families are analyzed, emphasizing their bandgap tunability, stability, toxicity profiles, and synthesis methodologies. Among these, PbS quantum dots (QDs) have been extensively explored and have achieved the most mature material control and device fabrication techniques, reaching near-industrial readiness. Secondly, the thin-film deposition processes critical to device performance are discussed. The review highlights solid-state and solution-phase ligand exchange methods crucial for converting discrete colloidal particles into highly dense and electrically conductive CQD films. Current approaches, including spin-coating, blade-coating, spray-coating, and inkjet printing, are analyzed, along with post-treatment strategies such as annealing and crosslinking to improve film uniformity, carrier mobility, and overall stability. These advancements have enabled precise control over film morphology and interface properties, significantly enhancing device efficiency and reproducibility. Thirdly, device architectures including photoconductors, photodiodes, and phototransistors are reviewed, with particular focus on photodiodes due to their superior performance in terms of dark current suppression, fast response, and low power consumption. Innovations in interface engineering, such as interfacial passivation, introduction of blocking layers, and heterojunction designs, have effectively reduced dark current densities to sub-nanoampere per square centimeter levels, enabling substantial improvements in signal-to-noise ratio and detectivity (D*). The review also extensively covers the key photodetector parameters, such as external quantum efficiency (EQE), responsivity (R), linear dynamic range (LDR), response speed, and noise characteristics. Recent breakthroughs demonstrate EQE surpassing 80%, responsivities over several amperes per watt, and LDR exceeding 120 dB. Meanwhile, advancements in interface engineering and low-capacitance design have pushed the device response time into the nanosecond regime, significantly broadening the potential application scope to include high-speed optical communications, time-of-flight imaging, and dynamic object tracking. Finally, the integration of CQD photodetectors with CMOS and thin-film transistor (TFT) readout circuits is discussed, showcasing successful demonstrations of SWIR imaging chips. Recent efforts from domestic and international research groups have led to significant milestones, including the realization of the first domestic 640 & times;512 pixel CMOS-integrated PbS CQD imaging chip and innovative vertical stacking strategies for multispectral imaging. In summary, this review provides a comprehensive evaluation of state-of-the-art CQD-based SWIR photodetection and imaging technology, highlighting current achievements, remaining challenges, and future research directions. Continuous development in material chemistry, film processing, device structure optimization, and intelligent system integration is expected to further establish CQDs as a cost-effective and highly capable technology for next-generation infrared imaging applications across industrial, biomedical, consumer, and defense sectors.
ABSTRACT Colloidal lead sulfide quantum dots are attractive for short‐wave infrared photodetectors due to their tunable bandgap and solution‐process compatibility, yet device performance is often limited by high dark current, inefficient carrier extraction, and poor stability. Here, we report a new strategy of combining thermal spin‐coating and annealing that improves quantum dot film quality by regulating solvent evaporation kinetics and stacking behavior during deposition. Elevating the substrate temperature during spin‐coating induces dense and uniform quantum dot assemblies with reduced trap density and improved interfacial contact. Photodetectors fabricated at an optimized temperature of 65°C exhibit substantially enhanced performance, including a responsivity of 0.765 A/W, a specific detectivity of 3.57 × 10 1 1 Jones, and a −3 dB bandwidth of 108 kHz, accompanied by over 50% reduction in dark current density. Importantly, the optimized devices show improved long‐term stability, retaining lower dark current and higher external quantum efficiency after prolonged storage without encapsulation. Leveraging these advantages, the photodetectors are further integrated into an imaging array and applied to non‐invasive glucose monitoring using dual‐wavelength ratiometric detection. This work establishes thermal spin‐coating as a simple and scalable route toward high‐performance, stable quantum dot infrared photodetectors for imaging and biomedical sensing applications.
Halide-capped PbS colloidal quantum dots (CQDs) prepared via solution-phase ligand exchange (SPLE) are promising materials for next-generation optoelectronic devices owing to their effective surface passivation. Nevertheless, deep traps and band-tail states in CQD solids are often intertwined, obscuring individual impacts on device performance. Here, we introduce two alkylamines, pentylamine (PA) and hexylamine (HA), as additives in a butylamine-based cosolvent system to decouple these electronic defects. The HA additive significantly suppresses deep trap states by improving halide passivation and directly coordinating with Pb on the CQD surface, whereas the PA additive promotes structural ordering and thus reduces band-tail states in CQD solids due to the formation of a 2D layered structure through its preferential interactions with the halide matrix. Incorporating the HA additive enables PbS CQD photodetectors (PDs) in zero-bias photovoltaic mode to achieve a remarkable responsivity of 0.76 A/W and an external quantum efficiency of 72% in the short-wave infrared (SWIR) region. Thus, device performance is dominated by deep traps at the CQD surface and interfacial defects in the device architecture, providing insights for high-performance CQD optoelectronic devices.
Despite the efficacy of self-assembled monolayers (SAMs) in ITO work function modulation, their impact on active layer crystallization kinetics, notably the donor/acceptor (D/A) nucleation mismatch, remains an underexplored efficiency-limiting factor in organic solar cells (OSCs). Herein, we propose an asymmetric pi-extended molecule, CbzPh, whose extra benzene ring affords a larger dipole than 4PACz (ITO work function: 5.28 eV vs. PEDOT:PSS's 4.87 eV) and strengthens non-covalent interactions with D/A molecules. The strong PM6-CbzPh interactions not only accelerate donor nucleation to promote balanced D/A film formation kinetics but also generate a donor-rich region near ITO, thereby enhancing charge selection and hole collection. Furthermore, this strategy minimizes D/A crystallization interference, improves polycrystalline orientation and coherence length, and suppresses trap states and energetic disorder, lowering non-radiative loss to 0.224 eV. With CbzPh replacing PEDOT:PSS, the PM6:L8-BO device achieves a FF of 81.14%, a PCE of 20.10% (up from 18.59%), and T-80 > 420 h. The universality of the strategy is testified across different systems with PCEs of 19.98%, 20.09%, 20.24% (certified 20.02%), and 20.88% (certified 20.48%) for PM6:BTP-eC9, PM6:L8-BO-C4, PM6:L8-BO-X, and D18:L8-BO, respectively. This work reveals that asymmetric pi-extended CbzPh suppresses non-radiative recombination via synchronous crystallization, providing new insights into SAM mechanisms for OSCs.
Engineering electron transport layer (ETL) interface is critical for high-efficiency and long-term stability in inverted perovskite solar cells (PSCs), yet co-assembled hybrid interlayer are rarely explored for this upper interface. This work integrates 4-aminobenzoate acid hydrochloride (4AA) with a dibenzo-18-crown-6 (DB18C6) to construct a hybrid interlayer at ETL interface. The 4AA molecules intercalate into DB18C6 aggregates, homogenizing the monolayer and boosting surface coverage (from 0.57 to 0.79) and strengthening the interfacial dipole moment (from 2 to 7 Debye). This interlayer provides dual passivation, in which the ─NH3 + and ─COOH groups of 4AA neutralize ionic defects, while DB18C6 optimizes perovskite crystallinity and energy level alignment. Therefore, modified devices achieve an efficiency of 26.33% (exceeding 22.92% of the control) with high open-circuit voltage (VOC) of 1.167 V and fill factor (FF) of 86.05% (compared to 1.130 V and 80.38% of the control). More importantly, the co-assembled hybrid interlayer serves as a barrier against environmental and ionic degradation. The unencapsulated device demonstrates outstanding operational stability, retaining 93.2% of initial efficiency after 1000 h of maximum power point tracking. This work demonstrates a co-assembly strategy to address efficiency and stability challenges at ETL interface, paving a reliable path toward high-performance and stable inverted PSCs.
To overcome the layer stacking effect in TiVC films, a laser writing technique was applied. With optimized laser power, an interlayer expansion of 23 times was achieved without compromising the structural integrity. This structural modification effectively facilitates ion transport while preserving the intrinsic high capacity of TiVC. As a result, the electrode retained 42.7% of its capacitance at an ultrahigh scan rate of 1000 mV s-1, demonstrating an exceptional combination of high capacity and outstanding rate performance.
The electrochemical performance of Ti3C2Tx MXene arises from chemical and electrostatic interactions between its surface terminations and interlayer molecules. Moving beyond the conventional paradigm of relying on the intercalation of external guest species to modulate this network, this study addresses a more fundamental question: can the interaction environment be intrinsically engineered from within the MXene lattice? Here, carbon (C) vacancies are introduced as a precise strategy to polarize the surface electronic structure, specifically enhancing the electronegativity of oxygen terminations. This polarization strengthens the hydrogen bonding (H-bonding) interactions with confined water, leading to the formation of a thermally stable, "active and fixed" interlayer architecture. This optimized structure results in a significant increase in intrinsic capacitance, with the Ti3C1.7 electrode achieving 348 F g-1 at 5 mV s-1, a 47% enhancement over the near-stoichiometric Ti3C2.0. Subsequent anodic oxidation alleviated ion diffusion limitations at high rates, synergistically improving rate capability. The co-engineered electrode achieved a high capacitance of 382 F g-1 while retaining 45% capacitance at an ultra-high scan rate of 5000 mV s-1. This work establishes the rational design of interfacial H-bonding networks as a core principle for advanced MXene electrodes, offering a pathway to high energy and power densities.
The temperature-dependent photoluminescence of CsPbBr3/SiO2 and CsPbI3/SiO2 nanocrystals was investigated to understand the thermal stability of SiO2 encapsulation. At increased temperature, intensity quenching, linewidth broadening, energy level shift, and decay dynamics were evaluated as quantified parameters. Comprehensive analysis of these parameters supports that CsPbI3/SiO2 nanocrystals show a stronger interaction with phonons compared with CsPbBr3/SiO2 nanocrystals. Despite SiO2 encapsulation, we conclude that trapping states are still present and the degree of localization can be characterized in terms of short-lived decay time and thermal activation energy.
Chiral vanadium oxide nanoparticles (V2O3 NPs) with different chiroptical signals were successfully prepared by employing tartaric acid, malic acid, and penicillamine as chirality-inducing agents. These chiral nanoparticles show sensitivity to pH values as they could express various optical transition modes such as charge transfer, d-d transitions, and surface plasmon resonance due to their rich electronic states, leading to tunable chiral optical activities in the UV-visible range. The different colors of V2O3 NPs with varied ligands at different pH values indicate the configuration variation of the chiral ligands as revealed by UV-visible absorption spectroscopy and circular dichroism (CD) characterizations. In addition, the as-synthesized chiral V2O3 NPs exhibit suitable properties for use as biomolecular probes and exhibit a limit of detection (LOD) of 3.185 mu M for H2O2 sensing, indicating that chiral V2O3 NPs could provide a highly sensitive and real-time sensing scheme, which may provide a useful strategy for the development of chiral materials in the areas of chiroptics and biosensors.
PbS colloidal quantum dots(QDs)show great promise for short-wave infrared(SWIR)photodetection due to their tunable photoresponse and cost-effective solution processability,positioning them as a strong competitor to InGaAs technologies.Inverted device architectures,essential for compatibility with complementary metal-oxide-semiconductor(CMOS)readout circuits,face performance challenges due to limitations in the hole transport layer(HTL),such as porous NiOx structures that cause surface recombination at low annealing temperatures.To overcome these challenges,herein,we develop a multi-HTL strategy integrating NiOx,1,2-ethanedithiol(EDT)-treated PbS,and self-assembled monolayers(SAMs)including[2-(9H-carbazol-9-yl)ethyl]phosphonic acid(2PACz)and[2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl]phosphonic acid(MeO-2PACz),significantly boosting the performance of inverted PbS QD photodetectors,with full-fullerene-based electron transport layers(ETLs).We confirm that the SAMs can effectively block electron transfer and passivate surface defects between the HTL and active layer,with 2PACz achieving an external quantum efficiency of 53%at 1200 nm and MeO-2PACz reducing dark current to 220 nA/cm2,yielding a specific detectivity of 1.64×1012 Jones,which represents the highest reported value under similar testing conditions and in this spectral region.This multi-HTL strategy enables high-performance SWIR imaging compatible with CMOS and thin-film transistor(TFT)circuits,advancing QD-based photodetection technologies.
Despite the rapid efficiency advancement of perovskite solar cells (PSCs), non-radiative recombination at the buried interface between self-assembled monolayers (SAMs) and perovskite remains a critical bottleneck, primarily due to interfacial defects and energy level mismatch. In this study, we demonstrate a bifunctional interlayer engineering strategy by introducing 4,5-diiodoimidazole (4,5-Di-I) at the Me-4PACz/perovskite interface. This approach uniquely addresses two fundamental limitations of SAM-based interfaces: the insufficient defect passivation capability of conventional Me-4PACz due to steric hindrance effects and the poor perovskite wettability on hydrophobic SAM surfaces that exacerbates interfacial voids. The imidazole derivatives not only form strong Pb–N coordination bonds with undercoordinated Pb2+ but also modulate the surface energy of Me-4PACz, enabling the growth of pinhole-free perovskite films with preferential crystal orientation. The champion device with 4,5-Di-I modification achieves a power conversion efficiency (PCE) of 24.10%, with a VOC enhancement from 1.12 V to 1.14 V, while maintaining 91% of initial PCE after 1300 h in N₂ atmosphere (25 °C), demonstrating superior stability under ISOS-L-2 protocols. This work establishes a universal strategy for interfacial multifunctionality design, proving that simultaneous defect suppression and crystallization control can break the long-standing trade-off between efficiency and stability in solution-processed photovoltaics.
Photodetectors based on emerging semiconductors such as quantum dots and perovskites have been under development for over two decades, but the use of diverse characterization methods and set-ups make it increasingly difficult to compare device performance. A more standardized approach to external quantum efficiency characterization is now essential.
Interfacial engineering using phenethyl-ammonium iodide (PEAI) is employed to improve inverted PbS quantum dot (QD) short-wave infrared photodetectors. Placement of a PEAI layer between NiOx and the QD active layer passivates defects, suppresses recombination, and reduces low-frequency noise. Optimal treatment lowers the 1 Hz noise current density from $3.06 \times 10^{-11}$ to $3.04 \times 10^{-12} ~\mathrm{A} / \sqrt{ } \text{Hz}$, yielding a specific detectivity enhancement from $\text{2. 8 5} \times \text{1 0}^{\mathrm{9}}$ to $\text{1. 4 2} \times \text{1 0}^{\text{1 0}}$ Jones at $\text{1 1 5 0 ~ n m}$. Bandwidth and temporal response are improved while maintaining operational stability, offering a CMOS-compatible pathway toward high-performance SWIR imaging.