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The diffusion length of quantum dot (QD) films is a critical parameter to improve the performance of QD-based optoelectronic devices. The dot-to-dot hopping transport mechanism results in shorter diffusion lengths compared to bulk solids. Herein, we present an experimental method to measure the diffusion length in PbS QD films using single layer graphene as a charge collector to monitor the density of photogenerated carriers. By producing devices with different thicknesses, we can construct light absorption and photocarrier density profiles, allowing extracting light penetration depths and carrier diffusion lengths for electrons and holes. We realized devices with small (size: ∼2.5 nm) and large (size: ∼4.8 nm) QDs, and use λ = 532 nm and λ = 635 nm wavelength illumination. For small QDs, we obtain diffusion lengths of 180 nm for holes and 500 nm for electrons. For large QDs, we obtain diffusion lengths of 120 nm for holes and 150 nm for electrons. Our results show that films made of small QD films have longer diffusion lengths for holes and electrons. We also observe that wavelength illumination may have a small effect, with electrons showing a diffusion length of 500 and 420 nm under λ = 532 nm and λ = 635 nm illumination, respectively, which may be due to increased interactions between photocarriers for longer wavelengths with deeper penetration depths. Our results demonstrate an effective technique to calculate diffusion lengths of photogenerated electrons and holes and indicate that not only QD size but also wavelength illumination can play important roles in the diffusion and electrical transport of photocarriers in QD films. [ABSTRACT FROM AUTHOR]

Lead sulfide quantum dots (QDs) have been widely used for various optoelectronic devices due to their high absorption coefficient and tunable bandgap. However, the low mobility of QD films results in poor charge collection and device performance. By combining QDs with graphene into hybrid graphene/QD photodetectors, photocarriers from QDs are transferred to graphene, improving charge collection and transport, drastically increasing the photoresponsivity. Herein, we carry a systematic analysis on how critical tuning parameters such as QD size and QD film thickness affect responsivity, spectral response, and time response. We report the absorption coefficient, refractive index (n, k), penetration depth, and energy bandgap of PbS QDs of different sizes. We study systematically how the photocurrent, photoresponsivity, time response, and power density dependence vary with QD size in hybrid Gr/QD. The bandgap of lead sulfide quantum dots was size-tuned between 0.86 and 1.39 eV. The time response shows that subsecond modulation can be achieved for different QD sizes with a responsivity up to 107 A/W at power densities of 10−5 mW/cm2. We also studied how the performance of the photodetectors is affected by the thickness, discussing the limitations on the thickness by the compromise between light absorption and charge collection. We describe how the optical response shifts toward the infrared as QD films get thicker. Time responses below 1 s are obtained for graphene/QD devices with thickness from 150 nm to 1 μm. This systematic study provides important guidelines to design hybrid graphene/QD photodetectors and tune their spectral response and performance. [ABSTRACT FROM AUTHOR]

Hybrid graphene and quantum dots (QDs) photodetectors merge the excellent conductivity and ambipolar electric field sensitivity of graphene, with the unique properties of QDs. The photoresponsivity of these devices depends strongly on the charge transfer at the graphene/QDs interface. Here 1‐pyrene butyric acid (PBA)‐coated PbS QDs with single layer graphene (SLG) are used to investigate the effect of pyrene as a π–π mediator to enhance charge transfer at the SLG/QDs junction under illumination. The surface chemistry at the QD–QD and SLG/QD interface is studied with the conventional tetrabutylammonium iodide (TBAI) QD linker. The hybrid SLG/QD photodetectors with PBA as a SLG‐QD linker demonstrate a photoresponse up to 30% higher than that recorded for devices where only TBAI is used, due to the strong electron coupling between SLG and QDs. Transconductance measurements show that PBA provokes electron depletion in SLG ascribed to the tendency to delocalize the QDs holes, favoring their transfer to SLG. This surface ligand is found to improve the interaction between the QDs light absorbers and the SLG charge collector, leading to an increased photodetection response. This demonstrates that ligand engineering can enhance charge dynamics and boost the performance of the hybrid device. [ABSTRACT FROM AUTHOR]

Developing sensing approaches that can exploit visible light for the detection of low-concentration hydrogen at room temperatures has become increasingly important for the safe use of hydrogen in many applications. In this study, heterostructures composed of monolayer MoS 2 and Pd nanoclusters (Pd/MoS 2 ) acting as photo- and hydrogen-sensitizers are successfully fabricated in a facile and scalable manner. The uniform deposition of morphologically isotropic Pd nanoclusters (11.5 ± 2.2 nm) on monolayer MoS 2 produces a plethora of active heterojunctions, effectively suppressing charge carrier recombination under light illumination. The dual photo- and hydrogen-sensitizing functionality of Pd/MoS 2 can enable its use as an active sensing layer in optoelectronic hydrogen sensors. Gas-sensing examinations reveal that the sensing performance of Pd/MoS 2 is enhanced three-fold under visible light illumination (17% for 140 ppm of H 2 ) in comparison with dark light (5% for 140 ppm of H 2 ). Photoactivation is also found to enable excellent sensing reversibility and reproducibility in the obtained sensor. As a proof-of-concept, the integration of Pd nanoclusters and monolayer MoS 2 can open a new avenue for light-induced hydrogen gas sensing at room temperature.