Quantum dots (QDs) offer several advantages in optoelectronics such as easy solution processing, strong light absorption and size tunable direct bandgap. However, their major limitation is their poor film mobility and short diffusion length (<250 nm). This has restricted the thickness of QD film to ∼200–300 nm due to the restriction that the diffusion length imposes on film thickness in order to keep efficient charge collection. Such thin films result in a significant decrease in quantum efficiency for λ > 700 nm in QDs photodetector and photovoltaic devices, causing a reduced photoresponsivity and a poor absorption towards the near-infrared part of the sunlight spectrum. Herein, we demonstrate 1 μm thick QDs photodetectors with intercalated graphene charge collectors that avoid the significant drop of quantum efficiency towards λ > 700 nm observed in most QD optoelectronic devices. The 1 μm thick intercalated QD films ensure strong light absorption while keeping efficient charge extraction with a quantum efficiency of 90%–70% from λ = 600 nm to 950 nm using intercalated graphene layers as charge collectors with interspacing distance of 100 nm. We demonstrate that the effect of graphene on light absorption is minimal. We achieve a time-modulation response of <1 s. We demonstrate that this technology can be implemented on flexible PET substrates, showing 70% of the original performance after 1000 times bending test. This system provides a novel approach towards high-performance photodetection and high conversion photovoltaic efficiency with quantum dots and on flexible substrates.
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This content will become publicly available on July 19, 2025
Intercalated Graphene and Colloidal Quantum Dots for Multispectral Photodetection
Hybrid photodetectors with 2D materials and quantum dots (QDs) offer new opportunities for spectral detection given their high mobilities and spectral tunability, respectively. Herein, the study presents a novel architecture of alternating PbS QDs with graphene monolayers positioned at different depths and with independent contacts. This geometry enables the probing of the photocurrent depth profile and therefore of different spectral bands. The study realizes devices with up to five graphene layers and five QD layers intercalated, using only one type of QDs (Single‐Bandgap devices) with an exciton absorption peak at 920 nm, as well as devices with different types of QDs (Multi‐Bandgap devices) with exciton peaks at 850, 1190, and 1350 nm. Since the absorption depth and photoresponse is wavelength dependent, each graphene has a different spectral response, which opens the path for spectral analysis. As expected, it is observed that top graphene layers have stronger response than deeper graphene layers, especially for short wavelengths. However, for the case of Multi‐Bandgap devices, a negative photoresponse coefficient is even observed for longer wavelengths, showing stronger response for deeper layers than for top layers. This intercalated architecture can be used for compact multispectral photodetection without any diffractive or beam splitting component.
more » « less- Award ID(s):
- 2046176
- PAR ID:
- 10524747
- Publisher / Repository:
- Wiley
- Date Published:
- Journal Name:
- Advanced Functional Materials
- ISSN:
- 1616-301X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Colloidal quantum dots/graphene (QD/Gr) nanohybrids have been studied intensively for photodetection in a broadband spectrum including ultraviolet, visible, near-infrared, and shortwave infrared (UV−vis-NIR-SWIR). Since the optoelectronic process in the QD/Gr nanohybrid relies on the photogenerated charge carrier transfer from QDs to graphene, understanding the role of the QD−QD and QD−Gr interfaces is imperative to the QD/Gr nanohybrid photodetection. Herein, a systematic study is carried out to probe the effect of these interfaces on the noise, photoresponse, and specific detectivity in the UV−vis-NIR-SWIR spectrum. Interestingly, the photoresponse has been found to be negligible without a 3-mercaptopropionic acid (MPA) ligand exchange, moderate with a single ligand exchange after all QD layers are deposited on graphene, and maximum if it is performed after each QD layer deposition up to five layers of total QD thickness of 260−280 nm. Furthermore, exposure of graphene to C-band UV (UVC) for a short period of 4−5 min before QD deposition leads to improved photoresponse via removal of polar molecules at the QD/Gr interface. With the combination of the MPA ligand exchange and UVC exposure, optimal optoelectronic properties can be obtained on the PbS QD/Gr nanohybrids with high specific detectivity up to 2.6 × 1011, 1.5 × 1011, 5 × 1010, and 1.9 × 109 Jones at 400, 550, 1000, and 1700 nm, respectively, making the nanohybrids promising for broadband photodetection.more » « less
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