Heterojunction nanohybrids based on low-dimension semiconductors, including colloidal quantum dots (QDs) and 2D atomic materials (graphene, transition metal chalcogenides, etc) provide a fascinating platform to design of new photonic and optoelectronic devices that take advantages of the enhanced light-solid interaction attributed to their strong quantum confinement and superior charge mobility for uncooled photodetectors with a high gain up to 1010. In these heterojunction nanohybrids, the van der Waals (vdW) interface plays a critical role in controlling the optoelectronic process including exciton dissociation by the interface built-in field that drives the follow-up charge injection and transport to graphene. In this paper, we present our recent progress in development of such heterostructures nanohybrids for uncooled infrared detectors including PbS and FeS2 QDs/graphene and 2D vdW heterostructures MoTe2/Graphene/SnS2 and GaTe/InSe. We have found that nonstoichiometric Fe1–xS2 QDs (x = 0.01–0.107) with strong localized surface plasmonic resonance (LSPR) can have much enhanced absorption in broadband from ultraviolet to short-wave infrared (SWIR, 1–3 μm). Consequently, the LSPR Fe1–xS2 QDs/graphene heterostructure photodetectors exhibit extraordinary photoresponsivity in exceeding 4.32 ×106 A/W and figure-of-merit detectivity D* < 7.50 ×1012 Jones in the broadband of UV–Vis–SWIR at room temperature. The 2D vdW heterostructures allows novel designs of interface band alignments with uncooled NIR-SWIR D* up to 1012 Jones. These results illustrate that the heterostructure nanohybrids provide a promising pathway for low-cost, printable and flexible infrared detectors and imaging systems.
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This content will become publicly available on April 9, 2025
Probing the Critical Role of Interfaces for Superior Performance in PbS Quantum Dot/Graphene Nanohybrid Broadband Photodetectors
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.
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- PAR ID:
- 10521255
- Publisher / Repository:
- ACS
- Date Published:
- Journal Name:
- ACS Applied Materials & Interfaces
- ISSN:
- 1944-8244
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Photodetectors based on colloidal quantum dots (QD)/graphene nanohybrids are quantum sensors due to strong quantum confinement in both QD and graphene. The optoelectronic properties of QD/graphene nanohybrids are affected by the quantum physics that predicts a high photoconductive gain and hence photoresponsivity (
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Nanohybrids represent a larger variety of functional materials consisting of one or more types of low‐dimensional semiconductor nanostructures, such as quantum dots, nanowires, nanotubes, 2D atomic materials (graphene, transition‐metal dichalcogenides, etc.) interfaced with one another, and/or with conventional material matrices (bulks, films, polymers, etc.). Heterojunction interfaces are characteristic in nanohybrids and play a critical role facilitating synergistic coupling of constituent materials of different functionalities, resulting in excellent electronic, optoelectronic, and mechanical properties. Therefore, nanohybrids provide fresh opportunities for designs of optoelectronic devices of extraordinary performance in addition to the benefits of low cost, large abundance, flexibility, and light weight. Herein, some recent achievements in exploiting new optoelectronic nanohybrids and understanding the underlying physics toward high‐performance optoelectronic nanohybrids that are competitive in commercialization of various optoelectronic devices are highlighted. Using nanohybrid photodetectors as an example, the importance in controlling the heterojunction interfaces and multiscale controlling of optoelectronic process of light absorption, exciton dissociation, photocarrier transfer, and transport from atomic to device scales and how this control impacts the photodetector performance are revealed. The current status, remaining challenges, and future perspectives in optoelectronic nanohybrids are also discussed.
