An official website of the United States government
Abstract Nanohybrids consisting of graphene and colloidal semiconductor quantum dots (QDs/graphene) can combine the benefits of strong quantum confinement in the constituent components, such as high carrier mobility in graphene and large exciton binding energy in QDs, to enable extraordinary photoconductive gain and hence high photoresponse. Furthermore, QDs/graphene nanohybrids are inherently flexible, making them ideal for flexible photodetectors. Despite exciting progress made in rigid and flexible QDs/graphene photodetectors in broadband from UV to short-wave infrared, flexible middle-wave infrared (MWIR) photodetectors remain a challenge. Herein, we report the first success in fabrication of HgTe QDs/graphene nanohybrid ultrabroadband (400–4000 nm wavelength) photodetectors on flexible polyimide substrates via resolving critical issues of device fabrication on flexible substrates, which allowed flexible device performance approaching their counterparts on rigid substrates. Specifically, the flexible HgTe QDs/graphene nanohybrids photodetectors exhibited high responsivity (R*) across the ultrabroadband spectrum at room temperature. At 550 nm, 1.5 μm and 4.0 μm wavelengths, anR* of up to 0.65 AW−1, 5.7 × 10−3AW−1and 0.9 × 10−3AW−1were achieved respectively. Bending tests confirmed performance stability of the flexible HgTe QDs/graphene nanohybrids photodetectors under repeated bending with up to 5.5 mm radius of curvature. Images taken in the ultrabroadband while the photodetectors in flat and bent states both show promising imaging quality. This result illustrates the potential applications of the uncooled, flexible HgTe QDs/graphene nanohybrids photodetectors in the ultrabroadband range of 400–4000 nm.
more »
« less
Decoupling of Photocurrent and Dark Current for Extraordinary Detectivity in Uncooled Middle-Wavelength Infrared Nanohybrid Photodetectors
Nanohybrids of graphene and colloidal semiconductor quantum dots (QDs/Gr) provide a promising quantum sensing scheme for photodetection. Despite exciting progress made in QDs/Gr photodetectors in broadband from ultraviolet to short-wave infrared, the device performance is limited in middle-wave infrared (MWIR) detection. A fundamental question arises as to whether the thermal noiseinduced dark current and hence poor signal-to-noise ratio in conventional uncooled MWIR photodetectors persist in QDs/ Gr nanohybrids. Herein, we investigated noise, responsivity (R*), and specific detectivity (D*) in HgTe QDs/Gr nanohybrids, revealing that the noise and R* are decoupled in nanohybrids and each can be optimized independently toward its theoretical limit. Specifically, the noise in the QDs/Gr nanohybrids is dominated by that of graphene with a negligible effect from the dark current in HgTe QDs and can be optimized to its intrinsic limit by removing charge doping of adsorbed polar molecules on graphene. Furthermore, the R* is proportional to the photoconductive gain enabled by the strong quantum confinement in QDs and Gr. Achieving high gain in the MWIR spectrum, however, is challenging and requires elimination of charge traps primarily from the surface states of the narrow-bandgap semiconductor HgTe QDs. Using grain-rotation-induced grain-coalescence growth of single-layer and core/shell HgTe QDs, we show the that HgTe QDs surface states caused by Te deficiency can be dramatically suppressed, resulting in high gain up to 4.0 × 107 in the MWIR spectrum. The optimized noise and R* have led to high uncooled MWIR D* up to 2.4 × 1011 Jones, making nanohybrids promising to surpass the fundamental dark-current limit in conventional photodetectors.
more »
« less
- PAR ID:
- 10599057
- Publisher / Repository:
- ACS
- Date Published:
- Journal Name:
- ACS Nano
- Volume:
- 19
- Issue:
- 9
- ISSN:
- 1936-0851
- Page Range / eLocation ID:
- 8520 to 8538
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Tong, Xin; Wu, Jiang; Wang, Zhiming (Ed.)Colloidal semiconductor quantum dot/graphene van der Waals heterostructure nanohybrids are emerging technologies for photodetection. These nanohybrids combine the advantages of the enhanced light-matter interaction and spectral tunability of quantum dots (QDs) and superior charge mobility in graphene, providing an affordable alternative for uncooled photodetectors with high gain or external quantum efficiency in a wide spectral range. In particular, the interfacing of QDs with high-mobility graphene as a charge transport pathway has provided an effective resolution to the critical issue of charge transport in QD-only photodetectors stemming from the low charge mobility associated with both QD surface defect states and QD-QD junctions. Furthermore, the achieved capability in industrial-scale fabrication of graphene, colloidal QDs, and QD/graphene nanohybrids has motivated efforts in researches of focal plane arrays that are expected to be not only high performance and low cost but also lightweight, flexible, and wearable. This chapter aims to provide an up-to-date review of the recent progress made in the research of QD/graphene nanohybrid photodetectors, together with a discussion on the challenges remaining and perspective in future research and development to make QD/graphene nanohybrids competitive for commercialization.more » « less
-
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.more » « less
-
ABSTRACT Colloidal quantum dot/graphene (QD/Gr) nanohybrids rely on strong quantum confinement and offer a promising platform to design high‐performance quantum sensors such as photodetectors. In QD/Gr nanohybrid photodetectors, QDs absorb the incident light, and the spectral range is determined by the QD's semiconductor bandgap with moderate tunability by QD size, which presents a challenge for QDs/Gr nanohybrids to be used for detection of photons beyond such a conventional bandgap‐determined spectral range. In this work, we explored coupled self‐scintillation and X‐ray photodetection in PbS QD/Gr nanohybrids of sub‐micron active layer thickness for compromised X‐ray self‐scintillation by Pb of high X‐ray cross section and high‐gain detection enabled by graphene on both rigid and flexible substrates. An additional critical step found to suppress noise induced by interaction of polar molecules with dangling bonds on the QD surface was achieved by a poly(methyl methacrylate) capping layer, resulting in significantly improved signal‐to‐noise ratio. This allows a maximum X‐ray sensitivity of 280 C Gy−1cm−2, together with high responsivity in visible to infrared range on the order of 10 A/W. This result has demonstrated that the conventional bandgap‐determined spectral range can be significantly expanded through design of the QD/Gr nanohybrids. The demonstrated performance and mechanical flexibility provide a pathway toward durable, flexible quantum dot‐based detectors for multi‐spectrum sensing.more » « less
-
Fulop, Gabor F.; Kimata, Masafumi; Zheng, Lucy; Andresen, Bjørn F.; Miller, John Lester (Ed.)Colloidal semiconductor quantum dots/graphene van der Waals (vdW) heterojunctions take advantages of the enhanced light-matter interaction and spectral tenability of quantum dots (QDs) and superior charge mobility in graphene, providing a promising alternative for uncooled infrared photodetectors with a gain or external quantum efficiency up to 1010. In these QD/graphene vdW heterostructures, the QD/graphene interface plays a critical role in controlling the optoelectronic process including exciton dissociation, charge injection and transport. Specifically, charge traps at the vdW interface can increase the noise, reduce the responsivity and response speed. This paper highlight our recent progress in engineering the vdW heterojunction interface towards more efficient charge transfer for higher photoresponsivity, D* and response speed. These results illustrate that the importance in vdW heterojunction interface engineering in QD/graphene photodetectors which may provide a promising pathway for low-cost, printable and flexible infrared detectors and imaging systems.more » « less
- Free Publicly Accessible Full Text
-
Accepted Manuscript
- Journal Article:
- https://doi.org/10.1021/acsnano.4c12802
