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.
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Coupled Self‐Scintillation and Photodetection in PbS Quantum Dots/Graphene X‐Ray Detectors
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.
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- Award ID(s):
- 2447841
- PAR ID:
- 10667754
- Publisher / Repository:
- Wiley
- Date Published:
- Journal Name:
- Advanced Optical Materials
- ISSN:
- 2195-1071
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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