skip to main content


Title: High resolution patterning of PbS quantum dots/graphene photodetectors with high responsivity via photolithography with a top graphene layer to protect surface ligands
Photodetectors based on colloidal quantum dots (CQDs) and single layer graphene (SLG) have shown high responsivity due to the synergy of strong light absorption from CQDs and high mobility from SLG. However, it is still challenging to achieve high-density and small-footprint devices on a chip to meet the demand for their integration into electronic devices. Even though there are numerous approaches to pattern the chemically fragile CQD films, usually they require non-conventional approaches such as stamping and surface modification that may be non-compatible with semiconductor processing. In this study, we show that conventional lithography and dry etching can be used to pattern QD active films by employing a graphene monolayer passivation/protective layer that protects the surface ligands of CQDs. This protective layer avoids damage induced by lithography process solvents that deteriorate the carrier mobility of CQDs and therefore the photoresponse. Herein we report patterning of CQDs using conventional UV photolithography, achieving reproducible five-micron length PbS CQDs/SLG photodetectors with a responsivity of 10 8 A W −1 . We have also fabricated thirty-six PbS CQDs/SLG photodetectors on a single chip to establish micron size photodetectors. This process offers an approach to pattern QDs with conventional UV lithography and dry etching semiconductor technology to facilitate their integration into current semiconductor commercial technology.  more » « less
Award ID(s):
2046176
NSF-PAR ID:
10335076
Author(s) / Creator(s):
; ;
Date Published:
Journal Name:
Nanoscale Advances
Volume:
3
Issue:
21
ISSN:
2516-0230
Page Range / eLocation ID:
6206 to 6212
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Hybrid graphene (Gr)–quantum dot (QD) photodetectors have shown ultrahigh photoresponsivity combining the strong light absorption of QDs with the high mobility of Gr. QDs absorb light and generate photocarriers that are efficiently transported by Gr. Typically, hybrid PbS–QD/graphene photodetectors operate by transferring photogenerated holes from the QDs to Gr while photoelectrons stay in the QDs inducing a photogating mechanism that achieves a responsivity of 6 × 107A W−1. However, despite such high gain, these systems have poor charge collection with quantum efficiency below 25%. Herein, a ZnO intermediate layer (PbS‐QD/ZnO/Gr) is introduced to improve charge collection by forming an effective p‐n PbS‐ZnO junction driving the electrons to the ZnO layer and then to Gr. This improves the photoresponsivity of the devices by nearly an order of magnitude with respect to devices without ZnO. Charge transfer to Gr is demonstrated by monitoring the change in Fermi level under illumination for conventional PbS‐QD/Gr and for ZnO intermediate PbS‐QD/ZnO/Gr devices. These results improve the capabilities of hybrid QD/Gr configurations for optoelectronic devices.

     
    more » « less
  2. Abstract

    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.

     
    more » « less
  3. Heterogeneous self-assembly of III–V nanostructures on inert two-dimensional monolayer materials enables novel hybrid nanosystems with unique properties that can be exploited for low-cost and low-weight flexible optoelectronic and nanoelectronic device applications. Here, the pseudo-van der Waals epitaxy (vdWE) growth parameter space for heterogeneous integration of InAs nanowires (NWs) with continuous films of single layer graphene (SLG) via metalorganic chemical vapor deposition (MOCVD) is investigated. The length, diameter, and number density of NWs, as well as areal coverage of parasitic islands, are quantified as functions of key growth variables including growth temperature, V/III ratio, and total flow rate of metalorganic and hydride precursors. A compromise between self-assembly of high aspect ratio NWs comprising high number density arrays and simultaneous minimization of parasitic growth coverage is reached under a selected set of optimal growth conditions. Exploration of NW crystal structures formed under various growth conditions reveals that a characteristic polytypic and disordered lattice is invariant within the explored parameter space. A growth evolution study reveals a gradual reduction in both axial and radial growth rates within the explored timeframe for the optimal growth conditions, which is attributed to a supply-limited competitive growth regime. Two strategies are introduced for further growth optimization. Firstly, it is shown that the absence of a pre-growth in situ arsine surface treatment results in a reduction of parasitic island coverage by factor of ∼0.62, while NW aspect ratio and number densities are simultaneously enhanced. Secondly, the use of a two-step flow-modulated growth procedure allows for realization of dense fields of high aspect ratio InAs NWs. As a result of the applied studies and optimization of the growth parameter space, the highest reported axial growth rate of 840 nm min −1 and NW number density of ∼8.3 × 10 8 cm −2 for vdWE of high aspect ratio (>80) InAs NW arrays on graphitic surfaces are achieved. This work is intended to serve as a guide for vdWE of self-assembled III–V semiconductor NWs such as In-based ternary and quaternary alloys on functional two-dimensional monolayer materials, toward device applications in flexible optoelectronics and tandem-junction photovoltaics. 
    more » « less
  4. 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
  5. 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