Pushing Absorption of Perovskite Nanocrystals into the Infrared.

To date, defect-tolerance electronic structure of lead halide perovskite nanocrystals is limited to an optical feature in the visible range. Here, we demonstrate that IR sensitization of formamidinium lead iodine (FAPI) nanocrystal array can be obtained by its doping with PbS nanocrystals. In this hybrid array, absorption comes from the PbS nanocrystals while transport is driven by the perovskite which reduces the dark current compared to pristine PbS. In addition, we fabricate a field-effect transistor using a high capacitance ionic glass made of hybrid FAPI/PbS nanocrystal arrays. We show that the hybrid material has an n-type nature with an electron mobility of 2 × 10-3 cm2 V-1 s-1. However, the dark current reduction is mostly balanced by a loss of absorption. To overcome this limitation, we couple the FAPI/PbS hybrid to a guided mode resonator that can enhance the infrared light absorption.

Field-Effect Transistor and Photo-Transistor of Narrow-Band-Gap Nanocrystal Arrays Using Ionic Glasses.

The gating of nanocrystal films is currently driven by two approaches: either the use of a dielectric such as SiO2 or the use of electrolyte. SiO2 allows fast bias sweeping over a broad range of temperatures but requires a large operating bias. Electrolytes, thanks to large capacitances, lead to the significant reduction of operating bias but are limited to slow and quasi-room-temperature operation. None of these operating conditions are optimal for narrow-band-gap nanocrystal-based phototransistors, for which the necessary large-capacitance gate has to be combined with low-temperature operation. Here, we explore the use of a LaF3 ionic glass as a high-capacitance gating alternative. We demonstrate for the first time the use of such ionic glasses to gate thin films made of HgTe and PbS nanocrystals. This gating strategy allows operation in the 180 to 300 K range of temperatures with capacitance as high as 1 µF·cm-2. We unveil the unique property of ionic glass gate to enable the unprecedented tunability of both magnitude and dynamics of the photocurrent thanks to high charge-doping capability within an operating temperature window relevant for infrared photodetection. We demonstrate that by carefully choosing the operating gate bias, the signal-to-noise ratio can be improved by a factor of 100 and the time response accelerated by a factor of 6. Moreover, the good transparency of LaF3 substrate allows back-side illumination in the infrared range, which is highly valuable for the design of phototransistors.

High current treated-passivated graphene (CTPG) towards stable nanoelectronic and spintronic circuits.

Achieving enhanced and stable electrical quality of scalable graphene is crucial for practical graphene device applications. Accordingly, encapsulation has emerged as an approach for improving electrical transport in graphene. In this study, we demonstrate high-current treatment of graphene passivated by AlOx nanofilms as a new means to enhance the electrical quality of graphene for its scalable utilization. Our experiments and electrical measurements on large-scale chemical vapor-deposited (CVD) graphene devices reveal that high-current treatment causes persistent and irreversible de-trapping density in both bare graphene and graphene covered by AlOx. Strikingly, despite possible interfacial defects in graphene covered with AlOx, the high-current treatment enhances its carrier mobility by up to 200% in contrast to bare graphene samples, where mobility decreases. Spatially resolved Raman spectroscopy mapping confirms that surface passivation by AlOx, followed by the current treatment, reduces the number of sp3 defects in graphene. These results suggest that for current treated-passivated graphene (CTPG), the high-current treatment considerably reduces charged impurity and trapped charge densities, thereby reducing Coulomb scattering while mitigating any electromigration of carbon atoms. Our study unveils CTPG as an innovative system for practical utilization in graphene nanoelectronic and spintronic integrated circuits.

Large-Scale Direct Growth of Monolayer MoS2 on Patterned Graphene for van der Waals Ultrafast Photoactive Circuits.

Two-dimensional (2D) van der Waals heterostructures combine the distinct properties of individual 2D materials, resulting in metamaterials, ideal for emergent electronic, optoelectronic, and spintronic phenomena. A significant challenge in harnessing these properties for future hybrid circuits is their large-scale realization and integration into graphene interconnects. In this work, we demonstrate the direct growth of molybdenum disulfide (MoS2) crystals on patterned graphene channels. By enhancing control over vapor transport through a confined space chemical vapor deposition growth technique, we achieve the preferential deposition of monolayer MoS2 crystals on monolayer graphene. Atomic resolution scanning transmission electron microscopy reveals the high structural integrity of the heterostructures. Through in-depth spectroscopic characterization, we unveil charge transfer in Graphene/MoS2, with MoS2 introducing p-type doping to graphene, as confirmed by our electrical measurements. Photoconductivity characterization shows that photoactive regions can be locally created in graphene channels covered by MoS2 layers. Time-resolved ultrafast transient absorption (TA) spectroscopy reveals accelerated charge decay kinetics in Graphene/MoS2 heterostructures compared to standalone MoS2 and upconversion for below band gap excitation conditions. Our proof-of-concept results pave the way for the direct growth of van der Waals heterostructure circuits with significant implications for ultrafast photoactive nanoelectronics and optospintronic applications.

Reconfigurable 2D/0D p-n Graphene/HgTe Nanocrystal Heterostructure for Infrared Detection.

Nanocrystals are promising building blocks for the development of low-cost infrared optoelectronics. Gating a nanocrystal film in a phototransistor geometry is commonly proposed as a strategy to tune the signal-to-noise ratio by carefully controlling the carrier density within the semiconductor. However, the performance improvement has so far been quite marginal. With metallic electrodes, the gate dependence of the photocurrent follows the gate-induced change of the dark current. Graphene presents key advantages: (i) infrared transparency that allows back-side illumination, (ii) vertical electric field transparency, and (iii) carrier selectivity under gate bias. Here, we investigate a configuration of 2D/0D infrared photodetectors taking advantage of a high capacitance ionic glass gate, large-scale graphene electrodes, and a HgTe nanocrystals layer of high carrier mobility. The introduction of graphene electrodes combined with ionic glass enables one to reconfigure selectively the HgTe nanocrystals and the graphene electrodes between electron-doped (n) and hole-doped (p) states. We unveil that this functionality enables the design a 2D/0D p-n junction that expands throughout the device, with a built-in electric field that assists charge dissociation. We demonstrate that, in this specific configuration, the signal-to-noise ratio for infrared photodetection can be enhanced by 2 orders of magnitude, and that photovoltaic operation can be achieved. The detectivity now reaches 109 Jones, whereas the device only absorbs 8% of the incident light. Additionally, the time response of the device is fast (<10 µs), which strongly contrasts with the slow response commonly observed for 2D/0D mixed-dimensional heterostructures, where larger photoconduction gains come at the cost of slower response.