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1.
ACS Nano ; 17(22): 22287-22298, 2023 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-37930899

RESUMO

Functional diversification at the single-device level has become essential for emerging optical neural network (ONN) development. Stable ferroelectricity harnessed with strong light sensitivity in α-In2Se3 holds great potential for developing ultrathin neuromorphic devices. Herein, we demonstrated an all-2D van der Waals heterostructure-based programmable synaptic field effect transistor (FET) utilizing a ferroelectric α-In2Se3 nanosheet and monolayer graphene. The devices exhibited reconfigurable, multilevel nonvolatile memory (NVM) states, which can be successively modulated by multiple dual-mode (optical and electrical) stimuli and thereby used to realize energy-efficient, heterosynaptic functionalities in a biorealistic fashion. Furthermore, under light illumination, the prototypical device can toggle between volatile (photodetector) and nonvolatile optical random-access memory (ORAM) logic operation, depending upon the ferroelectric-dipole induced band adjustment. Finally, plasticity modulation from short-term to prominent long-term characteristics over a wide dynamic range was demonstrated. The inherent operation mechanism owing to the switchable polarization-induced electronic band alignment and bidirectional barrier height modulation at the heterointerface was revealed by conjugated electronic transport and Kelvin-probe force microscopy (KPFM) measurements. Overall, robust (opto)electronic weight controllability for integrated in-sensor and in-memory logic processors and multibit ORAM systems was readily accomplished by the synergistic ferrophotonic heterostructure properties. Our presented results facilitate the technological implementation of versatile all-2D heterosynapses for next-generation perception, optoelectronic logic systems, and Internet-of-Things (IoT) entities.

2.
Science ; 381(6665): 1429-1432, 2023 Sep 29.
Artigo em Inglês | MEDLINE | ID: mdl-37769087

RESUMO

The spin-valley coupling between circularly polarized light and valley excitons in transition metal dichalcogenides provides the opportunity to generate and manipulate spin information by exploiting the valley degree of freedom. Here, we demonstrate a room-temperature valley-addressable tungsten disulfide monolayer laser in which the spin of lasing is controlled by the spin of pump without magnetic fields. This effect was achieved by integrating a tungsten disulfide monolayer into a photonic cavity that supports two orthogonal spin modes with high quality factors. The spin-pumped lasing effectively broke the population symmetry of valley excitons, resulting in highly coherent emission with valley-switchable radiation modes due to distinct laser thresholds. Our scheme provides a nanophotonic platform to develop versatile coherent spin-light sources operating at room temperature by actively manipulating spin-valley coupling in light-matter interactions.

3.
Nat Mater ; 22(9): 1085-1093, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37414946

RESUMO

Direct-bandgap transition metal dichalcogenide monolayers are appealing candidates to construct atomic-scale spin-optical light sources owing to their valley-contrasting optical selection rules. Here we report on a spin-optical monolayer laser by incorporating a WS2 monolayer into a heterostructure microcavity supporting high-Q photonic spin-valley resonances. Inspired by the creation of valley pseudo-spins in monolayers, the spin-valley modes are generated from a photonic Rashba-type spin splitting of a bound state in the continuum, which gives rise to opposite spin-polarized ±K valleys due to emergent photonic spin-orbit interaction under inversion symmetry breaking. The Rashba monolayer laser shows intrinsic spin polarizations, high spatial and temporal coherence, and inherent symmetry-enabled robustness features, enabling valley coherence in the WS2 monolayer upon arbitrary pump polarizations at room temperature. Our monolayer-integrated spin-valley microcavities open avenues for further classical and non-classical coherent spin-optical light sources exploring both electron and photon spins.

4.
ACS Appl Mater Interfaces ; 15(14): 18505-18515, 2023 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-37000129

RESUMO

Heterostructures based on two-dimensional materials offer the possibility to achieve synergistic functionalities, which otherwise remain secluded by their individual counterparts. Herein, ferroelectric polarization switching in α-In2Se3 has been utilized to engineer multilevel nonvolatile conduction states in a partially overlapping α-In2Se3-MoS2-based ferroelectric semiconducting field effect device. In particular, we demonstrate how the intercoupled ferroelectric nature of α-In2Se3 allows to nonvolatilely switch between n-i and n-i-n type junction configurations based on a novel edge state actuation mechanism, paving the way for subnanometric scale nonvolatile device miniaturization. Furthermore, the induced asymmetric polarization enables enhanced photogenerated carriers' separation, resulting in an extremely high photoresponse of ∼1275 A/W in the visible range and strong nonvolatile modulation of the bright A- and B- excitonic emission channels in the overlaying MoS2 monolayer. Our results show significant potential to harness the switchable polarization in partially overlapping α-In2Se3-MoS2 based FeFETs to engineer multimodal, nonvolatile nanoscale electronic and optoelectronic devices.

5.
Nanotechnology ; 34(12)2023 Jan 13.
Artigo em Inglês | MEDLINE | ID: mdl-36595332

RESUMO

Two dimensional (2D) van der Waals heterostructures (vdWHs) have unique potential in facilitating the stacking of layers of different 2D materials for optoelectronic devices with superior characteristics. However, the fabrication of large area all-2D heterostructures is still challenging towards realizing practical devices at a reduced cost. In the present work, we have demonstrated a rapid yet simple, impurity-free and efficient sonication-assisted chemical exfoliation approach to synthesize hybrid vdWHs based on 2D molybdenum disulphide (MoS2) and tungsten disulphide (WS2), with high yield. Microscopic and spectroscopic studies have confirmed the successful exfoliation of layered 2D materials and formation of their hybrid heterostructures. The co-existence of 2D MoS2and WS2in the vdWH hybrids is established by optical absorption and Raman shift measurements along with their chemical stiochiometry determined by x-ray photoelectron spectroscopy. The spectral response of the vdWH/Si (2D/3D) heterojunction photodetector fabricated using the as-synthesized material is found to exhibit broadband photoresponse compared to that of the individual 2D MoS2and WS2devices. The peak responsivity and detectivity are found to be as high as ∼2.15 A W-1and 2.05 × 1011Jones, respectively for an applied bias of -5 V. The ease of fabrication with appreciable performance of the chemically synthesized vdWH-based devices have revealed their potential use for large area optoelectronic applications on Si-compatible CMOS platforms.

6.
Mater Horiz ; 9(3): 1089-1098, 2022 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-35083477

RESUMO

2D-semiconductors with strong light-matter interaction are attractive materials for integrated and tunable optical devices. Here, we demonstrate room-temperature wavelength multiplexing of the two-primary bright excitonic channels (Ab-, Bb-) in monolayer transition metal dichalcogenides (TMDs) arising from a dark exciton mediated transition. We present how tuning dark excitons via an out-of-plane electric field cedes the system equilibrium from one excitonic channel to the other, encoding the field polarization into wavelength information. In addition, we demonstrate how such exciton multiplexing is dictated by thermal-scattering by performing temperature dependent photoluminescence measurements. Finally, we demonstrate experimentally and theoretically how excitonic mixing can explain preferable decay through dark states in MoX2 in comparison with WX2 monolayers. Such field polarization-based manipulation of excitonic transitions can pave the way for novel photonic device architectures.

7.
ACS Appl Mater Interfaces ; 14(1): 1699-1709, 2022 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-34932300

RESUMO

We report the superior broadband photodetection characteristics of few-layer phosphorene known as black phosphorus (BP) nanosheets integrated with silver nanoparticles (Ag NPs) using vertical heterojunctions on a Si platform. The exfoliation of BP nanosheets and preparation of an Ag NP:BP (Ag-BP) hybrid have been accomplished through environment-friendly and cost-effective chemical routes. The hybrid sample exhibits broadband light absorption with a strong plasmonic peak around ∼425 nm due to the localized surface plasmon resonance (LSPR) of Ag NPs of average size ∼6.0 nm. Spectroscopic analysis of the Ag-BP hybrid ascertains strong light-matter interactions around the LSPR band of Ag NPs. The size-dependent optical response of BP nanostructure/Si state-of-the-art broadband (300-1600 nm) photodiodes has been studied extensively. The enhancement of broadband photoresponse characteristics is demonstrated using the plasmonic Ag-BP 0D-2D hybrid nanostructure compared to pristine BP, where the peak responsivity in the former is shifted to the visible region (∼440 nm) compared to UV response (∼340 nm) of the latter. The tunable spectral responsivity with a peak value of ∼3.2 A/W (@ ∼440 nm and -5 V) for the Ag-BP/Si heterojunction device demonstrates the potential of plasmonic BP hybrids for future nanophotonic devices.

8.
J Environ Chem Eng ; 9(2): 104973, 2021 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-33462561

RESUMO

The world is presently infected by the biological fever of COVID-19 caused by SARS-CoV-2 virus. The present study is mainly related to the airborne transmission of novel coronavirus through airway. Similarly, our mother planet is suffering from drastic effects of air pollution. There are sufficient probabilities or evidences proven for contagious virus transmission through polluted airborne-pathway in formed aerosol molecules. The pathways and sources of spread are detailed along with the best possible green control technologies or ideas to hinder further transmission. The combined effects of such root causes and unwanted outcomes are similar in nature leading to acute cardiac arrest of our planet. To maintain environmental sustainability, the prior future of such emerging unknown biological hazardous air emissions is to be thoroughly researched. So it is high time to deal with the future of hazardous air pollution and work on its preventive measures. The lifetime of such an airborne virus continues for several hours, thus imposing severe threat even during post-lockdown phase. The world waits eagerly for the development of successful vaccination or medication but the possible outcome is quite uncertain in terms of equivalent economy distribution and biomedical availability. Thus, risk assessments are to be carried out even during the post-vaccination period with proper environmental surveillance and monitoring. The skilled techniques of disinfection, sanitization, and other viable wayouts are to be modified with time, place, and prevailing climatic conditions, handling the pandemic efficiently. A healthy atmosphere makes the earth a better place to dwell, ensuring its future lifecycle.

9.
ACS Appl Mater Interfaces ; 13(4): 5399-5405, 2021 Feb 03.
Artigo em Inglês | MEDLINE | ID: mdl-33464810

RESUMO

We present a novel maskless device fabrication technique for rapid prototyping of two-dimensional (2D)-based electronic materials. The technique is based on a thermally activated and self-developed cyclic polyphthalaldehyde (c-PPA) resist using a commercial Raman system and 532 nm laser illumination. Following the successful customization of electrodes to form field effect transistors based on MoS2 monolayers, the laser-induced electronic doping of areas beneath the metal contacts that were exposed during lithography was investigated using both surface potential mapping and device characterization. An effective change in the doping level was introduced depending on the laser intensity, i.e., low laser powers resulted in p-doping, while high laser powers resulted in n-doping. Fabricated devices present a low contact resistance down to 10 kΩ·µm at a back-gate voltage of VG = 80 V, which is attributed to the laser-induced n-type doping at the metal contact regions.

10.
ACS Nano ; 14(12): 17543-17553, 2020 Dec 22.
Artigo em Inglês | MEDLINE | ID: mdl-33210905

RESUMO

The formation of lateral heterojunction arrays within two-dimensional (2D) crystals is an essential step to realize high-density, ultrathin electro-optical integrated circuits, although the assembling of such structures remains elusive. Here we demonstrated a rapid, scalable, and site-specific integration of lateral 2D heterojunction arrays using few-layer indium selenide (In2Se3). We use a scanning laser probe to locally convert In2Se3 into In2O3, which shows a significant increase in carrier mobility and transforms the metal-semiconductor junctions from Schottky to ohmic type. In addition, a lateral p-n heterojunction diode within a single nanosheet is demonstrated and utilized for photosensing applications. The presented method enables high-yield, site-specific formation of lateral 2D In2Se3-In2O3-based hybrid heterojunctions for realizing nanoscale devices with multiple advanced functionalities.

11.
ACS Appl Mater Interfaces ; 12(39): 44345-44359, 2020 Sep 30.
Artigo em Inglês | MEDLINE | ID: mdl-32864953

RESUMO

The interface of transition-metal dichalcogenides (TMDCs) and high-k dielectric transition-metal oxides (TMOs) had triggered umpteen discourses because of the indubitable impact of TMOs in reducing the contact resistances and restraining the Fermi-level pinning for the metal-TMDC contacts. In the present work, we focus on the unresolved tumults of large-area TMDC/TMO interfaces, grown by adopting different techniques. Here, on a pulsed laser-deposited MoS2 thin film, a layer of TiO2 is grown by atomic layer deposition (ALD) and pulsed laser deposition (PLD). These two different techniques emanate the layer of TiO2 with different crystallinities, thicknesses, and interfacial morphologies, subsequently influencing the electronic and optical properties of the interfaces. Contrasting the earlier reports of n-type doping at the exfoliated MoS2/TiO2 interfaces, the large-area MoS2/anatase-TiO2 films had realized a p-type doping of the underneath MoS2, manifesting a boost in the extent of p-type doping with increasing thickness of TiO2, as emerged from the X-ray photoelectron spectra. Density functional analysis of the MoS2/anatase-TiO2 interfaces, with pristine and interfacial defect configurations, could correlate the interdependence of doping and the terminating atomic surface of TiO2 on MoS2. The optical properties of the interface, encompassing photoluminescence, transient absorption and z-scan two-photon absorption, indicate the presence of defect-induced localized midgap levels in MoS2/TiO2 (PLD) and a relatively defect-free interface in MoS2/TiO2 (ALD), corroborating nicely with the corresponding theoretical analysis. From the investigation of optical properties, we indicate that the MoS2/TiO2 (PLD) interface may act as a promising saturable absorber, having a significant nonlinear response for the sub-band-gap excitations. Moreover, the MoS2/TiO2 (PLD) interface had exemplified better phototransport properties. A potential application of MoS2/TiO2 (PLD) is demonstrated by the fabrication of a p-type phototransistor with the ionic-gel top gate. This endeavor to analyze and perceive the MoS2/TiO2 interface establishes the prospectives of large-area interfaces in the field of optics and optoelectronics.

12.
Nanotechnology ; 31(45): 455208, 2020 Nov 06.
Artigo em Inglês | MEDLINE | ID: mdl-32442984

RESUMO

Transition metal dichalcogenides (TMDs) and their heterojunctions are drawing immense research interest for various applications including infrared detection. They are being studied with different semiconductor materials to explore their heterojunction properties. In this regard, we report a MoSe2/Si heterojunction broadband photodiode which is highly sensitive for a wide spectral range from 405 nm to 2500 nm wavelength with the maximum responsivity of ∼522 mA W-1 for 1100 nm of incident light. The hydrothermal synthesis approach leads to the imperfect growth of the MoSe2, creating defects in the lattice, which was confirmed by x-ray photo-spectroscopy. These sub-bandgap defects caused high optical absorption of the SWIR light as observed in the absorption spectra. The speed of the device ranges to 18/10 µs for 10 kHz modulated light. Furthermore, the photodetector has been fully operational even at zero bias voltage, making it a potential contender for self-powered photodetection.

13.
Nanotechnology ; 31(13): 135203, 2020 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-31804224

RESUMO

The characteristics of a novel 0D/3D heterojunction photodetector fabricated using solution-processed colloidal MoS2 quantum dots (QDs) on GaAs is presented. MoS2 QDs with a dimension of ∼2 nm, synthesized by a standard sono-chemical exfoliation process with 2D layers have been used for the purpose. The microscopic and spectroscopic studies confirmed the formation of semiconducting (2H phase) MoS2 QDs. The photodetectors were fabricated using n-GaAs substrates with two different doping concentrations resulting in n-n heterojunctions between n-type 0D MoS2 QDs and bulk n-GaAs. The devices fabricated using GaAs with a higher doping concentration, showed an increase in the reverse current of the order of ∼102 upon illumination, while the same with a lower doping concentration showed an increase of the order of ∼103. All the heterojunction photodetector devices show a broadband operation over the visible wavelength range of 400-950 nm, with a peak responsivity of the devices being observed at 500 nm. The peak responsivity and detectivity are found to be ∼400 mA W-1 and ∼4 × 1012 Jones, respectively, even without any external applied bias, which are useful for self-powered photodetection. The results indicate that colloidal MoS2/GaAs based hybrid heterostructures provide a platform for fabricating broadband photodetectors by using highly absorbing MoS2 QDs, which may show the pathway towards next-generation optoelectronic devices with superior detection properties.

14.
Nanotechnology ; 31(14): 145701, 2020 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-31835257

RESUMO

While two-dimensional (2D) layered MoS2 nanosheets have been extensively studied owing to their fascinating optoelectronic properties, less attention has been paid to the corresponding zero-dimensional nano-crystals. In this contribution, we report the efficacy of MoS2 nanocrystals for their size tunable properties for optical and photocatalytic applications. We have synthesized differently sized (10-70 nm) crystalline, hexagonal 2H-MoS2 nanoparticles (NPs) dispersed in DMF solvent using a simple exfoliation technique. Synthesized NPs are found to exhibit size-dependent optical properties and excitation-dependent fluorescence characteristics in the visible region, which are otherwise not observed in bulk or 2D MoS2 layers. Size tunable bandgap and broad absorbance and emission spectrum covering the visible range could be exploited in the fabrication of various opto-electronic devices. Charge carrier emission dynamics of differently sized MoS2 NPs are investigated using time correlated single photon counting (TCSPC) spectroscopic technique. We found two time components, one in the order of several hundreds of ps, which arises due to the radiative recombination of charge carriers, while the other one is of the order of a few ns, which emanates from the defect states of MoS2 NPs. The average time constants are found to decrease with increase in particle size. A noticeable photocatalytic activity of the synthesized MoS2 NPs under visible light illumination for the degradation of brilliant green dye is also demonstrated for the first time and the effect of size variation of NPs in the dye degradation process is reported.

15.
Nanotechnology ; 30(48): 485202, 2019 11 29.
Artigo em Inglês | MEDLINE | ID: mdl-31426032

RESUMO

A unique light trapping mechanism associated with nano-conical textured black Si templates has been utilized to achieve improved photoresponse in MoS2QDs/Si heterojunctions over a wide wavelength range from visible to near infrared. Black Si templates have been fabricated by a simple and cost effective metal assisted chemical etching technique followed by spin-coating of colloidal MoS2 quantum dots (QDs) to form the heterojunction. A peak responsivity of as high as ∼1.39 A W-1 at ∼665 nm for a bias of 5 V has been achieved. The responsivity value is higher as compared to recently published results having similar device structure. The combination of MoS2 QDs and black Si has resulted in a broader spectral response with enhanced optical absorption in the nano-conical heterojunction devices. Finite element based optical simulation results revealed the superiority of MoS2 QDs/Si nano-conical heterojunctions due to improved light trapping. The results appear attractive for next generation Si CMOS compatible broad band photodetectors using two dimensional semiconductors.

16.
Sci Rep ; 6: 29016, 2016 06 30.
Artigo em Inglês | MEDLINE | ID: mdl-27357596

RESUMO

Silicon compatible wafer scale MoS2 heterojunctions are reported for the first time using colloidal quantum dots. Size dependent direct band gap emission of MoS2 dots are presented at room temperature. The temporal stability and decay dynamics of excited charge carriers in MoS2 quantum dots have been studied using time correlated single photon counting spectroscopy technique. Fabricated n-MoS2/p-Si 0D/3D heterojunctions exhibiting excellent rectification behavior have been studied for light emission in the forward bias and photodetection in the reverse bias. The electroluminescences with white light emission spectra in the range of 450-800 nm are found to be stable in the temperature range of 10-350 K. Size dependent spectral responsivity and detectivity of the heterojunction devices have been studied. The peak responsivity and detectivity of the fabricated heterojunction detector are estimated to be ~0.85 A/W and ~8 × 10(11) Jones, respectively at an applied bias of -2 V for MoS2 QDs of 2 nm mean diameter. The above values are found to be superior to the reported results on large area photodetector devices fabricated using two dimensional materials.

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