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Hot carrier based methods constitute a valuable approach for efficient and silicon compatible sub-bandgap photodetection. Although, hot electron excitation and transfer have been studied extensively on traditional materials such as Au and Ti, reports on alternative materials such as titanium nitride (TiN) are rare. Here, we perform hot hole photodetection measurements on a p-Si/metal thin film junction using Ti, Au and TiN. This material is of interest as it constitutes a refractory alternative to Au which is an important property for plasmonic applications where high field intensities can occur. In contrast to Au, a TiN/Si junction does not suffer from metal diffusion into the Si, which eases the integration with current Si-fabrication techniques. This work shows that a backside illuminated p-Si/TiN system can be used for efficient hot hole extraction in the IR, allowing for a responsivity of 1 mA/W at an excitation wavelength of 1250 nm and at zero bias. Via a comparison between TiN and other commonly used materials such as Au, the origin of this comparably high photoresponse can be traced back to be directly linked to a thin TiO2-x interfacial layer allowing for a distinct hot-hole transfer mechanism. Moreover, the fabrication of TiN nanodisk arrays is demonstrated which bears great promise to further boost the device efficiency.
Porphyrins are a class of conjugated molecules that structurally and functionally resemble natural photosynthetic and enzymatic chromophores. Crystalline solids self-assembled from anionic and cationic porphyrins yield a new class of multifunctional optoelectronic micro- and nanomaterials. In this article, we provide details on the concept of binary ionic self-assembly (ISA) and ionized forms of porphyrins, as well as formation of hierarchical structures, including nanotubes, rods and ribbons, sheets, and three-dimensional clover-like shapes, spheres, and sheaf-like structures. We summarize key physical properties from ultraviolet–visible characterizations of J-aggregate, exciton delocalization and extended π–π stacking, and related electronic and light-harvesting properties of the structures. Depending on the molecular subunits, the functionalities of the ISA materials are altered. These ISA nanostructures possess attractive light-harvesting and charge- and energy-transport functionalities and allow access to a novel class of nanomaterials with potential for applications in sensors, photovoltaics, photocatalysis, and solar power.
This work demonstrates the in situ growth of carbon nanowalls (CNWs) on diamond semiconductors by microwave plasma-assisted chemical vapor deposition. The resulting CNW/diamond junctions behave as photomemristors having both photocontrollable multiple resistance states and nonvolatile memory functions. The resistance state (high or low resistance) can be selected by irradiation with blue or violet light in conjunction with the application of a bias voltage, giving a large resistance switching ratio of ∼106. The photoinduced resistance switching behaviors are rarely observed and has only been observed in a few materials and/or heterostructures. These junctions also exhibit a photoresponsivity of ∼12 A/W, which is much larger than that obtained from photodiodes composed of other materials. These results suggest that CNW/diamond (i.e., carbon sp2/sp3) junctions could have applications in novel photocontrollable devices, which have photosensing, memory, and switching functions.
We report on the time-resolved measurements of photocarrier dynamics in InGaAs/InAlAs superlattices with epitaxial stresses in a wide range of optical pump fluences. We demonstrated that the contribution of free carrier absorption and two-photon absorption to the carrier dynamics decreases with an increase of epitaxial stresses. The lowest relaxation times of 1.7 and 8.3 ps, respectively attributed to carrier trapping and carrier recombination, were obtained for the structure with maximum epitaxial stresses.
This article discusses recent studies of piezotronics and piezo-phototronics of two-dimensional (2D) materials. Two-dimensional semiconductor materials have demonstrated excellent electronic and optoelectronic properties, and these ultrathin materials are candidates for next-generation devices. Among 2D semiconductors, transition-metal dichalcogenides in particular have large in-place piezoelectricity due to the noncentrosymmetry along the armchair direction. A strong coupling of piezoelectric and semiconducting properties has been reported for Schottky contacts and p–n junctions, even in single-layer materials. Since the carrier concentration of ultrathin 2D materials can be easily modulated by external piezocharges, layered composites of ferroelectric/2D materials also show promising piezotronic and piezo-phototronic properties.
Harnessing the nonvolatility of magnetism and the power of electric control, magnetoelectric devices that control magnetism electrically promise to deliver next-generation electronics systems that can store and compute large amounts of information with minimal power consumption and ultrafast processing speed. We highlight progress in magnetoelectric memory and logic prototypes using the voltage-controlled magnetic anisotropy (VCMA) effect. First, important performance metrics of VCMA-based magnetoelectric random access memory (MeRAM) are benchmarked against embedded complementary metal oxide semiconductor and other emerging embedded nonvolatile memories. We then discuss scaling of MeRAM from the physics and materials perspectives of the VCMA effect, as well as the use of magnetoelectric logic devices and circuits to realize new computing paradigms with VCMA. Finally, challenges to realize the full potential of VCMA-based memory and logic are presented: VCMA coefficient of 1000 fJ/V-m for energy-efficient write with low errors and tunneling magnetoresistance of 1000% for high density and low noise margin readout. New approaches for deterministic switching based on VCMA are needed. We share perspectives to address these challenges using new materials and device operation schemes.
Reduced graphene oxide (RGO) and its composites have a great potential for their applications in optoelectronic devices. In particular, small molecules can be used for tailoring optoelectronic properties of RGO. Here, we report the fabrication of a hybrid RGO/tetrasulfonate salt of the copper phthalocyanine (RGO/TSCuPc) nanocomposite phototransistor. The device shows p-type transistor behavior in the dark which changes to ambipolar behavior at the lower light intensity, and then shows a complete n-type property at the higher light intensity. The photoresponsivity of the device can be tuned by gate voltages, and the best photoresponsivity is recorded to be as high as ∼4.6 A/W for positive gate voltage and ∼6.3 A/W with a negative sign for negative gate voltage under solar light irradiation. The observations suggest that the photogenerated free electrons of TSCuPc molecules can be injected efficiently onto RGO sheets, resulting in increases in electron conduction and hole quenching.
The recently discovered orthorhombic allotrope of silicon, Si24, is an exciting prospective material for the future of solar energy due to a quasi-direct bandgap near 1.3 eV, coupled with the abundance and environmental stability of silicon. Synthesized via precursor Na4Si24 at high temperature and pressure (∼850 °C, 9 GPa), typical synthesis results have yielded polycrystalline samples with crystallites on the order of 20 μm. Several approaches to increase the crystal size have yielded success, including in-situ thermal spikes and refined selection of the starting materials. Microstructural analysis suggests that coherency exists between diamond silicon (d-Si) and Na4Si24. This hypothesis has led to the successful attempts at single crystal synthesis by selecting large crystals of d-Si along with metallic Na as the precursors rather than powdered and mixed precursor material. The new synthesis approach has yielded single crystals of Na4Si24 greater than 100 μm. These results represent a breakthrough in synthesis that enables further characterization and utility. The promise of Si24 for the future of solar energy generation and efficient electronics is strengthened through these advances in synthesis.
Ternary lead chalcogenides, such as PbSxSe1-x, offer the possibility of room-temperature infrared detection with engineered cut-off wavelengths within the important 3-5 micron mid-wave infrared (MWIR) wavelength range. We present growth and characterization of aqueous spray-deposited thin films of PbSSe. Complexing agents in the aqueous medium suppress unwanted homogeneous reactions so that growth occurs only by the heterogeneous reaction on the hydrophilic substrate. The strongly-adherent films are smooth with a mirror-like finish. The films comprise densely packed grains with tens of nm dimensions and a total film thickness of ∼400-500 nm. Measured optical constants reveal absorption out to at least 4.5 μm wavelength and a ∼0.3 eV bandgap intermediate between those of PbS and PbSe. The semiconducting films are p-type with resistivity ∼1 and 85 Ohm-cm at 300 and 80 K, respectively. Sharp x-ray diffraction peaks identify the films as Clausthalite-Galena solid-state solution with a lattice constant that indicates an even mixture of PbS and PbSe. The photoconductive response is observed at both nitrogen and room temperature up to at least 2 kHz chopping frequency.
In this work, a printable tungsten disulfide (WS2) based ink is developed from readily available WS2 powder (0.6 µm average particle size), and an ink-jet printing based deposition method for a tungsten disulfide film is presented. WS2 flake coverage and bulk electrical characteristics under three different irradiance conditions are examined and discussed. Presence of excitons in the absorbance of the inks is performed by optical UV-Vis spectrometry. Metrics using the A exciton peak generated by the few-layered flakes are used to calculate the average flake lateral dimensions, the concentration of WS2 in the inks after size selection and filtering, as well as the average monolayer count of the flakes. After printing, scanning electron microscopy is used to confirm average flake lateral size and average flake area coverage, while an atomic force microscope is used to confirm flake thickness.
Transition metal dichalcogenides (TMDC), such as MoS2, WS2 have attracted attention due to their mechanical and electronic properties in their two dimensional (2D) structures. Here, we report a facile growth of monolayer TMDC using oxide source materials with the assistant of NaCl. The addition of NaCl can enhance the lateral growth and widen the growth window of TMDC. Through carefully controlling the growth parameters, large area growth of TMDC can be achieved. Two steps E-beam lithography was utilized to fabricate electrodes of TMDC. The phototransistors made from the CVD grown TMDC show strong persistent photoconductivity (PPC). It was finally shown that TMDC device capping with h-BN could have suppressed PPC effects.
We describe the main experimental challenges toward the metrological calibration of photodetectors based on single semiconductor nanowires, and we propose a method for the quantification of their photoresponse, focusing in particular on GaAs nanowires. Spatially resolved measurements of the device’s photocurrent were performed with a far-field scanning optical setup and a laser excitation at λ = 656 nm. The photoresponse was quantitatively described by fitting the two-dimensional mapping of the photocurrent at different positions along the main nanowire axis. Our results indicate that the device’s photoresponse strongly depends on the position along the nanowire, which is attributed to the inhomogeneous properties of the device’s contacts. Furthermore, we show that its spatial profile across the nanowire can be directly compared with the profile of the laser beam by taking into account the angle between the scanning direction and the main nanowire axis as a geometrical factor. Finally, we discuss the impacts of laser-induced heating effects on the calibration of such nanoscale devices.
Novel approach to optimize quantum dot (QD) materials for specific optoelectronic applications is based on engineering of nanoscale potential profile, which is created by charged QDs. The nanoscale barriers prevent capture of photocarriers and drastically increase the photoelectron lifetime, which in turn strongly improves the photoconductive gain, responsivity, and sensitivity of photodetectors and decreases the nonradiative recombination losses of photovoltaic devices. QD charging may be created by various types of selective doping. To investigate effects of selective doping, we model, fabricated, and characterized AlGaAs/InAs QD structures with n-doping of QD layers, doping of interdot layers, and bipolar doping, which combines p-doping of QD layers with strong n-doping of the interdot space. We have measured spectral characteristics of photoresponse, photocurrent and dark current. The experimental data show that providing the same electron population of QDs, the bipolar doping creates the most contrasting nanoscale profile with the highest barriers around dots.
We present the first detailed structure-function study of a photoconducting ionic porphyrin supermolecular assembly, fabricated from tetra(N-methyl-4-pyridyl)porphyrin (TMPyP) and tetra(4-sulfonatophenyl)porphyrin (TSPP) in a 1:1 stoichiometric ratio. Rod like crystals large enough for single crystal diffraction studies were grown by utilizing a nucleation and growth model described in our previous work. The unit cell of the TMPyP:TSPP crystals is monoclinic P21/c and the cell constants are a = 8.3049(11) Å, b = 16.413(2) Å, c = 29.185(3) Å, β = 92.477(9)°. These crystals have smooth well defined facets and their internal structure consists of highly organized molecular columns of alternating porphyrin cations and anions that are stacked face to face. For the first time crystal morphology (habit) of an ionic porphyrin solid is predicted by using the crystal structure data and applying attachment energy (AE) model. The predicted habit is in good agreement with the experimental structural morphology observed in AFM and SEM images of the TMPyP:TSPP crystalline solid. The TMPyP:TSPP crystals are non-conducting in the dark and are photoconducting. The photoconductive response is significantly faster with excitation in the Q-band (Red) than with excitation in the Soret band (blue). DFT calculations were performed to determine their electronic band structure and density of states. The TMPyP:TSPP crystalline system is a useful model structure that combine the elements of molecular organization and morphology along with theory and correlate them with electronic and optical electronic properties.
Van der Waals (vdW) heterojunctions consisting of vertically-stacked individual or multiple layers of two-dimensional layered semiconductors, especially the transition metal dichalcogenides (TMDs), show novel optoelectronic functionalities due to the sensitivity of their electronic and optical properties to strong quantum confinement and interfacial interactions. Here, monolayers of n-type MoSe2 and p-type Mo1−xWxSe2 are grown by vapor transport methods, then transferred and stamped to form artificial vdW heterostructures with strong interlayer coupling as proven in photoluminescence and low-frequency Raman spectroscopy measurements. Remarkably, the heterojunctions exhibit an unprecedented photoconductivity effect that persists at room temperature for several days. This persistent photoconductivity is shown to be tunable by applying a gate bias that equilibrates the charge distribution. These measurements indicate that such ultrathin vdW heterojunctions can function as rewritable optoelectronic switches or memory elements under time-dependent photo-illumination, an effect which appears promising for new monolayer TMDs-based optoelectronic devices applications.
Amorphous oxide semiconductors (AOS) are important candidates for next generation display transistors, but instability under illumination with month-long transients is a significant drawback and may limit broader use. Several models have been developed to fit transient photoconductivity observed in AOS and relate it to a spectrum of weighted time constants, equivalent to either a density of states distribution of deep traps within the activated energy model, or to a time-dependent relaxation time constant in other models. In this work, we classify fits of the time constant spectrum to the transient data as either “descriptive” if they make no presumption about the spectral shape, or “predictive” if they assume a spectral shape a priori characterized by a few simple parameters. By fitting both descriptive and predictive models to simulated transients, it is observed that the best fit converges for the descriptive model if the measurement duration exceeds the mode (“peak”) value of the time constant distribution. The predictive models can converge orders of magnitude faster, but rely on a proper identification of the correct lineshape a priori. Therefore, it is recommended that first an unbiased descriptive model of sufficient measurement duration be performed. Then the known lineshape can be applied as a predictive model for future measurements, reducing subsequent measurement durations by orders of magnitude.
Working gas pressure during sputter deposition can significantly affect the conformality of a thin film when it is grown on a nanostructured surface. In this study, we fabricated core-shell nanostructured photodetectors, where n-type In2S3 nanorod arrays (core) were coated with p-type CuInS2 (CIS) films (shell) at relatively low and high Ar gas pressures. In2S3 nanorods were prepared by glancing angle deposition (GLAD) technique using a thermal evaporator unit. CIS films were deposited by RF sputtering at Ar pressures of 2.7x10-2 mbar (high pressure sputtering, HIPS) and 7.3x10-3 mbar (low pressure sputtering, LPS). The morphological characterization was carried out by means of SEM. The photocurrent measurement was conducted under 1.5 AM Sun under no bias. Nanostructured photodetectors of HIPS-CIS/GLAD-In2S3 (i.e. HIPS-GLAD) were shown to demonstrate enhanced photoresponse with a photocurrent value of 98 μA, which is about ∼230% higher than that of LPS-GLAD devices. The enhancement originates from the improved core-shell structure achieved by more conformal coating of the CIS shell. In addition, the results were compared to their counterpart thin-film devices incorporating an In2S3 film coated either with HIPS or LPS CIS layer. Nanorod devices with high and low pressure CIS films showed photocurrent values ∼20 times and ∼ 19 times higher compared to those of high and low pressure film devices, respectively. This finding can be explained by the higher light absorption property of nanorods, and the reduced inter-electrode distance as a result of core-shell structure, which allows the effective capture of the photo-generated carriers. Therefore, the results of this work can pave way to the development of high photoresponse core-shell semiconductor devices fabricated by physical vapor deposition techniques.
Two-Dimensional materials open up great prospects in photodetector applications owing to their sharp optical properties and the ability to combine them in layered heterostructures. Among this new class of materials, colloidal nanoplatelets (NPL) made of cadmium chalcogenides readily combine the thickness control at the atomic level together with the large scale production and ease of processing of colloidal materials. As a strategy to overcome the limited mobility inherent to nanocrystal based devices, the photocarrier lifetime is increased by building an electrolyte-gated phototransistor to passivate the electron traps. NPL can also be coupled with a graphene transport layer collecting the photogenerated charges, thus bypassing the transport bottleneck. We show that the charge transfer is driven by the large exciton binding energy of the NPL, which can be engineered by heterostructured NPL. This allows us to control the magnitude and the direction of the charge transfer to graphene. Eventually, we use nanotrench electrodes to decrease the transit time of the carriers, suppress the influence of film defects and provide an electric field large enough to overcome the large exciton binding energy of NPL.
Boron sub-2,3-naphthalocyanine chloride (SubNc) was investigated as a potential
red-sensitive organic photoconductive film (OPF). A photoconductive cell was
fabricated, and its current–voltage characteristics, both with and
without light irradiation, and external quantum efficiency (EQE) were
determined. The structure of the photoconductive cell was as follows, with
thicknesses in nm given in parentheses: glass
substrate/In–Zn–O (100)/spiro-2CBP (30)/SubNc
(50)/Alq3 (30)/Al (50) (spiro-2CBP =
2,7-bis(carbazol-9-yl)-9,9-spirobifluorene; Alq3 =
tris(8-hydroxyquinolinato)aluminum). The spiro-2CBP and Alq3 layers
were inserted between the SubNc layer and the electrodes to block dark current
injection. The three organic layers were successively deposited by evaporation
in a vacuum on the In–Zn–O-patterned substrate. SubNc film
absorbed light in the red region well, with an absorption peak at 695 nm. The
EQE of the cell reached 80% when the applied bias was 15 V. In addition, the
blocking layers effectively suppressed dark current in the OPF, which
corresponded to a current density of 20 nA/cm2 at 15 V. These results
indicate that SubNc is a promising candidate as a red-sensitive OPF.
We report on the formation of photoactive hybrid structures based on multilayer graphene nanobelts and CdSe/ZnS quantum dots (QDs) on Pt microelectrodes. We have found that heat treatment in mild conditions enhances rate of electrical photoresponse of the hybrid structures due to elimination of long-lived charge traps. We also show that the electrical photoresponse polarity depends on the energy level structure of the QDs.