High-performance broadband position-sensitive detector based on lateral photovoltaic effect of PbSe heterostructure.

PbSe has attracted considerable attention due to its promising applications in optoelectronics and energy harvesting. In this work, we explore the lateral photovoltaic effect (LPE) of PbSe films with a simple PbSe/Si heterostructure under nonuniform light illumination and zero-bias conditions. The LPE response is strongly dependent on the thickness of the PbSe film, but always shows a linear dependence on the laser spot position in an ultra-large working size of 5 mm and exhibits a wide photoresponse ranging from visible to near-infrared. The maximum position sensitivity can reach up to 190 mV/mm for the 15-nm-thick PbSe device at 1064 nm and nonlinearity is less than 4%, demonstrating its new potential application in novel position sensitive detectors (PSDs). Besides, the device also shows an ultrafast response speed, with the rise and fall time of ∼40 µs and ∼105 µs, respectively, and excellent reproducibility. These results bring great inspirations for developing high-performance broadband and self-powered PSDs based on the PbSe/Si heterostructure.

Photoluminescence characterization of wetting layer and carrier dynamics for coupled InGaAs/GaAs surface quantum dot pair structures.

The optical properties are investigated by spectroscopic characterizations for bilayer InGaAs/GaAs quantum dot (QD) structures consisting of a layer of surface quantum dots (SQDs) separated from a layer of buried quantum dots (BQDs) by different GaAs spacers with thicknesses of 7 nm, 10.5 nm and 70 nm. The coupling from the BQDs to SQDs leads to carrier transfer for the two samples with thin spacers, 7 nm and 10.5 nm, in which QD pairs are obtained while not for the 70 nm spacer sample. The carrier tunneling time is measured to be 0.145 ns and 0.275 ns from BQDs to SQD through the 7 nm and 10.5 nm spacers, respectively. A weak emission band can be observed at the wavelength of ∼ 960 nm, while the excitation intensity dependent PL and PLE spectra show that this is from the wetting layer (WL) of the SQDs. This WL is very important for carrier dynamics in bilayer structures of BQDs and SQDs, including for carrier generation, capture, relaxation, tunneling, and recombination. These results provide useful information for understanding the optical properties of InGaAs SQDs and for using such hybrid structures as building blocks for surface sensing devices.

Type-II GaSb quantum dots grown on InAlAs/InP (001) by droplet epitaxy.

GaSb quantum dots (QDs) have been grown by droplet epitaxy within InAlAs barrier layers on an InP (001) substrate. The droplet growth mode facilitates a larger size (average height ∼4.5 nm) and a lower density (∼6.3 × 109 cm-2) for the QDs than would be expected for the 4% lattice mismatch between GaSb and InAlAs. A type-II band alignment between the GaSb QDs and the InAlAs barriers is revealed by photoluminescence (PL) through a prominent blue-shift of ∼0.11 eV resulting from a six orders of magnitude increase in excitation power. Further confirmation of the type-II nature of these QDs is found through time-resolved PL studies showing a biexponential decay with a long carrier lifetime of ∼10.9 ns. These observations reveal new information for understanding the formation and properties of GaSb/InAlAs/InP QDs, which may be an optimum system for the development of both efficient memory cells and photovoltaic devices.

Correlation between photoluminescence and morphology for single layer self-assembled InGaAs/GaAs quantum dots.

Single layer self-assembled InGaAs quantum dots (QDs) are manipulated by using different arsenic species on GaAs (100) surface. The As4 molecules are experimentally observed to be more promising than As2 to promote the formation of one-dimensionally-aligned QD-chain arrays. The lateral alignment of QDs and the corresponding formation of dot chains are explained by the anisotropic surface kinetics in combination with the different reactivities of the two molecules with bonding sites on the GaAs (100) surface. Photoluminescence (PL) measurements demonstrate that the spectra of the QD-chains broaden to higher energy and increases in intensity with increasing excitation laser power. The PL band of the QD-chains also exhibits a 9 meV reduction in linewidth as temperature increases starting from 8 K. These observations confirm an efficient lateral coupling between neighboring QDs and thereafter polarized QD emission, whereas the randomly distributed QDs grown with As2 show no preferential polarization. Such QD-chains exhibiting anisotropic properties have the potential for nanophotonics applications like electro-optic modulators with very low drive voltage and ultra-wide bandwidth operation.

Lateral photovoltaic effect observed in doping-modulated GaAs/Al0.3Ga0.7As.

For photovoltaic effect (PE), both barrier height and carrier lifetime are all very important factors. However, how to distinguish their contributions to the PE is very difficult. In this paper, we prepared a series of GaAs/Al0.3Ga0.7As two dimensional electron gas (2DEG) with typical Al0.3Ga0.7As doping concentration of 0.6 × 1018/cm3, 1.2 × 1018/cm3, and 2.5 × 1018/cm3, respectively (sample number: #1, #2, #3), and studied their lateral photovoltaic effects (LPEs). It is found that their position sensitivities all increase with both laser wavelength and laser power. However, the position sensitivity exhibits a non-monotonic behavior with increasing doping concentration, which can be mainly ascribed to the doping concentration-dependent carrier lifetime, especially in the low power regime. With increasing laser power gradually, the position sensitivity difference between sample #1 and sample #2 is still large and increases a little, while the position sensitivity of sample #3 approaches to that of sample #2, suggesting that the doping concentration-dependent barrier height also starts to play an important role in the high power regime. Our results will provide important information for the design and development of novel and multifunctional PE devices.

Sb2S3 thickness-dependent lateral photovoltaic effect and time response observed in glass/FTO/CdS/Sb2S3/Au structure.

As an interesting one dimensional ribbon material, Sb2S3 has recently attracted much attention in recent years due to its exciting optical properties. However, Sb2S3-based photovoltaic or photoelectronic devices are still in research, and there are many things unknown to us and need to be well studied. In this work, the glass/FTO/CdS/Sb2S3/Au structures were successfully prepared with different Sb2S3 thicknesses, and the lateral photovoltaic effect (LPE) was firstly observed in this structure, suggesting its great potential in position sensitivity detectors (PSD). It is demonstrated that the crystallinity of Sb2S3 film increases, and Sb2S3 film tends to be vertical ribbon orientation with increasing thickness. Owing to the strong light absorption of the thicker Sb2S3 film and its one dimensional ribbon like crystal structure, the LPE in the glass/FTO/CdS/Sb2S3/Au structure improves with increasing Sb2S3 thickness from 350 nm to 800 nm, and the glass/FTO/CdS/Sb2S3(800 nm) structure exhibits an unprecedented performance with position sensitivity as large as 2230.4 mV/mm. Moreover, the time response of photovoltage was also firstly measured in this structure, it is observed that both the rise time and the fall time decrease with increasing thickness from 350 nm to 800 nm, and then increase quickly for 1100 nm film, further verifing that the Sb2S3 thickness-dependent LPE is strongly dependent on the carriers' longitudinal transport time. The very large LPE and the relatively fast response speed observed in the glass/FTO/CdS/Sb2S3(800 nm)/Au structure unveils its great potential applications in the optoelectronic detectors and also bring an insight that the suitable thickness is very crucial in Sb2S3-based devices.

Variations of thermoelectric performance by electric fields in bilayer MX2 (M = W, Mo; X = S, Se).

A gate electrode is usually used to controllably tune the carrier concentrations, further modulating the electrical conductivity and the Seebeck coefficient to obtain the optimum thermoelectric figure of merit (ZT) in two-dimensional materials. On the other hand, it is necessary to investigate how an electric field induced by a gate voltage affects the electronic structures, further determining the thermoelectric properties. Therefore, by using density functional calculations in combination with Boltzmann theory, the thermoelectric properties of bilayer MX2 (M = W, Mo; X = S, Se) with or without a 1 V nm-1 perpendicular electric field are comparatively investigated. First of all, the variations of the electrical conductivity (σ), electron thermal conductivity and Seebeck coefficient (S) with the carrier concentration are studied. Due to the trade-off relationship between S and σ, there is an optimum concentration to obtain the maximum ZT, which increases with the temperature due to the enhancement of the Seebeck coefficient. Moreover, N-type bilayers have larger optimum ZTs than P-type bilayers. In addition, the electric field results in the increase of the Seebeck coefficient in low hole-doped MS2 bilayers and high hole-doped MSe2 bilayers, thus leading to similar variations in ZT. The optimum ZTs are reduced from 2.11 × 10-2, 3.19 × 10-2, 2.47 × 10-2, and 2.58 × 10-2 to 1.57 × 10-2, 1.51 × 10-2, 2.08 × 10-2, and 1.43 × 10-2 for the hole-doped MoS2, MoSe2, and WSe2 bilayers, respectively. For N-type bilayers, the electric field shows a destructive effect, resulting in the obvious reduction of the Seebeck coefficient in the MSe2 layers and the low electron-doped MS2 bilayers. In electron-doped bilayers, the optimum ZTs will decrease from 3.03 × 10-2, 6.64 × 10-2, and 6.69 × 10-2 to 2.81 × 10-2, 3.59 × 10-2, and 4.39 × 10-2 for the MoS2, MoSe2, and WSe2 bilayers, respectively.

Flatbands in 2D boroxine-linked covalent organic frameworks.

Density functional calculations have been performed to analyze the electronic and mechanical properties of a number of 2D boroxine-linked covalent organic frameworks (COFs), which are experimentally fabricated from di-borate aromatic molecules. Furthermore, the band structures are surprising and show flat-band characteristics which are mainly attributed to the delocalized π-conjugated electrons around the phenyl rings and can be better understood within aromaticity theories. Next, the effects of branch sizes and hydrostatic strains on their band structures are systematically considered within generalized gradient approximations. It is found that their band gaps will start to saturate when the branch size reaches 9. For boroxine-linked COFs with only one benzene ring in the branch, the band gap is robust under compressive strain while it decreases with the tensile strain increasing. When the branch size is equal or greater than 2, their band gaps will monotonously increase with the strain increasing in the range of [-1.0, 2.0] Å. All boroxine-linked COFs are semiconductors with controllable band gaps, depending on the branch length and the applied strain. In comparison with other 2D materials, such as graphene, hexagonal boron nitride, and even γ-graphyne, all boroxine-linked COFs are much softer and even more stable. That is, they can maintain the planar features under a larger compressive strain, which means that they are good candidates in flexible electronics.

Thermoelectric properties of fullerene-based junctions: a first-principles study.

This study is built on density functional calculations in combination with the non-equilibrium Green's function, and we probe the thermoelectric transport mechanisms through C60 molecules anchored to Al nano-electrodes in three different ways, such as, the planar, pyramidal, and asymmetric surfaces. When the electrode is switched from the planar and pyramidal surfaces, the electrical conductance (σ) and electron's thermal conductance (κel) decrease almost two orders of magnitude due to the reduction of the molecule-electrode contact coupling, whereas the Seebeck coefficients (S) are reduced by ∼55%. Furthermore, the maximum electron's thermoelectric figure of merit (ZelT = S2σT/κel, assuming a vanishing phonon's thermal conductance) is about 0.12 in the asymmetric junction. In particular, all σ, S, κel, and ZelT increase along with the average temperature (T) in all C60-junctions, although their growth is really quite negligible in the pyramidal junction because the Fermi level is far away from the frontier orbitals. In addition, when the strain increases from the compressive (-1.0 Å) to tensile (1.0 Å) strain, the Seebeck coefficient in the planar junction increases drastically, while the Seebeck coefficients in the asymmetric and pyramidal junctions reach their maximum values at 0.2 Å tensile and -0.4 Å compressive strains, respectively. This is because the Seebeck coefficient is inversely proportional to the magnitudes and proportional to the slopes of the transmission spectrum around the Fermi level. Finally, it is found that the shift of the Fermi level is an effective scheme to obtain the maximum ZelT of any molecular junction, including fullerene-based junctions.

Enhanced thermoelectric performance in CdO by nano-SiO2 inclusions.

We report enhanced thermoelectric (TE) performance in CdO by using thermally insulating nano-particles to mimic nano pores in the composite. Through simply mechanical alloying, we fabricated CdO-SiO2 composites with varying nano-SiO2 concentration from 0.1 to 3 at%. Due to the very low thermal conductivity of nano-SiO2 distributed in the CdO matrix, the thermal conductivity of the composite was substantially reduced by about 80%, which lead to the dimensionless figure of merit (ZT) value increment about 28% (from 0.32 to 0.41) at 1000 K. TEM shows the nano inclusions formed within the CdO matrix and grain boundaries as well, which is thought to contribute to the reduction of thermal conductivity of the composite by additional scattering mechanism for the mid- to long-wavelength phonons. This facile and low-cost approach might be widely adopted and synergized to other TE materials systems to further improve their performance.

Dependence of oxygen content on transverse thermoelectric effect in tilted Bi2Sr2Co2Oy thin films.

The transverse thermoelectric (TE) effect has been investigated in c axis tilted Bi2Sr2Co2Oy thin films with different oxygen content. The film samples were fabricated by a chemical solution deposition method annealed under different atmospheres of O2, air, and N2, respectively. Open-circuit transverse voltage signals were observed when the surface of the films was heated by a pulsed laser as well as a continuous thermal source. With the increase of oxygen content in the films, the amplitude of the observed voltage signals increased while the response time decreased. The experimental results can be explained by a mechanism involving the transverse TE effect as well as the transport theory of TE materials.

The enhancement of photo-thermo-electric conversion in tilted Bi2Sr2Co2O(y) thin films through coating a layer of single-wall carbon nanotubes light absorber.

Light-induced transverse thermoelectric effect has been investigated in c-axis tilted Bi(2)Sr(2)Co(2)O(y) thin films coated with a single-wall carbon nanotubes light absorption layer. Open-circuit voltage signals were detected when the sample surface was irradiated by different lasers with wavelengths ranging from ultraviolet to near-infrared and the voltage sensitivity was enhanced as a result of the increased light absorption at the carbon nanotubes layer. Moreover, the enhancement degree was found to be dependent on the laser wavelength as well as the absorption coating size. This work opens up new strategy toward the practical applications of layered cobaltites in photo-thermo-electric conversion devices.

[Effects of morphology evolution on surface plasmon resonance of nano-Ag films treated by different thermal annealing temperatures].

The nano-Ag films were prepared by RF magnetron sputtering technique, and all of them were treated by rapid thermal annealing at different temperatures. The structure, the morphology and the optical properties of the annealed nano-Ag films were characterized by X-ray diffraction, scanning electron microscopy, and UV-Vis-NIR spectroscopy. The experimental results show that the open area fraction of the film and spacing between islands or nanoparticles increase with the increase of the annealing temperature, while the aspect ratio decreases. The anisotropic worm-like island films have been reshaped into isotropic nanospheres. The surface plasmon (SP) resonance band blue shifts and narrows continuously with increasing heating temperature. Analyses show that the SP resonance of the nano-Ag films can be modulated by morphology evolution induced by rapid thermal annealing.

[Study on the spectral properties of Ca7(SiO4)2Cl6 phosphor for white LED].

A bluish green Ca7 (SiO4)2Cl6 : Eu2+ phosphor used for UV excited white LED was synthesized by high temperature solid state method. The XRD patterns and luminescence properties were investigated. The results indicated that the sample was single Ca7 (SiO4)2Cl6 phase; the emission spectrum included two emission peaks located at 418 and 502 nm, respectively. Monitoring for the two emission peaks, the excitation spectra were two broad band peaks centered at 290 and 360 nm respectively, which illustrated that Eu2+ ions located at two different crystal lattice sites. The influence of Eu2+ ions concentration on the luminescence intensity was studied and the optimal doping concentration was 0.75 mol%. The results showed that this phosphor was a better candidate bluish phosphor for UV based white LED.

F-Type Pseudo-Halide Anions for High-Efficiency and Stable Wide-Band-Gap Inverted Perovskite Solar Cells with Fill Factor Exceeding 84.

The quality of wide-band-gap (WBG) perovskite films plays an important role in tandem solar cells. Therefore, it is necessary to improve the performance of WBG perovskite films for the development of tandem solar cells. Here, we employ F-type pseudo-halogen additives (PF6- or BF4-) into perovskite precursors. The perovskite films with F-type pseudo-halogen additives have a larger grain size and higher crystal quality with lower defect density. At the same time, the perovskite lattice increases due to substitution of F-type pseudo-halogen anions for I-/Br-, and the stress distortion in the film is released, which effectively suppresses the recombination of carriers, reduces the charge transfer loss, and inhibits the phase separation. Finally, the power conversion efficiency (PCE) of the inverted 1.67 eV perovskite devices is significantly improved to over 20% with an impressive fill factor of 84.02% and excellent device stability. In addition, the PCE of the four-terminal (4T) perovskite/silicon tandem solar cells reached 27.35% (PF6-) and 27.11% (BF4-), respectively. This provides important guidance for further improving WBG perovskite solar cell performance.

General heterostructure strategy of photothermal materials for scalable solar-heating hydrogen production without the consumption of artificial energy.

Solar-heating catalysis has the potential to realize zero artificial energy consumption, which is restricted by the low ambient solar heating temperatures of photothermal materials. Here, we propose the concept of using heterostructures of black photothermal materials (such as Bi2Te3) and infrared insulating materials (Cu) to elevate solar heating temperatures. Consequently, the heterostructure of Bi2Te3 and Cu (Bi2Te3/Cu) increases the 1 sun-heating temperature of Bi2Te3 from 93 °C to 317 °C by achieving the synergy of 89% solar absorption and 5% infrared radiation. This strategy is applicable for various black photothermal materials to raise the 1 sun-heating temperatures of Ti2O3, Cu2Se, and Cu2S to 295 °C, 271 °C, and 248 °C, respectively. The Bi2Te3/Cu-based device is able to heat CuOx/ZnO/Al2O3 nanosheets to 305 °C under 1 sun irradiation, and this system shows a 1 sun-driven hydrogen production rate of 310 mmol g-1 h-1 from methanol and water, at least 6 times greater than that of all solar-driven systems to date, with 30.1% solar-to-hydrogen efficiency and 20-day operating stability. Furthermore, this system is enlarged to 6 m2 to generate 23.27 m3/day of hydrogen under outdoor sunlight irradiation in the spring, revealing its potential for industrial manufacture.

Back-Contact Ionic Compound Engineering Boosting the Efficiency and Stability of Blade-Coated Perovskite Solar Cells.

Surface defect passivation, which plays a vital role in achieving high-efficiency perovskite solar cells (PSCs) in a spin-coating process, is rarely compatible with a printing process. Currently, printing PSCs with high efficiency remains a challenge, as only a few laboratories realized an efficiency of over 20%. In this work, zwitterionic compounds 2-hydroxyethyl trimethyl ammonium chloride (HETACl) and butyltrimethylammonium chloride (BTACl) were introduced, both of which can spontaneously adsorb on the surface perovskite and form an ultrathin passivation layer by a dip coating method. The complex formed by the strong interaction of HETACl with MAI on the surface of the perovskite film leads to the formation of a rough perovskite surface, which affects the enhancement of device performance. BTACl with a chemically inert side chain induces a weak interaction with the perovskite. It is demonstrated that BTACl not only passivates surface defects of the perovskite but also heals the grain boundaries and results in more uniform crystallizations. Finally, PSCs upon BTACl treatment were blade-coated in an ambient environment with a relative humidity of <50%, which produced a champion efficiency of 20.5% with negligible hysteresis, and the active area of the cell device was 0.095 cm2. After being stored in air for 30 days, unencapsulated PSCs treated with BTACl retained 95% of their initial efficiency, which is far superior to that of the control and those treated with HETACl.

High-Responsivity, Fast, and Self-Powered Narrowband Perovskite Heterojunction Photodetectors with a Tunable Response Range in the Visible and Near-Infrared Region.

In recent years, narrowband photodetectors (PDs) have been widely used in color imaging, spectral detection or discrimination, defense, and scientific research due to their special spectral selective responses. In this work, by combining organic-inorganic hybrid perovskite layers of different band gaps and thicknesses, a series of narrowband perovskite heterojunction PDs with a continuously adjustable spectral range in the visible and near-infrared range are designed and prepared. The PDs can achieve a narrowband photoresponse with a full width at half-maximum (FWHM) of less than 50 nm and a light rejection ratio (between 780 and 532 nm) of over 1100 and exhibit excellent photoresponse performances with an external quantum efficiency (EQE), responsivity (R), and detectivity (D*) as high as 50.3%, 0.331 A/W, and 4.27 × 1010 Jones, respectively. More importantly, the photoresponses of the PDs at zero bias are as good as those at the reverse bias voltages, indicating the outstanding self-powered property. In addition, a fast response time of ∼180/∼200 µs is obtained in the narrowband perovskite heterojunction, and the response speed nearly remains constant for different PDs in the whole tunable wavelength range, demonstrating the suitable and stable structure of the heterojunction, as well as the high crystalline quality of the perovskite layers. This work definitely provides a simple strategy for designing low-cost, high-photoresponsivity, fast speed, and self-powered narrowband PDs with a tunable spectral range.

Ambient sunlight-driven photothermal methanol dehydrogenation for syngas production with 32.9 % solar-to-hydrogen conversion efficiency.

Methanol dehydrogenation is an efficient way to produce syngas with high quality. The current efficiency of sunlight-driven methanol dehydrogenation is poor, which is limited by the lack of excellent catalysts and effective methods to convert sunlight into chemicals. Here, we show that atomically substitutional Pt-doped in CeO2 nanosheets (Pts-CeO2) exhibit excellent methanol dehydrogenation activity with 500-hr level catalytic stability, 11 times higher than that of Pt nanoparticles/CeO2. Further, we introduce a photothermal conversion device to heat Pts-CeO2 up to 299°C under 1 sun irradiation owning to efficient full sunlight absorption and low heat dissipation, thus achieving an extraordinarily high methanol dehydrogenation performance with a 481.1 mmol g-1 h-1 of H2 production rate and a high solar-to-hydrogen (STH) efficiency of 32.9%. Our method represents another progress for ambient sunlight-driven stable and active methanol dehydrogenation technology.

Additive Engineering for Efficient and Stable MAPbI3-Perovskite Solar Cells with an Efficiency of over 21.

The high density of defects in MAPbI3 perovskite films brings about severe carrier nonradiative recombination loss, which lowers the performance of MAPbI3-based perovskite solar cells (PSCs). Here, methylamine cyanate (MAOCN) molecules were introduced into MAPbI3 solutions to manipulate the crystallizatsion of the MAPbI3 films. MAOCN molecules can slow down the volatilization rate of the solvent and delay the crystallization process of the MAPbI3 film. The crystal quality of the MAPbI3 films is effectively optimized without an additive residue. Perovskite films treated by MAOCN have lower defect density and longer carrier lifetime, which lowers the carrier recombination loss. Meanwhile, the MAPbI3 film based on MAOCN has a more hydrophobic surface. The final MAPbI3-based device efficiency reached 21.28% (VOC = 1.126 V, JSC = 23.29 mA/cm2, and FF = 81.13). After 30 days of storage under atmospheric conditions, the efficiency of unencapsulated MAOCN-based PSCs only dropped by about 5%.