Exciton Dynamics and Optically Pumped Lasing in 1-Naphthylmethylamine-Based Quasi-2D Perovskite Films

Films of the quasi-2D perovskite based on 1-naphthylmethylamine (NMA) are promising as the gain medium for optically pumped lasing and future electrically pumped lasing because of its low lasing threshold and small electroluminescence efficiency rolloff. However, reasons for the low threshold and small efficiency rolloff are still unclear. Therefore, exciton dynamics are investigated in NMA-based quasi-2D perovskite films. It is found that quenching of bright excitons by other excitons or charge carriers is unlikely in NMA-based quasi-2D perovskite films, which is one reason for the low lasing threshold and small efficiency rolloff. Moreover, thermally stimulated current measurements reveal that the defect levels inside the band gap of the NMA-based quasi-2D perovskite are shallow, with a depth of ≈0.3 eV, causing a decrease in nonradiative exciton recombination through the defects. Therefore, population inversion can be easily achieved, leading to the low lasing threshold as well. For fabrication of NMA-based quasi-2D perovskite laser devices with even lower lasing thresholds, a circular-shaped optical resonator, and small-molecule-based defect passivation are used. Optically pumped lasing can be obtained from these devices, with a threshold of ≈1 µJ cm⁻², which is one of the lowest values ever reported in any perovskite lasers.     

Interstitial Cu: An Effective Strategy for High Carrier Mobility and High Thermoelectric Performance in GeTe

Dense point defects can strengthen phonon scattering to reduce the lattice thermal conductivity and induce outstanding thermoelectric performance in GeTe-based materials. However, extra point defects inevitably enlarge carrier scattering and deteriorate carrier mobility. Herein, it is found that the interstitial Cu in GeTe can result in synergistic effects, which include: 1) strengthened phonon scattering, leading to ultralow lattice thermal conductivity of 0.48 W m⁻¹ K⁻¹ at 623 K; 2) weakened carrier scattering, contributing to high carrier mobility of 80 cm² V⁻¹ s⁻¹ at 300 K; 3) optimized carrier concentration of 1.22 × 10²⁰ cm⁻³. Correspondingly, a high figure-of-merit of ≈2.3 at 623 K can be obtained in the Ge_0.93Ti_0.01Bi_0.06Te-0.01Cu, which corresponds to a maximum energy conversion efficiency of ≈10% at a temperature difference of 423 K. This study systematically investigates the doping behavior of the interstitial Cu in GeTe-based thermoelectric materials for the first time and demonstrates that the localized interstitial Cu is a new strategy to enhance the thermoelectric performance of GeTe-based thermoelectric materials.     

Carbon-related defects in microelectronics

In the present study electrically active carbon and hydrogen-related (CH) defects, which can act as strong recombination centers in high power devices and CMOS photodetectors, are investigated in n-type Si. Several different CH-related defects are observed by using the deep level transient spectroscopy (DLTS) technique on hydrogenated Si samples with different oxygen content. The concentration of these defects is determined as low as 10¹²–10¹³ cm^− 3. By comparing samples with different O, C, and H concentrations the origin of the CH-related defects is derived. We show that the concentration of the electrically inactive substitutional C can be estimated by a comparison of the depth profiles of the electrically active CH-related defects in a sample with those in a reference sample which has an identical oxygen and known carbon content. This approach is applicable even for concentrations of substitutional C lower than 10¹⁵ cm^− 3.     

Electronic properties of Si/Si-Ge Alloy/Si(100) heterostructures formed by ECR Ar plasma CVD without substrate heating

By using our low-energy Ar plasma enhanced chemical vapor deposition (CVD) at a substrate temperature below 100 °C during plasma exposure without substrate heating, modulation of valence band structures and infrared photoluminescence can be observed by change of strain in a Si/strained Si_0.4Ge_0.6/Si(100) heterostructure. For the strained Si_0.5Ge_0.5 film, Hall mobility at room temperature was confirmed to be as high as 660 cm² V⁻¹ s⁻¹ with a carrier concentration of 1.3×10¹⁸ cm⁻³ for n-type carrier, although the carrier origin was unclear. Moreover, good rectifying characteristics were obtained for a p⁺Si/nSi_0.5Ge_0.5 heterojunction diode. This indicates that the strained Si-Ge alloy and Si films and their heterostructures epitaxially grown by our low-energy Ar plasma enhanced CVD without substrate heating can be applicable effectively for various semiconductor devices utilizing high carrier mobility, built-in potential by doping and band engineering.     

Temperature dependent study of basal plane stacking faults in Ag:ZnO nanorods by Raman and photoluminescence spectroscopy

We report the specific features of basal plane stacking faults (BSFs) in ZnO nanorods (NRs), studied by temperature dependent photoluminescence and Raman spectroscopy. At low temperature (4 K) the intense band of emission at 3.321 eV is attributed to the presence of BSFs defects and Ag as an acceptor dopant in ZnO. This specific peak red-shifts with the temperature increase, occupying the position 3.210 eV at RT. The nature of the emission is explained as exciton recombination of the electrons, confined in the homo-heterojunction QW, with the holes, localized near the Ag atoms close to SFs. Raman spectroscopy revealed that Ag:ZnO nanorods have slightly downshifted positions of the modes 330 cm⁻¹ and 440 cm⁻¹ by 4 cm⁻¹, which we explain as due to the presence of BSFs. It was also observed, that the longitudinal optical phonon mode A^LO, which is common polar mode for ZnO, was not detected by Raman spectroscopy in the samples with high BSFs density. This feature can be explained as due to existence of the bound charge induced by the BSFs in the NRs.     

The influence of high energy electron irradiation on the Schottky barrier height and the Richardson constant of Ni/4H-SiC Schottky diodes

The influence of high energy electron (HEE) irradiation from a Sr-90 radio-nuclide on n-type Ni/4H–SiC samples of doping density 7.1×10¹⁵ cm⁻³ has been investigated over the temperature range 40–300 K. Current–voltage (I–V), capacitance–voltage (C–V) and deep level transient spectroscopy (DLTS) were used to characterize the devices before and after irradiation at a fluence of 6×10¹⁴ electrons-cm⁻². For both devices, the I–V characteristics were well described by thermionic emission (TE) in the temperature range 120–300 K, but deviated from TE theory at temperature below 120 K. The current flowing through the interface at a bias of 2.0 V from pure thermionic emission to thermionic field emission within the depletion region with the free carrier concentrations of the devices decreased from 7.8×10¹⁵ to 6.8×10¹⁵ cm⁻³ after HEE irradiation. The modified Richardson constants were determined from the Gaussian distribution of the barrier height across the contact and found to be 133 and 163 A cm⁻² K⁻² for as-deposited and irradiated diodes, respectively. Three new defects with energies 0.22, 0.40 and 0.71 eV appeared after HEE irradiation. Richardson constants were significantly less than the theoretical value which was ascribed to a small active device area.     

Water-gated phthalocyanine transistors: Operation and transduction of the peptide–enzyme interaction

The use of aqueous solutions as the gate medium is an attractive strategy to obtain high charge carrier density (10¹² cm⁻²) and low operational voltages (<1 V) in organic transistors. Additionally, it provides a simple and favorable architecture to couple both ionic and electronic domains in a single device, which is crucial for the development of novel technologies in bioelectronics. Here, we demonstrate the operation of transistors containing copper phthalocyanine (CuPc) thin-films gated with water and discuss the charge dynamics at the CuPc/water interface. Without the need for complex multilayer patterning, or the use of surface treatments, water-gated CuPc transistors exhibited low threshold (100 ± 20 mV) and working voltages (<1 V) compared to conventional CuPc transistors, along with similar charge carrier mobilities (1.2 ± 0.2) x 10⁻³ cm² V⁻¹ s⁻¹. Several device characteristics such as moderate switching speeds and hysteresis, associated with high capacitances at low frequencies upon bias application (3.4–12 μF cm⁻²), indicate the occurrence of interfacial ion doping. Finally, water-gated CuPc OTFTs were employed in the transduction of the biospecific interaction between tripeptide reduced glutathione (GSH) and glutathione S-transferase (GST) enzyme, taking advantage of the device sensitivity and multiparametricity.     

Characterization of the heavily (non-degenerate) boron-doped SiSiO2 interface

The influence of doping, crystallographic orientation and oxide thickness on the parameters of the boron-doped SiSiO₂ interface up to 3 × 10¹⁸ cm⁻³ for oxides thermally grown in a wet O₂ ambient is investigated. The fundamental surface recombination velocity, which is proportional to the product of the density of the effective recombination centers and of the associated capture cross section is nearly constant in the range of doping studied. The fixed-oxide charge density increases with doping concentration; this is probably due to the increasing importance of boron atoms segregating in the oxide and/or to the excess silicon interstitials increasing in density with dopant concentration.     

High Q-Factor and Low Threshold Continuous-Wave Near-Infrared Lasing with Quasi-2D Perovskites

Quasi-2D perovskites have shown great potential in achieving solution-processed electrically pumped laser diodes due to their multiple-quantum-well structure, which induces a carrier cascade process that can significantly enhance population inversion. However, continuous-wave (CW) optically pumped lasing has yet to be achieved with near-infrared (NIR) quasi-2D perovskites due to the challenges in obtaining high-quality quasi-2D films with suitable phase distribution and morphology. This study regulates the crystallization of a NIR quasi-2D perovskite ((NMA)₂FA_n−1Pb_nI_3n+1) using an 18-crown-6 additive, resulting in a compact and smooth film with a largely improved carrier cascade efficiency. The amplified spontaneous emission threshold of the film is reduced from 47.2 to 35.9 µJ cm⁻². Furthermore, by combining the film with a high-quality distributed feedback grating, this study successfully realizes a CW NIR laser of 809 nm at 110 K, with a high Q-factor of 4794 and a low threshold of 911.6 W cm⁻². These findings provide an important foundation for achieving electrically pumped laser diodes based on the unique quasi-2D perovskites.     

Analysis of the Annealing Budget of Metal Oxide Thin-Film Transistors Prepared by an Aqueous Blade-Coating Process

Metal oxide (MO) semiconductors are widely used in electronic devices due to their high optical transmittance and promising electrical performance. This work describes the advancement toward an eco-friendly, streamlined method for preparing thin-film transistors (TFTs) via a pure water-solution blade-coating process with focus on a low thermal budget. Low temperature and rapid annealing of triple-coated indium oxide thin-film transistors (3C-TFTs) and indium oxide/zinc oxide/indium oxide thin-film transistors (IZI-TFTs) on a 300 nm SiO₂ gate dielectric at 300 °C for only 60 s yields devices with an average field effect mobility of 10.7 and 13.8 cm² V⁻¹ s⁻¹, respectively. The devices show an excellent on/off ratio (>10⁶), and a threshold voltage close to 0 V when measured in air. Flexible MO-TFTs on polyimide substrates with AlO_x dielectrics fabricated by rapid annealing treatment can achieve a remarkable mobility of over 10 cm² V⁻¹ s⁻¹ at low operating voltage. When using a longer post-coating annealing period of 20 min, high-performance 3C-TFTs (over 18 cm² V⁻¹ s⁻¹) and IZI-TFTs (over 38 cm² V⁻¹ s⁻¹) using MO semiconductor layers annealed at 300 °C are achieved.     

Active Site Implantation for Ni(OH)2 Nanowire Network Achieves Superior Hybrid Seawater Electrolysis at 1 A cm−2 with Record-Low Cell Voltage

Direct seawater electrolysis provides a grand blueprint for green hydrogen (H₂) technology, while the high energy consumption has severely hindered its industrialization. Herein, a promising active site implantation strategy is reported for Ni(OH)₂ nanowire network electrode on nickel foam substrate by Ru doping (denoted as Ru Ni(OH)₂ NW²/NF), which can act as a dual-function catalyst for hydrazine oxidation and hydrogen evolution, achieving an ultralow working potential of 114.6 mV to reach 1000 mA cm⁻² and a small overpotential of 30 mV at 10 mA cm⁻², respectively. Importantly, using the two-electrode hydrazine oxidation assisted seawater electrolysis, it can drive a large current density of 500 mA cm⁻² at 0.736 V with over 200 h stability. To demonstrate the practicability, a home-made flow electrolyzer is constructed, which can realize the industry-level rate of 1 A cm⁻² with a record-low voltage of 1.051 V. Theoretical calculations reveal that the Ru doping activates Ni(OH)₂ by upgrading d-band centers, which raises anti-bonding energy states and thus strengthens the interaction between adsorbates and catalysts. This study not only provides a novel rationale for catalyst design, but also proposes a feasible strategy for direct alkaline seawater splitting toward sustainable, yet energy-saving H₂ production.     

Light Amplification and Efficient Electroluminescence from a Solution-Processable Diketopyrrolopyrrole Derivative via Triplet-to-Singlet Upconversion

Over the years, achieving efficient electroluminescence (EL) while simultaneously having low light amplification thresholds under optical excitation has been the key to progression toward the long-thought objective of electrically pumped organic lasers. While significant progress in this regard has been made for organic semiconductors emitting in the blue–green region of the visible spectrum, organic laser dyes with low-energy emission (>600 nm) still suffer from high amplified spontaneous emission (ASE) thresholds and low external quantum efficiencies (EQEs) in devices. Herein, low ASE thresholds and efficient EL are reported from a solution-processable organic laser dye dithiophenyl diketopyrrolopyrrole (DT-DPP). The ASE threshold of 4 µJ cm⁻² at the wavelength of 620 nm is obtained while making constructive use of triplet excitons by doping DT-DPP in a green-emitting host matrix, which exhibits thermally activated delayed fluorescence (TADF). The organic light-emitting diode fabricated from this system gives a high EQE of 7.9% due to the efficient utilization of triplet excitons. Transient EL studies further show that a high reverse intersystem crossing rate is crucial in achieving lasing under electrical pumping from such TADF-assisted fluorescent systems.     

Si/SiO2@Graphene Superstructures for High-Performance Lithium-Ion Batteries

The superstructure composed of various functional building units is promising nanostructure for lithium-ion batteries (LIBs) anodes with extreme volume change and structure instability, such as silicon-based materials. Here, a top-down route to fabricate Si/SiO₂@graphene superstructure is demonstrated through reducing silicalite-1 with magnesium reduction and depositing carbon layers. The successful formation of superstructure lies on the strong 3D network formed by the bridged-SiO₂ matrix coated around silicon nanoparticles. Furthermore, the mesoporous Si/SiO₂ with amorphous bridged SiO₂ facilitates the deposition of graphene layers, resulting in excellent structural stability and high ion/electron transport rate. The optimized Si/SiO₂@graphene superstructure anode delivers an outstanding cycling life for ≈1180 mAh g⁻¹ at 2 A g⁻¹ over 500 cycles, excellent rate capability for ≈908 mAh g⁻¹ at 12 A g⁻¹, great areal capacity for ≈7 mAh cm⁻² at 0.5 mA cm⁻², and extraordinary mechanical stability. A full cell test using LiFePO₄ as the cathode manifests a high capacity of 134 mAh g⁻¹ after 290 loops. More notably, a series of technologies disclose that the Si/SiO₂@graphene superstructure electrode can effectively maintain the film between electrode and electrolyte in LIBs. This design of Si/SiO₂@graphene superstructure elucidates a promising potential for commercial application in high-performance LIBs.     

Redox Poly-Counterion Doped Conducting Polymers for Pseudocapacitive Energy Storage

Conducting polymers (CPs) have been widely studied for electrochemical energy storage. However, the dopants in CPs are often electrochemically inactive, introducing “dead-weight” to the materials. Moreover, commercial-level electrode materials with high mass loadings (e.g., >10 mg cm⁻²) often encounter the problems of inferior electrical and ionic conductivity. Here, a redox-active poly-counterion doping concept is proposed to improve the electrochemical performance of CPs with ultra-high mass loadings. As a study prototype, heptamolybdate anion (Mo₇O₂₄⁶⁻) doped polypyrrole (PPy) is synthesized by electro-polymerization. A 2 mm thick PPy electrode with mass loading of ≈192 mg cm⁻² reaches a record-high areal capacitance of ≈47 F cm⁻², competitive gravimetric capacitance of 235 F g⁻¹, and volumetric capacitance of 235 F cm⁻³. With poly-counterion doping, the dopants also undergo redox reactions during charge/discharge processes, providing additional capacitance to the electrode. The interaction between polymer chains and the poly-counterions enhances the electrical conductivity of CPs. Besides, the poly-counterions with large steric hindrance could act as structural pillars and endow CPs with open structures for facile ion transport. The concept proposed in this work enriches the electrochemistry of CPs and promotes their practical applications.     

Effect of interface traps for ultra-thin high-k gate dielectric based MIS devices on the capacitance-voltage characteristics

The impact of states at the Al₂O₃/Si interface on the capacitance-voltage C-V characteristics of a metal/insulator/semiconductor heterostructure (MIS) capacitor was studied by a numerical simulation, by solving Schrodinger-Poisson equations and taking the electron emission rate from the interface state into account. Efficient computation and accurate physics based capacitance model of MOS devices with advanced ultra-thin equivalent oxide thickness (EOT) (down to 2.5 nm clearly considered here) were introduced for the near future integrated circuit IC technology nodes. Due to the importance of the interface state density for a low dimension and very low oxide thickness, a high frequency C-V model has been developed to interpret the effect of interface state density traps which communicate with the Al₂O₃/Si and their influence on the C-V characteristics. We found that these states are manifested by jumping capacity in the inversion zone, for a density of interface, higher than 1 × 10¹¹ cm^− 2 eV^− 1 during a p-doping of 1 × 10¹⁸ cm^− 3. This behavior has been investigated with various doping, temperature, frequency and energy levels on the C-V curves, and compared with the MIS structure that contains a standard SiO₂ insulator.     

High Optical Gain of Solution-Processed Mixed-Cation CsPbBr3 Thin Films towards Enhanced Amplified Spontaneous Emission

A solution-processed thin film made of all-inorganic CsPbBr₃ perovskite is a promising candidate for low-cost and flexible green-color lasers. However, the amplified spontaneous emission (ASE) of solution-processed CsPbBr₃ films still experiences a high threshold owing to poor morphology and insufficient optical gain. Here, a multiple-cation doping strategy is demonstrated to develop compact, smooth thin films of Cs_0.87(FAMA)_0.13PbBr₃/(NMA)₂PbBr₄ (FA: formamidinium; MA: methylammonium; NMA: naphthylmethylammonium) with a record high net modal optical gain of ≈ 3030 cm⁻¹ and low propagation loss of 1.0 cm⁻¹. The FA and MA cations improve the crystallization kinetics to form continuous films, and the NMA cations reduce the grain dimension, increase film dispersibility/uniformity, and enhance spatial confinement to promote optical gain. Room-temperature ASE is demonstrated under a low threshold of ≈ 3.8  µ J cm⁻² without degradation after four months of storage in glove box or excitation by 3 × 10⁷ laser pulses. These findings provide insights into enhancing the optical gain and lowering the threshold of perovskite lasers in terms of molecular synthesis and microstructure engineering.     

Effects of RTA temperatures on conductivity and micro-structures of boron-doped silicon nanocrystals in Si-rich oxide thin films

In this work, the B-doped Si rich oxide (SRO) thin films were deposited and then annealed using rapid thermal annealing (RTA) to form SiO₂-matrix silicon nanocrystals (Si NCs). The effects of the RTA temperatures on the structural properties, conduction mechanisms and electrical properties of B-doped SRO thin films (BSF) were investigated systematically using Hall measurements, Fourier transform infrared spectroscopy and Raman spectroscopy. Results showed that the crystalline fraction of annealed BSF increased from 41.3% to 62.8%, the conductivity was increased from 4.48×10⁻³ S/cm to 0.16 s/cm, the carrier concentration was increased from 8.74×10¹⁷ cm⁻³ to 4.9×10¹⁸ cm⁻³ and the carrier mobility was increased from 0.032 cm² V⁻¹ s⁻¹ to 0.2 cm² V⁻¹ s⁻¹ when the RTA temperatures increased from 1050 °C to 1150 °C. In addition, the fluctuation induced tunneling (FIT) theory was applicable to the conduction mechanisms of SiO₂-matrix boron-doped Si-NC thin films.     

Enhanced Thermoelectric Performance in GeTe by Synergy of Midgap state and Band Convergence

The good co-existence of midgap state and valence band degeneracy is realized in Bi-alloyed GeTe through the In-Cd codoping to play different but complementary roles in the valence band structure modification. In doping induces midgap state and results in a considerably improved Seebeck coefficient near room temperature, while Cd doping significantly increases the Seebeck coefficient in the mid-high temperature region by promoting the valence band convergence. The synergistic effects obviously increase the density of state effective mass from 1.39 to 2.65 m₀, and the corresponding carrier mobility still reaches 34.3 cm² V⁻¹ s⁻¹ at room temperature. Moreover, the Bi-In-Cd co-alloying introduces various phonon scattering centers including nanoprecipitates and strain field fluctuations and suppresses the lattice thermal conductivity to a rather low value of 0.56 W m⁻¹ K⁻¹ at 600 K. As a result, the Ge_0.89Bi_0.06In_0.01Cd_0.04Te sample obtains excellent thermoelectric properties of zT_max ≈2.12 at 650 K and zT_avg ≈1.43 between 300 and 773 K. This study illustrates that the thermoelectric performance of GeTe can be optimized in a wide temperature range through the synergy of midgap state and valence band convergence.     

High-Performance Photodetector and Angular-Dependent Random Lasing from Long-Chain Organic Diammonium Sandwiched 2D Hybrid Perovskite Non-Linear Optical Single Crystal

3D organic-inorganic metal halide perovskites are excellent materials for optoelectronic applications due to their exceptional properties, solution processability, and cost-effectiveness. However, the lack of environmental stability highly restricts them from practical applications. Herein, a stable centimeter-long 2D hybrid perovskite (N-MPDA)[PbBr₄] single crystal using divalent N1-methylpropane-1,3-diammonium (N-MPDA) cation as an organic spacer, is reported. The as-grown single crystal exhibits stable optoelectronic performance, low threshold random lasing, and multi-photon luminescence/multi-harmonic generation. A photoconductive device fabricated using (N-MPDA)[PbBr₄] single crystal exhibits an excellent photoresponsivity (≈124 AW⁻¹ at 405 nm) that is ≈4 orders of magnitudes higher than that of monovalent organic spacer-assisted 2D perovskites, such as (BA)₂PbBr₄ and (PEA)₂PbBr₄, and large specific detectivity (≈10¹² Jones). As an optical gain media, the (N-MPDA)[PbBr₄] single crystal exhibits a low threshold random lasing (≈6.5 µJ cm⁻²) with angular dependent narrow linewidth (≈0.1 nm) and high-quality factor (Q ≈ 2673). Based on these results, the outstanding optoelectronic merits of (N-MPDA)[PbBr₄] single crystal will offer a high-performance device and act as a dynamic material to construct stable future electronics and optoelectronic-based applications.     

High mobility and low operation voltage organic field effect transistors by using polymer-gel dielectric and molecular doping

In this work, we present a method to increase the performance in solution processed organic field effect transistors (OFET) by using gel as dielectric and molecular doping to the active organic semiconductor. In order to compare the performance improvement, Poly (methylmethacrylate) (PMMA) and Poly (3-hexylthiophene-2,5-diyl) P3HT material system were used as a reference. Propylene carbonate (PC) is introduced into PMMA to form the gel for using as gate dielectric. The mobility increases from 5.72×10⁻³ to 0.26 cm² V s^–1 and operation voltage decreases from −60 to −0.8 with gel dielectric. Then, the molecular dopant 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4-TCNQ) is introduced into P3HT via co-solution. The mobility increases up to 1.1 cm² V s^–1 and the threshold voltage downs to −0.09 V with doping. The increase in performance is discussed in terms of better charge inducing by high dielectric properties of gel and trap filling due to the increased carrier density in active semiconductor by molecular doping.