High Hole Mobility Research Articles

Influences of lattice strain and SiGe buffer layer thickness on electrical characteristics of strained Si/SiGe/Si(110) heterostructures

In previous studies, we reported on significantly high hole mobility in a strained Si/SiGe/Si(110) heterostructure pMOSFET. In this study, we investigated impact of strain on the hole mobility in this structure. 20-nm thick (110)-oriented strained Si films with different strain levels were formed using solid-source molecular beam epitaxy. A positive correlation between the hole mobility and the strain of the Si layer is verified. It is also shown that formation of growth twins and strain relaxation of SiGe layer in the [1‾10] direction deteriorate the hole mobility. The maximum mobility enhancement factor obtained in this study is about 3. In addition, the influence of the SiGe layer thickness on the off-state leakage current in pMOSFET operation is discussed. It is found that the upper part of the thick SiGe samples includes cause of the leakage current, indicating change of conductivity with the progress of the crystal growth of SiGe layer. This phenomenon is related to the formation process of the crystalline defects. Another finding is the existence of a current path through the substrate, which suggests a defect-assisted current flow across the SiGe/n-Si(110) junction.

Anisotropic Charge Transport in Cu(In,Ga)Se2 by Heavy Alkali Postdeposition Treatment for Reducing Cell‐to‐Module Efficiency Loss in Monolithically Integrated Photovoltaic Modules

The recent efficiency boosting of Cu(In,Ga)Se2 (CIGS) solar cells is undoubtedly triggered by heavy alkali postdeposition treatments (PDTs). However, the effects are not obvious under monolithically integrated CIGS modules where various current‐shunting sources can deteriorate the device performance. Herein, It is reported that KF PDT can effectively suppress the major shunting sources caused by P1 and P3 laser scribing for monolithic interconnection, reducing the cell‐to‐module (CTM) efficiency gap in CIGS photovoltaics. CIGS with NaF PDT exhibits nearly isotropic and high hole mobilities, causing a large CTM efficiency loss. CIGS with additional KF PDT, on the other hand, reveals much lower in‐plane hole mobility than the out‐of‐plane component, significantly increasing the P1 shunt resistance without exacerbating the photocarrier extraction in the active area. It is suggested that such anisotropic charge transport is due to carrier scattering by low‐conductivity phases at the CIGS grain boundaries. Furthermore, passivation of the front junction by KF PDT raises the tolerance to P3 scribing‐induced damage, increasing the P3 shunt resistance while preserving the junction property unlike the NaF PDT case. The work implies that the recent trend of employing heavy alkali PDTs for a high‐efficiency cell is also crucial for designing a high‐efficiency CIGS module.

Constructing hole transport channels in the photoactive layer connecting dopant-free hole transport layers to improve the power conversion efficiency of perovskite solar cells

Perovskite solar cells (PSCs) with dopant‐free hole transporting layers (HTLs) deserved extensive research by merits of their outstanding hydrophobicity and stability. However, the low carrier mobility and poor interfacial hole extraction lead to the inferior power conversion efficiency (PCE) than that of conventional Li+ doped Spiro-OMeTAD. Here, a design of triphenylamine groups grafted triphenylene derivative (T-6TPA) as dopant-free HTLs has been presented. The larger π-conjugation in T-6TPA give rise to high hole mobility of 2.06 × 10−3 cm2V−1s−1. Moreover, the interfacial hole extraction of T-6TPA was significantly promoted when the molecules were infiltrated into perovskite before HTL deposition. The infiltration method of anti-solvent dripping (An) strategy increased PCE from 18.5% up to 20.3%, which is superior to another additive doping strategy (Ad-strategy, 19.3%). The effectiveness of An-strategy can be attributed to the construction of a coherent and homogeneous hole transport channel. The hydrophobicity and high glass transition temperature of T-6TPA also granted excellent moisture and thermal stabilities that the initial PCE could remain 80% for 60 days in air or 600 h at 60 °C. This work highlights the synergistical optimization by design of highly hole-mobile materials as well as the interfacial network construction for charge transport.

Lead-Free Perovskite Homojunction-Based HTM-Free Perovskite Solar Cells: Theoretical and Experimental Viewpoints.

Simplifying the design of lead-free perovskite solar cells (PSCs) has drawn a lot of interest due to their low manufacturing cost and relative non-toxic nature. Focus has been placed mostly on reducing the toxic lead element and eliminating the requirement for expensive hole transport materials (HTMs). However, in terms of power conversion efficiency (PCE), the PSCs using all charge transport materials surpass the environmentally beneficial HTM-free PSCs. The low PCEs of the lead-free HTM-free PSCs could be linked to poorer hole transport and extraction as well as lower light harvesting. In this context, a lead-free perovskite homojunction-based HTM-free PSC was investigated, and the performance was then assessed using a Solar Cell Capacitance Simulator (SCAPS). A two-step method was employed to fabricate lead-free perovskite homojunction-based HTM-free PSCs in order to validate the simulation results. The simulation results show that high hole mobility and a narrow band gap of cesium tin iodide (CsSnI3) boosted the hole collection and absorption spectrum, respectively. Additionally, the homojunction's built-in electric field, which was identified using SCAPS simulations, promoted the directed transport of the photo-induced charges, lowering carrier recombination losses. Homojunction-based HTM-free PSCs having a CsSnI3 layer with a thickness of 100 nm, defect density of 1015 cm-3, and interface defect density of 1018 cm-3 were found to be capable of delivering high PCEs under a working temperature of 300 K. When compared to formamidinium tin iodide (FASnI3)-based devices, the open-circuit voltage (Voc), short-circuit density (Jsc), fill factor (FF), and PCE of FASnI3/CsSnI3 homojunction-based HTM-free PSCs were all improved from 0.66 to 0.78 V, 26.07 to 27.65 mA cm-2, 76.37 to 79.74%, and 14.62 to 19.03%, respectively. In comparison to a FASnI3-based device (PCE = 8.94%), an experimentally fabricated device using homojunction of FASnI3/CsSnI3 performs better with Voc of 0.84 V, Jsc of 22.06 mA cm-2, FF of 63.50%, and PCE of 11.77%. Moreover, FASnI3/CsSnI3-based PSC is more stable over time than its FASnI3-based counterpart, preserving 89% of its initial PCE. These findings provide promising guidelines for developing highly efficient and environmentally friendly HTM-free PSCs based on perovskite homojunction.

The electronic structure of β-TeO2 as wide bandgap p-type oxide semiconductor

Wide bandgap oxide semiconductors have gained significant attention in the fields from flat panel displays to solar cells, but their uses have been limited by the lack of high mobility p-type oxide semiconductors. Recently, β-phase TeO2 has been identified as a promising p-type oxide semiconductor with exceptional device performance. In this Letter, we report on the electronic structure of β-TeO2 studied by a combination of high-resolution x-ray spectroscopy and hybrid density functional theory calculations. The bulk bandgap of β-TeO2 is determined to be 3.7 eV. Direct comparisons between experimental and computational results demonstrate that the top of a valence band (VB) of β-TeO2 is composed of the hybridized Te 5s, Te 5p, and O 2p states, whereas a conduction band (CB) is dominated by unoccupied Te 5p states. The hybridization between spatially dispersive Te 5s2 states and O 2p orbitals helps us to alleviate the strong localization in the VB, leading to small hole effective mass and high hole mobility in β-TeO2. The Te 5p states provide stabilizing effect to the hybridized Te 5s-O 2p states, which is enabled by structural distortions of a β-TeO2 lattice. The multiple advantages of large bandgap, high hole mobility, two-dimensional structure, and excellent stability make β-TeO2 a highly competitive material for next-generation opto-electronic devices.

Synergistic Fluorine⋅⋅⋅Sulfur Intra‐ and Intermolecular Interactions on Dopant‐Free Hole Transport Material for Efficient and Stable Inverted Perovskite Solar Cells

Designing dopant‐free small‐molecule hole transport materials (HTMs) with self‐assembly behavior via noncovalent interactions is considered as one effective strategy to achieve high‐performance inverted perovskite solar cells (PSCs). Herein, two donor‐π bridge‐donor (D–π–D) HTMs are presented, TPASF and TPAOF, containing 3,6‐dimethoxythieno[3,2‐b]thiophene as a core part with 3‐fluoro‐N,N‐bis(4‐(methylthio)phenyl)aniline and 3‐fluoro‐N,N‐bis(4‐methoxyphenyl)aniline as side group. The synergistic F⋅⋅⋅S dipole–dipole intra‐ and intermolecular interactions in TPASF drive the self‐assembly of this molecule into a supramolecular nanofibrillar network, leading to high hole mobility, superior interfacial properties, and providing a good growth template for the perovskite layer atop. The corresponding dopant‐free TPASF‐based inverted devices exhibit a promising power conversion efficiency of 21.01% with a long T 80 lifetime of ≈632 h under operational conditions. This work paves the way for the further development of new dopant‐free self‐assembled HTM designs for highly efficient and stable inverted PSCs.

Tuning Hole Transport Properties via Pyrrole Derivation for High‐Performance Perovskite Solar Cells

AbstractHole transport materials (HTMs) with high hole mobility, good band alignment and ease of fabrication are highly desirable for perovskite solar cells (PSCs). Here, we designed and synthesized novel organic HTMs, named T3, which can be synthesized in high yields with commercially available materials, featuring a substituted pyrrole core and triphenylamine peripheral arms. The capability of functionalization in the final synthetic step provides an efficient way to obtain a variety of T3‐based HTMs with tunable energy levels and other properties. Among them, fluorine‐substituted T3 (T3‐F) exhibits the best band alignment and hole extraction properties, leading to PSCs with outstanding PCEs of 24.85 % and 24.03 % (certified 23.46 %) for aperture areas of 0.1 and 1 cm2, respectively. The simple structure and tunable performance of T3 can inspire further optimization for efficient PSCs.

Tuning Hole Transport Properties via Pyrrole Derivation for High-Performance Perovskite Solar Cells.

Hole transport materials (HTMs) with high hole mobility, good band alignment and ease of fabrication are highly desirable for perovskite solar cells (PSCs). Here, we designed and synthesized novel organic HTMs, named T3, which can be synthesized in high yields with commercially available materials, featuring a substituted pyrrole core and triphenylamine peripheral arms. The capability of functionalization in the final synthetic step provides an efficient way to obtain a variety of T3-based HTMs with tunable energy levels and other properties. Among them, fluorine-substituted T3 (T3-F) exhibits the best band alignment and hole extraction properties, leading to PSCs with outstanding PCEs of 24.85 % and 24.03 % (certified 23.46 %) for aperture areas of 0.1 and 1 cm2 , respectively. The simple structure and tunable performance of T3 can inspire further optimization for efficient PSCs.

Highly Conductive Ultrathin Layers of Conjugated Polymers for Metal-Free Coplanar Transistors with Single-Polymer Transport Layers.

Although metal or oxide conductive films are widely used as electrodes of electronic devices, organic electrodes would be more favorable for next-generation organic electronics. Here, using some model conjugated polymers as examples, we report a class of highly conductive and optically transparent polymer ultrathin layers. Vertical phase separation of semiconductor/insulator blends leads to a highly ordered two-dimensional (2D) ultrathin layer of conjugated-polymer chains on the insulator. Afterwards, the thermally evaporated dopants on the ultrathin layer lead to a conductivity of up to 103 S cm-1 and a sheet resistance 103 Ω/square for a model conjugated polymer poly(2,5-bis(3-hexadecylthiophen-2-yl)thieno[3,2-b]thiophenes) (PBTTT). The high conductivity is due to the high hole mobility (∼ 20 cm2 V-1 s-1), although doping-induced charge density is still in the moderate range of 1020 cm-3 with a 1 nm thick dopant. Metal-free monolithic coplanar field-effect transistors using the same conjugated-polymer ultrathin layer with alternatively doped regions as electrodes and a semiconductor layer are realized. The field-effect mobility of this monolithic transistor is over 2 cm2 V-1 s-1 for PBTTT, one order higher than that of the conventional PBTTT transistor using metal electrodes. The optical transparency of the single conjugated-polymer transport layer is over 90%, demonstrating a bright future for all-organic transparent electronics.

Effects of Charge Dopants in Quantum Spin Hall Materials.

Semiconductors' sensitivity to electrostatic gating and doping accounts for their widespread use in information communication and new energy technologies. It is demonstrated quantitatively and with no adjustable parameters that the presence of paramagnetic acceptor dopants elucidates a variety of hitherto puzzling properties of two-dimensional topological semiconductors at the topological phase transition and in the regime of the quantum spin Hall effect. The concepts of resonant states, charge correlation, Coulomb gap, exchange interaction between conducting electrons and holes localized on acceptors, strong coupling limit of the Kondo effect, and bound magnetic polaron explain a short topological protection length, high hole mobilities compared with electron mobilities, and different temperature dependence of the spin Hall resistance in HgTe and (Hg,Mn)Te quantum wells.

A Multifunctional Small-Molecule Hole-Transporting Material Enables Perovskite QLEDs with EQE Exceeding 20%

Hole-transporting materials (HTMs) play critical roles in the device performance and stability of perovskite quantum dot light-emitting diodes (Pe-QLEDs). However, the development of small-molecule HTMs for achieving high-performance Pe-QLEDs has proven to be very challenging because of their low hole mobility and poor solvent resistance. Herein, we tailor-made a multifunctional small-molecule HTM, termed X10, with methoxy as the substituents, for application in Pe-QLEDs. X10 features high hole mobility, good film-forming ability, and strong solvent resistance ability as well as defect passivation effect. Subsequently, Pe-QLEDs employing X10 as HTM presented a promising external quantum efficiency (EQE) of 20.18%, which is 7-fold higher than that of the reference HTM-TCTA-based ones (EQE ≈ 2.88%). To the best of our knowledge, this is the first case in which a small-molecule HTM displays a high EQE over 20% in Pe-QLEDs. Our work provides important guidance for the rational design of multifunctional small-molecule HTMs for high-performance Pe-QLEDs.

Quantum chemical investigation of Z-shaped heptazethrenes derivatives with detailed structural parameters and singlet fission for photovoltaic applications

A variety of organic solar cells has been discovered, but there is a need for efficient optoelectronic material to obtain high power conversion efficiency. In this study, we derived new molecules from Z-shaped heptazethrene. We measured its photovoltaic parameters, including frontier molecular orbitals (where the energy gap decreases to 16% as compared to the reference), molecular electrostatic potential maps (more nucleophilic core), the density of states (partial and total), absorbance in Vis-IR region (in the range of 650–1000 nm), transition density matrix, and hole-electron mobility in terms of reorganization energy that showed 11% higher electron mobility (λe) and 52% higher hole mobility (λh) as compared to the reference. A comparable power conversion efficiency (∼9%) is obtained from a single photon. Using the concept of singlet fission, we can increase the efficiency twice using a single photon (based on the diradical character of the molecule). The diradical character of the entitled molecules was also calculated. The designed molecules fulfil the criteria of singlet fission that generate two excited triplets from a single photon (ES1>2ET1). The designed molecules are more stable than the reference indicated by the singlet-triplet energy gap, which is 37% higher. Hence this work assists the researcher in enhancing the efficiency of the solar cell.

Review of Defect Passivation for NiOx-Based Inverted Perovskite Solar Cells

In recent years, organic–inorganic hybrid perovskite solar cells (PSCs) have attracted extensive attention due to their high power conversion efficiency (PCE) and simple preparation process. The selection and optimization of the hole transport layer (HTL) are very important for device performance. Compared to other HTLs, nickel oxide (NiOx) has been widely used in PSCs due to its good chemical stability, high hole mobility, and simple preparation method. This review begins with the application of NiOx HTL in planar PSCs and systematically introduces the influence of the structure and photoelectrical properties of devices by doping and surface modification. The effects of NiOx modification on the power conversion efficiency (PCE), filling factor (FF), open-circuit voltage (Voc), short-circuit current (Jsc), and stability of PSCs are reviewed in detail from the perspectives of energy-level matching, hole mobility, and crystallinity. Finally, the future of NiOx-based planar PSCs is discussed.

Engineering of Hole Transporting Interface by Incorporating the Atomic-Precision Ag6 Nanoclusters for High-Efficiency Blue Perovskite Light-Emitting Diodes.

Properties of the underlying hole transport layer (HTL) play a crucial role in determining the optoelectronic performance of perovskite light-emitting devices (PeLEDs). However, endowing the current HTL system with a deep highest occupied molecular orbital (HOMO) level concurrent with high hole mobility is still a big challenge, in particular being an open constraint toward high-efficiency blue PeLEDs. In this regard, employing the poly(9-vinylcarbazole) as a model, we perform efficient incorporation of the atomic-precision metal nanoclusters (NCs), [Ag6PL6, PL = (S)-4-phenylthiazolidine-2-thione], to achieve significant tailoring in both HOMO energy level and hole mobility. As a result, the as-modified PeLEDs exhibit an external quantum efficiency (EQE) of 14.29% at 488 nm. The presented study exemplifies the success of metal NC involved HTL engineering and offers a simple yet effective additive strategy to settle the blue PeLED HTL dilemma, which paves the way for the fabrication of highly efficient blue PeLEDs.

Tailoring the epitaxial growth of oriented Te nanoribbon arrays

As an elemental semiconductor, tellurium (Te) has been famous for its high hole-mobility, excellent ambient stability and topological states. Here, we realize the controllable synthesis of horizontal Te nanoribbon arrays (TRAs) with an angular interval of 60°on mica substrates by physical vapor deposition strategy. The growth of Te nanoribbons (TRs) is driven by two factors, where the intrinsic quasi-one-dimensional spiral chain structure promotes the elongation of their length; the epitaxy relationship between [110] direction of Te and [110] direction of mica facilitates the oriented growth and the expansion of their width. The bending of TRs which have not been reported is induced by grain boundary. Field-effect transistors based on TRs demonstrate high mobility and on/off ratio corresponding to 397cm2V-1s-1 and 1.5×105, respectively. These phenomena supply an opportunity to deep insight into the vapor-transport synthesis of low-dimensional Te and explore its underlying application in monolithic integration.

Toward Accurate Prediction of Ion Mobility in Organic Semiconductors by Atomistic Simulation.

A multiscale scheme (MLMS: Multi-Level Multi-Scale) to predict the ion mobility (μ) of amorphous organic semiconductors is proposed, which was successfully applied to the hole mobility predictions of 14 organic systems. An inverse relationship between μ and reorganization energy is observed due to local polaronic distortions. Another moderate inverse correlation between μ and distribution of site energy change exists, representing the effects of geometric flexibility. The former and the latter represent the intramolecular and intermolecular geometric effects, respectively. In addition, a linear correlation between transfer coupling and μ is observed, showing the importance of orbital overlaps between monomers. Especially, the highest hole mobility of C6-2TTN is due to its large transfer coupling. On the other hand, another high hole mobility of CBP turned out to come from the high first neighbor density (ρFND) of its first self-solvation, emphasizing the proper description of amorphous structural configurations with a sufficiently large number of monomers. In general, systems with either unusually high transfer coupling or high first neighbor density can potentially have high μ regardless of geometric effects. Especially, the newly suggested design parameter, ρFND, is pointing to a new direction as opposed to the traditional π-conjugation strategy.

Constructing D-π-A Type Polymers as Dopant-Free Hole Transport Materials for High-Performance CsPbI2Br Perovskite Solar Cells.

Hole-transporting materials (HTMs) play a major role in efficient and stable perovskite solar cells (PSCs), especially for CsPbI2Br inorganic PSC. Among them, dopant-free conjugated polymers attract more attention because of the advantages of high hole mobility and high stability. However, the relationship between the polymer structure and the photovoltaic performance is rarely investigated. In this work, we choose three similar D-π-A-type polymers, where the D unit and π-bridge are fixed into benzodithiophene and thiophene, respectively. By changing the A units from classic benzodithiophene-4,8-dione and benzotriazole to quinoxaline, three polymers PBDB-T, J52, and PE61 are utilized as dopant-free HTMs for CsPbI2Br PSCs. The energy levels, hole mobility, and molecular stacking of the three HTMs, as well as charge transfer between CsPbI2Br/HTMs, are fully investigated. Finally, the device based on PE61 HTM obtains the champion power conversion efficiency of 16.72%, obviously higher than PBDB-T (15.13%) and J52 (15.52%). In addition, the device based on PE61 HTM displays the best long-term stability. Those results demonstrate that quinoxaline is also an effective A unit to construct D-π-A-type polymers as HTMs and improve the photovoltaic performance of PSCs.

Laser-Induced Hole Coherence and Spatial Self-Phase Modulation in the Anisotropic 3D Weyl Semimetal TaAs.

Laser-induced electron coherence is a fascinating topic in manipulating quantum materials. Recently, it has been shown that laser-induced electron coherence in 2D materials can produce a third-order nonlinear optical response spatial self-phase modulation (SSPM), which has been used to develop a novel all-optical switching scheme. However, such investigations have mainly focused on electron coherence, whereas laser-induced hole coherence is rarely explored. Here, the observation of the optical Kerr effect in 3D Weyl semimetal TaAs flakes is reported. The nonlinear susceptibility (χ(3) ) is obtained, which exhibits a surprisingly high value (with = 9.9×10-9 e.s.u. or 1.4×10-16 m2 V-2 at 532nm). This cannot be explained by the conventional electron mobility, but can be well understood by the unique high anisotropic hole mobility of TaAs. The wind-chime model and χ(3) carrier mobility correlation adequately explain the results, suggesting the crucial role of laser-induced nonlocal ac hole coherence. These observations extend the understanding of SSPM from 2D to 3D quantum materials with anisotropic carrier mobility and from electron coherence to hole coherence.

Green‐solvent Processable Dopant‐free Hole Transporting Materials for Inverted Perovskite Solar Cells

AbstractThe commercialization of perovskite solar cells (PVSCs) urgently requires the development of green‐solvent processable dopant‐free hole transporting materials (HTMs). However, strong intermolecular interactions that ensure high hole mobility always compromise the solubility and film‐forming ability in green solvents. Herein, we show a simple but effective design strategy to solve this trade‐off, that is, constructing star‐shaped D‐A‐D structure. The resulting HTMs (BTP1‐2) can be processed by green solvent of 2‐methylanisole (2MA), a kind of food additive, and show high hole mobility and multiple defect passivation effects. An impressive efficiency of 24.34 % has been achieved for 2MA‐processed BTP1 based inverted PVSCs, the highest value for green‐solvent processable HTMs so far. Moreover, it is manifested that the charge separation of D‐A type HTMs at the photoinduced excited state can help to passivate the defects of perovskites, indicating a new HTM design insight.

Green-solvent Processable Dopant-free Hole Transporting Materials for Inverted Perovskite Solar Cells.

The commercialization of perovskite solar cells (PVSCs) urgently requires the development of green-solvent processable dopant-free hole transporting materials (HTMs). However, strong intermolecular interactions that ensure high hole mobility always compromise the solubility and film-forming ability in green solvents. Herein, we show a simple but effective design strategy to solve this trade-off, that is, constructing star-shaped D-A-D structure. The resulting HTMs (BTP1-2) can be processed by green solvent of 2-methylanisole (2MA), a kind of food additive, and show high hole mobility and multiple defect passivation effects. An impressive efficiency of 24.34% has been achieved for 2MA-processed BTP1 based inverted PVSCs, the highest value for green-solvent processable HTMs so far. Moreover, it is manifested that the charge separation of D-A type HTMs at the photoinduced excited state can help to passivate the defects of perovskites, indicating a new HTM design insight.