Yating Li, Mengmeng Niu, Junpeng Zeng, Quan Zhou, Xu Wu, Wei Ji, Yeliang Wang, Ren Zhu, Jingsi Qiao, Jianbin Xu, Yi Shi, Xinran Wang, and Daowei He
Abstract:
Organic semiconductors are highly promising as channel materials for energy-efficient, cost-effective, and flexible electronics. However, grain boundaries (GBs) can cause significant device performance variation, posing a major challenge for the development of high-performance organic circuits. In this work, we effectively passivated GB-induced traps in monolayer organic thin-film transistors (OTFTs) via p-type doping with the organic salt TrTPFB. The doping strategy broadens the mobility edge, effectively shielding GB-induced energy barriers and Coulomb scattering, and promotes deeper nonlocalized hybridization states for conduction. Consequently, the charge transport mechanism transitions from multiple trapping and release (MTR) to a more band-like behavior, even when GBs are present within the device channel. The doped OTFTs demonstrate ultralow mobility variation (1.4%) and threshold voltage variation (4.9%), as well as record-low contact resistant of RC = 0.6 Ω·cm, outperforming most single-crystal technologies. These performance metrics render doped monolayer polycrystalline films highly promising candidates for industrial-scale organic electronics.
Qingyang Wang, Mengmeng Niu, Weikang Zhou, Yicheng Ma, Chun Huang, Gege Yang, Yan Shao, Xu Wu, Cong Wang, Wei Ji*, Yeliang Wang*, Jingsi Qiao*
Abstract:
Two-dimensional (2D) multiferroic materials have significant application potential for novel storage devices due to their tunable magnetic and ferroelectric properties. Transition metal phosphorus chalcogenides MPX3 (X = S, Se, and Te) were found to be magnetic and multiferroic with excellent tunability, promising for multifunctionalized applications. In this study, we investigated the antiferromagnetic and antiferroelectric properties of two-dimensional FePX3 and CuFeP2X6 by density functional theory. Monolayer FePS3/FePSe3 and FePTe3 take intralayer zigzag and Neel antiferromagnetic ground states, respectively. This tunability of intralayer magnetism results from the competition between the spin-exchange interactions of the first and second nearest Fe atoms. Bilayer FePX3 shows weak interlayer interactions and keeps electronic and magnetic characteristics similar to those of the monolayer. Moreover, by introducing the nonmagnetic Cu atom into FePX3, the inversion symmetry broken induces CuFeP2X6 to be multiferroic materials. The transition barrier between ferroelectric (FE) and antiferroelectric (AFE) phases in CuFeP2S6 and CuFeP2Se6 is 0.09 and 0.04 eV/f.u., similar to well-known multiferroic CuCrP2S6. FE-to-AFE phase transition is expected to be achieved by applying an electric field and uniaxial strain. CuFeP2Te6 shows the ground state with a distorted paraelectric phase. Our results show the fundamental properties and in-depth understanding of 2D FePX3 and CuFeP2X6, guiding further investigation of 2D multifunctionalized magnetoelectric devices.
Xuanhao Wu, Mengmeng Niu, Xin Tian, Xiaoyan Peng, Pio John S. Buenconsej, Xu Wu, Yeliang Wang, Wei Ji, Yi Li, Jingsi Qiao,Jifang Tao, Mingming Zhang, Song Xiaof and Hongye Yuan
Abstract:
Developing sensitive metal–organic framework (MOF) systems to overcome the ubiquitous trade-off between porosity and conductivity remains a formidable yet sought-after endeavor. This pursuit is of great significance for the development of MOF-based chemiresistive sensors with enhanced sensitivity and selectivity. Herein, we present an innovative template assisted strategy that utilizes the two-dimensional properties and good conductivity of MXene nanosheets, as well as lattice matching between MXene (Nb2C) and selected Ni3(HITP)2, to achieve controllable self-assembly of Ni3(HITP)2 on MXene sheets. This results in Ni3(HITP)2/MXene (HITP: 2,3,6,7,10,11-hexaaminotriphenylene) heterostructures with considerable conductivity, porosity, and solution processability. The powder and film electrical conductivity are 4.8 × 103 and 5.3 × 105 S m−1, respectively, and the BET specific surface area can reach 797.8 m2 g−1. It is worth noting that excellent solution processability helps to prepare large-area films (23 cm × 9 cm) with good uniformity. Gas sensors based on Ni3(HITP)2/MXene heterostructures exhibit high sensitivity (LOD ∼ 5 ppb) and selectivity towards ultratrace ethanol at room temperature, setting a new benchmark. Such sensing behavior stems from the strong coupling of Ni3(HITP)2/MXene heterostructures and their enhanced interaction with ethanol, evidenced by experimental results and theoretical calculations. Real-time respiratory sensing assessments underscore their practicality in healthcare monitoring. This straightforward approach simplifies the integration of MOF-related materials on miniaturized devices with outstanding performance.
Xiaocang Han, Mengmeng Niu, Yan Luo, Runlai Li, Jiadong Dan, Yanhui Hong, Xu Wu, Alex V. Trukhanov, Wei Ji, Yeliang Wang, Jiahuan Zhou, Jingsi Qiao*, Jin Zhang* & Xiaoxu Zhao*
Abstract:
Scanning probe microscopy and scanning transmission electron microscopy (STEM) are powerful tools to trigger atomic-scale motions, pattern atomic defects and lead to anomalous quantum phenomena in functional materials. However, these techniques have primarily manipulated surface atoms or atoms located at the beam exit plane, leaving buried atoms, which govern exotic quantum phenomena, largely unaffected. Here we propose an electron-beam-triggered chemical etching approach to engineer shielded metal atoms sandwiched between chalcogen layers in monolayer transition metal dichalcogenide (TMDC). Various metal vacancies (V_MX_n, n=0−6) have been fabricated via atomically focused electron beam in STEM. The parent TMDC surface was modified with surfactants, facilitating the ejection of sandwiched metal vacancies via charge transfer effect. In situ sequential STEM imaging corroborated that a combined chemical-induced knock-on effect and chalcogen vacancy-assisted metal diffusion process result in atom-by-atom vacancy formation. This approach is validated in 16 different TMDCs. The presence of metal vacancies strongly modified their magnetic and electronic properties, correlated with the unpaired chalcogen p and metal d electrons surrounding vacancies and adjacent distortions. These findings show a generic approach for engineering interior metal atoms with atomic precision, creating opportunities to exploit quantum phenomena at the atomic scale.
Yang Yang#, Jijian Liu#, Chunyu Zhao#, Qingrong Liang, Weikang Dong, Jia Shi, Ping Wang, Denan Kong, Lu Lv, Lin Jia, Dainan Wang, Chun Huang, Shoujun Zheng, Meiling Wang, Fucai Liu, Peng Yu, Jingsi Qiao, Wei Ji, Jiadong Zhou*
Abstract:
The 2D ternary transition metal phosphorous chalcogenides (TMPCs) have attracted extensive research interest due to their widely tunable band gap, rich electronic properties, inherent magnetic and ferroelectric properties. However, the synthesis of TMPCs via chemical vapor deposition (CVD) is still challenging since it is difficult to control reactions among multi-precursors. Here, a subtractive element growth mechanism is proposed to controllably synthesize the TMPCs. Based on the growth mechanism, the TMPCs including FePS3, FePSe3, MnPS3, MnPSe3, CdPS3, CdPSe3, In2P3S9, and SnPS3 are achieved successfully and further confirmed by Raman, second-harmonic generation (SHG), and scanning transmission electron microscopy (STEM). The typical TMPCs–SnPS3 shows a strong SHG signal at 1064 nm, with an effective nonlinear susceptibility χ(2) of 8.41 × 10−11 m V−1, which is about 8 times of that in MoS2. And the photodetector based on CdPSe3 exhibits superior detection performances with responsivity of 582 mA W−1, high detectivity of 3.19 × 1011 Jones, and fast rise time of 611 µs, which is better than most previously reported TMPCs-based photodetectors. These results demonstrate the high quality of TMPCs and promote the exploration of the optical properties of 2D TMPCs for their applications in optoelectronics.
