In highest quality organic single-crystal field-effect transistors, electron transport occurs in the band-like regime, with the carrier mobility increasing upon lowering temperature. Neither the microscopic nature of this regime, nor why it occurs only in a small number of materials is currently understood. Here, comparative studies of closely related materials, exhibiting high-quality reproducible transport properties are needed. We performed a study of electron transport in single-crystals of different TCNQ (tetracyanoquinodimethane) molecules, combined with band structure calculations. We show that F2-TCNQ devices exhibit very high electron mobility and an unprecedented increase in mobility upon cooling, whereas in TCNQ and F4-TCNQ the mobility is substantially lower and decreases upon cooling. We analyze the crystal and electronic structures of these materials and find that F2-TCNQ crystals are indeed ideal to achieve outstanding transport properties. Our analysis also shows that to understand the difference between the three materials, studying their band structure is not sufficient, and that the electron-phonon coupling needs to be investigated as well. Besides the outstanding transport properties of F2-TCNQ, a key result of our work is the identification of the Fx-TCNQ family as a paradigm to investigate the most fundamental aspects of electronic transport in organic crystals.
Interfaces formed by two different organic semiconductors often exhibit a large conductivity, originating from transfer of charge between the constituent materials. The precise mechanisms driving charge transfer and determining its magnitude remain vastly unexplored, and are not understood microscopically. To start addressing this issue, we have performed a systematic study of highly reproducible single-crystal interfaces based on rubrene and Fx-TCNQ, a family of molecules whose electron affinity can be tuned by increasing the fluorine content. The combined analysis of transport and scanning K…
The kagome-lattice crystal hosts various intriguing properties including the frustrated magnetism, charge order, topological state, superconductivity and correlated phenomena. To achieve high-performance kagome-lattice compounds for electronic and spintronic applications, careful tuning of the band structure would be desired. Here, the electronic structures of kagome-lattice crystal Ni3In2S2 were investigated by transport measurements, angle-resolved photoemission spectroscopy as well as ab initio calculations. The transport measurements reveal Ni3In2S2 as a compensated semimetal with record-h…
First-principles predictions of carrier mobility with record accuracy using GW perturbation theory
Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin（德克萨斯大学奥斯汀分校奥登计算工程与科学学院）；Department of Physics, The University of Texas at Austin（德克萨斯大学奥斯汀分校物理系）；University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Mork Family Department of Chemical Engineering and Materials Science, University of Southern California（南加州大学莫克家族化学工程与材料科学系）
Material defects remain as the main bottleneck to the progress of topological insulators (TIs). In particular, efforts to achieve thin TI samples with dominant surface transport have always led to increased defects and degraded mobilities, thus making it difficult to probe the quantum regime of the topological surface states. Here, by utilizing a novel buffer layer scheme composed of an In2Se3/(Bi0.5In0.5)2Se3 heterostructure, we introduce a quantum generation of Bi2Se3 films with an order of magnitude enhanced mobilities than before. This scheme has led to the first observation of the quantum…
The two-dimensional electron gas (2DEG) at the non-isostructural interface between spinel gamma-Al2O3 and perovskite SrTiO3 is featured by a record electron mobility among complex oxide interfaces in addition to a high carrier density up to the order of 1E15 cm-2. Herein, we report on the patterning of 2DEG at the gamma-Al2O3/SrTiO3 interface grown at 650 °C by pulsed laser deposition using a hard mask of LaMnO3. The patterned 2DEG exhibits a critical thickness of 2 unit cells of gamma-Al2O3 for the occurrence of interface conductivity, similar to the unpatterned sample. However, its maximum c…
The Moore's law in the semiconducting industry has faltered as the three-dimensional (3D) Si-based transistors has approached their physical limit with the downscaling. The carrier mobility $\rm μ$, critical to the device's performance, will be degraded when the thickness of Si is scaled into several nanometers. In contrast to the bulk counterpart, two-dimensional (2D) semiconductors can be scaled into atomic-layer thickness without dangling bonds, maintaining its intrinsic carrier mobility and going beyond the limits of Si-based electronics. Hence, the development of novel 2D semiconducting m…
Ideal two-dimensional (2D) semiconductors with high mobility comparable to three-dimensional (3D) Si or GaAs are still lacking, hindering the development of high-performance 2D devices. Here in this work, using first-principles calculations and considering all the electron-phonon couplings, we show that monolayer BX (X = P, As, Sb) with honeycomb lattices have intrinsic phonon-limited carrier mobility reaching record-high values of 1200-14000 $cm^2V^{-1}s^{-1}$ at room temperature. Despite being polar and the band edges located at the K point with multiple valleys, these three systems unusuall…
Making a systematic effort, we have developed a single-crystalline ZnSnN2 on ZnO (0001) by reactive magnetron co-sputtering. Epitaxial growth was achieved at 350 C by co-sputtering from metal targets in nitrogen atmosphere, and confirmed by transmission electron microscopy (TEM) measurements. TEM verified that the layers are single-crystalline of hexagonal phase, exhibiting epitaxial relationship with the substrate. The screw-type threading dislocations originating from the interface were identified as dominant extended defects. More specifically, we report a pioneering measurement of the disl…
The rise of atomically thin materials has the potential to enable a paradigm shift in modern technologies by introducing multi-functional materials in the semiconductor industry. To date the growth of high quality atomically thin semiconductors (e.g. WS2) is one of the most pressing challenges to unleash the potential of these materials and the growth of mono- or bi-layers with high crystal quality is yet to see its full realization. Here, we show that the novel use of molecular precursors in the controlled synthesis of mono- and bi-layer WS2 leads to superior material quality compared to the …
Metal oxide thin-film transistors are fast becoming a ubiquitous technology for application in driving backplanes of organic light-emitting diode displays. Currently all commercial products rely on metal oxides processed via physical vapor deposition methods. Transition to simpler, higher throughput manufacturing methods such as solution-based processes, are currently been explored as cost-effective alternatives. However, developing printable oxide transistors with high carrier mobility and bias-stable operation has proved challenging. Here we show that hybrid multilayer channels composed of a…
Two-dimensional (2D) materials, such as graphene and transition metal dichalcogenides have attracted great attention because of the rich physics and potential applications in next-generation nano-sized electronic devices. Recently, atomically thin black phosphorus (BP) has become a new member of the 2D materials family with high theoretical mobility and tunable bandgap structure. However, degradation of properties under atmospheric conditions and high-density charge traps in BP have largely limited its mobility (~400 cm2/Vs at room temperature) and thus restricted its future applications. Here…
The quality of the semiconductor-barrier interface plays a pivotal role in the demonstration of high quality reproducible quantum dots for quantum information processing. In this work, we have measured SiMOSFET Hall bars on undoped Si substrates in order to investigate the quality of the devices fabricated in a full CMOS process. We report a record mobility of 17'500 cm2/Vs with a sub-10 nm oxide thickness indicating a high quality interface, suitable for future qubit applications. We also study the influence of gate materials on the mobilities and discuss the underlying mechanisms, giving ins…
In this letter, fin-shape tri-gate $β$-Ga$_{2}$O$_{3}$ lateral MESFETs are demonstrated with a high power figure of merit of 0.95 GW/cm$^{2}$ - a record high for any $β$-Ga$_{2}$O$_{3}$ transistor to date. A low-temperature undoped buffer-channel stack design is developed which demonstrates record high Hall and drift electron mobilities in doped $β$-Ga$_{2}$O$_{3}$ channels allowing for low ON resistances R$_{ON}$ in $β$-Ga$_{2}$O$_{3}$ MESFETs. Fin-widths (W$_{fin}$) were 1.2-1.5 $μ$m and there were 25 fins (N$_{fin}$) per device with a trench depth of $\sim$1$μ$m. A $β$-Ga$_2$O$_3$ MESFET wi…
High surface-mobility, which is attributable to topological protection, is a trademark of three-dimensional topological insulators (3DTIs). Exploiting surface-mobility indicates successful application of topological properties for practical purposes. However, the detection of the surface-mobility has been hindered by the inevitable bulk conduction. Even in the case of high-quality crystals, the bulk state forms the dominant channel of the electrical current. Therefore, with electrical transport measurement, the surface-mobility can be resolved only below-micrometer-thick crystals. The evaluati…
Very recently, it was demonstrated that the carrier mobility of a molecular monolayer dioctylbenzothienobenzothiophene (C8-BTBT) on boron nitride can reach 10 cm2/Vs, the highest among the previously reported monolayer molecular field-effect transistors. Here we show that the high-quality single crystal of the C8-BTBT monolayer may be the key origin of the record-high carrier mobility. We discover that the C8-BTBT molecules prefer layer-by-layer growth on both hexagonal boron nitride and graphene. The flatness of these substrates substantially decreases the C8-BTBT nucleation density and enabl…
We demonstrate a new substrate cleaning and buffer growth scheme in $β$-Ga$_2$O$_3$ epitaxial thin films using metalorganic vapor phase epitaxy (MOVPE). For the channel structure, a low-temperature (LT, 600 $^\circ$C) undoped Ga$_2$O$_3$ buffer is grown followed by transition layers to a high-temperature (HT, 810 $^\circ$C) Si-doped Ga$_2$O$_3$ channel layers without growth interruption. The (010) Ga$_2$O$_3$ Fe-doped substrate cleaning uses solvent cleaning followed by an additional HF (49% in water) treatment for 30 mins before the epilayer growth. This step is shown to compensate the parasi…
The combination of high-quality Al2O3 dielectric and thiol chemistry passivation can effectively reduce the density of interface traps and Coulomb impurities of WS2, leading to a significant improvement of the mobility and a transition of the charge transport from the insulating to the metallic regime. A record high mobility of 83 cm2/Vs (337 cm2/Vs) is reached at room temperature (low temperature) for monolayer WS2. A theoretical model for electron transport is also developed.
Graphene with high carrier mobility μ is required both for graphene-based electronic devices and for the investigation of the fundamental properties of graphene's Dirac fermions. It is largely accepted that the mobility-limiting factor in graphene is the Coulomb scattering off of charged impurities that reside either on graphene or in the underlying substrate. This is true both for traditional graphene devices on SiO2 substrates and possibly for the recently reported high-mobility suspended and supported devices. An attractive approach to reduce such scattering is to place graphene in an envir…
InvDesMobility: a reliability-gated first-principles feedback framework for closed-loop materials discovery
School of Physics and Key Laboratory of Quantum State Construction and Manipulation (Ministry of Education), Renmin University of China（物理学院和量子态构造与操控重点实验室（教育部） ，中国人民大学）
