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Schematic and characterization of the 2D SnO/In2O3 heterostructure. a) Schematic illustration of the 2D vdW transfer technique of SnO/In2O3 sheets from liquid metals. The crystal structure of SnO exhibits trigonal symmetry with cell parameters of a = 3.79 Å and b = 3.79 Å and c = 4.84 Å,27 where In2O3 sheets exhibits cubic crystal structure with cell parameters of a = 10.12 Å and b = 10.12 Å and c = 10.12 Å.34 b) Optical image of the 2D SnO/In2O3 heterostructure. c) HRTEM image of the 2D SnO/In2O3 heterostructure sheets. d) HRTEM image showing a highly crystalline structure with continuous lattice fringes across the SnO/In2O3 heterostructure interface. e) SAED pattern taken across the heterostructure interface, with each diffraction spot consisting of a pair diffraction peaks with indexed lattice spacings of 2.70 Å (321), 1.64 Å (532) for In2O3 sheets and 2.68 Å (110), 1.6 Å (211) for SnO sheets (see inset for magnified view for the diffraction spots to lattice plane (110) of SnO and (321) of In2O3). f,g) AFM image of the SnO/In2O3 heterostructure with a step height of ≈5.5 nm.
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Heterostructures assembled from atomically thin materials have led to a new paradigm in the development of the next‐generation high‐performing functional devices. However, the construction of the ultrathin van der Waals (vdW) heterostructures is challenging and/or limited to materials with layered crystal structures. Herein, liquid metal vdW transf...
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Citations
... Thus, they have been intensely investigated recently. For instance, scientists have fabricated LM electrodes used in many basic electronic devices 47 , such as capacitors 48,49 , inductors [49][50][51] , memristors [52][53][54] , and optoelectronic devices [55][56][57] , achieving good performances in electrical biomedical facilities. Moreover, LM-based devices, such as bone cement, e-vessels, and exoskeletons, can excellently conform with human movement, due to their superior stretchability performance. ...
Pursuit of improved living quality has stimulated great demand for high-performance conformal healthcare devices in modern human society. However, manufacturing of efficient, comfortable and stretchable biomedical apparatus faces huge challenges using traditional materials. Liquid metals (LMs) show remarkable potential to solve this problem due to their extraordinary biocompatibility, stretchability, thermal and electrical conductivity. In recent years, tremendous explorations have attempted to make stretchable biomedical devices with LMs. Herein, we review the stretchable LM-based biomedical devices on the topics of disease treatment and human function augmenting. The representative and up-to-date neural interfaces, alloy cement, e-vessels, soft heaters, exoskeletons, and e-skins are summarized. The existing issues of LMs applied for biomedical devices are also discussed. This review can provide guidance for the follow-up research in LM-based biomedical devices.
... An atomic-level oxide film formed by self-oxidation of liquid metal at room temperature is considered as a new generation of two-dimensional semiconductor materials [52,56,[63][64][65][66][67][68][69][70][71][72]. Unlike the common layered material exfoliation, the liquid metal core is a disordered structure made of metal bonds. ...
... Subsequent articles have prepared other types of ultrathin 2D nanostructures by means of liquid metal synthesis. In 2009, Ali Zavabeti subsequently construct liquid metal Van der Waals (VdW) transfer method (refer to sticking method) is used to construct largearea heterostructures of atomically thin metal oxides of p-SnO/n-In2O3 with ease, which is shown in Figure 2c [71]. The liquid metal synthesis and transfer method therefore can potentially provide access to a variety of other heterostructures which are made of oxide layers that do not naturally exist as layered materials leading to interesting new discoveries. ...
With the continuous exploration of low-dimensional nanomaterials, two dimensional metal oxides (2DMOs) has been received great interest. However, their further development is limited by the high cost in the preparation process and the unstable states caused by the polarization of surface chemical bonds. Recently, obtaining mental oxides via liquid metals have been considered a surprising method for obtaining 2DMOs. Therefore, how to scientifically choose different preparation methods to obtain 2DMOs applying in different application scenarios is an ongoing process worth discussing. This review will provide some new opportunities for the rational design of 2DMOs based on liquid metals. Firstly, the surface oxidation process and in situ electrical replacement reaction process of liquid metals are introduced in detail, which provides theoretical basis for realizing functional 2DMOs. Secondly, by simple sticking method, gas injection method and ultrasonic method, 2DMOs can be obtained from liquid metal, the characteristics of each method are introduced in detail. Then, this review provides some prospective new ideas for 2DMOs in other energy-related applications such as photodegradation, CO2 reduction and battery applications. Finally, the present challenges and future development prospects of 2DMOs applied in liquid metals are presented.
... Fig. 2(d) shows the corresponding work function curve obtained from the solid line marked in a, as shown in the figure, the work function was 4.32 eV, which is close to the relevant values reported in the literature. 34 Scanning tunneling microscopy (STS) is an effective approach to obtain the band structure of two-dimensional nanomaterials. To improve precision, we collected 24 sets of I-V data. ...
High-performance gas sensors have been developed to meet the demand for the trace detection of NO2 given the adverse effects of NO2 posed to the environment and human health. Two-dimensional...
... 38 Additionally, deposition of one metal oxide sheet on top of another can lead to 2D van der Waals heterostructures. 108 By patterning and functionalizing the substrate, deposition of metal oxides on selective areas is possible, which can be utilized for electronic device fabrication. Functionalization of the substrates, which tunes the surface energy, offers control of the surface adhesion and transferring process. ...
The nascent field of liquid metals, metals, and alloys of low melting points has provided opportunities for synthesizing low-dimensional materials. Located between transition- and non-metals in the periodic table, post-transition elements exhibit unique properties in particular low melting points. Taking on a liquid form at low temperature, post-transition liquid metals can be used as solvents for metallic solutes. The enigmatic surface of liquid metals is also ultra-active and smooth, offering opportunities for fabricating and templating two-dimensional (2D) films. So far, various 2D materials have been harvested from the surface of liquid metals including 2D metal compounds and nonmetallic materials. Utilizing different extraction and transfer techniques, the produced 2D films can be uniformly deposited on desired substrates at large lateral dimensions. Here, we present a comprehensive overview of the fundamentals underlying post-transition-elements-based liquid metals and alloys and explain the effect of atomic level electron configurations on their characteristics. We discuss the key physical properties of liquid metals including the origin of their low melting points and their high thermal and electrical conductivities. We illustrate their boundary-induced layering and oxidation as essential traits for creating 2D films. Afterward, the interfacial synthesis of 2D materials is depicted with the discussion of surface oxidation, reduction and exfoliation. We present different types of devices using liquid metal-induced 2D synthesis processes, including field-effect transistors, optoelectronic devices, systems that use 2D dielectric and conductive layers, and piezoelectric devices. Eventually, we discuss future prospects and outline how liquid metals can contribute to exciting future applications.
... Liquid metal printing is a vacuum-free route to depositing ultrathin (<5 nm) metal oxide semiconductors generated by spontaneous surface oxidation 20 . This method has been utilized for synthesis of various metal oxides 21 (SnO 2 , SbO x , InSnO x , GaO x , etc.) for applications to transparent conductive films 14 , photodetectors 22,23 , as well as switching devices 24 . A powerful feature of liquid metal synthesis distinguishing it from contact-based adhesive 2D material transfer is the liquid metal's mechanical compliance which leads to its ability to transfer continuous nanosheets at the cm 2 scale 25 . ...
Ultrathin single-nm channels of transparent metal oxides offer unparalleled opportunities for boosting the performance of low power, multifunctional thin-film electronics. Here we report a scalable and low-temperature liquid metal printing (LMP) process for unlocking the ultrahigh mobility of 2-dimensional (2D) InOx. These continuous nanosheets are rapidly (60 cm s−1) printed over large areas (30 cm2) directly from the native oxide skin spontaneously formed on molten indium. These nanocrystalline LMP InOx films exhibit unique 2D grain morphologies leading to exceptional conductivity as deposited. Quantum confinement and low-temperature oxidative postannealing control the band structure and electronic density of states of the 2D InOx channels, yielding thin-film transistors with ultrahigh mobility (μ0 = 67 cm2 V−1s−1), excellent current saturation, and low hysteresis at temperatures down to 165 °C. This work establishes LMP 2D InOx as an ideal low-temperature transistor technology for high-performance, large area electronics such as flexible displays, active interposers, and thin-film sensors.
... Interesting new strategy was recently employed to fabricate vdW heterostructured 2D layered materials via stacking of various 2D layered crystals extracted from their liquid-based metals and alloys. A p-n heterojunction was developed by the vdW exfoliation of 2D SnO and In 2 O 3 films [167]. In this method, 2D SnO/In 2 O 3 vdW heterostructures developed [167] by the vdW transfer of surface oxide film of liquid tin (p-SnO) on top of the natural surface oxide of indium (n-In 2 O 3 ). ...
... A p-n heterojunction was developed by the vdW exfoliation of 2D SnO and In 2 O 3 films [167]. In this method, 2D SnO/In 2 O 3 vdW heterostructures developed [167] by the vdW transfer of surface oxide film of liquid tin (p-SnO) on top of the natural surface oxide of indium (n-In 2 O 3 ). The developed 2D heterostructured film finally composed of p-SnO/n-In 2 O 3 2D films attached on top of each other via vdW forces (Fig. 13a, b) [167]. ...
... In this method, 2D SnO/In 2 O 3 vdW heterostructures developed [167] by the vdW transfer of surface oxide film of liquid tin (p-SnO) on top of the natural surface oxide of indium (n-In 2 O 3 ). The developed 2D heterostructured film finally composed of p-SnO/n-In 2 O 3 2D films attached on top of each other via vdW forces (Fig. 13a, b) [167]. The following microstructural studies in atomic scale levels confirmed the formation of a vdW heterointerfaces between SnO/In 2 O 3 films with two crystalline structures with the different characteristics fabricated over Si/SiO 2 substrate (Fig. 13c). ...
Two-dimensional (2D) semiconductors beyond graphene represent the thinnest stable known nanomaterials. Rapid growth of their family and applications during the last decade of the twenty-first century have brought unprecedented opportunities to the advanced nano- and opto-electronic technologies. In this article, we review the latest progress in findings on the developed 2D nanomaterials. Advanced synthesis techniques of these 2D nanomaterials and heterostructures were summarized and their novel applications were discussed. The fabrication techniques include the state-of-the-art developments of the vapor-phase-based deposition methods and novel van der Waals (vdW) exfoliation approaches for fabrication both amorphous and crystalline 2D nanomaterials with a particular focus on the chemical vapor deposition (CVD), atomic layer deposition (ALD) of 2D semiconductors and their heterostructures as well as on vdW exfoliation of 2D surface oxide films of liquid metals.
... For example, the large area heterostructures of atomically thin p-SnO/n-In 2 O 3 exhibit both outstanding photodetectivity and photoresponsivity under the illumination of the 280 nm light. This excellent performance is due to the narrow bandgap of the staggered band at the p-n junction formed by the high-quality SnO/In 2 O 3 heterostructure (Alsaif et al., 2019a). Low-dimensional magnetic materials (including 2D oxides, etc.) possess excellent magnetic properties which originate from the defects such as vacancy, doping, adatom, and dangling bonds, which can be important in advancing electronics, data storage, and even biomedical fields. ...
... Therefore, for the liquid metal with a non-self-limiting reaction, precisely controlling the oxygen content and adjusting the oxidation time of the liquid metal may lead to a surface layer with a specific thickness and surface composition. Various 2D MOXs (Bi 2 O 3 (Messalea et al., 2018), In 2 O 3 (Alsaif et al., 2019a), ZnO (Mahmood et al., 2021), and PbO (Ghasemian et al., 2020)) were successfully obtained based on the Cabrera-Mott model and the exfoliation technique by printing or gas injection method. ...
Atomically thin two-dimensional (2D) metal oxides exhibit unique optical, electrical, magnetic, and chemical properties, rendering them a bright application prospect in high-performance smart devices. Given the large variety of both layered and non-layered 2D metal oxides, the controllable synthesis is the critical prerequisite for enabling the exploration of their great potentials. In this review, recent progress in the synthesis of 2D metal oxides is summarized and categorized. Particularly, a brief overview of categories and crystal structures of 2D metal oxides is firstly introduced, followed by a critical discussion of various synthesis methods regarding the growth mechanisms, advantages, and limitations. Finally, the existing challenges are presented to provide possible future research directions regarding the synthesis of 2D metal oxides. This work can provide useful guidance on developing innovative approaches for producing both 2D layered and non-layered nanostructures and assist with the acceleration of the research of 2D metal oxides.
... As shown in Fig. 1f, atomically thin oxide skin of the liquid tin and indium (i.e. SnO and In 2 O 3 ) were stacked to produce a large-area 2D p -n heterostructure [64]. However, such a method is also limited with a finite number of choices of 2D materials with relatively high densities of bubbles or wrinkles formed in the heterojunction interface. ...
The emerging two-dimensional (2D) materials have led to the revolution across many fields in optics, electronics, optoelectronics, and sensors. Physical sensors such as photodetector and chemical sensors like gas and biological sensors play important roles in optical communications, imaging, environmental monitoring, remediation, as well as healthcare and medical industries. The implementation of 2D materials can significantly enhance the performances of such sensors due to their ultra-thin planar surface, large surface-to-volume ratio, and unique physiochemical properties. Peculiar features such as tunable band structures and relatively large charge carrier mobilities in certain 2D materials further provide additional dimensions to realize high-performance sensors from optical, electronic, and optoelectronic transducing platforms. Enabled by the weak van der Waals (vdW) force, individual 2D materials can be artificially stacked to realize the atomically thin 2D heterostructures, producing unprecedented features which are not accessible in the individual 2D counterparts or other low-dimensional heterostructures. Here, the atomically thin 2D heterostructures are comprehensively reviewed by firstly summarizing their controllable and scalable synthesis. Meanwhile, the band structure alignment and interfacial charge transfer behavior of 2D heterostructures are specifically introduced and their influences on physical and chemical sensing are revealed. In addition, the state-of-the-art progress is reported and critically discussed. Finally, the current challenges and prospects of 2D heterostructure-based sensors are provided.
... The rise time (t rise ) and fall time (t fall ) are defined as the time required for the current to rise from 10% to 90% and decrease from 90% to 10% of the peak intensity. 38,49,50 A t rise and t fall of 42 s and 87 s were determined, respectively. The observed comparatively slow rise and decay times are likely linked to the defect-induced trap states inside the bandgap of 2D indium oxysulfide. ...
Metal oxychalcogenides are emerging as a new motif of group VI-A semiconductors with unique electronic properties. Among this family, two dimensional (2D) oxysulfide materials have been increasingly involved in the development of next-gen electronic and optoelectronic devices. However, current synthesis routes for 2D metal oxysulfides are still limited to vapor phase deposition techniques, hindering access to ultra-thin, well-defined, and highly crystalline structures. Herein, we report a new synthesis approach for atomically thin and large-area indium oxysulfide nanosheets (2D In2O3-xSx, x is from 0 to 0.41). The process consists of printing indium oxide skins out of molten indium metal and a subsequent sulfur insertion conducted in a trisulfur radical anion solution. Back-gated field-effect transistors (FETs) based on 2D In2O3-xSx reveal a notably high electron mobility of ∼20.4 cm2 V-1 s-1, corresponding to approximately 270% mobility enhancement over as-synthesized indium oxide. In addition, 2D In2O3-xSx based photodetectors exhibit an excellent performance in ultraviolet (UV) region, with a photoresponsivity of ∼3.4×103 A W-1 greatly surpassing that of many commercial materials. More importantly, the same reaction parameters can be employed to obtain 2D bismuth oxysulfide and 2D tin oxysulfide, offering a furnace-free approach for 2D oxysulfide semiconductor fabrication.
... 37,38 Given certain post-transition metals such as Ga, In, Sn, and Bi are with relatively low melting points, the adherence of such a 2D large-area surface oxide layer to these metals in the liquid form is weak due to the absence of covalent bonds, which can be easily delaminated through external force (e.g., screenprinting). Recent attempts in producing atomically thin Ga 2 O 3 , 39 In 2 O 3 , 40 SnO, 37 and Bi 2 O 3 41 have been demonstrated. It should be noted that such a synthesis approach is distinctly different from those of other reported printable Gabased TCOs, in which liquid Ga was first printed on the substrate and subsequently underwent thermal oxidation to transform into TCOs. ...
Ultrathin transparent conductive oxides (TCOs) are emerging candidates for next-generation transparent electronics. Indium oxide (In2O3) incorporated with post-transition-metal ions (e.g., Sn) has been widely studied due to their excellent optical transparency and electrical conductivity. However, their electron transport properties are deteriorated at the ultrathin two-dimensional (2D) morphology compared to that of intrinsic In2O3. Here, we explore the domain of transition-metal dopants in ultrathin In2O3 with the thicknesses down to the single-unit-cell limit, which is realized in a large area using a low-temperature liquid metal printing technique. Zn dopant is selected as a representative to incorporate into the In2O3 rhombohedral crystal framework, which results in the gradual transition of the host to quasimetallic. While the optical transmittance is maintained above 98%, an electron field-effect mobility of up to 87 cm2 V-1 s-1 and a considerable sub-kΩ-1 cm-1 ranged electrical conductivity are achieved when the Zn doping level is optimized, which are in a combination significantly improved compared to those of reported ultrathin TCOs. This work presents various opportunities for developing high-performance flexible transparent electronics based on emerging ultrathin TCO candidates.
