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1.
J Mol Diagn ; 22(5): 720-727, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-32142899

RESUMO

PCR amplification, a key step in next-generation sequencing (NGS) library construction, can generate an unlimited amount of product from limited input; however, it cannot create more information than was present in the original template. Thus, NGS libraries can be made from very little DNA, but reducing the input may compromise assay sensitivity in ways that are difficult to ascertain unless library complexity (ie, the number of unique DNA molecules represented in the library) and depth of coverage with unique sequence reads (those derived from input DNA molecules) versus duplicate sequence reads (those resulting from overamplification of particular molecules) are discretely measured. A series of experiments was performed to explore the impact of low DNA input on an amplicon-based NGS assay using unique molecular identifiers to track unique versus duplicate reads. At high sequencing depths, unique and total (unique plus duplicate) read coverage are not well correlated, so increasing the number of sequenced reads does not necessarily improve sensitivity. Unique coverage depth tends to improve with more input, but improvements are not consistent. Fluctuations in library complexity complicated variant detection using both standardized and clinical specimens, often resulting in technical replicates with vastly different estimates of variant allelic fraction. In conclusion, depth of coverage with unique reads must be tracked in clinical NGS to ensure that sensitivity and accuracy are maintained.

2.
Nat Mater ; 2020 Mar 10.
Artigo em Inglês | MEDLINE | ID: mdl-32157191

RESUMO

Atomically thin two-dimensional (2D) metals may be key ingredients in next-generation quantum and optoelectronic devices. However, 2D metals must be stabilized against environmental degradation and integrated into heterostructure devices at the wafer scale. The high-energy interface between silicon carbide and epitaxial graphene provides an intriguing framework for stabilizing a diverse range of 2D metals. Here we demonstrate large-area, environmentally stable, single-crystal 2D gallium, indium and tin that are stabilized at the interface of epitaxial graphene and silicon carbide. The 2D metals are covalently bonded to SiC below but present a non-bonded interface to the graphene overlayer; that is, they are 'half van der Waals' metals with strong internal gradients in bonding character. These non-centrosymmetric 2D metals offer compelling opportunities for superconducting devices, topological phenomena and advanced optoelectronic properties. For example, the reported 2D Ga is a superconductor that combines six strongly coupled Ga-derived electron pockets with a large nearly free-electron Fermi surface that closely approaches the Dirac points of the graphene overlayer.

3.
Nature ; 578(7793): 75-81, 2020 02.
Artigo em Inglês | MEDLINE | ID: mdl-32025010

RESUMO

Complex-oxide materials exhibit a vast range of functional properties desirable for next-generation electronic, spintronic, magnetoelectric, neuromorphic, and energy conversion storage devices1-4. Their physical functionalities can be coupled by stacking layers of such materials to create heterostructures and can be further boosted by applying strain5-7. The predominant method for heterogeneous integration and application of strain has been through heteroepitaxy, which drastically limits the possible material combinations and the ability to integrate complex oxides with mature semiconductor technologies. Moreover, key physical properties of complex-oxide thin films, such as piezoelectricity and magnetostriction, are severely reduced by the substrate clamping effect. Here we demonstrate a universal mechanical exfoliation method of producing freestanding single-crystalline membranes made from a wide range of complex-oxide materials including perovskite, spinel and garnet crystal structures with varying crystallographic orientations. In addition, we create artificial heterostructures and hybridize their physical properties by directly stacking such freestanding membranes with different crystal structures and orientations, which is not possible using conventional methods. Our results establish a platform for stacking and coupling three-dimensional structures, akin to two-dimensional material-based heterostructures, for enhancing device functionalities8,9.

4.
ACS Nano ; 13(9): 9781-9810, 2019 Sep 24.
Artigo em Inglês | MEDLINE | ID: mdl-31430131

RESUMO

Since the isolation of graphene in 2004, there has been an exponentially growing number of reports on layered two-dimensional (2D) materials for applications ranging from protective coatings to biochemical sensing. Due to the exceptional, and often tunable, electrical, optical, electrochemical, and physical properties of these materials, they can serve as the active sensing element or a supporting substrate for diverse healthcare applications. In this review, we provide a survey of the recent reports on the applications of 2D materials in biosensing and other emerging healthcare areas, ranging from wearable technologies to optogenetics to neural interfacing. Specifically, this review provides (i) a holistic evaluation of relevant material properties across a wide range of 2D systems, (ii) a comparison of 2D material-based biosensors to the state-of-the-art, (iii) relevant material synthesis approaches specifically reported for healthcare applications, and (iv) the technological considerations to facilitate mass production and commercialization.

5.
Nanoscale ; 11(33): 15440-15447, 2019 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-31393495

RESUMO

Intercalation of atomic species through epitaxial graphene on silicon carbide began only a few years following its initial report in 2004. The impact of intercalation on the electronic properties of the graphene is well known; however, the intercalant itself can also exhibit intriguing properties not found in nature. This realization has inspired new interest in epitaxial graphene/silicon carbide (EG/SiC) intercalation, where the scope of the technique extends beyond modulation of graphene properties to the creation of new 2D forms of 3D materials. The mission of this minireview is to provide a concise introduction to EG/SiC intercalation and to demonstrate a simplified approach to EG/SiC intercalation. We summarize the primary techniques used to achieve and characterize EG/SiC intercalation, and show that thermal evaporation-based methods can effectively substitute for more complex synthesis techniques, enabling large-scale intercalation of non-refractory metals and compounds including two-dimensional silver (2D-Ag) and gallium nitride (2D-GaNx).

6.
ACS Appl Mater Interfaces ; 10(47): 40831-40837, 2018 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-30384598

RESUMO

The utilization of alkali salts, such as NaCl and KI, has enabled the successful growth of large single domain and fully coalesced polycrystalline two-dimensional (2D) transition-metal dichalcogenide layers. However, the impact of alkali salts on photonic and electronic properties is not fully established. In this work, we report alkali-free epitaxy of MoS2 on sapphire and benchmark the properties against alkali-assisted growth of MoS2. This study demonstrates that although NaCl can dramatically increase the domain size of monolayer MoS2 by 20 times, it can also induce strong optical and electronic heterogeneities in as-grown, large-scale films. This work elucidates that utilization of NaCl can lead to variation in growth rates, loss of epitaxy, and high density of nanoscale MoS2 particles (4 ± 0.7/µm2). Such phenomena suggest that alkali atoms play an important role in Mo and S adatom mobility and strongly influence the 2D/sapphire interface during growth. Compared to alkali-free synthesis under the same growth conditions, MoS2 growth assisted by NaCl results in >1% tensile strain in as-grown domains, which reduces photoluminescence by ∼20× and degrades transistor performance.

7.
Nanotechnology ; 29(47): 47LT02, 2018 Nov 23.
Artigo em Inglês | MEDLINE | ID: mdl-30207301

RESUMO

The experimental realization of two-dimensional (2D) gallium nitride (GaN) has enabled the exploration of 2D nitride materials beyond boron nitride. Here we demonstrate one possible pathway to realizing ultra-thin nitride layers through a two-step process involving the synthesis of naturally layered, group-III chalcogenides (GIIIC) and subsequent annealing in ammonia (ammonolysis) that leads to an atomic-exchange of the chalcogen and nitrogen species in the 2D-GIIICs. The effect of nitridation differs for gallium and indium selenide, where gallium selenide undergoes structural changes and eventual formation of ultra-thin GaN, while indium selenide layers are primarily etched rather than transformed by nitridation. Further investigation of the resulting GaN films indicates that ultra-thin GaN layers grown on silicon dioxide act as effective 'seed layers' for the growth of 3D GaN on amorphous substrates.

8.
Nanoscale ; 10(31): 15023-15034, 2018 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-30052245

RESUMO

Two-dimensional materials have shown great promise for implementation in next-generation devices. However, controlling the film thickness during epitaxial growth remains elusive and must be fully understood before wide scale industrial application. Currently, uncontrolled multilayer growth is frequently observed, and not only does this growth mode contradict theoretical expectations, but it also breaks the inversion symmetry of the bulk crystal. In this work, a multiscale theoretical investigation aided by experimental evidence is carried out to identify the mechanism of such an unconventional, yet widely observed multilayer growth in the epitaxy of layered materials. This work reveals the subtle mechanistic similarities between multilayer concentric growth and spiral growth. Using the combination of experimental demonstration and simulations, this work presents an extended analysis of the driving forces behind this non-ideal growth mode, and the conditions that promote the formation of these defects. Our study shows that multilayer growth can be a result of both chalcogen deficiency and chalcogen excess: the former causes metal clustering as nucleation defects, and the latter generates in-domain step edges facilitating multilayer growth. Based on this fundamental understanding, our findings provide guidelines for the narrow window of growth conditions which enables large-area, layer-by-layer growth.

9.
Nano Lett ; 18(3): 1849-1855, 2018 03 14.
Artigo em Inglês | MEDLINE | ID: mdl-29415536

RESUMO

A two-dimensional (2D) heterobilayer system consisting of MoS2 on WSe2, deposited on epitaxial graphene, is studied by scanning tunneling microscopy and spectroscopy at temperatures of 5 and 80 K. A moiré pattern is observed, arising from lattice mismatch of 3.7% between the MoS2 and WSe2. Significant energy shifts are observed in tunneling spectra observed at the maxima of the moiré corrugation, as compared with spectra obtained at corrugation minima, consistent with prior work. Furthermore, at the minima of the moiré corrugation, sharp peaks in the spectra at energies near the band edges are observed for spectra acquired at 5 K. The peaks correspond to discrete states that are confined within the moiré unit cells. Conductance mapping is employed to reveal the detailed structure of the wave functions of the states. For measurements at 80 K, the sharp peaks in the spectra are absent, and conductance maps of the band edges reveal little structure.

10.
Nano Lett ; 18(2): 1049-1056, 2018 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-29342357

RESUMO

A multistep diffusion-mediated process was developed to control the nucleation density, size, and lateral growth rate of WSe2 domains on c-plane sapphire for the epitaxial growth of large area monolayer films by gas source chemical vapor deposition (CVD). The process consists of an initial nucleation step followed by an annealing period in H2Se to promote surface diffusion of tungsten-containing species to form oriented WSe2 islands with uniform size and controlled density. The growth conditions were then adjusted to suppress further nucleation and laterally grow the WSe2 islands to form a fully coalesced monolayer film in less than 1 h. Postgrowth structural characterization demonstrates that the WSe2 monolayers are single crystal and epitaxially oriented with respect to the sapphire and contain antiphase grain boundaries due to coalescence of 0° and 60° oriented WSe2 domains. The process also provides fundamental insights into the two-dimensional (2D) growth mechanism. For example, the evolution of domain size and cluster density with annealing time follows a 2D ripening process, enabling an estimate of the tungsten-species surface diffusivity. The lateral growth rate of domains was found to be relatively independent of substrate temperature over the range of 700-900 °C suggesting a mass transport limited process, however, the domain shape (triangular versus truncated triangular) varied with temperature over this same range due to local variations in the Se/W adatom ratio. The results provide an important step toward atomic level control of the epitaxial growth of WSe2 monolayers in a scalable process that is suitable for large area device fabrication.

11.
ACS Nano ; 12(2): 965-975, 2018 02 27.
Artigo em Inglês | MEDLINE | ID: mdl-29360349

RESUMO

Atomically thin transition metal dichalcogenides (TMDs) are of interest for next-generation electronics and optoelectronics. Here, we demonstrate device-ready synthetic tungsten diselenide (WSe2) via metal-organic chemical vapor deposition and provide key insights into the phenomena that control the properties of large-area, epitaxial TMDs. When epitaxy is achieved, the sapphire surface reconstructs, leading to strong 2D/3D (i.e., TMD/substrate) interactions that impact carrier transport. Furthermore, we demonstrate that substrate step edges are a major source of carrier doping and scattering. Even with 2D/3D coupling, transistors utilizing transfer-free epitaxial WSe2/sapphire exhibit ambipolar behavior with excellent on/off ratios (∼107), high current density (1-10 µA·µm-1), and good field-effect transistor mobility (∼30 cm2·V-1·s-1) at room temperature. This work establishes that realization of electronic-grade epitaxial TMDs must consider the impact of the TMD precursors, substrate, and the 2D/3D interface as leading factors in electronic performance.

12.
Nanoscale ; 10(1): 336-341, 2017 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-29215125

RESUMO

Two and three-dimensional (2D/3D) hybrid materials have the potential to advance communication and sensing technologies by enabling new or improved device functionality. To date, most 2D/3D hybrid devices utilize mechanical exfoliation or post-synthesis transfer, which can be fundamentally different from directly synthesized layers that are compatible with large scale industrial needs. Therefore, understanding the process/property relationship of synthetic heterostructures is priority for industrially relevant material architectures. Here we demonstrate the scalable synthesis of molybdenum disulfide (MoS2) and tungsten diselenide (WSe2) via metal organic chemical vapor deposition (MOCVD) on gallium nitride (GaN), and elucidate the structure, chemistry, and vertical transport properties of the 2D/3D hybrid. We find that the 2D layer thickness and transition metal dichalcogenide (TMD) choice plays an important role in the transport properties of the hybrid structure, where monolayer TMDs exhibit direct tunneling through the layer, while transport in few layer TMDs on GaN is dominated by p-n diode behavior and varies with the 2D/3D hybrid structure. Kelvin probe force microscopy (KPFM), low energy electron microscopy (LEEM) and X-ray photoelectron spectroscopy (XPS) reveal a strong intrinsic dipole and charge transfer between n-MoS2 and p-GaN, leading to a degraded interface and high p-type leakage current. Finally, we demonstrate integration of heterogeneous 2D layer stacks of MoS2/WSe2 on GaN with atomically sharp interface. Monolayer MoS2/WSe2/n-GaN stacks lead to near Ohmic transport due to the tunneling and non-degenerated doping, while few layer stacking is Schottky barrier dominated.

13.
Sci Rep ; 7(1): 16938, 2017 12 05.
Artigo em Inglês | MEDLINE | ID: mdl-29209000

RESUMO

Evaluating and tuning the properties of two-dimensional (2D) materials is a major focus of advancing 2D science and technology. While many claim that the photonic properties of a 2D layer provide evidence that the material is "high quality", this may not be true for electronic performance. In this work, we deconvolute the photonic and electronic response of synthetic monolayer molybdenum disulfide. We demonstrate that enhanced photoluminescence can be robustly engineered via the proper choice of substrate, where growth of MoS2 on r-plane sapphire can yield >100x enhancement in PL and carrier lifetime due to increased molybdenum-oxygen bonding compared to that of traditionally grown MoS2 on c-plane sapphire. These dramatic enhancements in optical properties are similar to those of super-acid treated MoS2, and suggest that the electronic properties of the MoS2 are also superior. However, a direct comparison of the charge transport properties indicates that the enhanced PL due to increased Mo-O bonding leads to p-type compensation doping, and is accompanied by a 2x degradation in transport properties compared to MoS2 grown on c-plane sapphire. This work provides a foundation for understanding the link between photonic and electronic performance of 2D semiconducting layers, and demonstrates that they are not always correlated.

14.
Sci Adv ; 3(10): e1701661, 2017 10.
Artigo em Inglês | MEDLINE | ID: mdl-29062892

RESUMO

Integration of transition metal dichalcogenides (TMDs) into next-generation semiconductor platforms has been limited due to a lack of effective passivation techniques for defects in TMDs. The formation of an organic-inorganic van der Waals interface between a monolayer (ML) of titanyl phthalocyanine (TiOPc) and a ML of MoS2 is investigated as a defect passivation method. A strong negative charge transfer from MoS2 to TiOPc molecules is observed in scanning tunneling microscopy. As a result of the formation of a van der Waals interface, the ION/IOFF in back-gated MoS2 transistors increases by more than two orders of magnitude, whereas the degradation in the photoluminescence signal is suppressed. Density functional theory modeling reveals a van der Waals interaction that allows sufficient charge transfer to remove defect states in MoS2. The present organic-TMD interface is a model system to control the surface/interface states in TMDs by using charge transfer to a van der Waals bonded complex.

15.
ACS Appl Mater Interfaces ; 9(34): 29255-29264, 2017 Aug 30.
Artigo em Inglês | MEDLINE | ID: mdl-28805363

RESUMO

To fabricate practical devices based on semiconducting two-dimensional (2D) materials, the source, channel, and drain materials are exposed to ambient air. However, the response of layered 2D materials to air has not been fully elucidated at the molecular level. In the present report, the effects of air exposure on transition metal dichalcogenides (TMD) and metal dichalcogenides (MD) are studied using ultrahigh-vacuum scanning tunneling microscopy (STM). The effects of a 1-day ambient air exposure on MBE-grown WSe2, chemical vapor deposition (CVD)-grown MoS2, and MBE SnSe2 are compared. Both MBE-grown WSe2 and CVD-grown MoS2 display a selective air exposure response at the step edges, consistent with oxidation on WSe2 and adsorption of hydrocarbon on MoS2, while the terraces and domain/grain boundaries of both TMDs are nearly inert to ambient air. Conversely, MBE-grown SnSe2, an MD, is not stable in ambient air. After exposure in ambient air for 1 day, the entire surface of SnSe2 is decomposed to SnOx and SeOx, as seen with X-ray photoelectron spectroscopy. Since the oxidation enthalpy of all three materials is similar, the data is consistent with greater oxidation of SnSe2 being driven by the weak bonding of SnSe2.

16.
ACS Appl Mater Interfaces ; 9(29): 25006-25013, 2017 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-28715196

RESUMO

Poly(vinyl alcohol) (PVA) and LiClO4, a solid polymer electrolyte with a glass transition temperature (Tg) of 80 °C, is used to electrostatically gate graphene field-effect transistors. The ions in PVA:LiClO4 are drifted into place by field-effect at T > Tg, providing n- or p-type doping, and when the device is cooled to room temperature, the polymer mobility and, hence ion mobility are arrested and the electric double layer (EDL) is "locked" into place in the absence of a gate bias. Unlike other electrolytes used to gate two-dimensional devices for which the Tg, and therefore the "locking" temperature, is well below room temperature, the electrolyte demonstrated in this work provides a route to achieve room-temperature EDL stability. Specifically, a 6 orders of magnitude increase in the room temperature EDL retention time is demonstrated over the commonly used electrolyte, poly(ethylene oxide) (PEO) and LiClO4. Hall measurements confirm that large sheet carrier densities can be achieved with PVA:LiClO4 at top gate programming voltages of ±2 V (-6.3 ± 0.03 × 1013 cm-2 for electrons and 1.6 ± 0.3 × 1014 cm-2 for holes). Transient drain current measurements show that at least 75% of the EDL is retained after more than 4 h at room temperature. Unlike PEO-based electrolytes, PVA:LiClO4 is compatible with the chemicals used in standard photolithographic processes enabling the direct deposition of patterned, metal contacts on the surface of the electrolyte. A thermal instability in the electrolyte is detected by both I-V measurements and differential scanning calorimetry, and FTIR measurements suggest that thermally catalyzed cross-linking may be driving phase separation between the polymer and the salt. Nevertheless, this work highlights how the relationship between polymer and ion mobility can be exploited to tune the state retention time and the charge carrier density of a 2D crystal transistor.

17.
Sci Rep ; 7(1): 4151, 2017 06 23.
Artigo em Inglês | MEDLINE | ID: mdl-28646133

RESUMO

The remarkable electronic properties of layered semiconducting transition metal dichalcogenides (TMDs) make them promising candidates for next-generation ultrathin, low-power, high-speed electronics. It has been suggested that electronics based upon ultra-thin TMDs may be appropriate for use in high radiation environments such as space. Here, we present the effects of irradiation by protons, iron, and silver ions at MeV-level energies on a WSe2/6H-SiC vertical heterostructure studied using XPS and UV-Vis-NIR spectroscopy. It was found that with 2 MeV protons, a fluence of 1016 protons/cm2 was necessary to induce a significant charge transfer from SiC to WSe2, where a reduction of valence band offset was observed. Simultaneously, a new absorption edge appeared at 1.1 eV below the conduction band of SiC. The irradiation with heavy ions at 1016 ions/cm2 converts WSe2 into a mixture of WOx and Se-deficient WSe2. The valence band is also heavily altered due to oxidation and amorphization. However, these doses are in excess of the doses needed to damage TMD-based electronics due to defects generated in common dielectric and substrate materials. As such, the radiation stability of WSe2-based electronics is not expected to be limited by the radiation hardness of WSe2, but rather by the dielectric and substrate.

18.
Nat Nanotechnol ; 12(9): 883-888, 2017 09.
Artigo em Inglês | MEDLINE | ID: mdl-28650442

RESUMO

Monolayer transition metal dichalcogenide crystals, as direct-gap materials with strong light-matter interactions, have attracted much recent attention. Because of their spin-polarized valence bands and a predicted spin splitting at the conduction band edges, the lowest-lying excitons in WX2 (X = S, Se) are expected to be spin-forbidden and optically dark. To date, however, there has been no direct experimental probe of these dark excitons. Here, we show how an in-plane magnetic field can brighten the dark excitons in monolayer WSe2 and permit their properties to be observed experimentally. Precise energy levels for both the neutral and charged dark excitons are obtained and compared with ab initio calculations using the GW-BSE approach. As a result of their spin configuration, the brightened dark excitons exhibit much-increased emission and valley lifetimes. These studies directly probe the excitonic spin manifold and reveal the fine spin-splitting at the conduction band edges.

20.
Sci Rep ; 7: 43214, 2017 02 22.
Artigo em Inglês | MEDLINE | ID: mdl-28225066

RESUMO

Using quantum tunneling of electrons into vibrating surface atoms, phonon oscillations can be observed on the atomic scale. Phonon interference patterns with unusually large signal amplitudes have been revealed by scanning tunneling microscopy in intercalated van der Waals heterostructures. Our results show that the effective radius of these phonon quasi-bound states, the real-space distribution of phonon standing wave amplitudes, the scattering phase shifts, and the nonlinear intermode coupling strongly depend on the presence of defect-induced scattering resonance. The observed coherence of these quasi-bound states most likely arises from phase- and frequency-synchronized dynamics of all phonon modes, and indicates the formation of many-body condensate of optical phonons around resonant defects. We found that increasing the strength of the scattering resonance causes the increase of the condensate droplet radius without affecting the condensate fraction inside it. The condensate can be observed at room temperature.

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