The optical emission efficiency of two dimensional layered transition metal dichalcogenides (TMDs) is one of the most important parameter that affects their optoelectronic performance. Optimization of growth parameters of chemical vapor deposition (CVD) to achieve optoelectronics-grade quality TMDs is therefore highly desirable. Here, we present a systematic photoluminescence (PL) spectroscopic approach to assess the intrinsic optical and crystalline quality of CVD grown MoS2. We suggest that the intensity ratio between PL measured in air and vacuum could be used as an effective way to monitor the intrinsic optical quality of CVD MoS2. Low temperature PL measurements are also used to evaluate the structural defects in MoS2 by defect-associated bound exciton emission, which is well correlated with the field effect carrier mobilities of MoS2 grown at different temperatures. This work therefore provides a sensitive, noninvasive method to characterize the optical properties of TMDs, allow tuning of growth parameters for the development of optoelectronic devices.
In this work, the effect of the ion fluence-dependent defect formation on the modification of surface electronic and optical properties of graphene has been investigated. The chemical vapor deposited (CVD) graphene was irradiated with swift heavy ion (SHI) (70 MeV Si+5) beam at different fluence to study the defect formation mechanism and the role of it in modulating its surface electronic property such as work function. At low ion dose, acceptor doping via vacancy creation was observed; whereas dense electronic excitation dominated extended defects was realized at higher dose, which subsequen…
Weyl semimetal Td-phase WTe2 possesses the spin-resolved band structure with strong spin-orbit coupling, holding promises as a useful spin source material. The noncentrosymmetric crystalline structure of Td-WTe2 endows the generation of the out-of-plane polarized spin, which is of great interest in magnetic memory applications. Previously, WTe2 was explored in spin devices based on mechanically exfoliated single crystal flakes with a size of micrometers. For practical spintronics applications, it is highly desirable to implement wafer-scale thin films. In this work, we utilize centimeter-scale…
Notwithstanding numerous density functional studies on the chemically induced transformation of multilayer graphene into a diamond-like film, a comprehensive convincing experimental proof of such a conversion is still lacking. We show that the fluorination of graphene sheets in Bernal (AB)-stacked bilayer graphene (AB-BLG) grown by chemical vapor deposition on a single crystal CuNi(111) surface triggers the formation of interlayer carbon-carbon bonds, resulting in a fluorinated diamond monolayer (F-diamane). Induced by fluorine chemisorption, the phase transition from AB-BLG to single layer di…
The electronic spins of the nitrogen-vacancy centers (NV centers) in Chemical-Vapor-Deposition (CVD) grown diamonds form ideal probes of magnetic fields and temperature, as well as promising qu-bits for quantum information processing. Studying and controlling the magnetic environment of NV centers in such high purity crystals is thus essential for these applications. We demonstrate optical detection of paramagnetic species, such as hydrogen-related complexes, in a CVD-grown diamond. The resonant transfer of the NV centers' polarized electronic spins to the electronic spins of these species gen…
Tailoring the interlayer twist angle of bilayer graphene (BLG) has a significant influence on its electronic properties, including superconductivity, topological transitions, ferromagnetic states and correlated insulating states. These exotic electronic properties are sensitively dependent on the work functions of bilayer graphene samples. Here, the twisted angle-dependent work functions of CVD-grown twisted bilayer graphene (tBLG) are detailed investigated by Kelvin Probe Force Microscopy (KPFM) in combination with Raman spectra. The thickness-dependent surface potentials of Bernal-stacked mu…
Using temperature dependent photoluminescence (PL), polarization resolved PL and Raman spectroscopy, we investigate the effect of in situ vacuum annealing as well as the relaxation of strain on the luminescence and the valley polarization properties of large area strictly monolayer (1L)-MoS$_2$, grown on sapphire and SiO$_2$/Si substrates by a microcavity based chemical vapor deposition (CVD) technique. The study shows that the strain as well as the physisorption of air molecules at the sulfur vacancy ($V_S$) sites play key roles in governing the optical quality of CVD grown 1L-MoS$_2$. Remova…
The results of magneto-optical spectroscopy investigations of excitons in a CVD grown monolayer of WSe2 encapsulated in hexagonal boron nitride are presented. The emission linewidth for the 1s state is of 4:7 meV, close to the narrowest emissions observed in monolayers exfoliated from bulk material. The 2s excitonic state is also observed at higher energies in the photoluminescence spectrum. Magneto-optical spectroscopy allows for the determination of the g-factors and of the spatial extent of the excitonic wave functions associated with these emissions. Our work establishes CVD grown monolaye…
Silicon-based quantum bits with electron spins in quantum dots or nuclear spins on dopants are serious contenders in the race for quantum computation. Added to process integration maturity, the lack of nuclear spins in the most abundant $^{28}$silicon isotope host crystal for qubits is a major asset for this silicon quantum technology. We have grown $^{28}$silicon epitaxial layers (epilayers) with an isotopic purity greater than 99.992 % on 300mm natural abundance silicon crystals. The quality of the mono-crystalline isotopically purified epilayer conforms to the same drastic quality requireme…
We present a comprehensive temperature dependent Raman measurements for horizontally aligned CVD grown layered MoS2 in a temperature range of 4 to 330 K under resonance condition. Our analysis of temperature dependent phonon frequency shift and linewidth suggest a finite role of three and four phonon anharmonic effect. We observed Davydov splitting of the out-of-plane (A1g ) and in-plane (E12g ) modes, attributed to the weak interlayer interaction, and reflected in the appearance of additional modes with decreasing temperature for both 3 layers and few layers system. We also observed that the …
Through a combination of monitoring the Raman spectral characteristics of 2D materials grown on copper catalyst layers, and wafer scale automated detection of the fraction of transferred material, we reproducibly achieve transfers with over 97.5% monolayer hexagonal boron nitride and 99.7% monolayer graphene coverage, for up to 300 mm diameter wafers. We find a strong correlation between the transfer coverage obtained for graphene and the emergence of a lower wavenumber 2D- peak component, with the concurrent disappearance of the higher wavenumber 2D+ peak component during oxidation of the cat…
Although chemical vapor deposition (CVD) is one of the preferred routes to synthetic diamond crystals, a full knowledge of the point defects produced during growth is still incomplete. Here we exploit the charge and spin properties of nitrogen-vacancy (NV) centers in type-1b CVD diamond to expose an optically and magnetically dark point defect, so far virtually unnoticed despite an abundance comparable to (if not greater than) that of substitutional nitrogen. Indirectly-detected photo-luminescence spectroscopy indicates a donor state 1.6 eV above the valence band, although the defect's microsc…
We show the emergence of fractional quantum Hall states in dry-transferred chemical vapor deposition (CVD) derived graphene assembled into heterostructures for magnetic fields from below 3 T to 35 T. Effective composite-fermion filling factors up to $ν^* = 4$ are visible and higher order composite-fermion states (with four flux quanta attached) start to emerge at the highest fields. Our results show that the quantum mobility of CVD-grown graphene is comparable to that of exfoliated graphene and, more specifically, that the $p/3$ fractional quantum Hall states have energy gaps of up to 30 K, we…
Method for Transferring High-Mobility CVD-Grown Graphene with Perfluoropolymers
使用无定形聚合物通过化学气相沉积（CVD）生长的石墨烯的转移代表了用于石墨烯基电子器件制造的广泛实施的方法。然而，最常用的聚合物聚甲基丙烯酸甲酯（PMMA）会在石墨烯上留下残留物，从而限制了移动性。在这里，我们报告了一种石墨烯转移和图案化的方法，该方法采用全氟聚合物-Hyronium-作为转移手柄，并保护石墨烯免受光刻胶或其他聚合物的污染。以这种方式转移到LaAlO $_3$ /SrTiO $_3$异质结构上的CVD生长的石墨烯在原子上是干净的，在2 K下在狄拉克点附近具有高迁移率（~ 30，000 cm $^2$ V $^{-1}$ s $^{-1}$）和清晰的量化霍尔和磁阻。局部控制的LaAlO $_3$ /SrTiO $_3$界面金属-绝缘体过渡-通过石墨烯-保留与此转移方法。全氟聚合物（诸如Hyplane）与CVD生长的石墨烯和其他2D材料的使用可以容易地与其他聚合物或光致抗蚀剂一起实施。
Raman spectroscopic characterization of stacking configuration and interlayer coupling of twisted multilayer graphene grown by chemical vapor deposition
Effects of annealing on chemical vapor deposited graphene are investigated via a weak localization magnetoresistance measurement. Annealing at \SI{300}{\celsius} in inert gases, a common cleaning procedure for graphene devices, is found to raise the dephasing rate significantly above the rate from electron-electron interactions, which would otherwise be expected to dominate dephasing at 4 K and below. This extra dephasing is apparently induced by local magnetic moments activated by the annealing process, and depends strongly on the backgate voltage applied.
Graphene layers grown by chemical vapour deposition (CVD) method and transferred from Cu-foils to the oxidized Si-substrates were investigated by spectroscopic ellipsometry (SE), Raman and X-Ray Photoelectron Spectroscopy (XPS) methods. The optical properties of transferred CVD graphene layers do not always correspond to the ones of the exfoliated graphene due to the contamination from the chemicals used in the transfer process. However, the real thickness and the mean properties of the transferred CVD graphene layers can be found using ellipsometry if a real thickness of the SiO2 layer is tak…
Improved topological conformity enhances heat conduction across metal contacts on transferred graphene
转移的石墨烯（trG）上的金属接触的热导率可以显着降低从原生石墨烯（grG）上的类似接触的固有值，由于增加的粗糙度，残留物，氧化物和空隙的额外电阻。在本文中，我们比较了Al/trG/Cu界面的热导率（G）与Al/grG/Cu界面的热导率，以了解转移石墨烯上金属接触的热传递。我们的样品是通过化学气相沉积（CVD）在Cu箔上生长的多晶石墨烯和CVD生长的石墨烯转移到蒸发的Cu薄膜上。我们发现，对于生长的CVD石墨烯的Al/grG/Cu界面，在室温下G = 31 MW m ^{-2} K ^{-1}，比Al/Cu界面低两个数量级。对于大多数在Cu膜上转移的石墨烯，G = 20 MW m ^{-2} K ^{-1}，比生长的CVD石墨烯低35%。我们仔细排除了残留物，原生氧化物和界面粗糙度的贡献，并将生长和转移的CVD石墨烯的热导率的差异归因于石墨烯对Cu衬底的不同程度的一致性。我们发现，50%的接触面积仅使热导率降低了35%，这表明在石墨烯界面处的空隙中发生了少量的热传递。我们通过在300 ° C下退火样品成功地改善了转移石墨烯与衬底的一致性，从而将转移石墨烯的热导率提高到本征值。从Al/trG/Cu和Al/grG/Cu界面的G的温度依赖性测量，我们还证实了声子是金属/石墨烯/金属界面上的主要热载体，尽管石墨烯中诱导的载流子浓度为3 × 10 ^{12} cm ^{-2}。
Direct integration of ferroelectric Hf0.5Zr0.5O2 (HZO) on the inert surface of graphene is challenging. Here, using nucleation layers to promote atomic layer deposition of HZO was investigated. Different metals were deposited as nucleation layers via dc sputtering. Ta, which oxidizes in air to form a sub-stoichiometric oxide, was compared to Pt, which offers a more stable electrode. For thicker interlayers, Ta leads to unstable switching behavior of the HZO film. Conversely, at smaller thicknesses, a higher Pr can be achieved with an oxidized Ta interlayer. In both cases, Pt offers higher endu…
Combining MoS$_2$ monolayers to form multilayers allows to access new functionalities. In this work, we examine the correlation between the stacking order and the interlayer coupling of valence states in MoS$_2$ homobilayer samples grown by chemical vapor deposition (CVD) and artificially stacked bilayers from CVD monolayers. We show that hole delocalization over the bilayer is allowed in 2H stacking and results in strong interlayer exciton absorption and also in a larger A-B exciton separation as compared to 3R bilayers, where both holes and electrons are confined to the individual layers. Co…
Probing phonons, quasi-particle excitations and their coupling has enriched our understanding of these 2D materials and proved to be crucial for developing their potential applications. Here, we report comprehensive temperature, 4-330 K, and polarization-dependent Raman measurements on mono and bilayer MoSe2. Phonon's modes up to fourth-order are observed including forbidden Raman and IR modes, understood considering Frohlich mechanism of exciton-phonon coupling. Most notably, anomalous variations in the phonon linewidths with temperature pointed at the significant role of electron-phonon coup…
We report on the study of optical properties of mist CVD grown alpha Gallium oxide with the observation of excitonic absorption in spectral responsivity measurements. 163 nm of Gallium oxide was grown on sapphire using Gallium acetylacetonate as the starting solution at a substrate temperature of 450 deg C. The film was found to be crystalline and of alpha phase with an on axis full width at half maximum of 92 arcsec as confirmed from X ray diffraction scans. The Taucs plot extracted from absorption spectroscopy exhibited two transitions in the UV regime at 5.3 eV and 5.6 eV, corresponding to …
Transport in Nanoribbon Interconnects Obtained from Graphene Grown by Chemical Vapor Deposition
我们研究了石墨烯纳米管（GNR）的互连从石墨烯化学气相沉积（CVD）生长。我们报告低场和高场的电气测量在很宽的温度范围内，从1.7到900 K。室温迁移率在100至500 cm 2/V/s的范围内，与来自剥离的石墨烯的GNR相当，这表明体缺陷或晶界在小于CVD石墨烯微晶尺寸的器件中几乎不起作用。在高电场下，峰值电流密度受到焦耳加热的限制，但少量的热工程使我们能够达到约2 x 10^9 A/cm 2，这是纳米级CVD石墨烯互连的最高报告。在低于~5 K的温度下，短GNR充当量子点，其尺寸与其长度相当，突出了金属接触在限制传输中的作用。我们的研究说明了CVD生长GNRs的机会，同时揭示了可变性和接触作为未来的挑战。
Transport Properties of Graphene Nanoribbon Transistors on Transport Properties of Graphene Nanoribbon Transistors on Chemical-Vapor-Deposition Grown Wafer-Scale Graphene
Monolayer transition metal dichalcogenides (TMDCs) are two-dimensional (2D) materials with many potential applications. Chemical vapour deposition (CVD) is a promising method to synthesize these materials. However, CVD-grown materials generally have poorer quality than mechanically exfoliated ones and contain more defects due to the difficulties in controlling precursors' distribution and concentration during growth where solid precursors are used. Here, we propose to use thiol as a liquid precursor for CVD growth of high quality and uniform 2D MoS2. Atomic-resolved structure characterizations…
Chemical vapor deposition (CVD) allows growing transition metal dichalcogenides (TMDs) over large surface areas on inexpensive substrates. In this work, we correlate the structural quality of CVD grown MoS$_2$ monolayers (MLs) on SiO$_2$/Si wafers studied by high-resolution transmission electron microscopy (HRTEM) with high optical quality revealed in optical emission and absorption from cryogenic to ambient temperatures. We determine a defect concentration of the order of 10$^{13}$ cm$^{-2}$ for our samples with HRTEM. To have access to the intrinsic optical quality of the MLs, we remove the …
Synergetic effect of edge states and point defects to tune ferromagnetism in CVD-grown vertical nanostructured MoS2: A correlation between electronic structure and theoretical study
Graphene has been widely used in the form of micro-flakes to fabricate composite materials with enhanced mechanical properties. Due to the small size of the inclusions and their random orientation within the matrix, the superior mechanical properties of graphene cannot be fully exploited. Recently, attempts have been made to fabricate nanolaminate composites by interleaving large sheets of chemical vapor deposition (CVD) monolayer graphene between thin layers of polymer matrices. However, CVD graphene is inevitably accompanied by wrinkles that are formed in the synthesis process, and it remain…
CVD grown bilayer MoS2 based artificial optoelectronic synapses for arithmetic computing and image recognition applications
Indian Institute of Technology, Bombay（孟买印度理工学院）；National Institute for Materials Science（日本国立材料研究所）；Jackson State University（杰克逊州立大学）；Institute of Physics, Bhubaneswar（布巴内斯瓦尔物理研究所）；Homi Bhabha National Institute（霍米·巴巴国家研究所）
Fe filled carbon nanotubes were synthesized by atmospheric pressure chemical vapor deposition using a simple mixture of iron acetylacetonate with a conventional photoresist and the effect of growth temperature from 550 to 950 °C on Fe filled nanotubes has been studied. Scanning electron microscopy results show that, as the growth temperature increases from 550 to 950 °C, the average diameter of the nanotubes increases while their number density decreases. High resolution transmission electron microscopy along with energy dispersive X-ray investigation shows that the nanotubes have a multi-wall…
We present inverted spin-valves fabricated from CVD-grown bilayer graphene (BLG) that show more than a doubling in device performance at room temperature compared to state-of-the art bilayer graphene spin-valves. This is made possible by a PDMS droplet-assisted full-dry transfer technique that compensates for previous process drawbacks in device fabrication. Gate-dependent Hanle measurements show spin lifetimes of up to 5.8 ns and a spin diffusion length of up to 26 $μ$m at room temperature combined with a charge carrier mobility of $\approx$ 24 000 cm$^{2}$(Vs)$^{-1}$ for the best device. Our…
Defects play a significant role in optical properties of semiconducting two-dimensional transition metal dichalcogenides (TMDCs). In ultra-thin MoSe2, a remarkable feature at ~250 cm-1 in Raman spectra is ascribed to be a defect-related mode. Recent attempts failed to explain the origin of this peak, leaving it being a mystery. Here in this work, we demonstrate that this peak is a Se vacancy induced defect mode. Heat effect and hydrogen etching are two main factors to introduce Se vacancies in CVD process of growing MoSe2. A phonon confinement model can well explain the behaviors of intrinsic …
We report on the fabrication and characterization of high-quality chemical vapor-deposited (CVD) bilayer graphene (BLG). In particular, we demonstrate that CVD-grown BLG can mechanically be detached from the copper foil by an hexagonal boron nitride (hBN) crystal after oxidation of the copper-to-BLG interface. Confocal Raman spectroscopy reveals an AB-stacking order of the BLG crystals and a high structural quality. From transport measurements on fully encapsulated hBN/BLG/hBN Hall bar devices we extract charge carrier mobilities up to 180,000 cm$^2$/(Vs) at 2 K and up to 40,000 cm$^2$/(Vs) at…
