The Raman shift, broadening, and relative Raman intensities of bilayer graphene are computed as functions of the electron concentration. We include dynamic effects for the phonon frequencies and we consider the gap induced in the band structure of bilayer graphene by an external electric field. We show that from the analysis of the Raman spectra of gated bilayer graphene it is possible to quantitatively identify the amount of charges coming from the atmosphere and from the substrate. These findings suggest that Raman spectroscopy of bilayer graphene can be used to characterize the electrostatic environment of few-layers graphene.
We investigate the effects of lattice disorders on the low frequency Raman spectra of bilayer MoS2. The bilayer MoS2 was subjected to defect engineering by irradiation with a 30 keV He+ ion beam and the induced morphology change was characterized by transmission electron microscopy. With increasing ion dose the shear mode is observed to redshift and it is also suppressed sharply compared to other Raman peaks. We use the linear chain model to describe the changes to the Raman spectra. Our observations suggest that crystallite size and orientation are the dominant factors behind the changes to t…
The most important bands for the evaluation of strain in graphene (the 2D and 2D prime modes) are investigated. It is shown that for Bernal-stacked bilayers, the two-phonon Raman features have three different components that can be assigned to processes originating solely from the top graphene layer, bottom graphene layer, and from a combination of processes originating both from the top and bottom layers. The individual components of the 2D and 2D prime modes are disentangled. The reported results enable addressing the properties of individual graphene layers in isotopically labelled turbostr…
Magnetic-Field-Dependent Raman Scattering in Multiferroic Bilayer Films: Evidence for Stress-Mediated Magnetoelectric Coupling
首次报道了Pb（Zr，Ti）O_3-CoFe_2 O_4双层多铁体系的磁场相关拉曼散射研究。纳米双层膜的声子频率随着磁场的变化而发生明显的变化，而单层Pb（Zr，Ti）O3膜则没有这种变化。CoFe 2 O 4层的磁致伸缩产生机械传递到Pb（Zr，Ti）O3层的应力，导致模式变化。观察到的磁场诱导软化的软模式的Pb（Zr，Ti）O3层承担着一个惊人的相似的直接磁电输出的双层，提供证据的应力介导的磁电耦合机制的多铁性双层。
Twisted van der Waals heterostructures unravel a new platform to study strongly correlated quantum phases. The interlayer coupling in these heterostructures is sensitive to twist angles ($θ$) and key to controllably tune several exotic properties. Here, we demonstrate a systematic evolution of the interlayer coupling strength with twist angle in bilayer $\mathrm{MoS_{2}}$ using a combination of Raman spectroscopy and classical simulations. At zero doping, we show a \textit{monotonic} increment of the separation between the $\mathrm{A_{1g}}$ and $\mathrm{E^{1}_{2g}}$ mode frequencies as $θ$ dec…
Comment on "Raman spectra of misoriented bilayer graphene"
在最近的论文[Phys.Rev.B78，113407（2008）]中，Poncharal等人研究了取向错误的双层石墨烯的拉曼光谱。他们发现，相对于单层石墨烯，错位石墨烯的2D带的蓝移显示出对激发激光能量的强烈依赖性。蓝移随激发能的降低而增加。这一发现与我们对折叠/错误取向的石墨烯的费米速度降低的解释相矛盾[Ni et al.Phys.Rev.B77，235403（2008）]。在这篇评论中，我们提出了更多的实验结果，从我们的小组以及从其他人表明，蓝移确实只是弱依赖于激发能。因此，我们认为，我们的解释的二维蓝移的折叠石墨烯由于费米速度的降低仍然是有效的。
The vibrational properties of twisted bilayer graphene (tBLG) show complex features, due to the intricate energy landscape of its low-symmetry configurations. A machine learning-based approach is developed to provide a continuous model between the twist angle and the simulated Raman spectra of tBLGs. Extracting the structural information of the twist angle from Raman spectra corresponds to solving a complicated inverse problem. Once trained, the machine learning regressors (MLRs) quickly provide predictions without human bias and with an average of 98% of the data variance being explained by t…
The temperature evolution of the resonant Raman scattering from high-quality bilayer 2H-MoS$_{2}$ encapsulated in hexagonal BN flakes is presented. The observed resonant Raman scattering spectrum as initiated by the laser energy of 1.96 eV, close to the A excitonic resonance, shows rich and distinct vibrational features that are otherwise not observed in non-resonant scattering. The appearance of 1$^{st}$ and 2$^{nd}$ order phonon modes is unambiguously observed in a broad range of temperatures from 5 K to 320 K. The spectrum includes the Raman-active modes, $i.e.$ E$_\textrm{1g}^{2}$($Γ$) and…
Van der Waals layered materials with well-defined twist angles between the crystal lattices of individual layers have attracted increasing attention due to the emergence of unexpected material properties. As many properties critically depend on the exact twist angle and its spatial homogeneity, there is a need for a fast and non-invasive characterization technique of the local twist angle, to be applied preferably right after stacking. We demonstrate that confocal Raman spectroscopy can be utilized to spatially map the twist angle in stacked bilayer graphene for angles between 6.5° and 8° when…
With the increasing interest in twisted bilayer graphene (tBLG) of the past years, fast, reliable, and non-destructive methods to precisely determine the twist angle are required. Raman spectroscopy potentially provides such method, given the large amount of information about the state of the graphene that is encoded in its Raman spectrum. However, changes in the Raman spectra induced by the stacking order can be very subtle, thus making the angle identification tedious. In this work, we propose the use of machine learning (ML) analysis techniques for the automated classification of the Raman …
University of Warsaw（华沙大学）；Wrocław University of Science and Technology（弗罗茨瓦夫科技大学）；Peking University Shenzhen Graduate School（北京大学深圳研究生院）；CNRS（法国国家科学研究中心）
In 1H monolayer transition metal dichalcogenide, the inversion symmetry is broken, while the reflection symmetry is maintained. On the contrary, in the bilayer, the inversion symmetry is restored, but the reflection symmetry is broken. As a consequence of these contrasting symmetries, here we show that bilayer WS$_2$ exhibits a quantum confined Stark effect (QCSE) that is linear with the applied out-of-plane electric field, in contrary to a quadratic one for a monolayer. The interplay between the unique layer degree of freedom in the bilayer and the field driven partial inter-conversion betwee…
Twisted 2D bilayer materials are created by artificial stacking of two monolayer crystal networks of 2D materials with a desired twisting angle $θ$. The material forms a moiré superlattice due to the periodicity of both top and bottom layer crystal structure. The optical properties are modified by lattice reconstruction and phonon renormalization, which makes optical spectroscopy an ideal characterization tool to study novel physics phenomena. Here, we report a Raman investigation on a full period of the twisted bilayer (tB) WSe$_2$ moiré superlattice (\textit i.e. 0° $\leq θ\leq$ 60°). We obs…
Twisted bilayer graphene (TBLG) has emerged as an exciting new material with tunable electronic properties ranging from superconductivity to correlated insulating phases. But current methods of fabrication and identification of TBLG are painstaking and laborious. In this work, we combine Raman spectroscopy with the Gaussian mixture model (GMM) data clustering algorithm to identify areas with particular twist angles, from a TBLG sample with a mixture of orientations. We present two approaches to this cluster analysis: training the GMM on Raman parameters returned by peak fits, and on full Raman…
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…
The twist angle between the monolayers in van der Waals heterostructures provides a new degree of freedom in tuning material properties. We compare the optical properties of WSe2 homobilayers with 2H and 3R stacking using photoluminescence, Raman spectroscopy, and reflectance contrast measurements under ambient and cryogenic temperatures. Clear stacking- dependent differences are evident for all temperatures, with both photoluminescence and reflectance contrast spectra exhibiting a blue shift in spectral features in 2H compared to 3R bilayers. Density functional theory (DFT) calculations eluci…
We describe how the out-of-plane dielectric polarizability of monolayer graphene influences the electrostatics of bilayer graphene -- both Bernal (BLG) and twisted (tBLG). We compare the polarizability value computed using density functional theory with the output from previously published experimental data on the electrostatically controlled interlayer asymmetry potential in BLG and data on the on-layer density distribution in tBLG. We show that monolayers in tBLG are described well by polarizability $α_{exp} = 10.8 \unicode{x212B}^3$ and effective out-of-plane dielectric susceptibility $ε_z …
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…
We investigate the electron-hole two-stream instability (or Coulomb drag) in intrinsic bilayer graphene in the hydrodynamic regime, accounting for the effects of temperature, initial drift velocity, magnetic field, and collisions. The threshold drift speed for the onset of instabilities is of the order of the thermal velocity of the carriers. We put in evidence an unprecedented purely electrostatic mechanism leading to current relaxation, giving rise to a well-defined dc longitudinal conductivity $\propto T^{3/2}$. Due to competition between electrostatic and collisional processes, two distinc…
Isolating the natural edges of bilayer graphene in gate-defined mesoscopic devices
University of Basel（巴塞尔大学）；Advanced Materials Laboratory, National Institute for Materials Science（国家材料科学研究所先进材料实验室）；Solid State Physics Laboratory, ETH Zürich（苏黎世联邦理工学院固体物理实验室）；Swiss Nanoscience Institute（瑞士纳米科学研究所）
Correct defect quantification in graphene samples is crucial both for fundamental and applied re-search. Raman spectroscopy represents the most widely used tool to identify defects in graphene. However, despite its extreme importance the relation between the Raman features and the amount of defects in multilayered graphene samples has not been experimentally verified. In this study we intentionally created defects in single layer graphene, turbostratic bilayer graphene and Bernal stacked bilayer graphene by oxygen plasma. By employing isotopic labelling, our study reveals substantial differenc…
Among the most common few-layers transition metal dichalcogenides (TMDs), WSe2 is the most challenging material from the lattice dynamics point of view. Indeed, for a long time the main two phonon modes (A1g and E12g) have been wrongly assigned. In the last few years, these two modes have been properly interpreted, and their quasi-degeneracy in the monolayer has been used for its identification. In this work, we show that this approach has a limited validity and we propose an alternative, more general approach, based on multi-phonon bands. Moreover, we show and interpret all the peaks (about 4…
Disorder-induced symmetry breaking in moiré bands of marginally twisted bilayer MoS$_2$
Monash University（蒙纳士大学）；University of Pennsylvania（宾夕法尼亚大学）；University of Antwerp（安特卫普大学）；John A. Paulson School of Engineering and Applied Sciences, Harvard University（哈佛大学约翰·A·保尔森工程与应用科学学院）；Nanyang Technological University Singapore（新加坡南洋理工大学）；Washington University（华盛顿大学）；Universidad Autónoma de Madrid（马德里自治大学）
Graphene is an ideal platform to study the coherence of quantum interference pathways by tuning doping or laser excitation energy. The latter produces a Raman excitation profile that provides direct insight into the lifetimes of intermediate electronic excitations and, therefore, on quantum interference, which has so far remained elusive. Here, we control the Raman scattering pathways by tuning the laser excitation energy in graphene doped up to 1.05eV, above what achievable with electrostatic doping. The Raman excitation profile of the G mode indicates its position and full width at half maxi…
Wannier Function Approach to Realistic Coulomb Interactions in Layered Materials and Heterostructures
我们介绍了一种方法来获得现实的库仑相互作用项在独立的层状材料和垂直异质结构从从头计算模拟相应的散装材料。为此，我们建立了一个组合的计算框架内的约束随机相位近似，Wannier函数表示的库仑矩阵元素在一些低能量希尔伯特空间和连续介质静电，我们称之为Wannier函数连续静电（WFCE）。对于单层和双层石墨烯，我们再现完整的从头计算的库仑矩阵元素的精度为$0.2$ eV或更好。我们表明，在双层石墨烯中的现实库仑相互作用可以通过不同的电介质和金属环境在eV尺度上进行操纵。与[M. M. Scherer等人，Phys.Rev.B85，235408（2012）]提出双层石墨烯的电子基态是层状反铁磁体，并且令人惊讶地保持不受库仑相互作用中的这些强变化的影响。
