We study hot electron transport in short-channel suspended multilayer graphene devices created by a distinct experimental approach. For devices with semi-transparent contact barriers, a dip of differential conductance (dI/dV) has been observed at source drain bias Vd = 0, along with anomalies at higher Vd likely induced by optical phonon scattering. For devices with low contact barriers, only the dI/dV dip at Vd = 0 is observed, and we find a well-fit logarithmic dependence of dI/dV on both the bias Vd and the temperature T. The logarithmic Vd dependence is explained with the hot electron effect and the logarithmic T dependence could be attributed to the weak-localization in two-dimensions.
We study hot carrier transport under magnetic fields up to 15 T in suspended graphitic multilayers through differential conductance (dI/dV) spectroscopy. Distinct high-energy dI/dV anomalies have been observed and shown to be related to intrinsic phonon-emission processes in graphite. The evolution of such dI/dV anomalies under magnetic fields is further understood as a consequence of inter-Landau level cyclotron-phonon resonance scattering. The observed magneto-phonon effects not only shed light on the physical mechanisms responsible for high-current transport in graphitic systems, but also o…
We report a tunable magnetoresistance (MR) behavior in suspended graphitic multilayers through point defect engineering by ion implantation. We find that ion implantation drastically changes the MR behavior: the linear positive MR in pure graphitic multilayers transforms into a negative MR after introducing significant short-range disorders (implanted boron or carbon atoms), consistent with recent non-Markovian transport theory. Our experiments suggest the important role of the non-Markovian process in the intriguing MR behavior for graphitic systems, and open a new window for understanding tr…
The high-bias electrical transport properties of suspended metallic single-walled carbon nanotubes (SWNTs) are investigated at various temperatures in vacuum, in various gases and when coated with molecular solids. It is revealed that non-equilibrium optical phonon effects in suspended nanotubes decrease as the ambient temperature increases. Gas molecules surrounding suspended SWNTs assist the relaxation of hot phonons and afford enhanced current flow along nanotubes. Molecular solids of carbon dioxide frozen onto suspended SWNTs quench the non-equilibrium phonon effect. The discovery of stron…
Freely suspended metallic single-wall carbon nanotubes (SWNTs) exhibit reduced current carrying ability compared to those lying on substrates, and striking negative differential conductance (NDC) at low electric fields. Theoretical analysis reveals significant self-heating effects including electron scattering by hot non-equilibrium optical phonons. Electron transport characteristics under strong self-heating are exploited for the first time to probe the thermal conductivity of individual SWNTs (~ 3600 Wm-1K-1 at T=300 K) up to ~700 K, and reveal a 1/T dependence expected for Umklapp phonon sc…
High bias electrical transport characteristics of freely suspended metallic single-walled carbon nanotubes (SWNTs) are investigated at 250-400K in vacuum and various gases. Self-heating is exploited to examine the temperature dependence of phonon transport and optical phonon decay in SWNTs. The acoustic phonon thermal conductivity of a SWNT follows ~1/T at high temperatures. Non-equilibrium optical phonon effects in suspended nanotubes decrease as the ambient temperature increases. Gas molecules assist the relaxation of hot optical phonons along the tube length and enable enhanced current flow…
Near infrared pump-probe spectroscopy has been used to measure the ultrafast dynamics of photoexcited charge carriers in monolayer and multilayer graphene. We observe two decay processes occurring on 100 fs and 2 ps timescales. The first is attributed to the rapid electron-phonon thermalisation in the system. The second timescale is found to be due to the slow decay of hot phonons. Using a simple theoretical model we calculate the hot phonon decay rate and show that it is significantly faster in monolayer flakes than in multilayer ones. In contrast to recent claims, we show that this enhanced …
We carried out measurements on nanoelectromechanical systems based on multilayer graphene sheets suspended over trenches in silicon oxide. The motion of the suspended sheets was electrostatically driven at resonance using applied radio-frequency voltages. The mechanical vibrations were detected using a novel form of scanning probe microscopy, which allowed identification and spatial imaging of the shape of the mechanical eigenmodes. In as many as half the resonators measured, we observed a new class of exotic nanoscale vibration eigenmodes not predicted by the elastic beam theory, where the am…
Suspended Bernal-stacked graphene multilayers up to an unexpectedly large thickness exhibit a broken-symmetry ground state, whose origin remains to be understood. Here we show that a finite-temperature second order phase transition occurs in multilayers whose critical temperature Tc increases from 12 K in bilayers to 100 K in heptalayers. A comparison of the data to a phenomenological model inspired by a mean field approach suggests that the transition is associated with the appearance of a self-consistent valley- and spin-dependent staggered potential changing sign from one layer to the next,…
We report the synthesis of AB-stacked multilayer graphene via ambient pressure chemical vapor deposition on Cu foils, and demonstrate a method to construct suspended multilayer graphene devices. In four-terminal geometry, such devices were characterized by hot carrier transport at temperatures down to 240 mK and in magnetic fields up to 14 T. The differential conductance (dI/dV) shows a characteristic dip at longitudinal voltage bias V=0 at low temperatures, indicating the presence of hot electron effect due to a weak electron-phonon coupling. Under magnetic fields, the magnitude of the dI/dV …
We report a method to promote photoluminescence emission in graphene materials by enhancing carrier scattering instead of directly modifying band structure in multilayer reduced graphene oxide (rGO) nanospheres. We intentionally curl graphene layers to form nanospheres by reducing graphene oxide with spherical polymer templates to manipulate the carrier scattering. These nanospheres produce hot-carrier luminescence with more than ten-fold improvement of emission efficiency as compared to planar nanosheets. With increasing excitation power, hot-carrier luminescence from nanospheres exhibits abn…
The development of nanoscale solid-state devices exploiting the promising topological surface states of topological insulator materials requires careful device engineering and improved materials quality. For instance, the introduction of a substrate, device contact or the formation of oxide layers can cause unintentional doping of the material, spoiling the sought-after properties. In support of this, nanoscale imaging tools can provide useful materials information without the need for complex device fabrication. Here we study Bi$_2$Se$_3$ nanoribbons suspended across multiple material stacks …
We study the emission of femtosecond spin current pulses at Fe/Au interfaces. Using optical second harmonic generation we demonstrate the control of pulse shape and duration by varying the emitter thickness and show that it is determined by the parameters of hot electrons emission and the diffusive transport. Using a simple model of electron emission we develop a description of superdiffusive spin transport in Au allowing to extract electron velocity and scattering rates from the experimental data. The importance of carrier multiplication in Fe is demonstrated.
A general expression for calculating the thermal power transferring from 3-dimensional electron to any D-dimensional phonon subsystem is derived in this paper. Electron-phonon coupling in a free suspended cylindrical nanoshell is studied, in which acoustic phonons are confined to quasi-one dimension but electrons behave three-dimensionally. The temperature dependence of the thermal power is obtained analytically, and the low-temperature crossover from the $T^{3}$ to $T^{3}/(1-ν^2)+9γT^4/[T^*(1-ν^2)^{3/2}]$ dependence is also observed. The corresponding quantities are estimated for the material…
Close to charge neutrality, the low-energy properties of high-quality suspended devices based on atomically thin graphene layers are determined by electron-electron interactions. Bernal-stacked layers, in particular, have shown a remarkable even-odd effect with mono- and tri-layers remaining gapless conductors, and bi- and tetra-layers becoming gapped insulators. These observations $-$at odds with the established notion that (Bernal) trilayers and thicker multilayers are semi-metals$-$ have resulted in the proposal of a physical scenario leading to a surprising prediction, namely that even-lay…
The measured frequencies and intensities of different first- and second- order Raman peaks of suspended graphene are used to show that optical phonons and different acoustic phonon polarizations are driven out of local equilibrium inside a sub-micron laser spot. The experimental results are correlated with a first principles-based multiple temperature model to suggest a considerably lower equivalent local temperature of the flexural phonons than those of other phonon polarizations. The finding reveals weak coupling between the flexural modes with hot electrons and optical phonons. Since the ul…
We show that graphene-dielectric multilayers give rise to an unusual tunability of the Casimir-Lifshitz forces, and allow to easily realize completely different regimes within the same structure. Concerning thermal effects, graphene-dielectric multilayers take advantage from the anomalous features predicted for isolated suspended graphene sheets, even though they are considerably affected by the presence of the dielectric substrate. They can also archive the anomalous non-monotonic thermal metallic behavior by increasing the graphene sheets density and their Fermi energy. In addition to a stro…
A suspended layer made up of ferromagnetically ordered spins could be created between two mono/multilayer graphene through intercalation. Stability and electronic structure studies show that, when fluorine molecules are intercalated between two mono/multilayer graphene, their bonds get stretched enough ($\sim$ 1.9$-$2.0 Å) to weaken their molecular singlet eigenstate. Geometrically, these stretched molecules form a pseudoatomized fluorine layer by maintaining a van der Waals separation of $\sim$ 2.6 Å from the adjacent carbon layers. As there is a significant charge transfer from the adjacent …
In van der Waals bonded or rotationally disordered multilayer stacks of two-dimensional (2D) materials, the electronic states remain tightly confined within individual 2D layers. As a result, electron-phonon interactions occur primarily within layers and interlayer electrical conductivities are low. In addition, strong covalent in-plane intralayer bonding combined with weak van der Waals interlayer bonding results in weak phonon-mediated thermal coupling between the layers. We demonstrate here, however, that Coulomb interactions between electrons in different layers of multilayer epitaxial gra…
The excellent electronic and mechanical properties of graphene allow it to sustain very large currents, enabling its incandescence through Joule heating in suspended devices. Although interesting scientifically and promising technologically, this process is unattainable in ambient environment, because graphene quickly oxidises at high temperatures. Here, we take the performance of graphene-based incandescent devices to the next level by encapsulating graphene with hexagonal boron nitride (hBN). Remarkably, we found that the hBN encapsulation provides an excellent protection for hot graphene fi…
We present fabrication and optical characterization of micro-cavities made of multilayer graphene (MLG) cantilevers clamped by metallic electrodes and suspended over Si/Si02 substrate. Graphene cantilevers act as a semi-transparent mirrors closing an air-wedge optical cavity. This simple geometry implements a standing-wave optical resonator along with a mechanical one. Equal thickness interference fringes are observed in both Raman and Rayleigh backscattered signals with interfringe given by their specific wavelength.Chromatic dispersion within the cavity makes possible spatial modulation of g…
Using transient absorption (TA) microscopy as a hot electron thermometer we show disorder-assisted acoustic-phonon supercollisions (SCs) best describes the rate-limiting relaxation step in graphene over a wide range of lattice temperatures ($T_l=$5-300 K), Fermi energies ($E_F=\pm0.35$ eV), and optical probe energies (~0.3 - 1.1 eV). Comparison with simultaneously collected transient photocurrent, an independent hot electron thermometer, confirms the rate-limiting optical and electrical response in graphene are best described by the SC-heat dissipation rate model, $H=A(T^3_e- T^3_l)$. Our data…
We present a proof of concept for a spectrally selective near-infrared (NIR) and short-wavelength infrared (SWIR) photodetector based on nanopatterned multilayer graphene intercalated with FeCl$_3$ (NPMLG-FeCl$_3$), enabling large modulation p-doping of graphene. The localized surface plasmons (LSPs) on the graphene sheets in NPMLG-FeCl$_3$ allow for electrostatic tuning of the photodetection in the NIR and SWIR regimes from $λ=1.3$ $μ$m to 3 $μ$m, which is out of range for nanopatterned monolayer graphene (NPG). Most importantly, the LSPs along with an optical cavity increase the absorbance f…
The interfacial band structures of multilayer systems play a crucial role for the ultrafast charge and spin carrier dynamics at interfaces. Here, we study the energy- and momentum-dependent quasiparticle lifetimes of excited states of a lead monolayer film on Ag(111) prior and after the adsorption of a monolayer of 3,4,9,10-perylene-tetracarboxylic-dianhydride (PTCDA). Using time-resolved two-photon momentum microscopy, we show that the electron dynamics of the bare Pb/Ag(111) bilayer system is dominated by isotropic intraband scattering processes within the quantum well state as well as inter…
We study the infrared dynamics of low-energy atoms interacting with a sample of suspended graphene at finite temperature. The dynamics exhibits severe infrared divergences order by order in perturbation theory as a result of the singular nature of low-energy flexural phonon emission. Our model can be viewed as a two-channel generalization of the independent boson model with asymmetric atom-phonon coupling. This allows us to take advantage of the exact non-perturbative solution of the independent boson model in the stronger channel while treating the weaker one perturbatively. In the low-energy…
We monitor the dynamics of hot carriers in InSe by means of two photons photoelectron spectroscopy (2PPE). The electrons excited by photons of 3.12 eV experience a manifold relaxation. First, they thermalize to the electronic states degenerate with the $\bar M$ valley. Subsequently, the electronic cooling is dictated by Fröhlich coupling with phonons of small momentum transfer. Ab-initio calculations predict cooling rates that are in good agreement with the observed dynamics. We argue that electrons accumulating in states degenerate with the $\bar M$ valley could travel through a multilayer fl…
We describe a theoretical approach for spin-polarized hot-electron transport, as it occurs after excitation by ultrafast optical pulses in heterostructures formed by ferromagnetic and normal metals. We formulate a spin-dependent particle-in-cell model that solves the Boltzmann equation for excited electrons. It includes lifetimes and transmission coefficients as parameters, which can be taken from ab-initio calculations or experiment, and can be easily extended to multilayer systems. This approach is capable of describing electron transport in the ballistic, super-diffusive and diffusive regim…
Being used in optoelectronic devices as ultra-thin conductor-insulator junctions, detailed investigations are needed about how exactly h-BN and graphene hybridize. Here, we present a comprehensive ab initio study of hot carrier dynamics governed by electron-phonon scattering at the h-BN/graphene interface, using graphite (bulk), monolayer and bilayer graphene as benchmark materials. In contrast to monolayer graphene, all multilayer structures possess low-energy optical phonon modes that facilitate carrier thermalization. We find that the h-BN/graphene interface represents an exception with com…
Many promising optoelectronic devices, such as broadband photodetectors, nonlinear frequency converters, and building blocks for data communication systems, exploit photoexcited charge carriers in graphene. For these systems, it is essential to understand, and eventually control, the cooling dynamics of the photoinduced hot-carrier distribution. There is, however, still an active debate on the different mechanisms that contribute to hot-carrier cooling. In particular, the intrinsic cooling mechanism that ultimately limits the cooling dynamics remains an open question. Here, we address this que…
Graphene and its multilayers have attracted considerable interest owing to the fourfold spin and valley degeneracy of their charge carriers, which enables the formation of a rich variety of broken-symmetry states and raises the prospect of controlled phase transitions among them. In especially clean samples, electron-electron interactions were recently shown to produce surprising patterns of symmetry breaking and phase transitions in the integer quantum Hall regime. Although a series of robust fractional quantum Hall states was also recently observed in graphene, their rich phase diagram and t…
Feasibility study of continuous electronic Pomeranchuk cooling with a flavor-degenerate Wigner crystal
RWTH Aachen University（亚琛工业大学）；JARA Fundamentals of Future Information Technology（JARA未来信息技术基础）；nd Institute of Physics, RWTH Aachen University（亚琛工业大学第二物理研究所）；HFML-FELIX（荷兰强磁场实验室FELIX中心）；Radboud University（拉德堡德大学）；Max Planck Institute for the Structure and Dynamics of Matter（马普物质结构与动力学研究所）；Center for Free Electron Laser Science（自由电子激光科学中心）；University of Hamburg（汉堡大学）；I. Institute for Theoretical Physics, University of Hamburg（汉堡大学第一理论物理研究所）；Institute for Theoretical Physics and Astrophysics, University of Würzburg（维尔茨堡大学理论与天体物理研究所）；Peter Grünberg Institute (PGI-9), Forschungszentrum Jülich（于利希研究中心彼得·格林贝格研究所（PGI-9））
