Graphene is conceivably the most nonlinear optoelectronic material we know. Its nonlinear optical coefficients in the terahertz frequency range surpass those of other materials by many orders of magnitude. Here, we show that the terahertz nonlinearity of graphene, both for ultrashort single-cycle and quasi-monochromatic multicycle input terahertz signals, can be efficiently controlled using electrical gating, with gating voltages as low as a few volts. For example, optimal electrical gating enhances the power conversion efficiency in terahertz third-harmonic generation in graphene by about two orders of magnitude. Our experimental results are in quantitative agreement with a physical model of the graphene nonlinearity, describing the time-dependent thermodynamic balance maintained within the electronic population of graphene during interaction with ultrafast electric fields. Our results can serve as a basis for straightforward and accurate design of devices and applications for efficient electronic signal processing in graphene at ultrahigh frequencies.
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 the relaxation dynamics after photoexcitation. These dynamics contain a sub-100 fs thermalization phase, which occurs through carrier–carrier scattering and leads to a carrier distribution with an elevated temperature. This is followed by a picosecond cooling phase, where different phonon systems play a role: graphene acoustic and optical phonons, and substrate phonons. Here, we address the cooling pathway of two technologically relevant systems, both consisting of high-quality graphene with a mobility >10 000 cm 2 V –1 s –1 and environments that do not efficiently take up electronic heat from graphene: WSe 2 -encapsulated graphene and suspended graphene. We study the cooling dynamics using ultrafast pump–probe spectroscopy at room temperature. Cooling via disorder-assisted acoustic phonon scattering and out-of-plane heat transfer to substrate phonons is relatively inefficient in these systems, suggesting a cooling time of tens of picoseconds. However, we observe much faster cooling, on a time scale of a few picoseconds. We attribute this to an intrinsic cooling mechanism, where carriers in the high-energy tail of the hot-carrier distribution emit optical phonons. This creates a permanent heat sink, as carriers efficiently rethermalize. We develop a macroscopic model that explains the observed dynamics, where cooling is eventually limited by optical-to-acoustic phonon coupling. These fundamental insights will guide the development of graphene-based optoelectronic devices.
Combining the quantum optical properties of single-photon emitters with the strong near-field interactions available in nanophotonic and plasmonic systems is a powerful way of creating quantum manipulation and metrological functionalities. The ability to actively and dynamically modulate emitter-environment interactions is of particular interest in this regard. While thermal, mechanical and optical modulation have been demonstrated, electrical modulation has remained an outstanding challenge. Here we realize fast, all-electrical modulation of the near-field interactions between a nanolayer of erbium emitters and graphene, by in-situ tuning the Fermi energy of graphene. We demonstrate strong interactions with a >1000-fold increased decay rate for ~25% of the emitters, and electrically modulate these interactions with frequencies up to 300 kHz – orders of magnitude faster than the emitter’s radiative decay (~100 Hz). This constitutes an enabling platform for integrated quantum technologies, opening routes to quantum entanglement generation by collective plasmon emission or photon emission with controlled waveform.
Due to its outstanding electrical properties and chemical stability, graphene finds widespread use in various electrochemical applications. Although the presence of electrolytes strongly affects its electrical conductivity, the underlying mechanism has remained elusive. Here, we employ terahertz spectroscopy as a contact-free means to investigate the impact of ubiquitous cations (Li+, Na+, K+, and Ca2+) in aqueous solution on the electronic properties of SiO2-supported graphene. We find that, without applying any external potential, cations can shift the Fermi energy of initially hole-doped graphene by ∼200 meV up to the Dirac point, thus counteracting the initial substrate-induced hole doping. Remarkably, the cation concentration and cation hydration complex size determine the kinetics and magnitude of this shift in the Fermi level. Combined with theoretical calculations, we show that the ion-induced Fermi level shift of graphene involves cationic permeation through graphene. The interfacial cations located between graphene and SiO2 electrostatically counteract the substrate-induced hole doping effect in graphene. These insights are crucial for graphene device processing and further developing graphene as an ion-sensing material.
The characteristic performance of n-type and p-type inversion (IM) mode, accumulation (AC) mode and junctionless (JL) mode, bulk Germanium FinFET device with 3-nm gate length (L G ) are demonstrated by using 3-D quantum transport device simulation. The simulated bulk Ge FinFET device exhibits favorable short channel characteristics, including drain-induced barrier lowering (DIBL<10mV/V), sub threshold slope (SS~64mV/dec.). Electron density distributions in ON-state and OFFstate also show that the simulated devices have large I ON /I OFF ratios. Homogenous source/drain doping is maintained and only the channel doping is varied among different operating modes. Also, a constant threshold voltage |V TH |~0.31V is maintained. Moreover, the calculated quantum capacitance (C Q ) values of the Ge nanowire emphasizes the importance of quantum confinement effects (QCE) on the performance of the ultra-scaled devices.
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 question by studying two technologically relevant systems, consisting of high-quality graphene with a mobility >10,000 cm 2 V −1 s −1 and environments that do not efficiently take up electronic heat from graphene: WSe2-encapsulated graphene and suspended graphene. We study the cooling dynamics of these two high-quality graphene systems using ultrafast pump-probe spectroscopy at room temperature. Cooling via disorder-assisted acoustic phonon scattering and out-of-plane heat transfer to the environment is relatively inefficient in these systems, predicting a cooling time of tens of picoseconds. However, we observe much faster cooling, on a timescale of a few picoseconds. We attribute this to an intrinsic cooling mechanism, where carriers in the hot-carrier distribution with enough kinetic energy emit optical phonons. During phonon emission, the electronic system continuously re-thermalizes, re-creating carriers with enough energy to emit optical phonons. We develop an analytical model that explains the observed dynamics, where cooling is eventually limited by optical-to-acoustic phonon coupling. These fundamental insights into the intrinsic cooling mechanism of hot carriers in graphene will play a key role in guiding the development of graphene-based optoelectronic devices.
High mobility is a crucial requirement for a large variety of electronic device applications. The state-of-the-art for high quality graphene devices is based on heterostructures made with graphene encapsulated in > 80 nm-thick flakes of hexagonal boron nitride (hBN). Unfortunately, scaling up multilayer hBN while precisely controlling the number of layers remains an elusive challenge, resulting in a rough material unable to enhance the mobility of graphene. This leads to the pursuit of alternative, scalable materials, which can be simultaneously used as substrate and encapsulant for graphene. Tungsten disulfide (WS2) is a transition metal dichalcogenide, which was successfully grown in large (∼mm-size) multi-layers by chemical vapour deposition. However, the resistance vs gate voltage characteristics when gating graphene through WS2 exhibit largely hysteretic shifts of the charge neutrality point (CNP) in the order of ∆n ∼2.6•10 11 cm −2 , hindering the use of WS2 as a reliable encapsulant. The hysteresis originates due to the charge traps from sulfur vacancies present in WS2. In this work, we report for the first time the use of WS2 as a substrate and the overcoming of hysteresis issues by chemically treating WS2 with a super-acid, which passivates these vacancies and strips the surface from contaminants. The hysteresis is significantly reduced below the noise level by at least a factor five (to ∆n <5•10 10 cm −2 ) and, simultaneously, the roomtemperature mobility of WS2-encapsulated graphene is as high as ∼6.2•10 4 cm −2 V −1 s −1 at a carrier density n ∼1•10 12 cm −2 . Our results promote WS2 to a valid alternative to hBN as encapsulant for high-performance graphene devices.
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