Raman Spectroscopy of Electrochemically-Gated Graphene Transistors: Geometrical Capacitance, Electron-Phonon, Electron-Electron, and Electron-Defect Scattering

Abstract

We report a comprehensive micro-Raman scattering study of electrochemically-gated graphene field-effect transistors. The geometrical capacitance of the electrochemical top-gates is accurately determined from dual-gated Raman measurements, allowing a quantitative analysis of the frequency, linewidth and integrated intensity of the main Raman features of graphene. The anomalous behavior observed for the G-mode phonon is in very good agreement with theoretical predictions and provides a measurement of the electron-phonon coupling constant for zone-center ($\Gamma$ point) optical phonons. In addition, the decrease of the integrated intensity of the 2D-mode feature with increasing doping, makes it possible to determine the electron-phonon coupling constant for near zone-edge (K and K' points) optical phonons. We find that the electron-phonon coupling strength at $\Gamma$ is five times weaker than at K (K'), in very good agreement with a direct measurement of the ratio of the integrated intensities of the resonant intra- (2D') and inter-valley (2D) Raman features. We also show that electrochemical reactions, occurring at large gate biases, can be harnessed to efficiently create defects in graphene, with concentrations up to approximately $1.4\times 10^{12}\mathrm{c}{\mathrm{m}}^{-2}$. At such defect concentrations, we estimate that the electron-defect scattering rate remains much smaller than the electron-phonon scattering rate. The evolution of the G- and 2D-mode features upon doping remain unaffected by the presence of defects and the doping dependence of the D mode closely follows that of its two-phonon (2D mode) overtone. Finally, the linewidth and frequency of the G-mode phonon as well as the frequencies of the G- and 2D-mode phonons in doped graphene follow sample-independent correlations that can be utilized for accurate estimations of the charge carrier density.

18 pages, 14 figures, 1 table

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• Electrical Control over Phonon Polarization in Strained Graphene
• Theory of resonant Raman scattering: Toward a comprehensive \textit{ab initio} description
• Strongly Absorbing Nanoscale Infrared Domains within Graphene Bubbles
• Photochemical reaction on graphene surfaces controlled by substrate-surface modification with polar self-assembled monolayers
• Self-aligned local electrolyte gating of 2D materials with nanoscale resolution
• Adsorbates as a charge-carrier reservoir for electrostatic carrier doping to graphene
• Single- and narrow-line photoluminescence in a boron nitride-supported MoSe${}_2$/graphene heterostructure
• Mass inversion at the Lifshitz transition in monolayer graphene by diffusive, high-density, on-chip, doping
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• Dynamic strain in gold nanoparticle supported graphene induced by focused laser irradiation
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• Optoelectronics of confined semiconductors : the case of colloidal nanocrystals and their application to photodetection
• Non-adiabatic phonon self-energy due to electrons with finite linewidths
• Many-body effects in suspended graphene probed through magneto-phonon resonances
• Insulating Electronic States Near the Dirac Point Arising from Twisted Stacking and Curvature in 3D Nanoporous Graphene