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Broadband electromagnetic response and ultrafast dynamics of few-layer epitaxial graphene (0903.0577v2)

Published 3 Mar 2009 in cond-mat.mtrl-sci

Abstract: We study the broadband optical conductivity and ultrafast carrier dynamics of epitaxial graphene in the few-layer limit. Equilibrium spectra of nominally buffer, monolayer, and multilayer graphene exhibit significant terahertz and near-infrared absorption, consistent with a model of intra- and interband transitions in a dense Dirac electron plasma. Non-equilibrium terahertz transmission changes after photoexcitation are shown to be dominated by excess hole carriers, with a 1.2-ps mono-exponential decay that reflects the minority-carrier recombination time.

Citations (213)

Summary

  • The paper reports that non-equilibrium THz spectroscopy reveals a 1.2 ps decay time for minority-carrier recombination in few-layer epitaxial graphene.
  • The study employs FTIR, LEEM, ARPES, and STM to detail layer-dependent optical conductivity and electronic morphology.
  • The findings underscore the impact of substrate-induced doping and a dense Dirac electron plasma in driving graphene’s fast electromagnetic response.

Broadband Electromagnetic Properties and Ultrafast Dynamics of Few-Layer Epitaxial Graphene

This paper presents a detailed examination of the broadband optical conductivity and ultrafast carrier dynamics in few-layer epitaxial graphene. Utilizing both equilibrium infrared spectroscopy and non-equilibrium terahertz (THz) spectroscopy, the researchers evaluated monolayer, buffer, and multilayer epitaxial graphene grown on SiC substrates. This work builds on previous understandings and explores new dimensions in the electromagnetic response of graphene, particularly in the field of engineered graphene layers as potential components in future high-speed electronic devices.

Methodology and Measurements

The research employed Fourier-Transform Infrared (FTIR) spectroscopy and time-domain THz spectroscopy to measure the electromagnetic response across a range from the far-infrared to the near-infrared spectrum. The paper focused on graphene layers of varying thickness, confirming their morphology and electronic state through low-energy electron microscopy (LEEM), angle-resolved photoemission spectroscopy (ARPES), and scanning tunneling microscopy (STM). Such characterization was crucial as these thin films exhibit nanoribbon-like monolayer terraces.

The equilibrium paper revealed significant absorption in both the terahertz and near-infrared regimes, indicative of intra- and interband transitions within a dense Dirac electron plasma. Additionally, non-equilibrium THz spectroscopy highlighted ultrafast changes in transmission post photoexcitation, driven primarily by excess hole carriers and characterized by a 1.2 ps mono-exponential decay. This decay time reflects the minority-carrier recombination time, an important parameter for understanding the interplay of electron and hole dynamics in these materials.

Theoretical Analysis and Implications

The article's theoretical framework relied on modeling the real part of the optical sheet conductivity, accounting for variations in film layer thickness and carrier concentrations. The results indicate that the epitaxial graphene's optical response significantly differs from exfoliated counterparts due to substrate interactions that induce high doping levels. Consequently, the dense electron environment deeply influences the THz transient response, particularly emphasizing the non-linear dependency of the Drude spectral weight on carrier distribution.

The findings demonstrate that despite photoexcitation creating both electron and hole populations, hole dynamics predominantly dictate the non-equilibrium THz response in the studied samples. This observation aligns with graphene’s unique electronic properties, where material responses are strongly coupled to the quasi-relativistic behavior of Dirac fermions.

Broader Impact and Future Directions

The characterization of ultrafast dynamics and broadband conductivity in few-layer epitaxial graphene informs potential applications in high-frequency optoelectronic devices and terahertz technologies. Understanding the recombination dynamics and spectral weight distribution can be pivotal for designing devices that exploit graphene's carrier mobility and photonic properties.

Looking forward, further exploration into layer-by-layer variation, doping control, and substrate impacts could refine epitaxial graphene's optoelectronic capabilities. Advanced techniques, possibly even spanning beyond optical frequencies into the X-ray region, may offer deeper insights into the complex interplay of charge-carrier dynamics. Moreover, integration with other two-dimensional materials might pave the way for novel heterostructures with tailored electromagnetic properties, driving advancements in both fundamental research and functional device engineering.

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