Competing Ultrafast Energy Relaxation Pathways in Photoexcited Graphene

• Published in: Nano letters Vol. 14; no. 10; pp. 5839 - 5845
• Main Authors: Jensen, S. A, Mics, Z, Ivanov, I, Varol, H. S, Turchinovich, D, Koppens, F. H. L, Bonn, M, Tielrooij, K. J
• Format: Journal Article
• Language: English
• Published: Washington, DC American Chemical Society 08.10.2014
• Subjects: Applied sciences; Carriers; Condensed matter: electronic structure, electrical, magnetic, and optical properties; Cross-disciplinary physics: materials science; rheology; Electronic structure and electrical properties of surfaces, interfaces, thin films and low-dimensional structures; Electronic structure of nanoscale materials : clusters, nanoparticles, nanotubes, and nanocrystals; Electronics; Exact sciences and technology; Fermi surfaces; Fluence; Fullerenes and related materials; diamonds, graphite; Graphene; Heating; Materials science; Molecular electronics, nanoelectronics; Optical properties and condensed-matter spectroscopy and other interactions of matter with particles and radiation; Optical properties of low-dimensional, mesoscopic, and nanoscale materials and structures; Pathways; Phonons; Physics; Scattering; Semiconductor electronics. Microelectronics. Optoelectronics. Solid state devices; Specific materials; pump−probe; Graphene; terahertz; hot carrier; ultrafast; Optoelectronics; Doping; Heat treatments; Nanoelectronics; Optical phonons; Relaxation; Electronic structure; THz range; Fermi level; High energy; Optical properties; Photoconductivity
• ISSN: 1530-6984; 1530-6992
• DOI: 10.1021/nl502740g

For most optoelectronic applications of graphene, a thorough understanding of the processes that govern energy relaxation of photoexcited carriers is essential. The ultrafast energy relaxation in graphene occurs through two competing pathways: carrier–carrier scattering, creating an elevated carrier temperature, and optical phonon emission. At present, it is not clear what determines the dominating relaxation pathway. Here we reach a unifying picture of the ultrafast energy relaxation by investigating the terahertz photoconductivity, while varying the Fermi energy, photon energy and fluence over a wide range. We find that sufficiently low fluence (≲4 μJ/cm2) in conjunction with sufficiently high Fermi energy (≳0.1 eV) gives rise to energy relaxation that is dominated by carrier–carrier scattering, which leads to efficient carrier heating. Upon increasing the fluence or decreasing the Fermi energy, the carrier heating efficiency decreases, presumably due to energy relaxation that becomes increasingly dominated by phonon emission. Carrier heating through carrier–carrier scattering accounts for the negative photoconductivity for doped graphene observed at terahertz frequencies. We present a simple model that reproduces the data for a wide range of Fermi levels and excitation energies and allows us to qualitatively assess how the branching ratio between the two distinct relaxation pathways depends on excitation fluence and Fermi energy.