Two-probe study of hot carriers in reduced graphene oxide

Journal of Applied Physics (Impact Factor: 2.21). 03/2011; 109. DOI:10.1063/1.3573674
Source: arXiv

ABSTRACT The energy relaxation of carriers in reduced graphene oxide thin films is
studied using optical pump-probe spectroscopy with two probes of different
colors. We measure the time difference between peaks of the carrier density at
each probing energy by measuring a time-resolved differential transmission and
find that the carrier density at the lower probing energy peaks later than that
at the higher probing energy. Also, we find that the peak time for the lower
probing energy shifts from about 92 to 37 fs after the higher probing energy
peak as the carrier density is increased from 1.5E12 to 3E13 per square
centimeter, while no noticeable shift is observed in that for the higher
probing energy. Assuming the carriers rapidly thermalize after excitation, this
indicates that the optical phonon emission time decreases from about 50 to
about 20 fs and the energy relaxation rate increases from 4 to 10 meV/fs. The
observed density dependence is inconsistent with the phonon bottleneck effect.

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    ABSTRACT: Carrier dynamics in single-layer graphene grown by chemical vapor deposition (CVD) is studied using spatially and temporally resolved pump-probe spectroscopy by measuring both differential transmission and differential reflection. By studying the expansion of a Gaussian spatial profile of carriers excited by a 1500-nm pump pulse with a 1761-nm probe pulse, we observe a diffusion of hot carriers of 5500 square centimeter per second. We also observe that the expansion of the carrier density profile decreases to a slow rate within 1 ps, which is unexpected. Furthermore, by using an 810-nm probe pulse we observe that both the differential transmission and reflection change signs, but also that this sign change can be permanently removed by exposure of the graphene to femtosecond laser pulses of relatively high fluence. This indicates that the differential transmission and reflection at later times may not be directly caused by carriers, but may be from some residue material from the sample fabrication or transfer process.
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    ABSTRACT: 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 abnormal spectral redshift with dynamic feature associated to the strengthened electron-phonon coupling. These experimental results can be well understood by considering the screened Coulomb interactions. With increasing carrier density, the reduced screening effect promotes carrier scattering which enhances hot-carrier emission from such multilayer rGO nanospheres. This carrier-scattering scenario is further confirmed by pump-probe measurements.
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