Direct Observation of Single Layer Graphene Oxide Reduction through Spatially Resolved, Single Sheet Absorption/Emission Microscopy

• Autores: Sokolov, Denis A.; Morozov, Yurii V.; McDonald, Matthew P.; Vietmeyer, Felix; Hodak, Jose Hector; Kuno, Masaru
• Año de publicación: 2014
• Idioma: inglés
• Tipo de recurso: artículo
• Materia: Graphene Oxide; Reduced Graphene Oxide; Photolysis; Absorption; Emission; Absorption Coefficient
• Institución: Consejo Nacional de Investigaciones Científicas y Técnicas

Laser reduction of graphene oxide (GO) offers unique opportunities for the rapid, nonchemical production of graphene. By tuning relevant reduction parameters, the band gap and conductivity of reduced GO can be precisely controlled. In situ monitoring of single layer GO reduction is therefore essential. In this report, we show the direct observation of laser-induced, single layer GO reduction through correlated changes to its absorption and emission. Absorption/emission movies illustrate the initial stages of single layer GO reduction, its transition to reduced-GO (rGO) as well as its subsequent decomposition upon prolonged laser illumination. These studies reveal GO’s photoreduction life cycle and through it native GO/rGO absorption coefficients, their intrasheet distributions as well as their spatial heterogeneities. Extracted absorption coefficients for unreduced GO are α405 nm ≈ 6.5 ± 1.1 × 104 cm–1, α520 nm ≈ 2.1 ± 0.4 × 104 cm–1, and α640 nm ≈ 1.1 ± 0.3 × 104 cm–1 while corresponding rGO α-values are α405 nm ≈ 21.6 ± 0.6 × 104 cm–1, α520 nm ≈ 16.9 ± 0.4 × 104 cm–1, and α640 nm ≈ 14.5 ± 0.4 × 104 cm–1. More importantly, the correlated absorption/emission imaging provides us with unprecedented insight into GO’s underlying photoreduction mechanism, given our ability to spatially resolve its kinetics and to connect local rate constants to activation energies. On a broader level, the developed absorption imaging is general and can be applied toward investigating the optical properties of other two-dimensional materials, especially those that are nonemissive and are invisible to current single molecule optical techniques.
Fil: Sokolov, Denis A.. University Of Notre Dame-Indiana; Estados Unidos
Fil: Morozov, Yurii V.. University Of Notre Dame-Indiana; Estados Unidos. Taras Shevchenko National University of Kiev; Rusia
Fil: McDonald, Matthew P.. University Of Notre Dame-Indiana; Estados Unidos
Fil: Vietmeyer, Felix. University Of Notre Dame-Indiana; Estados Unidos
Fil: Hodak, Jose Hector. Consejo Nacional de Investigaciones Científicas y Técnicas. Oficina de Coordinación Administrativa Ciudad Universitaria. Instituto de Química, Física de los Materiales, Medioambiente y Energía. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales. Instituto de Química, Física de los Materiales, Medioambiente y Energía; Argentina
Fil: Kuno, Masaru. University Of Notre Dame-Indiana; Estados Unidos