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High-throughput optical imaging and spectroscopy of individual carbon nanotubes in devices

Abstract

Single-walled carbon nanotubes are uniquely identified by a pair of chirality indices (n,m), which dictate the physical structures and electronic properties of each species1. Carbon nanotube research is currently facing two outstanding challenges: achieving chirality-controlled growth and understanding chirality-dependent device physics2,3,4,5,6. Addressing these challenges requires, respectively, high-throughput determination of the nanotube chirality distribution on growth substrates and in situ characterization of the nanotube electronic structure in operating devices. Direct optical imaging and spectroscopy techniques are well suited for both goals7,8,9, but their implementation at the single nanotube level has remained a challenge due to the small nanotube signal and unavoidable environment background10,11,12,13,14,15,16,17. Here, we report high-throughput real-time optical imaging and broadband in situ spectroscopy of individual carbon nanotubes on various substrates and in field-effect transistor devices using polarization-based microscopy combined with supercontinuum laser illumination. Our technique enables the complete chirality profiling of hundreds of individual carbon nanotubes, both semiconducting and metallic, on a growth substrate. In devices, we observe that high-order nanotube optical resonances are dramatically broadened by electrostatic doping, an unexpected behaviour that points to strong interband electron–electron scattering processes that could dominate ultrafast dynamics of excited states in carbon nanotubes.

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Figure 1: Scheme of polarization-based optical microscopy for single-nanotube imaging and spectroscopy.
Figure 2: Optical imaging and spectroscopy of an individual nanotube on substrates and in devices.
Figure 3: High-throughput chirality profiling of 402 single-walled carbon nanotubes from one growth condition.
Figure 4: Gate-variable nanotube optical transitions in field-effect devices.

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Acknowledgements

Nanotube synthesis and optical spectroscopy were supported by a National Science Foundation (NSF) CAREER grant (no. 0846648), the NSF Center for Integrated Nanomechanical Systems (no. EEC-0832819) and NSF grant no. CHE-1213469. Support for device fabrication and characterization instrumentation was provided by the Director, Office of Energy Research, Materials Sciences and Engineering Division, of the US Department of Energy (contract nos. DE-SC0003949 and DE-AC02-05CH11231). J.L. and W.Z. also acknowledge support from Duke SMiF (Shared Materials Instrumentation Facilities).

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Contributions

F.W., K.L. and X.H. conceived the experiment. K.L., X.H. and F.W. carried out optical measurements. X.H. and K.L. carried out electrical measurements. Q.Z., K.L. and A.Z. fabricated and characterized the device. J.L., W.Z. and J.L. grew nanotubes for chirality profiling. K.L., Q.Z. and A.Z. grew nanotubes for the device. C.J., E.G. and F.W. performed the theoretical analysis. All authors discussed the results and wrote the manuscript.

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Correspondence to Feng Wang.

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The authors declare no competing financial interests.

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Liu, K., Hong, X., Zhou, Q. et al. High-throughput optical imaging and spectroscopy of individual carbon nanotubes in devices. Nature Nanotech 8, 917–922 (2013). https://doi.org/10.1038/nnano.2013.227

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