Time-Resolved Cathodoluminescence in a TEM

Sophie Meuret^a, Luiz Tizei^b, Nikolay Cherkashin^a, Yves Auad^b, Robin Cours^a, Sebastien Weber^a, Florent Houdellier^a, Mathieu Kociak^b, Arnaud Arbouet^a

^aCEMES-CNRS Université de Toulouse UPS 29 rue Jeanne Marvig BP 94347 Toulouse, Cedex 04, France

^bLaboratoire LPS CNRS/Université Paris-Saclay, Bâtiment 510, Orsay, France

Proceedings of Electron Beam Spectroscopy for Nanooptics 2021 (EBSN2021)

Online, Spain, 2021 June 14th - 15th

Organizers: Mathieu Kociak and Nahid Talebi

Oral, Sophie Meuret, presentation 016
Publication date: 8th June 2021

The development of time-resolved Cathodoluminescence (TR-CL) in a scanning electron microscope (SEM) enabled the measurement of the lifetime of excited states in semiconductors with a sub-wavelength spatial resolution. It was used for example to measure the influence of stacking faults on the GaN exciton lifetime ¹, to probe the role of a silver layer on the dynamics of a YAG crystal ^2, or to show the influence of stress on the optical properties of ZnO nanowires ³. These results demonstrate that TR-CL is essential to study the correlation between semiconductor optical and structural properties (composition, defects, strain…). Despite giving invaluable information, TR-CL in a scanning electron microscope is still limited in spatial resolution. CL in the transmission electron microscope (TEM) proved to dramatically improve the spatial resolution with respect to SEM-CL, in addition, to give access to multiple complementary analysis tools (from atomic-scale imaging to electron energy loss spectroscopy). The advent of the yet undemonstrated TR-CL in a STEM is therefore expected to be a major next step for the investigation of the optical properties of nanomaterials.

In this presentation, we will discuss our first experimental demonstration of time-resolved cathodoluminescence within a transmission electron microscope. They were performed in a unique femtosecond pulsed transmission electron microscope, with a cold-FEG electron gun ⁴. This technology allows among other things sub-ps temporal resolution while preserving a spatial resolution of a few nanometers, essential for the study of nanophotonic materials. We will present the first lifetime maps acquired in a TEM both on nano-diamonds and InGaN quantum wells and discuss the unique features and opportunities of this technique.

References:

[1] Corfdir, P. et al. Exciton localization on basal stacking faults in a-plane epitaxial lateral overgrown GaN grown by hydride vapor phase epitaxy. J. Appl. Phys. 105, 043102 (2009).

[2] Moerland, R. J., Weppelman, I. G. C., Garming, M. W. H., Kruit, P. & Hoogenboom, J. P. Time-resolved cathodoluminescence microscopy with sub-nanosecond beam blanking for direct evaluation of the local density of states. Opt. Express 24, 24760 (2016).

[3] Fu, X. et al. Exciton Drift in Semiconductors under Uniform Strain Gradients: Application to Bent ZnO Microwires. ACS Nano 8, 3412–3420 (2014).

[4] Houdellier, F., Caruso, G. M., Weber, S., Kociak, M. & Arbouet, A. Development of a high brightness ultrafast Transmission Electron Microscope based on a laser-driven cold field emission source. Ultramicroscopy 186, 128–138 (2018).

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