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Light-Induced Charge Carrier Dynamics at Nanostructured Interfaces Investigated by Ultrafast Electron Diffractive Photovoltammetry

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Quantum Dot Solar Cells

Part of the book series: Lecture Notes in Nanoscale Science and Technology ((LNNST,volume 15))

Abstract

We present an ultrafast photovoltammetry framework to investigate the surface charge carrier dynamics at the nanometer scale. This diffraction-based method utilizes the feature-gated nanomaterial diffraction pattern to identify the scattering sites and to deduce the associated charge dynamics from the nanocrystallographic refraction-shift observed in the ultrafast electron diffraction patterns. From applying this methodology on SiO2/Si interface, and surfaces decorated with nanoparticles and water–ice adsorbed layer, we are able to elucidate the localized charge injection, dielectric relaxation, and carrier diffusion, with direct resolution in the charge state and possibly correlated structural dynamics at these interfaces, which are central to nanoelectronics, photovoltaics, and photocatalysis development. These new results highlight the high sensitivity of the interfacial charge transfer to the nanoscale modification, environment, and surface plasmonics enhancement and demonstrate the diffraction-based ultrafast surface voltage probe as a unique and powerful method to resolve the nanometer scale charge carrier dynamics.

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Notes

  1. 1.

    The shift in diffraction due to electron wavlength change in the materials, which is on the level of 3 ×10− 5 per 1 V in photovoltage for 30 keV electron beam, is small compared to refraction shift, which is on the 10− 2 level under the same condition.

  2. 2.

    The persistence length here refers to the length of the crystal in the sample that allow the probing electron to scatter coherently to form diffraction pattern. The persistence length can be limited by the size of the crystal, the coherence length of the probing electron, or the penetration depth of the probing electron, which ever is the smallest.

  3. 3.

    The electrostatics calculations were performed using the Charged Particle Toolkit software from Field Precision. The geometry was setup according to Fig. 13.22a, c. In both cases, a potential of \(V _{\mathrm{ s}} = -5\) V was imposed. For nanoparticle simulations, the relative permittivity of the dielectric layer was set to 2.5. The Si(111) was treated as a grounded metal because of the high carrier density under photoexcitation. The potential far away from the nanoparticle was set to 0. Electrons of 30 keV were initialized at different launch angles (1°–5°) and positions along the height of the dielectric layer (1/3, 1/2, and 2/3). The slab model calculations were also carried out with this software, with varying capacitor slab separations.

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Acknowledgements

The researches discussed in this lecture note were largely supported under grant DE-FG02-06ER46309 from the US Department of Energy. The analytic work on the charge dynamics was supported by US National Science Foundation under grant NSF-DMR 1126343. Partial support for R.A. Murdick is under grant 45982-G10 from the Petroleum Research Fund of the American Chemical Society.

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  1. Department of Physics and Astronomy, Michigan State University, East Lansing, MI, 48824, USA

    Kiseok Chang, Ryan A. Murdick, Tzong-Ru T. Han, Fei Yuan & Chong-Yu Ruan

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  1. Kiseok Chang
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  1. State Key Laboratory of Electronic Thin, University of Electronic Science and Technology of China, Chengdu, China, People's Republic

    Jiang Wu

  2. State Key Laboratory of Electronic, University of Electronic Science and Technology, Chengdu, China, People's Republic

    Zhiming M. Wang

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Chang, K., Murdick, R.A., Han, TR.T., Yuan, F., Ruan, CY. (2014). Light-Induced Charge Carrier Dynamics at Nanostructured Interfaces Investigated by Ultrafast Electron Diffractive Photovoltammetry. In: Wu, J., Wang, Z. (eds) Quantum Dot Solar Cells. Lecture Notes in Nanoscale Science and Technology, vol 15. Springer, New York, NY. https://doi.org/10.1007/978-1-4614-8148-5_13

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