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Terahertz-Driven Stark Spectroscopy of CdSe and CdSe–CdS Core–Shell Quantum Dots

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journal contribution
posted on 24.10.2019, 15:48 by Brandt C. Pein, Chee Kong Lee, Liang Shi, JiaoJian Shi, Wendi Chang, Harold Y. Hwang, Jennifer Scherer, Igor Coropceanu, Xiaoguang Zhao, Xin Zhang, Vladimir Bulović, Moungi G. Bawendi, Adam P. Willard, Keith A. Nelson
The effects of large external fields on semiconductor nanostructures could reveal much about field-induced shifting of electronic states and their dynamical responses and could enable electro-optic device applications that require large and rapid changes in optical properties. Studies of quasi-dc electric field modulation of quantum dot (QD) properties have been limited by electrostatic breakdown processes observed under high externally applied field levels. To circumvent this, here we apply ultrafast terahertz (THz) electric fields with switching times on the order of 1 ps. We show that a pulsed THz electric field, enhanced by a microslit field enhancement structure (FES), can strongly manipulate the optical absorption properties of a thin film of CdSe and CdSe–CdS core–shell QDs on the subpicosecond time scale with spectral shifts that span the visible to near-IR range. Numerical simulations using a semiempirical tight binding model show that the band gap of the QD film can be shifted by as much a 79 meV during these time scales. The results allow a basic understanding of the field-induced shifting of electronic levels and suggest electro-optic device applications.