Terahertz-Driven Luminescence and Colossal Stark Effect in CdSe–CdS Colloidal Quantum Dots

Pein, Brandt C.; Chang, Wendi; Hwang, Harold Y.; Scherer, Jennifer; Coropceanu, Igor; Zhao, Xiaoguang; Zhang, Xin; Bulović, Vladimir; Bawendi, Moungi; Nelson, Keith A.

doi:10.1021/acs.nanolett.7b01837

Title: Terahertz-Driven Luminescence and Colossal Stark Effect in CdSe–CdS Colloidal Quantum Dots

Journal Article · Wed Aug 23 00:00:00 EDT 2017 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.7b01837· OSTI ID:1375963

^[1]; Chang, Wendi ^[1]; Hwang, Harold Y. ^[2]; Scherer, Jennifer ^[1]; Coropceanu, Igor ^[1]; Zhao, Xiaoguang ^[3]; Zhang, Xin ^[3]; Bulović, Vladimir ^[1];

^[1]; Nelson, Keith A. ^[1]

Department of Chemistry and Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States
Massachusetts Institute of Technology Lincoln Laboratory, Lexington, Massachusetts 02420, United States
Department of Mechanical Engineering, Boston University, Boston, Massachusetts 02215, United States

Optical properties of colloidal semiconductor quantum dots (QDs), arising from quantum mechanical confinement of charge, present a versatile testbed for the study of how high electric fields affect the electronic structure of nanostructured solids. Studies of quasi-DC electric field modulation of QD properties have been limited by electrostatic breakdown processes under high externally applied electric fields, which have restricted the range of modulation of QD properties. In contrast, here we drive CdSe–CdS core–shell QD films with high-field THz-frequency electromagnetic pulses whose duration is only a few picoseconds. Surprisingly, in response to the THz excitation, we observe QD luminescence even in the absence of an external charge source. Our experiments show that QD luminescence is associated with a remarkably high and rapid modulation of the QD bandgap, which changes by more than 0.5 eV (corresponding to 25% of the unperturbed bandgap energy). We show that these colossal energy shifts can be explained by the quantum confined Stark effect even though we are far outside the regime of small field-induced shifts in electronic energy levels. Our results demonstrate a route to extreme modulation of material properties and to a compact, high-bandwidth THz detector that operates at room temperature.

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Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: C0001088; SC0001088

OSTI ID:: 1375963

Alternate ID(s):: OSTI ID: 1523280

Journal Information:: Nano Letters, Journal Name: Nano Letters Vol. 17 Journal Issue: 9; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 40 works

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