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

被引:54
作者
Pein, Brandt C. [1 ,2 ]
Chang, Wendi [1 ,2 ]
Hwang, Harold Y. [3 ]
Scherer, Jennifer [1 ,2 ]
Coropceanu, Igor [1 ,2 ]
Zhao, Xiaoguang [4 ]
Zhang, Xin [4 ]
Bulovic, Vladimir [1 ,2 ]
Bawendi, Moungi [1 ,2 ]
Nelson, Keith A. [1 ,2 ]
机构
[1] MIT, Dept Chem, Cambridge, MA 02139 USA
[2] MIT, Dept Elect Engn & Comp Sci, Cambridge, MA 02139 USA
[3] MIT, Lincoln Lab, Lexington, MA 02420 USA
[4] Boston Univ, Dept Mech Engn, Boston, MA 02215 USA
基金
美国国家科学基金会;
关键词
Terahertz; quantum dots; luminescence; Stark effect; LIGHT-EMITTING-DIODES; FIELD-EFFECT TRANSISTORS; NANOCRYSTAL SOLIDS; CHARGE INJECTION; ELECTRON; ELECTROLUMINESCENCE; TRANSPORT; EMISSION; LEDS;
D O I
10.1021/acs.nanolett.7b01837
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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 Tliz detector that operates at room temperature.
引用
收藏
页码:5375 / 5380
页数:6
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