Terahertz-driven Luminescence and Colossal Stark Effect in CdSe:CdS Colloidal Quantum Dots
Brandt C. Pein, Wendi Chang, Harold Y. Hwang, Jennifer Scherer, Igor Coropceanu, Xiaoguang Zhao, Xin Zhang, Vladimir Bulović, Moungi Bawendi, Keith A. Nelson
Unique optical properties of colloidal semiconductor quantum dots (QDs), arising from quantum mechanical confinement of charge within these structures, present a versatile testbed for the study of how high electric fields affect the electronic structure of nanostructured solids. Earlier studies of quasi-DC electric field modulation of QD properties have been limited by the electrostatic breakdown processes under the high externally applied electric fields, which have restricted the range of modulation of QD properties. In contrast, in the present work 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 band-gap, which is changing by more than 0.5 eV (corresponding to 25% of the unperturbed bandgap energy) within the picosecond timeframe of THz field profile. We show that these colossal energy shifts can be consistently explained by the quantum confined Stark effect. Our work demonstrates a route to extreme modulation of material properties without configurational changes in material sets or geometries. Additionally, we expect that this platform can be adapted to a novel compact THz detection scheme where conversion of THz fields (with meV-scale photon energies) to the visible/near-IR band (with eV-scale photon energies) can be achieved at room temperature with high bandwidth and sensitivity.
Stimulated Emission from 2D CdSe/CdS Nanoplatelets Integrated in a Liquid-Core Fiber
Leibniz University Hannover(汉诺威莱布尼茨大学);Leibniz Institute of Photonic Technology(莱布尼茨光子技术研究所);Institute of Applied Optics and Biophysics(应用光学与生物物理研究所);Otto Schott Institute of Material Research(奥托·肖特材料研究所);University Tübingen(蒂宾根大学)
Studies on Size Dependent Structures and Optical Properties of CdSeS Clusters
研究了CdSeS纳米团簇在水介质中的尺寸依赖性结构和光学性质。采用密度泛函理论/含时密度泛函理论(DFT/TDDFT)研究了不同尺寸Cd $_n$ Se $_m$ S $_p$纳米团簇(n=6)的稳定性.基态(S $_0$)和激发态(S $_1$,S $_2$,S $_3$)的计算结果通过紫外-可见光谱得到了实验验证。计算从头算结果表明,CdSeS团簇是显着更超极化相比,CdX(X= S,Se,Te)团簇。还观察到结构依赖的响应特性,特别是对于n>3。较大的超极化率($β$和$γ$)、电荷变化和轨道分析确定Cd $_4$ Se $_m$ S $_p$团簇为非线性光学活性量子点(QD)。
Optical and X-ray Photo-emission Spectroscopies of Core/Shell Colloidal CdSe/CdS Quantum Dots: Modeling and Experimental Determination of Band Alignment