Attractive versus Repulsive Excitonic Interactions of Colloidal Quantum Dots Control Blue- to Red-Shifting (and Non-shifting) Amplified Spontaneous Emission

Autor: Ozan Yerli, Halime Gul Yaglioglu, Burak Guzelturk, Ahmet Fatih Cihan, Hilmi Volkan Demir, Yusuf Kelestemur, Ayhan Elmali, Ulaş Kürüm
Přispěvatelé: Demir, Hilmi Volkan
Rok vydání: 2013
Předmět:
Wave-guides
Amplified spontaneous emission
TPA cross sections
Spontaneous emission
Luminescence of organic solids
Physics::Optics
CdSe/CdS
quantum dots
Semiconductor Nanocrystals
Two-photon absorption
amplified spontaneous emission
Two-photon absorptions
Regime
Computer Science::Networking and Internet Architecture
Semiconductor quantum dots
two-photon absorption
General Materials Science
Stimulated emission
Physical and Theoretical Chemistry
Absorption (electromagnetic radiation)
Physics
Energy
Colloidal quantum dots
business.industry
Excitonic interaction
near-unity efficiency
Two photon processes
Condensed Matter::Mesoscopic Systems and Quantum Hall Effect
Dynamics
Nanocrystals
Wavelength
Light Amplification
Quantum dot
exciton-exciton interactions
Amplified spontaneous emissions
Optoelectronics
Stimulated-emission
Quantum efficiency
Optical Gain
business
Quantum mechanical model
Inverted Core/shell Nanocrystals
Confinement
Light polarization
Zdroj: Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters
ISSN: 1948-7185
DOI: 10.1021/jz402211m
Popis: Tunable, high-performance, two-photon absorption (TPA)-based amplified spontaneous emission (ASE) from near-unity quantum efficiency colloidal quantum dots (CQDs) is reported. Besides the absolute spectral tuning of ASE, the relative spectral tuning of ASE peak with respect to spontaneous emission was shown through engineering excitonic interactions in quasi-type-II CdSe/CdS core/shell CQDs. With core-shell size adjustments, it was revealed that Coulombic exciton-exciton interactions can be tuned to be attractive (type-I-like) or repulsive (type-II-like) leading to red- or blue-shifted ASE peak, respectively, and that nonshifting ASE can be achieved with the right core-shell combinations. The possibility of obtaining ASE at a specific wavelength from both type-I-like and type-II-like CQDs was also demonstrated. The experimental observations were supported by parametric quantum-mechanical modeling, shedding light on the type-tunability. These excitonically engineered CQD-solids exhibited TPA-based ASE threshold as low as 6.5 mJ/cm2 under 800 nm excitation, displaying one of the highest values of TPA cross-section of 44 660 GM. © 2013 American Chemical Society.
Databáze: OpenAIRE