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Room-Temperature Electron Spin Generation by Femtosecond Laser Pulses in Colloidal CdS Quantum Dots.

ABSTRACT: We present an experimental investigation of optical spin orientation in colloidal CdS quantum dots (QDs) by a femtosecond laser pulse at room temperature. The spin carrier and its spin-generation process are clarified. Firstly, the observed spin signals of CdS QDs in time-resolved Faraday rotation measurements are shown to belong to electron carriers, by comparing the spin dephasing dynamics and Landé g factor between CdS QDs and bulk materials. Secondly, spin dynamics unaffected by the faster carrier recombination suggests that the spin-polarized electrons are not photoexcited but resident in the dots. Moreover, hole spins should dephase very fast compared with electron spins, otherwise the trion (two electrons with opposite spin orientations and one hole) recombination process will affect the resident electron spin signals. The electron spin is generated in a short time of which the excitation light is absorbed and the resident electron is excited to trion states, i.e., of pulse durations. Due to fast hole spin dephasing, trion recombination gives null spin signals, and the subsequent electron spin dynamics is controlled by its intrinsic mechanisms.

SUBMITTER: Tong H

PROVIDER: S-EPMC5452855 | biostudies-other | 2013 Oct

REPOSITORIES: biostudies-other

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Project description:Pairs of coupled quantum dots with controlled coupling between the two potential wells serve as an extremely rich system, exhibiting a plethora of optical phenomena that do not exist in each of the isolated constituent dots. Over the past decade, coupled quantum systems have been under extensive study in the context of epitaxially grown quantum dots (QDs), but only a handful of examples have been reported with colloidal QDs. This is mostly due to the difficulties in controllably growing nanoparticles that encapsulate within them two dots separated by an energetic barrier via colloidal synthesis methods. Recent advances in colloidal synthesis methods have enabled the first clear demonstrations of colloidal double quantum dots and allowed for the first exploratory studies into their optical properties. Nevertheless, colloidal double QDs can offer an extended level of structural manipulation that allows not only for a broader range of materials to be used as compared with epitaxially grown counterparts but also for more complex control over the coupling mechanisms and coupling strength between two spatially separated quantum dots. The photophysics of these nanostructures is governed by the balance between two coupling mechanisms. The first is via dipole-dipole interactions between the two constituent components, leading to energy transfer between them. The second is associated with overlap of excited carrier wave functions, leading to charge transfer and multicarrier interactions between the two components. The magnitude of the coupling between the two subcomponents is determined by the detailed potential landscape within the nanocrystals (NCs). One of the hallmarks of double QDs is the observation of dual-color emission from a single nanoparticle, which allows for detailed spectroscopy of their properties down to the single particle level. Furthermore, rational design of the two coupled subsystems enables one to tune the emission statistics from single photon emission to classical emission. Dual emission also provides these NCs with more advanced functionalities than the isolated components. The ability to better tailor the emission spectrum can be advantageous for color designed LEDs in lighting and display applications. The different response of the two emission colors to external stimuli enables ratiometric sensing. Control over hot carrier dynamics within such structures allows for photoluminescence upconversion. This Account first provides a description of the main hurdles toward the synthesis of colloidal double QDs and an overview of the growing library of synthetic pathways toward constructing them. The main discoveries regarding their photophysical properties are then described in detail, followed by an overview of potential applications taking advantage of the double-dot structure. Finally, a perspective and outlook for their future development is provided.

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Room-Temperature Electron Spin Generation by Femtosecond Laser Pulses in Colloidal CdS Quantum Dots.

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