Kira Patty

Enhancement of emission efficiency of colloidal CdSe quantum dots on silicon substrate via an ultra-thin layer of aluminum oxide

We demonstrate that an ultra-thin layer of aluminum oxide can significantly enhance the emission efficiency of colloidal quantum dots on a Si substrate. For an ensemble of single quantum dots, our results show that this super brightening process can increase the fluorescence of CdSe quantum dots, forming well-resolved spectra, while in the absence of this layer the emission remains mostly at the noise level. We demonstrate that this process can be further enhanced with irradiation of the quantum dots, suggesting a significant photo-induced fluorescence enhancement via considerable suppression of non-radiative decay channels of the quantum dots. We study the impact of the Al oxide thickness on Si and interdot interactions, and discuss the results in terms of photo-induced catalytic properties of the Al oxide and the effects of such an oxide on the Coulomb blockade responsible for suppression of photo-ionization of the quantum dots.

Suppression of quantum decoherence via infrared-driven coherent exciton-plasmon coupling: Undamped field and Rabi oscillations

We show that when a semiconductor quantum dot is in the vicinity of a metallic nanoparticle and driven by a mid-infrared laser field, its coherent dynamics caused by interaction with a visible laser field can become free of quantum decoherence. We demonstrate that this process, which can offer undamped Rabi and field oscillations, is the result of coherent normalization of the “effective” polarization dephasing time of the quantum dot (T2*). This process indicates formation of infrared-induced coherently forced oscillations, which allows us to control the value of T2* using the infrared laser. The results offer decay-free ultrafast modulation of the effective field experienced by the quantum dot when neither the visible laser field nor the infrared laser changes with time.

Probing the structural dependency of photoinduced properties of colloidal quantum dots using metal-oxide photo-active substrates

We used photoactive substrates consisting of about 1 nm coating of a metal oxide on glass substrates to investigate the impact of the structures of colloidal quantum dots on their photophysical and photochemical properties. We showed during irradiation these substrates can interact uniquely with such quantum dots, inducing distinct forms of photo-induced processes when they have different cores, shells, or ligands. In particular, our results showed that for certain types of core-shell quantum dot structures an ultrathin layer of a metal oxide can reduce suppression of quantum efficiency of the quantum dots happening when they undergo extensive photo-oxidation. This suggests the possibility of shrinking the sizes of quantum dots without significant enhancement of their non-radiative decay rates. We show that such quantum dots are not influenced significantly by Coulomb blockade or photoionization, while those without a shell can undergo a large amount of photo-induced fluorescence enhancement via such blockade when they are in touch with the metal oxide.

Ultrafast dynamics induced by coherent exciton–plasmon coupling in quantum dot-metallic nanoshell systems

We study ultrafast coherent-plasmonic dynamics of hybrid systems consisting of one semiconductor quantum dot and one metallic nanoshell when they interact with a laser field with a step-like amplitude rise. It is shown that such dynamics is generated when quantum coherence in these systems can generate a retarded super-enhanced local field. This process happens in the picosecond range when the applied laser field ceases to be time-dependent. We show such a field generates a strong impulse, leading to a dramatic upheaval of the collective properties of the system. These include ultrafast oscillations of the effective transition energy and linewidth of the quantum dot, and generation of a polarization pulse. Within this pulse the Forster resonance energy transfer from the quantum dot to the nanoshell happens at a significantly high rate, while after that it is blocked nearly completely. We study the collective molecular resonances of this system using Rayleigh scattering and show how the frequency of the field impulse can be tuned. The intrinsic differences between such resonances and those involving spherical metallic nanoparticles are discussed.

Miniaturized Scanning Electron Microscope for In-Situ Planetary Studies

The exploration of remote planetary surfaces calls for the advancement of low-power, low-mass, highly-miniaturized instrumentation. Multi-functional instruments of this nature will prove to be particularly useful in preparation for human return to the moon, and in exploring increasingly remote locations in the Solar System. To this end, our group has been developing a miniaturized Scanning Electron Microscope (mSEM) capable of remote investigations of mineralogical samples through in-situ topographical and chemical analysis on a fine scale. Specifically, the fabrication and testing of a proof-of-concept assembly has begun, and consists of a cold-fieldemission electron gun and custom high-voltage power supply, electrostatic electronbeam focusing column, and scanning-imaging electronics plus backscatter electron detector. The functioning of an SEM is well known: an electron beam is focused down to nanometer- scale onto a given sample resulting in emissions such as backscattered and secondary electrons, x rays, and visible light. Raster-scanning the primary electron beam across the sample results in a fine-scale image of the surface topography (texture), crystalline structure and orientation, with accompanying elemental composition. The flexibility in the types of measurements the mSEM is capable of makes it ideally suited for a variety of applications. The mSEM is appropriate for use on multiple planetary surfaces, and for a variety of mission goals (from science to non-destructive analysis to in-situ resource utilization). The current status of the development and potential mSEM applications for planetary exploration are summarized here.

Quantum-biological control of energy transfer in hybrid quantum dot-metallic nanoparticle systems

We show theoretically that when a semiconductor quantum dot and metallic nanoparticle system interacts with a laser field, quantum coherence can introduce a new landscape for the dynamics of Forster resonance energy transfer (FRET). We predict adsorption of biological molecules to such a hybrid system can trigger dramatic changes in the way energy is transferred, blocking FRET while the distance between the quantum dot and metallic nanoparticle (R) and other structural specifications remain unchanged. We study the impact of variation of R on the FRET rate in the presence of quantum coherence and its ultrafast decay, offering a characteristically different dependency than the standard 1/R6. Application of the results for quantum nanosensors is discussed.

Control of photoinduced fluorescence enhancement of colloidal quantum dots using metal oxides

It is well known that irradiation of colloidal quantum dots can dramatically enhance their emission efficiencies, leading to so-called photoinduced fluorescence enhancement (PFE). This process is the result of the photochemical and photophysical properties of quantum dots and the way they interact with the environment in the presence of light. It has been shown that such properties can be changed significantly using metal oxides. Using spectroscopic techniques, in this paper we investigate emission of different types of quantum dots (with and without shell) in the presence of metal oxides with opposing effects. We observed significant increase of PFE when quantum dots are deposited on about one nanometer of aluminum oxide, suggesting such oxide can profoundly increase quantum yield of such quantum dots. On the other hand, copper oxide can lead to significant suppression of emission of quantum dots, making them nearly completely dark instantly.