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Light management with quantum nanostructured dots-in-host semiconductors

ABSTRACT: Insightful knowledge on quantum nanostructured materials is paramount to engineer and exploit their vast gamut of applications. Here, a formalism based on the single-band effective mass equation was developed to determine the light absorption of colloidal quantum dots (CQDs) embedded in a wider bandgap semiconductor host, employing only three parameters (dots/host potential barrier, effective mass, and QD size). It was ascertained how to tune such parameters to design the energy level structure and consequent optical response. Our findings show that the CQD size has the biggest effect on the number and energy of the confined levels, while the potential barrier causes a linear shift of their values. While smaller QDs allow wider energetic separation between levels (as desired for most quantum-based technologies), the larger dots with higher number of levels are those that exhibit the strongest absorption. Nevertheless, it was unprecedently shown that such quantum-enabled absorption coefficients can reach the levels (104–105 cm−1) of bulk semiconductors. Development of a simple yet insightful model to understand the optical behavior of dots-in-host semiconductors. Unprecedentedly shown that quantum-enabled absorption coefficients can reach levels close to that of bulk semiconductors.

SUBMITTER: Alexandre M

PROVIDER: S-EPMC8595380 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:The rapid emergence of superbugs, or multi-drug resistant (MDR) organisms, has prompted a search for novel antibiotics, beyond traditional small-molecule therapies. Nanotherapeutics are being investigated as alternatives, and recently superoxide-generating quantum dots (QDs) have been shown as important candidates for selective light-activated therapy, while also potentiating existing antibiotics against MDR superbugs. Their therapeutic action is selective, can be tailored by simply changing their quantum-confined conduction-valence band (CB-VB) positions and alignment with different redox half-reactions-and hence their ability to generate specific radical species in biological media. Here, we show the design of superoxide-generating QDs using optimal QD material and size well-matched to superoxide redox potential, charged ligands to modulate their uptake in cells and selective redox interventions, and core/shell structures to improve their stability for therapeutic action. We show that cadmium telluride (CdTe) QDs with conduction band (CB) position at -0.5 V with respect to Normal Hydrogen Electron (NHE) and visible 2.4 eV bandgap generate a large flux of selective superoxide radicals, thereby demonstrating the effective light-activated therapy. Although the positively charged QDs demonstrate large cellular uptake, they bind indiscriminately to cell surfaces and cause non-selective cell death, while negatively charged and zwitterionic QD ligands reduce the uptake and allow selective therapeutic action via interaction with redox species. The stability of designed QDs in biologically-relevant media increases with the formation of core-shell QD structures, but an appropriate design of core-shell structures is needed to minimize any reduction in charge injection efficiency to adsorbed oxygen molecules (to form superoxide) and maintain similar quantitative generation of tailored redox species, as measured using electron paramagnetic resonance (EPR) spectroscopy and electrochemical impedance spectroscopy (EIS). Using these findings, we demonstrate the rational design of QDs as selective therapeutic to kill more than 99% of a priority class I pathogen, thus providing an effective therapy against MDR superbugs.

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Light management with quantum nanostructured dots-in-host semiconductors

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