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Tailoring Photoluminescence from Si-Based Nanocrystals Prepared by Pulsed Laser Ablation in He-N2 Gas Mixtures

DOI:10.3390/molecules25030440 期刊:Molecules 出版年份:2020 更新时间:2025-09-19 17:13:59
摘要: Using methods of pulsed laser ablation from a silicon target in helium (He)-nitrogen (N2) gas mixtures maintained at reduced pressures (0.5–5 Torr), we fabricated substrate-supported silicon (Si) nanocrystal-based ?lms exhibiting a strong photoluminescence (PL) emission, which depended on the He/N2 ratio. We show that, in the case of ablation in pure He gas, Si nanocrystals exhibit PL bands centered in the “red - near infrared” (maximum at 760 nm) and “green” (centered at 550 nm) spectral regions, which can be attributed to quantum-con?ned excitonic states in small Si nanocrystals and to local electronic states in amorphous silicon suboxide (a-SiOx) coating, respectively, while the addition of N2 leads to the generation of an intense “green-yellow” PL band centered at 580 nm. The origin of the latter band is attributed to a radiative recombination in amorphous oxynitride (a-SiNxOy) coating of Si nanocrystals. PL transients of Si nanocrystals with SiOx and a-SiNxOy coatings demonstrate nonexponential decays in the micro- and submicrosecond time scales with rates depending on nitrogen content in the mixture. After milling by ultrasound and dispersing in water, Si nanocrystals can be used as e?cient non-toxic markers for bioimaging, while the observed spectral tailoring e?ect makes possible an adjustment of the PL emission of such markers to a concrete bioimaging task.
作者: Anastasiya A. Fronya,Sergey V. Antonenko,Alexander Yu. Kharin,Andrei V. Muratov,Yury A. Aleschenko,Sergey I. Derzhavin,Nikita V. Karpov,Yaroslava I. Dombrovska,Alexander A. Garmash,Nikolay I. Kargin,Sergey M. Klimentov,Victor Yu. Timoshenko,Andrei V. Kabashin
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Investigating the photoluminescence (PL) emission properties of silicon nanocrystals prepared by pulsed laser ablation in He-N2 gas mixtures for bioimaging applications.

The addition of nitrogen to helium atmosphere during pulsed laser ablation of silicon target drastically changed PL properties of the prepared Si-based nanostructured films, enabling the generation of a five-fold stronger PL band in the green-yellow spectral range. This tuning opportunity for the PL properties looks very promising for projected bioimaging applications.

The study is limited to the characterization of PL properties of Si nanocrystals prepared by pulsed laser ablation in He-N2 gas mixtures. The potential bioimaging applications are suggested but not experimentally validated in this study.

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