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Radioluminescence Properties of the Cdse/Zns Quantum Dots

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Radioluminescence Properties of the Cdse/Zns Quantum Dots *Manuscript Click here to view linked References 1 2 3 4 5 6 Radioluminescence properties of the CdSe/ZnS 7 8 9 10 Quantum Dot nanocrystals with analysis of long-memory 11 12 13 trends. 14 15 16 17 D. Nikolopoulosa, I. Valaisb,*, C. Michailb, A. Bakasc, C. Fountzoulad, D. Cantzose, D. 18 19 Bhattacharyyaf, I. Sianoudisg, G. Fountosb, P. Yannakopoulosa, G. Panayiotakish and I. 20 21 b 22 Kandarakis 23 a 24 Piraeus University of Applied Sciences, Department of Electronic Computer Systems 25 26 Engineering, Petrou Ralli & Thivon 250, GR-12244 Aigaleo, Greece 27 28 29 b Radiation Physics, Materials Technology and Biomedical Imaging Laboratory, 30 31 32 Department of Biomedical Engineering, Technological Educational Institute of Athens, 33 34 Egaleo, 122 10 Athens, Greece 35 36 c 37 Department of Medical Radiologic Technology, Technological Educational Institute of 38 39 Athens, 122 10 Athens, Greece 40 41 42 d Department of Medical Laboratories Faculty of Health and Caring Profession, 43 44 45 Technological Educational Institute of Athens, 122 10 Athens, Greece 46 47 ePiraeus University of Applied Sciences (TEI of Piraeus), Department of Automation 48 49 50 Engineering, Petrou Ralli & Thivon 250, GR-12244 Aigaleo, Greece 51 52 f Cranfield University, Surface Engineering and Nanotechnology Institute, Bedfordshire, 53 54 55 MK43 0AL, United Kindom 56 57 58 59 60 61 -1- 62 63 64 65 1 2 3 4 5 g Department of Optics and Optometry, Technological Educational Institute of Athens, 122 6 7 8 10 Athens, Greece 9 10 h University of Patras, School of Medicine, Department of Medical Physics, GR-15310, 11 12 13 Rion, Greece 14 15 16 17 18 ABSTRACT 19 20 21 This paper reports radioluminescence properties of the CdSe/ZnS quantum dots. Three quantum dot samples 22 23 were prepared with concentrations 14.2x10-5 mg/mL, 21.3x10-5 mg/mL and 28.5x10-5 mg/mL, respectively. 24 25 The ultraviolet induced emission spectra of CdSe/ZnS dots exhibited a peak at 550 nm ranging between 450 26 27 nm and 650 nm. Discrepancies observed between 250 nm and 450 nm were attributed to the solvent and 28 29 cuvette. The absolute efficiency calculated from random fractional-Gaussian luminescence segments varied. 30 31 Long-memory fractional-Brownian segments were also found. The quantum dot solution with concentration 32 33 of 21.3 x10-5 mg/mL exhibited the maximum absolute efficiency value at 90 kVp. The CdSe/ZnS dots have 34 35 demonstrated potential for detection of X-rays in the medical imaging energy range. 36 37 38 39 40 Corresponding author. 41 42 43 E-mail address: [email protected] (I. Valais) 44 45 46 47 KEYWORDS: Quantum Dots; Absolute Luminescence Efficiency; CdSe/ZnS 48 49 50 51 52 53 54 55 56 57 58 59 60 61 -2- 62 63 64 65 1 2 3 4 5 1. Introduction 6 7 8 9 10 Radiation based Medical Imaging (RMI) has facilitated several fields of medicine by 11 12 13 achieving increased levels of diagnostic accuracy. However, despite the on-going progress 14 15 in RMI, it remains entangled to accomplish low-cost designs of enhanced image quality 16 17 18 and low radiation risk to human (Van Eijk, 2008). Both, the experimental and the 19 20 computational techniques, offer an extensive methodology to incorporate new and 21 22 innovative RMI designs, especially, in the modalities which utilise radiation sensors 23 24 25 (Knoll, 2010). The current approaches aim to employ new fast light-emitting materials 26 27 with efficient coupling to state-of-the art optical sensors (Michail, 2015a). In particular, the 28 29 30 new methods look promising to integrate novel nanophosphors with appealing 31 32 characteristics, well-established Complementary Metal Oxide Semiconductors (CMOS), 33 34 35 e.g. Si-CMOS-based technology (Seferis et al., 2013, Michail et al., 2015b) and Quantum 36 37 Dots (QDs) as gain materials (Krasnyj et al., 2007, Del Sordo et al., 2009, Hobson et al., 38 39 40 2011). The related research extends both at the spectral emission and the radiation 41 42 detection domains (Michail et al., 2007, Michail et al., 2014a, David et al., 2016). Apart 43 44 from X-ray imaging, the phosphor-based sensing materials have been employed also in 45 46 47 optoelectronic devices, nuclear medicine, dosimetry and in high energy physics 48 49 experiments (Beierholm et al., 2008, Valais et al., 2010, Kobayashi et al., 2012, Yanagida 50 51 52 et al., 2014). It becomes evident that the radiation sensors constitute critical structural parts 53 54 of detectors of RMI systems (Blasse and Grabmaier, 1994, Kandarakis and Cavouras 2001, 55 56 57 Rodnyi, 2001, Doi, 2006, Gupta et al., 2006, Ross et al., 2006, Van Eijk, 2008, Yaffe et al., 58 59 60 61 -3- 62 63 64 65 1 2 3 4 5 2008, Michail et al., 2013, 2014b, David et al., 2016). Optimisation of existing RMI 6 7 8 materials can be achieved by introducing new materials of higher radiation efficiency and 9 10 better optical properties (Blasse and Grabmaier, 1994, Seferis et al., 2014, Prochazkova et 11 12 13 al., 2016). Simultaneously, the novel designs need to be explored through a combination of 14 15 modelling and experimentation. Noteworthy advances in this field of research include the 16 17 18 construction of sensors of small size (Rodnyi, 2001, Michail et al., 2015a), nanophosphors 19 20 (Kalyvas et al., 2011, Seferis et al., 2014, 2015) and QDs (Zych et al., 2003, Kim et al., 21 22 2007, Konstantatos et al., 2007, Del Sordo et al., 2009, Rauch et al., 2009, Stodilka et al., 23 24 25 2009, Baharin et al., 2010, Malyukin, 2010, Hobson et al., 2011, Konstantatos and Sargent, 26 27 2011, Lawrence et al., 2012). QDs resemble particle size of the order of 1nm-20nm 28 29 30 (Goncharova et al., 2004). Due to their unique optical and electrical properties they have 31 32 been already utilised in optoelectronic sensors (Guo et al., 2000, Eychmuller, 2000, Ma et 33 34 35 al., 2003, Wang et al., 2006, Gbur et al., 2013), as radiation sensors (Sordo et al., 2009, 36 37 Stodilka et al., 2009, Baharin et al., 2010, Hobson et al., 2011, Nistor et al., 2013, Sahi and 38 39 40 Chen 2013) and theranostics in nuclear medicine (Assadi et al., 2011). Recent studies 41 42 suggest also that QDs can be employed in optical diffusion applications of high sensitivity 43 44 (e.g. in nuclear medical imaging), nuclear physics to X-ray and gamma-ray astronomy 45 46 47 (Pang et al., 2005, Voitenko et al., 2007, Del Sordo et al., 2009, Klassen et al., 2009, Xing 48 49 et al., 2009), as well as in modalities where high light spatial resolution is required (e.g. in 50 51 52 X-ray projection medical imaging) (Kandarakis et al., 2005, Jacobsohn et al., 2007, Del 53 54 Sordo et al., 2009, Stodilka et al., 2009, Baharin et al., 2010, Hobson et al., 2011, Seferis et 55 56 57 al., 2014, 2015). 58 59 60 61 -4- 62 63 64 65 1 2 3 4 5 QDs can be grouped also as semiconductor sensors that have progressed during the last 6 7 8 decade. Moreover, QD-polymer composite films scintillate upon exposure to ionising 9 10 radiation (Dai et al., 2002, Letant and Wang, 2006a, 2006b), and this has been attributed to 11 12 13 the transportation of charge within the QD polymer host, where the electron and hole 14 15 localise and recombine to emit light (Lawrence et al., 2012). 16 17 18 As can be deduced, there is noteworthy scientific scope for studying the detection 19 20 capabilities of QDs as potential semiconductor nanosensors of ionising radiation in RMI 21 22 applications. Nevertheless, despite the relevant scientific evidence, only some 23 24 25 investigations have dealt with the application of QDs as ionising radiation sensors (Dai et 26 27 al., 2002, Letant and Wang, 2006a, 2006b, Cevik et al., 2008, Waheed et al., 2009, 28 29 30 Lawrence et al., 2012, Sahi and Chen, 2013) and even less (Baharin et al., 2010, Hobson et 31 32 al., 2011, Lawrence et al., 2012, Valais et al., 2015) for potential uses in RMI. In the above 33 34 35 consensus, this paper has focused on the radiation detection properties of Cadmium 36 37 Selenide/Zinc Sulfide (CdSe/ZnS) core-shell type QDs for potential technological 38 39 40 applications in X-ray radiology and for radiation safety monitoring e.g. in X-ray RMI 41 42 installation rooms or in the natural radiation environment. The investigation was 43 44 multidirectional in the sense that different experimental and computational techniques were 45 46 47 utilised in order to explore possible factors which might affect the optical response of QDs 48 49 after X-ray irradiation. The paper firstly reports various measurements and calculations of 50 51 52 luminescence spectra after excitation of QDs by two types of ultraviolet (UV) lamps. The 53 54 luminescence efficiency (LE) of different QD solutions is then reported, after their 55 56 57 irradiation to X-rays generated by a diagnostic radiology RMI unit. Since the X-ray 58 59 60 61 -5- 62 63 64 65 1 2 3 4 5 irradiation employs several factors (high voltage generator, type, motion and status of the 6 7 8 anode, collimator arrangements, filter, phototimers, general irradiation-handling electronic 9 10 circuits (Doi, 2006) and the light detection is multilevel (photomultiplier tube, integration 11 12 13 sphere, analog-to-digital converters, light-to-current measurement etc.
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