lanthanum oxyfluoride nanostructures prepared by modified sonochemical method and their use in the fields of optoelectronics and biotechnology

Accepted Manuscript Original article Lanthanum oxyfluoride nanostructures prepared by modified sonochemical method and their use in the fields of optoelectronics and biotechnology C Suresh, H Nagabhushana, G.P Darshan, R.B Basavaraj, B Daruka Prasad, S.C Sharma, M.K Sateesh, J.P Shabaaz Begum PII: DOI: Reference: S1878-5352(17)30064-3 http://dx.doi.org/10.1016/j.arabjc.2017.03.006 ARABJC 2070 To appear in: Arabian Journal of Chemistry Received Date: Revised Date: Accepted Date: 17 September 2016 12 March 2017 15 March 2017 Please cite this article as: C Suresh, H Nagabhushana, G.P Darshan, R.B Basavaraj, B Daruka Prasad, S.C Sharma, M.K Sateesh, J.P Shabaaz Begum, Lanthanum oxyfluoride nanostructures prepared by modified sonochemical method and their use in the fields of optoelectronics and biotechnology, Arabian Journal of Chemistry (2017), doi: http://dx.doi.org/10.1016/j.arabjc.2017.03.006 This is a PDF file of an unedited manuscript that has been accepted for publication As a service to our customers we are providing this early version of the manuscript The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain Lanthanum oxyfluoride nanostructures prepared by modified sonochemical method and their use in the fields of optoelectronics and biotechnology C Suresh1, 2, H Nagabhushana1*, G P Darshan3, R B Basavaraj1, B Daruka Prasad4, S.C Sharma5, M.K Sateesh6, J.P Shabaaz Begum6 Prof C.N.R Rao Centre for Advanced Materials, Tumkur University, Tumkur- 572 103, India Department of Physics, Govt First Grade College, Tumkur -572 103, India Department of Physics, Acharya Institute of Graduate Studies, Bangalore 560 107, India Department of Physics, B M S Institute of Technology and Management, Affiliated to VTU, Belagavi, Bangalore 560 064, India Department of Mechanical Engineering Jain University, Advisor, Jain group of Institutions, Bangalore 560069, India Molecular diagnostics and Nanotechnology laboratories, Department of Microbiology and Biotechnology, Bangalore University, Bangalore -560 056, India * Corresponding author: +91- 9663177440, E-mail: bhushanvlc@gmail.com (H Nagabhushana) Abstract Dysprosium doped lanthanum oxyfluoride nanostructures were prepared by modified sonochemical method using Aloe Vera gel as a bio-surfactant The morphology of the product was systematically studied by varying different experimental parameters including concentration of surfactant, sonication time, pH and sonication power It was found that some of these above parameters play a key role in tuning the morphology of the product The photoluminescence studies exhibited characteristic emission peaks at ~ 483 nm, 574 nm and 674 nm attributed to 4F9/2→6H15/2, 4F9/2→6H13/2 and 4F9/2→6H11/2 transitions of Dy3+ ions respectively The optimal concentration of Dy3+ ions was found to be ~ mol % The photometric studies revealed that the prepared samples were quite useful for the fabrication of white light emitting diodes The optimized product was also tested for their capability as an antigen against the bacterial and fungal pathogens The present method of preparation may be scaled up easily to the larger production for industrial applications The optimized sample showed an effective visualization of latent fingerprints on various forensic relevant materials Keywords: Sonochemical method; Photoluminescence; Latent fingerprint; antimicrobial; antifungal 1 Introduction In the recent years, the development of white light-emitting diodes (WLEDs) replaced all the conventional incandescent or fluorescent lamps due to its long life time, high brightness, ecofriendly and high efficiency characteristics (Lin et al., 2011; Park et al., 2003; Im et al., 2009) The phosphors converted WLEDs (pc-WLEDs) consists of near ultraviolet chips which finds wide range of applications due to excellent color stability and reproducibility (Chen et al., 2012; Zhang et al., 2013) Commercially available pc-WLEDs constitutes of InGaN chip with Y3Al5O12:Ce3+ (YAG: Ce) phosphor suffers from low color rendering index and high correlated color temperature (CCT) due to the lack of red component in it (Hecht et al., 2009; Jung et al., 2006) Hence, rare earth doped particularly lanthanide-doped luminescent materials are considered to be an ideal hosts for better luminescence properties due to their high refractive index and low phonon energy Further, these materials created new avenues for researches due to their possible applications in various biomedical fields such as biological labels, biosensors, multimodal bio-imaging, photodynamic therapy and drug delivery etc (Ruirui Xing., 2016a; Ruiyun Zhang., 2016; Ruirui Xing., 2016b; Ruirui Xing., 2016c) Ruirui Xing synthesized functional hybrid multilayer films of collagen-capped gold nanoparticles by layer-by-layer assembly technique Prepared samples showed efficient regulating cell growth and detachments (Ruirui Xing., 2016d) So far, various synthesis routes were used including solution combustion, sol – gel, co- precipitation, solid state reaction, hydrothermal methods etc (Hu et al., 1999; Xia et al., 2009; Gai et al., 2014; Tana et al., 2011; Kaczmarek et al., 2013) Morphologies of the compounds not only control their properties but also enhance the effectiveness for the various applications (Alivisatos, 1996) However, in some of these routes it is difficult to control over the morphology, size and stoichiometric compositions Therefore, a lot of research has been needed for the improvement of versatile synthesis routes Ultrasound assisted sonochemical route was considered to be one of the better synthesis route for fabrication of well-defined nano/superstructured materials In this method, during the synthesis, ultrasound irradiation provides remarkable reaction conditions to initiate the chemical reaction (Suslick, 1990) The impact of the ultrasound force to acoustic cavitation leads to the formation, growth and implosive collapse of bubbles of the reaction mixture leads to superstructures (Suslick, 1996) Generally fingerprints (FPs) encompasses a mixture of substances originating from the sweat glands namely epidermis, secretory glands in the dermis along with intrinsic components including drugs, medication traces, metabolites and extrinsic contaminants namely blood, food contaminants, dirt and grease, hair and moistures (Darshan et al., 2016a) The ridge arrangement of the skin on human finger create a distinctive FP By touching an object, sweat emitted through the pores in the skin can be moved to the surface to leave an impression of the ridge pattern Such invisible prints were recognized as a Latent finger prints (LFPs) which are useful for the recognition and detection of individuals at forensic science For the past few decades, various visualization methods were established to enhance LFPs Nevertheless, there still exist a lack of sensitivity and selectivity (Saif, 2013) Presently nanoparticles were utilized in forensic investigations due to small crystalline size, flexibility and ability to precisely tune their surface properties The surface modification versatility of these materials may lead to accurate targeting and to increase selectivity (Cadd et al., 2015) Powder dusting was simple and most frequently used method for revealing the LFPs (Champod et al., 2004) in which powder of bronze, ferric oxide and rosin were used These powders were unable to reveal LFPs on some relevant forensic surfaces as it was hazardous and uneven crystallite size Alternatively, use of powder-based luminescent nanophosphors was the best solution to conquer such limitations Rare earth doped nanophosphors have been C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an extensively investigated as a potential labeling agents to visualize LFPs with high contrast, good sensitivity and reduced background hindrance due to smaller crystallite size and better adhesion efficiency (Darshan et al., 2016 b) Furthermore, it was well established that the lanthanide ions were bio-compatible with low toxicity Therefore, use of stable synthesized LaOF: Dy3+ in powder dusting method creates a significant interest for scientific community to visualize the LFPs as a labeling agents The present work describes the synthesis of LaOF: Dy3+ (1-11 mol %) nanostructures (NS) by facile ultrasound assisted sonochemical route using A.V gel as bio-surfactant The effectiveness and unique properties of ultrasound for the fabrication of nanostructured materials was successfully explored Further, to evaluate the potential applications of the prepared samples, the photoluminescence (PL) and photometric properties (CIE and CCT) were studied in detail The optimized sample was used as a labeling agent for the visualization of LFPs on various forensic relevant surfaces Experimental 2.1 Synthesis The precursors used for the preparation of LaOF NS were of analytical grade without further purification The chemicals used were lanthanum nitrate [La (NO3)3.4H2O (Sigma Aldrich; 99.9 %)], ammonium fluoride [NH4F; (Sigma Aldrich; 99.9 %)] and dysprosium nitrate [Dy (NO3)3; (Sigma Aldrich; 99.9 %)] A.V gel was used as a bio-surfactant and the detailed preparation procedure for obtaining A.V gel from aloe vera plant was reported elsewhere (Kavyashree et al., 2015) Stoichiometric quantities of the precursors and 50 ml of A.V gel (bio-surfactant) and 150 ml of double distilled water were dissolved and mixed using magnetic stirrer for ~ 25 to get a clear solution Resulting mixture was divided into various wt% from 5% to 30% W/V and subjected to sonochemical treatment with the help of Mrc Laboratory equipment model-AC 120H, probe, ultrasonic frequency of ~ 20 kHz, power Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an of ~ 300 W and sonication time ~ - h at a fixed temperature of 80 C NaOH was used as a precipitating agent and used to adjust pH value The precipitate obtained at the end of the reaction was filtered several times using double distilled water and alcohol The powder was dried at 80 C for h in a hot air oven and then heat treated at ~ 700 oC for h The schematic illustration for the ultrasound assisted sonochemical synthesis was shown in Fig.1 2.2 Characterization Phase purity and structural analysis of the product was done by using Shimadzu made powder X-ray diffractometer (PXRD) Morphology was examined by Hitachi scanning electron microscopy (SEM) Particle size was determined by Hitachi (H-8100) made transmission electron microscope (TEM) equipped with EDAX The Fourier transform infrared (FTIR) studies were done by Perkin Elmer Spectrometer (Spectrum 1000) The DRS of the samples was recorded on Lambda-35, Perkin Elmer spectrophotometer Jobin Yvon Spectroflourimeter Fluorolog-3 was used for photoluminescence (PL) studies 2.3 Visualization of LFPs by using LaOF: Dy3+ (3 mol %) NS The fresh FPs were deposited on various surfaces including glass, CD, mobile screen, marble, computer mouse and pet bottle Before deposition, the standard procedure was followed to get the finger prints as reported elsewhere (Darshan, G.P et al., 2016) The optimized (3 mol %) NS were smoothly applied on the LFPs by powder dusting method and excess powder was removed by smooth brushing A Nikon D3100/ AF-S Nikkor 50 mm f/1.8G ED lens digital camera and a 254 nm UV light was used for the visualization of FPs The schematic representation for the revelation of LFPs was shown in Fig.2 2.4 Evaluation of bactericidal activity of LaOF: Dy3+nanostructures against Test micro organisms Test Microorganisms and reference strain Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an Four American Type Culture Collection (ATCC) (Table 1), registered bacterial isolates were used for bactericidal activity of A.V gel mediated LaOF: Dy3+ NS All the glassware’s were sterilized by autoclaving at 121 °C for 15 m before using in the assay In the present investigation, four bacteria were cultured on Mueller-Hinton agar (Hi-Media, Mumbai, India) and plates were incubated for 24 h in aerobic conditions at 37 °C A single colony from the stock bacterial culture was used for preparing the bacterial suspensions 20 ml of sterile Mueller-Hinton broth and 100 ml Erlenmeyer flask were inoculated and these were kept in a shaker at 200 rpm for 24 ± h and again incubated at ~ 37 °C Further, an optical density of McFarland of 0.5 (1 × 108 CFU/mL) with bacterial suspension was made separately with isotonic solution of NaCl (0.85%) Later, the bacterial suspension was diluted ten times (1 × 107 CFU/mL) and used as inoculum in testing for bactericidal activity 2.5 Determination of Minimum Inhibitory Concentration (MIC) and Minimum Bactericidal Concentration (MBC) by Micro broth dilution method The MIC was determined by employing Clinical and Laboratory Standards with some slight modifications using 96 well micro broth dilution plate and bacterial strains concentration A stock suspension was obtained by suspending the prepared of LaOF: Dy3+ NS in milli-Q water to meet a final concentration 100 µg/mL (Balouiri et al., 2016) Then the aliquot was mixed with Mueller-Hinton broth for subsequent experiments Further, bacterial strains were exposed to LaOF: Dy3+ (3 mol %) NS ranging from 25 to 0.000025 μg/mL in ten-fold dilution series The similar procedure was employed for determination of MIC for both positive (tetracycline-25 μg/mL) and negative (sterile Mueller-Hinton broth without NS) controls 20 μL of the bacterial suspension was added to each microtitre well and incubated at 37 °C for 24 h To obtain better results, all the experiments were repeated in triplicates Afterward, MIC values of the NS were revealed by adding 25 μL of iodonitrotetrazolium Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an chloride (INT at 0.5 mg/mL) in each well after 24 h The microtitre plates were additionally incubated at 37 °C for 60 m MICs of test compounds were resolved for the lowest concentration of NS or drug that restricted the color change from colorless to red MBC determined by subculting of 50 μL cultured suspension (without INT) by streaking on Mueller-Hinton (MH) agar in petriplate and later incubated for 24 h at 37 °C MBC was the lowest concentration that completely stops the bacterial growth on MH agar surface 2.6 Evaluation of Antifungal Activity of LaOF: Dy3+ (3 mol %) NS F oxysporum, phytopathogenic fungi of tomato blight was procured from the culture collection at Centre of the Molecular Diagnostics Laboratory, Department of Microbiology and Biotechnology, Bangalore University, Bangalore, India The F oxysporum was grown on SDA at 25 ± 10 °C and incubated with alternative cycle of 12 h (dark and light) Evaluation of antifungal activity was performed by the food poison technique with slight modifications The sterilized SDA media was amended with synthesized NS of different concentrations (100 μg/mL, 300 μg/mL, 500 μg/mL, 700 μg/mL and 900 μg/mL) The medium without NS (control) were decanted into the petri dishes The mycelial agar disc (5 mm) was bored aseptically with the help of sterile cork-borer for days Such mycelial agar was inoculated to each petri dish containing different concentrations of synthesized NS and control media (without NS) All the Petri dishes were incubated for days at 25 ± °C The antifungal activity of LaOF: Dy3+ NS on F oxysporum was determined by measuring the radial growth (in cm) Further, antifungal activities of NS were compared with traditional fungicide bavistin (carbendazim) The antifungal effect of nanoparticles was determined as mentioned below Percent inhibition of F oxysporum growth  dc - dt 100 dc - (1) where dc ; the average increase in F oxysporum growth (control) and dt ; the average increase in F oxysporum growth (tested samples) Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an 2.7 Statistical Analysis The antifungal experimental data was analyzed by mean ± SE subjected to multivariate analysis Further, the mean ± SE separated by Duncan’s multiple range test at 0.5 significance (P < 0.05) using SPSS software (version 19) Results and discussion PXRD profiles of pure and Dy3+ (1-11 mol %) doped LaOF NS was shown in Fig.3 (a) All the patterns exhibit sharp and broad diffraction peaks and well matched with the standard JCPDS card No.89-5168 (Dhananjaya et al., 2016) Further, no impurity peaks were observed with increase of Dy3+ concentration indicating that the product was pure The broad diffraction peaks in the present studies was normally associated with crystallite size or strain present in the prepared sample Debye – Scherrer’s relation was utilized to determine the average crystallite sizes as reported elsewhere (Venkataravanappa et al., 2016a) In order to compare the crystallite sizes as well as strain present in the sample W – H plots were utilized and the obtained plots is given in Fig.3 (b) (Venkataravanappa et al., 2017b) Further, the estimated average crystallite size as well as the lattice strains were given in Table As can be evident from the table the lattice strain was found to be increase with Dy3+ concentration due to lattice distortion (Nagabhushana et al., 2016) Rietveld refinement method was used to evaluate the various structural parameters namely Pseudo-Voigt profile function (u, v and w), isothermal temperature factors (B iso), backgrounds scale factor, atomic coordinates etc (Daruka Prasad et al., 2014) The observed, calculated and the difference PXRD profiles of LaOF: Dy3+ (3 mol %) was shown in Fig (c) The experimental and calculated profiles showed nearly to zero in the intensity scale as illustrated by a line (Y obs–Ycalc) The refined structural parameters for LaOF: Dy3+ (1- 11 mol %) NS was summarized in Table It was noticed that a slight variation in structural Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an parameters with addition of Dy3+ ions in LaOF The acceptable percentage difference between Dy and La in LaOF matrix was estimated using the relation (Darshan et al., 2016c): Dr  Rm  Rd Rm - (2) where Rm and Rd; radii of host material and dopant ion respectively The estimated value of Dr was found to be ~ 25 % Further it was clear that the dopant Dy3+ substituted into La3+ ions in LaOF host lattice From the Diamond software, packing diagram was simulated by using the refined lattice parameters as well as atomic positions and shown in Fig.3 (d) It was evident that La3+/ Dy3+ ions were co-ordinate by four oxide and four fluoride anions as well as occupy the six-fold 6cWyckoff positions and the symmetry for La3+ ions was C3v (Dhananjaya et al., 2016) Fig.4 shows the SEM micrographs of LaOF: Dy3+ (3 mol %) NS prepared at different sonication times (1 – h) with 30 ml of A.V gel and pH = When the sonication time was ~1 h, all the structures appear to be almost spherical in shape and form a network structure (Fig.4 (a & b)) When the sonication time was increased to h, it forms a spherical shaped network structure derive together to form a layer like structure consist of several hollow pores (Fig (c & d)) Further, when the sonication time was increased to and h, pores were found to be reduced (Fig.4 (e, f)) Finally, when the sonication time was further increased to and h, these hollow pores were almost reduced (Fig.4 (g, h)) The effect of concentration of bio - surfactant (A.V gel) on the morphology of the prepared samples was also studied and was shown in Fig.5 Initially, when the A.V gel concentration was ~ ml small plate like structures were observed (Fig.5 (a)) When the concentration of A.V gel was increased to 10 and 15 ml, the plate like structures were oriented in multi directions (Fig.5 (b & c)) Further when the A.V gel concentration increased to 20 and 30 ml, plate like structures were undergoing self – assembly in a particular direction (Fig.5 (d & e)) Table shows the list of Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an a) b) mm mm c) d) mm mm e) f) mm mm Figure.17 Finger print images visualized by using LaOF: Dy3+ (3 mol %) NS on (a) glass (b) marble (c) computer mouse (d) CD (e) mobile screen and (f) PET bottle 39 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an Sweat pores Core Termination Island Bifurcation Bridge Hook Figure.18 High-resolution fluorescence image of finger print The magnified images shows minutiae ridge patterns (1) core, (2) termination, (3) bifurcation, (4) island, (5) bridge, (6) Hook and (7) sweat pores a) b) mm mm 40 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an Figure.19 Fingerprint images visualized by LaOF: Dy3+ (3 mol %) NS (a) loop and (b) Whorl Figure.20 Antibacterial activity of LaOF: Dy3+ (3 mol %) NS synthesized using different concentrations A.V gel (A-1 %, B-3 %, C-5 %, D-7 %, E-9 %, F-11 %) on effects bacterial & fungal pathogens 41 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an Figure.21 Antifungal effect of LaOF: Dy3+ (3 mol %) NS on F oxysporum (Concentration in µg/ml) 42 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an % of fungal growth inhibition 100 90 80 70 60 50 40 30 20 10 100 200 300 400 500 600 700 PC NC Concentration µg/mL Fig.22.The effective inhibition of Fusarium oxysporum by LaOF: Dy3+ (3 mol %) NS by dose dependent manner Table 1: Four reference strains of bacteria used for evaluation of bactericidal activity LaOF: Dy3+ (3 mol %) NS Bacteria Gram reaction Gram Negative Gram Negative Gram Negative Escherichia coli Klebsiellapneumoniae Pseudomonas aerguinosa Gram Positive Staphylococcus aureus 43 Strain Number ATCC 8739 ATCC 13883 ATCC 9027 ATCC 6538 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an Table 2: Estimated crystallite size, micro strain, lattice strain, dislocation density, stacking fault and energy gap (Eg) values of LaOF: Dy3+ (1-11 mol %) NS Micro Strain (x 10-4) Lattice strain є (10−3) 33 1.06 3.19 6.24 0.45 4.13 29 38 1.11 2.76 10.33 0.42 4.36 30 35 1.06 2.62 6.91 0.46 4.17 32 30 1.08 3.34 9.14 0.43 4.29 28 37 1.18 3.14 12.11 0.44 4.25 11 26 34 1.19 3.18 9.61 0.40 4.53 Crystallite size(nm) Dy3+ conc (mol %) D-S relation 26 W-H plots 44 Dislocation density δ Stacking (1014) Fault −2 lin m ) (mJm-2) Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn Eg (eV) C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an Table 3: Rietveld refinement parameters of LaOF: Dy3+ (1- 11 mol %) NS Crystal system Tetragonal Space group P 4/n mm Hall symbol P 4ab 2ab -1ab Lattice parameters (Å) 1mol % mol % mol % mol % mol % 11mol % a=b 4.0794 4.0798 4.0766 4.0758 4.0701 4.0699 c 5.8196 5.8213 5.8146 5.8050 5.8005 5.8053 Unit cell volume (Å3) 96.845 96.895 96.629 96.432 96.090 96.157 ATOMIC COORDINATES La x 0.0000 0.0000 0.0000 0.0000 0.0000 0.0000 y 0.5000 0.5000 0.5000 0.5000 0.5000 0.5000 z 0.7791 0.7781 0.7801 0.7774 0.7761 0.7787 x 0.0000 0.0000 0.0000 0.0000 0.0000 0.0000 y 0.0000 0.0000 0.0000 0.0000 0.0000 0.0000 z 0.5000 0.5000 0.5000 0.5000 0.5000 0.5000 O 45 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an F x 0.0000 0.0000 0.0000 0.0000 0.0000 0.0000 y 0.0000 0.0000 0.0000 0.0000 0.0000 0.0000 z 0.0000 0.0000 0.0000 0.0000 0.0000 0.0000 RP 5.08 4.87 5.75 6.11 6.03 5.60 RWP 6.64 6.49 7.60 8.10 7.86 7.15 RExp 6.68 6.63 8.12 8.39 8.16 7.87 2 0.99 0.96 0.88 0.93 0.93 0.82 GoF 0.99 0.98 0.95 0.97 0.96 0.91 RBragg 9.27 5.87 7.22 7.24 7.85 8.62 RF 9.80 6.13 6.02 4.28 12.40 8.37 X-ray density (g/cc3) 5.86 5.96 5.98 5.81 6.01 6.01 Table 4: List of major phytochemicals extracted in A V gel confirmed from GCMS Name Molecular Weight Molecular formula Tetracontane 562 C40H82 Guanosine 283 C10H13N5O5 Ethanone, 1-Phenyl 120 C8H8O Pentadecanoic Acid 242 C15H30O2 46 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an Table 5: Photometric parameters of LaOF: Dy3+ (1-11 mol %) NS Dy3+ Concentration (mol %) CIE CP (%) CCT (K) X Y 0.3439 0.4159 30 5059 0.3783 0.4286 41 4341 0.3567 0.4192 34 4832 0.3483 0.4158 31 5050 0.3230 0.4053 25 5802 11 0.3336 0.4088 26 5466 47 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an Table 6: Evaluation of bactericidal activity of LaOF: Dy3+ (3 mol %) NS on pathogenic bacteria with different concentration of A.V gel Bacteria E coli K pneumoniae P aeruginosa S aureus A.V gel concentration MIC 1% 0.25 3% 2.5 5% 2.5 7% 2.5 9% 2.5 11 % 2.5 MBC 2.5 25 25 25 25 25 MIC 0.025 0.25 0.25 2.5 2.5 2.5 MBC 0.25 2.5 2.5 25 25 25 MIC 0.025 0.25 0.25 2.5 2.5 2.5 MBC 0.25 2.5 2.5 25 25 25 MIC 0.25 2.5 2.5 2.5 2.5 2.5 MBC 2.5 25 25 25 25 25 48 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an Table 7: The A.V gel concentration dependent antifungal effect of LaOF: Dy3+ (3 mol %) NS against F oxysporum Concentration in µg/ml (LaOF: Dy3+ (3 mol %)) Percent Inhibition (Mean ± standard error) 100 12.10 ± 0.1143 200 26.52 ± 0.0583 300 46.19 ± 0.0639 400 71.41 ± 0.0583 500 81.21 ± 0.0577 600 86.38 ± 0.0639 700 93.92 ± 0.0578 POSITIVE CONTROL 100 NEGATIVE CONTROL 49 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an Research highlights  Modified sonochemical method was used for the synthesis of LaOF: Dy3+  Superstructure morphologies were obtained by tuning the experimental parameters  CIE and CCT results exhibit that the compounds were useful in wLED’s  Prepared compounds exhibited superior antibacterial and antifungal activities  The optimized compound was effectively used for forensic applications 50 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn C.33.44.55.54.78.65.5.43.22.2.4 22.Tai lieu Luan 66.55.77.99 van Luan an.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.C.33.44.55.54.78.655.43.22.2.4.55.22 Do an.Tai lieu Luan van Luan an Do an.Tai lieu Luan van Luan an Do an F9/2-6H13/2 F9/2-6H11/2 F9/2-6H15/2 450 500 550 600 650 Wavelength (nm) 51 Stt.010.Mssv.BKD002ac.email.ninhd 77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77.77.99.44.45.67.22.55.77.C.37.99.44.45.67.22.55.77t@edu.gmail.com.vn.bkc19134.hmu.edu.vn.Stt.010.Mssv.BKD002ac.email.ninhddtt@edu.gmail.com.vn.bkc19134.hmu.edu.vn (m Co D y 3+ 11 nc ol %) LaOF:Dy3+ Exci = 354 nm PL Intensity (a.u.) 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