Abstract

Highly luminescent CdS nanocrystals (NCs) grown in a dielectric (borosilicate glass) matrix have been synthesized by the melt quenching technique. NC sizes are varied by controlling the post thermal treatment durations in the glass matrix and their optical properties have been investigated. The sizes of the CdS NCs calculated from the transmission electron microscopic (TEM) images are found to alter in the range of 4–40 nm. Field emission scanning electron microscopic (FESEM) images reveal the presence of 30–100 nm CdS nanostructures. Photoluminescence (PL) of CdS–glass nanocomposites reveals a sharp green emission peak (508nm) due to direct electron–hole recombination along with a broad trap-related emission band. The sharpness, tuning ability of the absorption spectra, and PL covering the visible spectral range are the highest reported to date for any compound semiconductor–dielectric nanocomposite and one single nanocomposite, synthesized by this method, advocating for their potential utilization as functional materials in the fabrication of multiple devices such as luminescent solar concentrators (LSCs), optical color filters, and solid-state lasers.

© 2014 Optical Society of America

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  44. F. Zhang, S.-W. Chan, J. E. Spanier, E. Apak, Q. Jin, R. D. Robinson, and I. P. Herman, “Cerium oxide nanoparticles: size-selective formation and structure analysis,” Appl. Phys. Lett. 80, 127–129 (2002).
    [CrossRef]
  45. H. Mao, J. Chen, J. Wang, Z. Li, N. Dai, and Z. Zhu, “Photoluminescence investigation of CdSe quantum dots and the surface state effect,” Physica E 27, 124–128 (2005).
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  46. C. Dey, A. R. Molla, A. Tarafder, M. K. Mishra, G. De, M. Goswami, G. P. Kothiyal, and B. Karmakar, “Single-step in-situ synthesis and optical properties of ZnSe nanostructured dielectric nanocomposites,” J. Appl. Phys. 115, 134309 (2014).
    [CrossRef]
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2014

C. Dey, A. R. Molla, A. Tarafder, M. K. Mishra, G. De, M. Goswami, G. P. Kothiyal, and B. Karmakar, “Single-step in-situ synthesis and optical properties of ZnSe nanostructured dielectric nanocomposites,” J. Appl. Phys. 115, 134309 (2014).
[CrossRef]

2013

M. K. Mishra, A. Mandal, J. Saha, and G. De, “CdS nanoparticles incorporated onion-like mesoporous silica films: ageing-induced large Stokes shifted intense PL emission,” Opt. Mater. 35, 2604–2612 (2013).
[CrossRef]

S. Chen, M.-L. Zheng, X.-Z. Dong, Z.-S. Zhao, and X.-M. Duan, “Nondegenerate two-photon absorption in a zinc blende-type ZnS single crystal using the femtosecond pump–probe technique,” J. Opt. Soc. Am. B 30, 3117–3122 (2013).
[CrossRef]

K. Senthilkumar, T. Kalaivani, S. Kanagesan, V. Balasubramanian, and J. Balakrishnan, “Wurtzite ZnSe quantum dots: synthesis, characterization and PL properties,” J. Mater. Sci Mater. Electron. 24, 692–696 (2013).

2012

S. Kim, T. Kim, M. Kang, S. K. Kwak, T. W. Yoo, L. S. Park, I. Yang, S. Hwang, J. E. Lee, S. K. Kim, and S.-W. Kim, “Highly luminescent InP/GaP/ZnS nanocrystals and their application to white light-emitting diodes,” J. Am. Chem. Soc. 134, 3804–3809 (2012).
[CrossRef]

L. Zhao, L. Hu, and X. Fang, “Growth and device application of CdSe nanostructures,” Adv. Funct. Mater. 22, 1551–1566 (2012).
[CrossRef]

2011

X. Fang, T. Zhai, U. K. Gautam, L. Li, L. Wua, Y. Bando, and D. Golberg, “ZnS nanostructures: from synthesis to applications,” Prog. Mater. Sci. 56, 175–287 (2011).
[CrossRef]

Z. R. Khan, M. Zulfequar, and M. S. Khan, “Chemical synthesis of CdS nanoparticles and their optical and dielectric studies,” J. Mater. Sci. 46, 5412–5416 (2011).
[CrossRef]

2010

S. V. Alyshev, A. O. Zabezhaylov, R. A. Mironov, V. I. Kozlovsky, and E. M. Dianov, “Formation of three-dimensional ZnSe-based semiconductor nanostructures,” Semiconductors 44, 72–75 (2010).
[CrossRef]

2009

X. Fang, S. Xiong, T. Zhai, Y. Bando, M. Liao, U. K. Gautam, Y. Koide, X. Zhang, Y. Qian, and D. Golberg, “High-performance blue/ultraviolet-light-sensitive ZnSe-nanobelt photodetectors,” Adv. Mater. 21, 5016–5021 (2009).
[CrossRef]

K. D. Patel, G. K. Solanki, J. R. Gandhi, and S. G. Patel, “Structural and optical characterization of ZnSe crystals grown by physical vapor transport technique,” Chalcogenide Lett. 6, 45–50 (2009).

2008

S. Wageh, A. S. Eid, S. El-Rabaie, and A. A. Higazy, “CdSe nanocrystals in novel phosphate glass matrix,” Physica E 40, 3049–3054 (2008).
[CrossRef]

S. M. Reda, “Synthesis and optical properties of CdS quantum dots embedded in silica matrix thin films and their applications as luminescent solar concentrators,” Acta Mater. 56, 259–264 (2008).
[CrossRef]

2007

S. J. Gallagher, B. C. Rowan, J. Doran, and B. Norton, “Quantum dot solar concentrator: device optimization using spectroscopic techniques,” Sol. Energy 81, 540–547 (2007).
[CrossRef]

C.-L. Weng, I.-C. Chen, and Y.-C. Tsai, “Electron–acoustic-phonon interaction in core/shell nanocrystals and in quantum-dot quantum wells,” Phys. Rev. B 76, 195313 (2007).
[CrossRef]

H. Liu, Q. Liu, and X. Zhao, “Crystal growth and optical properties of CdS-doped lead silicate glass,” Mater. Charact. 58, 96–100 (2007).
[CrossRef]

S. K. Gayen, M. Brito, B. B. Das, G. Comanescu, X. C. Liang, M. Alrubaiee, R. R. Alfano, C. Gonzalez, A. H. Byro, D. L. V. Bauer, and V. Balogh-Nair, “Synthesis and optical spectroscopy of a hybrid cadmium sulfide–dendrimer nanocomposite,” J. Opt. Soc. Am. B 24, 3064–3071 (2007).
[CrossRef]

2006

S. K. Apte, B. B. Kale, R. S. Sonawane, S. D. Naik, S. S. Bodhale, and B. K. Das, “Homogeneous growth of CdS/CdSSe nanoparticles in glass matrix,” Mater. Lett. 60, 499–503 (2006).
[CrossRef]

2005

M. J. Bowers, J. R. McBride, and S. J. Rosenthal, “White-light emission from magic-sized cadmium selenide nanocrystals,” J. Am. Chem. Soc. 127, 15378–15379 (2005).
[CrossRef]

H. Mao, J. Chen, J. Wang, Z. Li, N. Dai, and Z. Zhu, “Photoluminescence investigation of CdSe quantum dots and the surface state effect,” Physica E 27, 124–128 (2005).
[CrossRef]

2004

G. Jose, G. Jose, V. Thomas, C. Joseph, M. A. Ittyachen, and N. V. Unnikrishnan, “Optical characterization of Eu3+ ions in CdSe nanocrystal containing silica glass,” J. Fluoresc. 14, 733–738 (2004).
[CrossRef]

2003

D. Battaglia, J. J. Li, Y. Wang, and X. Peng, “Colloidal two-dimensional systems: CdSe quantum shells and wells,” Angew. Chem., Int. Ed. 42, 5035–5039 (2003).
[CrossRef]

N. S. Pesika, K. J. Stebe, and P. C. Searson, “Relationship between absorbance spectra and particle size distributions for quantum-sized nanocrystals,” J. Phys. Chem. B 107, 10412–10415 (2003).
[CrossRef]

2002

F. Zhang, S.-W. Chan, J. E. Spanier, E. Apak, Q. Jin, R. D. Robinson, and I. P. Herman, “Cerium oxide nanoparticles: size-selective formation and structure analysis,” Appl. Phys. Lett. 80, 127–129 (2002).
[CrossRef]

M. Kazes, D. Y. Lewis, Y. Ebenstein, T. Mokari, and U. Banin, “Lasing from semiconductor quantum rods in a cylindrical microcavity,” Adv. Mater. 14, 317–321 (2002).
[CrossRef]

W. W. Yu and X. Peng, “Formation of high-quality CdS and other II–VI semiconductor nanocrystals in noncoordinating solvents: tunable reactivity of monomers,” Angew. Chem., Int. Ed. 41, 2368–2371 (2002).

K. E. Andersen, C. Y. Fong, and W. E. Pickett, “Quantum confinement in CdSe nanocrystallites,” J. Non-Cryst. Solids 299–302, 1105–1110 (2002).
[CrossRef]

2001

K. Rajeshwar, N. R. de Tacconi, and C. R. Chenthamarakshan, “Semiconductor-based composite materials: preparation, properties, and performance,” Chem. Mater. 13, 2765–2782 (2001).
[CrossRef]

X.-D. Zhou and W. Huebner, “Size-induced lattice relaxation in CeO2 nanoparticles,” Appl. Phys. Lett. 79, 3512–3514 (2001).
[CrossRef]

P. Mukherjee, “Transmission electron microscopy (TEM) of silicate glasses containing CdSxSe1−x,” J. Mater. Sci. Lett. 20, 605–609 (2001).
[CrossRef]

2000

M. Rajalakshmi, A. K. Arora, B. S. Bendre, and S. Mahamuni, “Optical phonon confinement in zinc oxide nanoparticles,” J. Appl. Phys. 87, 2445–2448 (2000).
[CrossRef]

M. Jacobsohn and U. Banin, “Size dependence of second harmonic generation in CdSe nanocrystal quantum dots,” J. Phys. Chem. B 104, 1–5 (2000).
[CrossRef]

K. Barnham, J. L. Marques, J. Hassard, and P. O’Brien, “Quantum-dot concentrator and thermodynamic model for the global redshift,” Appl. Phys. Lett. 76, 1197–1199 (2000).
[CrossRef]

1999

A. M. Kapitonov, A. P. Stupak, S. V. Gaponenko, E. P. Petrov, A. L. Rogach, and A. Eychmuller, “Luminescence properties of thiol-stabilized CdTe nanocrystals,” J. Phys. Chem. B 103, 10109–10113 (1999).
[CrossRef]

K. K. Nanda, S. N. Sarangi, and S. N. Sahu, “Visible light emission from CdS nanocrystals,” J. Phys. D 32, 2306–2310 (1999).
[CrossRef]

1996

H. Yukselici and P. D. Persans, “High temperature optical properties of CdS crystals in borosilicate glass,” J. Non-Cryst. Solids 203, 206–210 (1996).
[CrossRef]

S. H. Risbud, “Nucleation and coalescence phenomena in the transformation of semiconductor-doped glasses,” Thermochim. Acta 280–281, 319–332 (1996).
[CrossRef]

U. Woggon, O. Wind, V. Sperling, M. Portune, and C. Klingshirn, “Nonlinear and electro-optic properties of II–VI semiconductor nanocrystals and polymer and glass matrices,” Surf. Rev. Lett. 3, 1089–1094 (1996).
[CrossRef]

1995

H. Yukselici, P. D. Persans, and T. M. Hayes, “Optical studies of the growth of Cd1-xZnxS nanocrystals in borosilicate glass,” Phys. Rev. B 52, 11763–11772 (1995).
[CrossRef]

V. C. S. Reynoso, A. M. de Paula, R. F. Cuevas, J. A. M. Neto, O. L. Alves, C. L. Cesar, and L. C. Barbosa, “PbTe quantum dot doped glasses with absorption edge in the 1.5  pm wavelength region,” Electron. Lett. 31, 1013–1015 (1995).
[CrossRef]

1994

H. Okamoto, J. Matsuoka, H. Nasu, K. Kamiya, and H. Tanaka, “Effect of cadmium to sulfur ratio on the photoluminescence of CdS doped glasses,” J. Appl. Phys. 75, 2251–2256 (1994).
[CrossRef]

T. Vossmeyer, L. Katsikas, M. Gienig, I. G. Popovic, K. Diesner, A. Chemseddine, A. Eychmiiller, and H. Weller, “CdS nanoclusters: synthesis, characterization, size dependent oscillator strength, temperature shift of the excitonic transition energy, and reversible absorbance shift,” J. Phys. Chem. 98, 7665–7673 (1994).
[CrossRef]

M. S. Hybertsen, “Absorption and emission of light in nanoscale silicon structures,” Phys. Rev. Lett. 72, 1514–1517 (1994).
[CrossRef]

1992

V. S. Dneprovskii, V. I. Klimov, D. K. Okoroko, and Y. V. Vandyshev, “Ultrafast light induced transmission changes and laser emission of semiconductor quantum dots,” Phys. Status Solidi B 173, 405–406 (1992).
[CrossRef]

1990

G. D. Stucky and J. E. Mac Doudall, “Quantum confinement and host/guest chemistry: probing a new dimension,” Science 247, 669–678 (1990).
[CrossRef]

1988

A. P. Alivisatos, T. D. Harris, L. E. Brus, and A. Jayaraman, “Resonance Raman scattering and optical absorption studies of CdSe microclusters at high pressure,” J. Chem. Phys. 89, 5979–5982 (1988).
[CrossRef]

Y. Kayanuma, “Quantum-size effects of interacting electrons and holes in semiconductor microcrystals with spherical shape,” Phys. Rev. B 38, 9797–9805 (1988).
[CrossRef]

1987

N. F. Borrelli, D. W. Hall, H. J. Holland, and D. W. Smith, “Quantum confinement effects of semiconducting microcrystallites in glass,” J. Appl. Phys. 61, 5399–5409 (1987).
[CrossRef]

1984

K. C. Rustagi and C. Flytzanis, “Optical nonlinearities in semiconductor-doped glasses,” Opt. Lett. 9, 344–346 (1984).
[CrossRef]

L. E. Brus, “Electron–electron and electron–hole interactions in small semiconductor crystallites: the size dependence of the lowest excited electronic state,” J. Chem. Phys. 80, 4403–4409 (1984).
[CrossRef]

Alfano, R. R.

Al-Ghamdi, A. A.

S. Han, L. Hu, N. Gao, A. A. Al-Ghamdi, and X. Fang, “Efficient self-assembly synthesis of uniform CdS spherical nanoparticles-Au nanoparticles hybrids with enhanced photoactivity,” Adv. Funct. Mater., doi: 10.1002/adfm.201400012 (2014).
[CrossRef]

Alivisatos, A. P.

A. P. Alivisatos, T. D. Harris, L. E. Brus, and A. Jayaraman, “Resonance Raman scattering and optical absorption studies of CdSe microclusters at high pressure,” J. Chem. Phys. 89, 5979–5982 (1988).
[CrossRef]

Alrubaiee, M.

Alves, O. L.

V. C. S. Reynoso, A. M. de Paula, R. F. Cuevas, J. A. M. Neto, O. L. Alves, C. L. Cesar, and L. C. Barbosa, “PbTe quantum dot doped glasses with absorption edge in the 1.5  pm wavelength region,” Electron. Lett. 31, 1013–1015 (1995).
[CrossRef]

Alyshev, S. V.

S. V. Alyshev, A. O. Zabezhaylov, R. A. Mironov, V. I. Kozlovsky, and E. M. Dianov, “Formation of three-dimensional ZnSe-based semiconductor nanostructures,” Semiconductors 44, 72–75 (2010).
[CrossRef]

Andersen, K. E.

K. E. Andersen, C. Y. Fong, and W. E. Pickett, “Quantum confinement in CdSe nanocrystallites,” J. Non-Cryst. Solids 299–302, 1105–1110 (2002).
[CrossRef]

Apak, E.

F. Zhang, S.-W. Chan, J. E. Spanier, E. Apak, Q. Jin, R. D. Robinson, and I. P. Herman, “Cerium oxide nanoparticles: size-selective formation and structure analysis,” Appl. Phys. Lett. 80, 127–129 (2002).
[CrossRef]

Apte, S. K.

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Figures (15)

Fig. 1.
Fig. 1.

Dilatometric thermograms of CS-1 (base glass) and CS-2-0h (5 wt. % CdS-added as-prepared glass).

Fig. 2.
Fig. 2.

Representative refractive index variation with wavelength of CS-1 and CS-2-50h. The continuous lines are the Cauchy fitted curve of the experimental points (black squares).

Fig. 3.
Fig. 3.

(a) UV–visual absorption spectra of samples CS-1, CS-2-0h, CS-2-10h, CS-2-20h, CS-2-30h, CS-2-40h, CS-2-50h, and CS-2-100h. The inset shows the variation of the absorption edge position with heat treatment time. The lines are drawn to guide the eye. (b) Photographs of the samples are laid over the parallel lines to show their transparency.

Fig. 4.
Fig. 4.

(αhυ)2 versus hυ curve of the samples CS-2-0h, CS-2-10h, CS-2-20h, CS-2-30h, CS-2-40h, CS-2-50h, and CS-2-100h. The straight-line portions (inset) are extrapolated to obtain the edge energies as intercepts at (αhυ)2=0. These values are labeled as 2.53, 2.48, and 2.45 eV for 30, 50, and 100 h heat-treated samples, respectively.

Fig. 5.
Fig. 5.

Calculated size dependence of the lowest excitation energies of a CdS sphere for the carrier and exciton confinement cases. Absorbance onset (the curve shown in the inset) and bandgap enlargement versus particle radius for CdS in the nanocomposite are also plotted using a suitable model.

Fig. 6.
Fig. 6.

Representative TEM image of (a) CS-2-50h. (b) EDS analysis of CS-2-50h.

Fig. 7.
Fig. 7.

FESEM images of (a) and (b) CS-2-40h. (c) EDS analysis of CS-2-40h. (d) FESEM image of as-received CdS particles.

Fig. 8.
Fig. 8.

Representative XRD patterns of (a) CS-2-50h and (b) CS-1 (base glass). (c) JCPDS file for comparison.

Fig. 9.
Fig. 9.

PL spectra of CS-1, CS-2-0h, CS-2-10h, CS-2-20h, CS-2-30h, CS-2-40h, CS-2-50h, and CS-2-100h. The excitation wavelength is 446 nm with a constant power of a 0.73 W diode laser.

Fig. 10.
Fig. 10.

Representative deconvoluted PL spectra of (a) CS-2-20h and (b) CS-2-100h showing three peaks. Two sharp peaks are due to size-dependent emission and the broad peak is due to trap state emissions.

Fig. 11.
Fig. 11.

Variation of (a) photoluminescence intensity and (b) peak position γr of the sample CS-2-30h with heat treatment time.

Fig. 12.
Fig. 12.

Energy scale diagram of the luminescence spectra for both the bulk-like NCs and relatively small NCs of CdS. The emissions labeled as γ1, γ2, γ3, and γ4 are from the defect states. The horizontal dashed levels just below the conduction band are virtual levels. The luminescence mechanism with sample photographs under 446 nm laser excitation is also shown.

Fig. 13.
Fig. 13.

(a) Chromaticity diagram corresponding to light emitted from the glass nanocomposite when excited at 446 nm. The point ‘p’ represents chromaticity coordinates (0.364, 0.569) of the emitted light for the sample CS-2-30h. Luminescence photographs of sample (b) CS-2-0h (front view and side view), (c) CS-2-20h (front view and side view), and that of (d) CS-2-30h (front view and side view) are also shown when excited at 446 nm with a diode laser.

Fig. 14.
Fig. 14.

Variation of photoluminescence intensity with excitation power for sample CS-2-30h. The excitation wavelength is 446 nm. The inset shows the linear fitting of Log (intensity) with Log (power).

Fig. 15.
Fig. 15.

Diagram of an LSC portraying a number of processes. (1) Light enters from the upper surface and is absorbed by the CdS NCs in the nanocomposite (LSC). (2) Light is reabsorbed by another CdS NC. (3) Light is re-emitted and trapped inside the LSC due to total internal reflection. (4) Light is absorbed by the matrix. (5) Light passes through the LSC without absorption. (6) Light is concentrated upon the photovoltaic cell. (7) Re-emitted light incident upon the top surface with an angle smaller than the critical angle escapes the LSC.

Tables (6)

Tables Icon

Table 1. Composition and Some Properties of Nanocomposites

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Table 2. Some Thermal Properties of the Base Glass and Nanocomposite

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Table 3. Wavelength Dependent Refractive Indices and Abbe Numbers of the Base Glass and Nanocomposites

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Table 4. PL Peak Positions and FWHM Values Recorded from the Photoluminescence Spectra of Nanocomposites

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Table 5. Comparison of PL Peak Positions and the Band Edge Energy of the Nanocomposites

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Table 6. Photometric Properties of the Glass Nanocomposites CS-2-0h to CS-2-100h

Equations (8)

Equations on this page are rendered with MathJax. Learn more.

n=A+Bλ2+Cλ4,
VD=nD1nFnC,
α(hν)=C*(hνEgbulk)12,
α=2.303Ax.
E*Egbulk+2π22r2(1mem0+1mhm0)1.8e24πε0εr.
aB=ε0εh2πμe2,
1μ=(1mem0+1mhm0).
E*EgbulkEb+h2[8(mem0+mhm0)(rηaB)]2,

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