J. Semicond. > 2023, Volume 44 > Issue 12 > 122502, doi: 10.1088/1674-4926/44/12/122502
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ARTICLES

Hyperfine splitting and ferromagnetism in CdS : Mn nanoparticles for optoelectronic device applications

Madhavi Sharad Darekar and Praveen Beekanahalli Mokshanatha

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 Corresponding author: Madhavi Sharad Darekar, madhavi_darekar28@rediff.com

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Abstract: Manganese (Mn) doped cadmium sulphide (CdS) nanoparticles were synthesized using a chemical method. It was possible to decrease CdS : Mn particle size by increasing Mn concentration. Investigation techniques such as ultraviolet−visible (UV−Vis) absorption spectroscopy and photoluminescence (PL) spectroscopy were used to determine optical properties of CdS : Mn nanoparticles. Size quantization effect was observed in UV−Vis absorption spectra. Quantum efficiency for luminescence or the internal magnetic field strength was increased by doping CdS nanoparticles with Mn element. Orange emission was observed at wavelength ~630 nm due to 4T1 → 6A1 transition. Isolated Mn2+ ions arranged in tetrahedral coordination are mainly responsible for luminescence. Luminescence quenching and the effect of Mn doping on hyperfine interactions in the case of CdS nanoparticles were also discussed. The corresponding weight percentage of Mn element actually incorporated in doping process was determined by atomic absorption spectroscopy (AAS). Crystallinity was checked and the average size of nanoparticles was estimated using the X-ray diffraction (XRD) technique. CdS : Mn nanoparticles show ferromagnetism at room temperature. Transmission electron microscopy (TEM) images show spherical clusters of various sizes and selected area electron diffraction (SAED) patterns show the polycrystalline nature of the clusters. The electronic states of diluted magnetic semiconductors (DMS) of Ⅱ−Ⅵ group CdS nanoparticles give them great potential for applications due to quantum confinement. In this study, experimental results and discussions on these aspects have been given.

Key words: synthesis, characterization, undoped CdS nanoparticles, Mn-doped CdS nanoparticles, non-aqueous chemical method



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Fig. 1.  Luminescence mechanism scheme of Mn-doped CdS nanoparticles[19].

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Fig. 2.  UV−Vis absorption spectra of Mn-doped CdS nanoparticles (samples A to J).

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Fig. 3.  Variation of energy gap with atomic weight percentage of Mn in Mn-doped CdS nanoparticles (samples A to J).

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Fig. 4.  UV−Vis absorption spectrum of Mn-doped CdS nanoparticles (sample K).

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Fig. 5.  UV−Vis absorption spectra of Mn-doped CdS nanoparticles (samples R to Z).

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Fig. 6.  Variation of energy gap with particle size in Mn-doped CdS nanoparticles (samples R to Z).

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Fig. 7.  UV−Vis absorption spectra of Mn-doped CdS nanoparticles (samples A’, B’, C’ and D’).

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Fig. 8.  XRD spectra of Mn-doped CdS nanoparticles (samples A to J).

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Fig. 9.  Excitation and emission spectra of Mn-doped CdS nanoparticles (samples A to J).

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Fig. 10.  Variation of PL intensity with atomic weight percentage of Mn in samples A to J.

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Fig. 11.  ESR spectra of Mn-doped CdS nanoparticles (samples A to J).

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Fig. 12.  Variation of line width with atomic weight percentage of Mn (samples A to J).

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Fig. 13.  ESR spectra of manganese sulphide nanoparticles.

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Fig. 14.  ESR spectra of Mn-doped CdS nanoparticles (samples R to Z).

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Fig. 15.  Variation of line width with weight percentage of Mn in samples R to Z.

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Fig. 16.  ESR spectra of Mn-doped CdS nanoparticles (samples A’, B’, C’ and D’).

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Fig. 17.  Variation of line width with atomic weight percentage of Mn in samples A’, B’, C’, and D’.

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Fig. 18.  M(H) curves of two Cd1 – xMnxS samples (x = 0.04, 0.05) at 300 K.

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Fig. 19.  Temperature dependence of magnetization for Cd0.96Mn0.04S at 1 KOe. The inset shows the best fit to the Bloch law M(T) = M(0) × (1 − AT3/2) (shown by the marked line).

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Fig. 20.  Total energy difference ∆EFM-AFM between ferromagnetic and anti-ferromagnetic configurations for Mn-doped CdS nanoparticles as a function of Mn concentration in the “short” (squares) and “far” (circles) configurations.

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Fig. 21.  (a) TEM image of Mn-doped CdS nanoparticles (sample A) with magnification of 200 nm and (b) SAED pattern of Mn-doped CdS nanoparticles (sample A).

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Fig. 22.  (a) TEM image of Mn-doped CdS nanoparticles (sample J) with magnification of 200 nm and (b) SAED pattern of Mn-doped CdS nanoparticles (sample J).

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Table 1.   Properties of thioglycerol.

ParameterSHCH2CH(OH)CH2OH
Density1.295 gm/mL
Molecular weight108.16 gm/mole
Purity99%
Molarity11.9 M
Boiling point118 °C
Freezing point110 °C
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Table 2.   UV−Vis absorption values, band gap values and particle sizes of Mn-doped CdS nanoparticles (samples A to J).

Sample Wt.% of Mn used for chemical reaction Wt.% of Mn found by AAS At. Wt.% of Mn found by AAS UV−Vis absorp-
tion (nm)		 Band gap
Eg (eV)		 Particle size (nm)
A 15 3.72 0.068 358 3.46 5.28
B 25 4.56 0.083 365 3.40 5.36
C 35 5.66 0.103 350 3.54 5.18
D 45 6.48 0.118 340 3.65 5.06
E 50 6.87 0.125 336 3.69 5.02
F 55 7.20 0.131 330 3.76 4.95
G 60 7.53 0.137 318 3.90 4.81
H 65 7.80 0.142 315 3.94 4.78
I 70 8.02 0.146 310 4.00 4.73
J 80 8.46 0.154 300 4.14 4.61
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Table 3.   UV−Vis absorption values, band gap values and particle sizes of Mn-doped CdS nanoparticles (samples R to Z).

SampleWt.% of Mn used for
chemical reaction		Wt.% of Mn found by
AAS		At. Wt.% of Mn found by AASUV−Vis absorption (nm)Band gap Eg (eV)Particle size (nm)
R6.4 × 10−50.026 ± 0.0020.00053463.595.13
S8 × 10−50.0780.00143503.545.18
T2 × 10−40.1320.00243503.545.18
U3 × 10−40.1520.00283523.525.21
V4 × 10−40.240.00443553.495.24
W5 × 10−40.30.00553573.475.27
X7 × 10−40.620.01133603.455.29
Y1 × 10−31.240.02263663.395.37
Z5 × 10−33.720.06713703.355.42
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Table 4.   UV−Vis absorption values, band gap values and particle sizes of Mn-doped CdS nanoparticles (samples A’, B’, C’, and D’).

Sample At. Wt.% of Mn found by AAS UV−Vis absorption (nm) Band gap Eg (eV) Particle size (nm)
A’ 0.0080 370 3.35 5.42
B’ 0.0085 350 3.54 5.18
C’ 0.0176 336 3.69 5.02
D’ 0.0602 320 3.88 4.83
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Table 5.   XRD parameters of Mn-doped CdS nanoparticles (samples A to J).

Sample Wt.% of Mn used for chemical reaction Wt.% of Mn found
by AAS		 At. Wt.% of Mn found by AAS XRD average particle size, d’ (nm) and inter planar distance, d (Å)
A 15 3.72 0.068 2$ \theta $ = 29°
d’ = 5.27 nm
d = 3.08 Å		 2$ \theta $ = 47.8°
d’ = 3.72 nm
d = 1.90 Å
B 25 4.56 0.083 2$ \theta $ = 28.6°
d’ = 5.70 nm
d = 3.12 Å		 2$ \theta $ = 47.7°
d’ = 3.81 nm
d = 1.90 Å
C 35 5.66 0.103 2$ \theta $ = 28.7°
d’ = 5.33 nm
d = 3.11 Å		 2$ \theta $ = 47.5°
d’ = 3.62 nm
d = 1.91 Å
D 45 6.48 0.118 2$ \theta $ = 29.2°
d’ = 4.89nm
d = 3.05 Å		 2$ \theta $ = 47.6°
d’ = 4.58 nm
d = 1.91 Å
E 50 6.87 0.125 2$ \theta $ = 28.6°
d’ = 5.19 nm
d = 3.12 Å		 2$ \theta $ = 47.4°
d’ = 4.28 nm
d = 1.92 Å
F 55 7.20 0.131 2$ \theta $ = 28.8°
d’ = 4.89 nm
d = 3.1 Å		 2$ \theta $ = 47.3°
d’ = 3.56 nm
d = 1.92 Å
G 60 7.53 0.137 2$ \theta $ = 28.5°
d’ = 5.4 nm
d = 3.13 Å		 2$ \theta $ = 47.5°
d’ = 3.81 nm
d = 1.91 Å
H 65 7.80 0.142 2$ \theta $ = 28.6°
d’ = 4.94 nm
d = 3.12 Å		 2$ \theta $ = 47.2°
d’ = 3.84 nm
d = 1.92 Å
I 70 8.02 0.146 2$ \theta $ = 28.8°
d’ = 3.73 nm
d = 3.1 Å		 2$ \theta $ = 47.1°
d’ = 2.83 nm
d = 1.93 Å
J 80 8.46 0.154 2$ \theta $ = 28.7°
d’ = 4.77 nm
d = 3.11 Å		 2$ \theta $ = 47.7°
d’ = 3.53 nm
d = 1.90 Å
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Table 6.   PL parameters of Mn-doped CdS nanoparticles (samples A to J).

Sample Wt.% of Mn used for chemical reaction Wt.% of Mn found by AAS At. Wt.% of Mn found by AAS
 PL intensity
Excitation
λex (nm)		 Emission λem (nm)
A 15 3.72 0.068 391.3 625
B 25 4.56 0.083 389.2 626
C 35 5.66 0.103 393.1 628
D 45 6.48 0.118 392.9 631
E 50 6.87 0.125 391.9 634
F 55 7.20 0.131 391.3 638
G 60 7.53 0.137 389 634
H 65 7.80 0.142 387.9 633
I 70 8.02 0.146 389 642
J 80 8.46 0.154 386.1 631
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Table 7.   ESR parameters of Mn-doped CdS nanoparticles (samples A to J).

Sample At. Wt.% of Mn Line width
(Gauss)		 Spectroscopic splitting factor (g) Bra
(Gauss)		 ESR intensity (× 105) ESR intensity/gain No. of CdS molecules No. of Mn atoms
A 0.068 225.69 2.0079 3465.8418 1.9101743 1.9101743 6909 1008
B 0.083 243.05 2.0079 3462.2744 4.7703872 1.1925968 4078 628
C 0.103 294.11 2.0128 3457.3715 4.4982699 4.4982699 8038 1053
D 0.118 302.76 2.0077 3466.022 2.7958911 2.7958911 4754 561
E 0.125 302.76 2.0077 3466.022 3.7125768 3.7125768 1998 250
F 0.131 302.76 2.0178 3445.1535 8.6626791 5.4141 6582 934
G 0.137 328.71 2.0178 3448.7209 5.6189461 3.5118413 6625 908
H 0.142 397.92 2.0178 3448.7209 5.0669891 5.0669891 3897 401
I 0.146 501.73 2.0028 3474.6725 2.4355177 19.4841 5231 434
J 0.154 527.68 1.9854 3504.9493 2.561721 16.010756 5384 307
a: Br is the magnetic field at the center of the two resonance lines.
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Table 8.   ESR parameters of Mn-doped CdS nanoparticles (samples R to Z).

Sample At. Wt.% of Mn found by AAS Spectroscopic splitting factor (g) Line width (Gauss)
R 0.0005 1.9904 10
S 0.0014 1.9904 19.16
T 0.0024 1.9910 54.17
U 0.0028 1.9902 55
V 0.0044 1.9902 55.87
W 0.0055 1.9902 56.7
X 0.0113 1.9910 59.2
Y 0.0226 1.9909 60
Z 0.0671 1.9904 80.8
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Table 9.   ESR parameters of Mn-doped CdS nanoparticles (samples A’, B’, C’, and D’).

Sample Wt.% of Mn found by AAS At. Wt.% of Mn found by AAS Line width (Gauss) Br (Gauss) ESR intensity
(×105)		 Spectroscopic splitting factor (g)
A’ 0.439 0.0080 97.7 3370.5 0.1055 2.068
B’ 0.469 0.0085 101.7 2535.7 2.5 2.050
C’ 0.969 0.0176 144.7 3374.4 0.955 2.066
D’ 3.309 0.0602 164.2 3384.2 1.087 2.060
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Table 10.   VSM parameters of two Cd1 – xMnxS powder samples (x = 0.04, 0.05).

SampleMs at 300 K
(emu/g)		Ms at 5 K
(emu/g)		Hc at 300 K
(Oe)		Hc at 5 K
(Oe)
Cd0.95Mn0.05S~1.61 × 10−3~1.59 × 10−2~105~250
Cd0.96Mn0.04S~3.07 × 10−3~3.84 × 10−2~100~98
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[1]
Gadalla A, Almokhtar M, Abouelkhir A N. Effect of Mn doping on structural, optical and magnetic properties of CdS diluted magnetic semiconductor nanoparticles. Chalcogenide Letters, 2018, 15, 207
[2]
Chaure S. Investigation of the effect of manganese doping in CdS nanocrystalline thin films. Mater Res Express, 2018, 6, 025912 doi: 10.1088/2053-1591/aad4e1
[3]
Venkatesan D, Deepan D, Ramkumar J, et al. Synthesis and characterization of sodium bis (2-ethylhexyl) sulfonsuccinate (AOT) capped pure and Mn-doped CdS nanoparticles. J Nanomater, 2012, 2012, 1 doi: 10.1155/2012/492573
[4]
Maity P, Kumar R, Jha S N, et al. Investigation of the Physical Properties of Mn-doped CdS Diluted Magnetic Semiconductor Quantum Dots: Non-linear Band Gap variation with Downwards Bowing. Available at SSRN 4066164
[5]
Levy L, Ingert D, Feltin N, et al. Cd1− y Mn y S nanoparticles: Absorption and photoluminescence properties. J Cryst Growth, 1998, 184/185, 377 doi: 10.1016/S0022-0248(97)00780-X
[6]
Hofmann D M, Hofstaetter A, Leib U, et al. EPR and ENDOR investigations on CdS : Mn nanocrystals. J Cryst Growth, 1998, 184/185, 383 doi: 10.1016/S0022-0248(98)80081-X
[7]
Counio G, Esnouf S, Gacoin T, et al. CdS : Mn nanocrystals in transparent xerogel matrices: synthesis and luminescence properties. J Phys Chem, 1996, 100, 20021 doi: 10.1021/jp961937i
[8]
Bhargava R N, Gallagher D, Hong X, et al. Optical properties of manganese-doped nanocrystals of ZnS. Phys Rev Lett, 1994, 72, 416 doi: 10.1103/PhysRevLett.72.416
[9]
Khosravi A A, Kundu M, Jatwa L, et al. Green luminescence from copper doped zinc sulphide quantum particles. Appl Phys Lett, 1995, 67, 2702 doi: 10.1063/1.114298
[10]
Khosravi A A, Kundu M, Kuruvilla B A, et al. Manganese doped zinc sulphide nanoparticles by aqueous method. Appl Phys Lett, 1995, 67, 2506 doi: 10.1063/1.114440
[11]
Bhargava R N, Gallagher D, Welker T, et al. Doped nanocrystals of semiconductors - a new class of luminescent materials. J Lumin, 1994, 60/61, 275 doi: 10.1016/0022-2313(94)90146-5
[12]
Bhargava R N. Nanoparticles and their use for multifunctional bioimaging. J Lumin, 1996, 70, 85 doi: 10.1016/0022-2313(96)00046-4
[13]
Norris D J, Yao N, Charnock F T, et al. High-quality manganese-doped ZnSe nanocrystals. Nano Lett, 2001, 1, 3 doi: 10.1021/nl005503h
[14]
Ochsenbein S T, Gamelin D R. Quantum oscillations in magnetically doped colloidal nanocrystals. Nat Nanotechnol, 2011, 6, 112 doi: 10.1038/nnano.2010.252
[15]
Beaulac R, Ochsenbein S, Gamelin D, et al. Colloidal transition-metal-doped quantum dots. In nanocrystal quantum dots. CRC Press, 2010, 397
[16]
Yu J H, Liu X Y, Kweon K E, et al. Giant Zeeman splitting in nucleation-controlled doped CdSe : Mn2+ quantum nanoribbons. Nat Mater, 2010, 9, 47 doi: 10.1038/nmat2572
[17]
Wood V, Halpert J E, Panzer M J, et al. Alternating Current driven electroluminescence from ZnSe/ZnS : Mn/ZnS nanocrystals. Nano Lett, 2009, 9, 2367 doi: 10.1021/nl900898t
[18]
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    Received: 04 June 2023 Revised: 27 June 2023 Online: Accepted Manuscript: 26 October 2023Uncorrected proof: 22 November 2023Published: 10 December 2023

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      Article Navigation >  Journal of Semiconductors  > 2023  >  44(12): 122502
      Madhavi Sharad Darekar, Praveen Beekanahalli Mokshanatha. Hyperfine splitting and ferromagnetism in CdS : Mn nanoparticles for optoelectronic device applications[J]. Journal of Semiconductors, 2023, 44(12): 122502. doi: 10.1088/1674-4926/44/12/122502 M S Darekar, P Beekanahalli Mokshanatha. Hyperfine splitting and ferromagnetism in CdS : Mn nanoparticles for optoelectronic device applications[J]. J. Semicond, 2023, 44(12): 122502. doi: 10.1088/1674-4926/44/12/122502Export: BibTex EndNote
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      Madhavi Sharad Darekar, Praveen Beekanahalli Mokshanatha. Hyperfine splitting and ferromagnetism in CdS : Mn nanoparticles for optoelectronic device applications[J]. Journal of Semiconductors, 2023, 44(12): 122502. doi: 10.1088/1674-4926/44/12/122502

      M S Darekar, P Beekanahalli Mokshanatha. Hyperfine splitting and ferromagnetism in CdS : Mn nanoparticles for optoelectronic device applications[J]. J. Semicond, 2023, 44(12): 122502. doi: 10.1088/1674-4926/44/12/122502
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      Hyperfine splitting and ferromagnetism in CdS : Mn nanoparticles for optoelectronic device applications

      doi: 10.1088/1674-4926/44/12/122502

      • Department of Physics, Institute of Engineering and Technology, Srinivas University, Mukka, Surathkal, Mangalore-574146, Karnataka, India

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        Madhavi Sharad Darekar Madhavi Sharad Darekar received her Ph.D. (Physics) in the field of synthesis and characterization of undoped and doped semiconductor nanoparticles from the Department of Physics, Savitribai Phule Pune University, India, in 2006. She received a Post-Doctoral Fellow degree in Nanotechnology from the Department of Nanotechnology, Srinivas University, India, in 2023. At present, she is pursuing a Post-Doctoral Fellow course in Physics in the Department of Physics, Srinivas University, India. Her research involves synthesis of undoped and doped semiconductor nanoparticles by chemical method, thin film deposition by spin coating method, dip coating method, chemical bath deposition etc., their characterizations and applications

      • Corresponding author: madhavi_darekar28@rediff.com
      • Received Date: 2023-06-04
      • Revised Date: 2023-06-27
        • Available Online: 2023-10-26

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