Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu₆PS₅I-based thin films deposited using magnetron sputtering

Cu₆PS₅I-based thin films were deposited using non-reactive radio-frequency magnetron sputtering. Structural studies of thin films were performed by scanning electron microscopy, and their chemical composition was determined using energy-dispersive X-ray spectroscopy. As-deposited thin films were irr...

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Опубліковано в: :Semiconductor Physics Quantum Electronics & Optoelectronics
Дата:2017
Автори: Studenyak, I.P., Kutsyk, M.M., Bendak, A.V., Izai, V.Yu., Kus, P., Mikula, M.
Формат: Стаття
Мова:Англійська
Опубліковано: Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України 2017
Онлайн доступ:https://nasplib.isofts.kiev.ua/handle/123456789/214924
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Цитувати:Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu₆PS₅I-based thin films deposited using magnetron sputtering / I.P. Studenyak, M.M. Kutsyk, A.V. Bendak, V. Yu. Izai, P. Kus, M. Mikula // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 2. — С. 246-249. — Бібліогр.: 12 назв. — англ.

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Digital Library of Periodicals of National Academy of Sciences of Ukraine
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author Studenyak, I.P.
Kutsyk, M.M.
Bendak, A.V.
Izai, V.Yu.
Kus, P.
Mikula, M.
author_facet Studenyak, I.P.
Kutsyk, M.M.
Bendak, A.V.
Izai, V.Yu.
Kus, P.
Mikula, M.
citation_txt Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu₆PS₅I-based thin films deposited using magnetron sputtering / I.P. Studenyak, M.M. Kutsyk, A.V. Bendak, V. Yu. Izai, P. Kus, M. Mikula // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 2. — С. 246-249. — Бібліогр.: 12 назв. — англ.
collection DSpace DC
container_title Semiconductor Physics Quantum Electronics & Optoelectronics
description Cu₆PS₅I-based thin films were deposited using non-reactive radio-frequency magnetron sputtering. Structural studies of thin films were performed by scanning electron microscopy, and their chemical composition was determined using energy-dispersive X-ray spectroscopy. As-deposited thin films were irradiated with wideband radiation of a Cu-anode X-ray tube at different exposure times. Optical transmission spectra of X-ray irradiated Cu₅.₅₆P1.₆₆S₄.₉₃I₀.₈₅ thin films were measured depending on irradiation time. The Urbach absorption edge and dispersion of refractive index for X-rays irradiated Cu₅.₅₆P1.₆₆S₄.₉₃I₀.₈₅ thin films were studied. It has been revealed that the nonlinear decrease of energy pseudogap and the nonlinear increase of refractive index occur with the increase of X-ray irradiation time.
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fulltext Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 2. P. 246-249. doi: https://doi.org/10.15407/spqeo20.02.246 © 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine 246 PACS 78.40.Ha, 77.80.Bh Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu6PS5I-based thin films deposited using magnetron sputtering I.P. Studenyak1, M.M. Kutsyk1, A.V. Bendak1, V.Yu. Izai1, P. Kúš2, M. Mikula2 1Uzhhorod National University, Faculty of Physics, 3, Narodna Sq., 88000 Uzhhorod, Ukraine 2Comenius University, Faculty of Mathematics, Physics and Informatics, Mlynska dolina, 84248 Bratislava, Slovakia, E-mail:studenyak@dr.com Abstract. Cu6PS5I-based thin films were deposited using non-reactive radio-frequency magnetron sputtering. Structural studies of thin films were performed by scanning electron microscopy, their chemical composition were determined using energy- dispersive X-ray spectroscopy. As-deposited thin films were irradiated with wideband radiation of Cu-anode X-ray tube at different exposition times. Optical transmission spectra of X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films were measured depending on irradiation time. The Urbach absorption edge and dispersion of refractive index for X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films were studied. It has been revealed the nonlinear decrease of energy pseudogap and nonlinear increase of refractive index with increase of X-ray irradiation time. Keywords: thin film, magnetron sputtering, X-ray irradiation, optical absorption, refractive index. Manuscript received 31.01.17; revised version received 16.05.17; accepted for publication 14.06.17; published online 18.07.17. 1. Introduction Cu6PS5I compounds belong to an argyrodite family and are known as highly-efficient superionic conductors [1]. They are promising materials for creating new types of solid electrolyte batteries, ionistors, and electrochemical sensors [2]. Optical properties (absorption, lumine- scence, Raman scattering, refractive index dispersion) for Cu6PS5I crystals were extensively studied in Refs. [2-4]. Cu6PS5I thin films for the first time were deposited onto silicate glass substrates by non-reactive radio- frequency magnetron sputtering [5]. Structural studies show formation of a homogeneous two-dimensional amorphous structure. No phase transitions are observed in the temperature interval 77…300 K; however, at 470 K the film is partially destructed and detached from the substrate. A typical Urbach bundle is observed, temperature dependences of the energy pseudogap and the Urbach energy are described in the Einstein model. The influence of annealing on the optical absorption edge parameters of Cu6PS5I thin films was investigated in Ref. [6]. It should be noted that the energy pseudogap decreases due to the annealing, but at the same time the Urbach energy increases more than 30%. Optical properties of sulphur and phosphorous implanted Cu6PS5I thin films as well as the influence of ionic implantation on energy pseudogap, Urbach energy and refraction indexes were studied in Ref. [7]. Electrical studies have shown that the total electric conductivity of the Cu6PS5I-based thin films increases Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 2. P. 246-249. doi: https://doi.org/10.15407/spqeo20.02.246 © 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine 247 with increase of Cu atoms content [8]. Thus, with the Cu content increase in the interval from Cu5.37P1.88S5.04I0.71 to Cu7.55P0.89S3.44I1.12, the electric conductivity increases from 0.044 to 0.066 S/m. Besides, with the Cu content increase, a red shift of the optical transmission spectra as well as a typical Urbach bundle, explained by strong electron-phonon interaction, are observed. It is shown that the Urbach tail of the investigated thin films caused by the influence of different type disordering and mainly determined by the contribution of static structural disordering into the film Urbach energy. In this paper, we report on the influence of X-ray irradiation on the optical transmission spectra, Urbach absorption edge parameters and refractive indexes in Cu6PS5I-based thin films. 2. Experimental Thin films were deposited from polycrystalline Cu6PS5I target onto a silicate glass substrate at room temperature by using the non-reactive radio-frequency magnetron sputtering. The structure of the deposited films was analyzed by X-ray diffraction and scanning electron microscopy (SEM) technique (Hitachi S-4300). The diffraction pattern shows the films to be amorphous. The thin film chemical composition (Cu5.56P1.66S4.93I0.85) was determined using the energy-dispersive X-ray spectro- scopy (EDX) studies, which enabled us to check the chemical composition in different points of the film surface. The deposited Cu5.56P1.66S4.93I0.85 thin film is observed to be depleted by copper, sulphur, iodine and enriched with phosphorous. SEM-studies of the thin films confirm formation of a uniform two-dimensional structure (Fig. 1). Fig. 1. SEM image of Cu5.56P1.66S4.93I0.85 thin film. X-ray irradiation was performed for the different exposition times (30, 60 and 120 min) using wideband radiation of Cu-anode X-ray tube with approximately 400 W of power applied (33 kV, 13 mA). Optical transmission spectra of Cu6PS5I-based thin films were studied at room temperature with MDR-3 grating monochromator. Spectral dependences of absorption coefficient and dispersion dependences of refractive index of thin films were calculated using the well-known method [9]. 3. Results and discussion Fig. 2 presents optical transmission spectra for various irradiation times at room temperature for X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films. With irradiation time increase, the red shift of the short-wave part of transmission spectra and interference maxima are observed. Spectral dependences of the absorption coefficient at various irradiation times at room temperature for X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films are shown in Fig. 3. In Ref. [8], it was shown that the optical absorption edge for non-irradiated Cu6PS5I- based thin films in the region of its exponential behaviour is described by the Urbach rule [10] ( ) ⎥ ⎦ ⎤ ⎢ ⎣ ⎡ −ν ⋅α=να )( exp, U 0 0 TE Eh Th , (1) where EU(T) is the Urbach energy, α0 and E0 are the coordinates of the convergence point in the Urbach bundle, hν and T are the photon energy and temperature, respectively. In the X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films, we also observed the Urbach behaviour of the optical absorption edge. It should be noted that the optical absorption edge for X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films is shifted to the long wave region with the irradiation time increase. Fig. 2. Optical transmission spectra of non-irradiated (1) and X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films at various irradiation times: (2) 30, (3) 90 and (4) 210 min. Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 2. P. 246-249. doi: https://doi.org/10.15407/spqeo20.02.246 © 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine 248 Fig. 3. Spectral dependences of the absorption coefficient of non-irradiated (1) and X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films at various irradiation times: (2) 30, (3) 90 and (4) 210 min. To characterize the absorption edge spectral position, such parameter as the energy pseudogap α gE ( α gE is the energy position of the exponential absorption edge) at a fixed absorption coefficient value α was determined. We used the α gE values taken at α = 104 cm−1 for thin films (Table). The observed variation of the optical absorption edge leads to the α gE value decrease and EU value increase with irradiation time increase (from 2.835 to 2.655 eV and from 249 to 404 meV, respectively). The dependences of α gE and UE for X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films on irradiation time are presented in Fig. 4. It is well-known that Urbach energy EU characte- rizes the disordering degree in the investigated system and is described by the equation [11] ( ) ( )XT EEE UUU += , (2) where ( )TEU and ( )XEU are the contributions of temperature and structural disordering to EU, respecti- vely. The Urbach energy EU increase is the evidence of the structural disordering increase caused by X-ray irradiation. Table. Optical parameters of non-irradiated and X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films. Irradiation time (min) 0 30 90 210 n 2.443 2.450 2.455 2.461 α gE (eV) 2.835 2.792 2.699 2.655 UE (meV) 249.3 357.5 382.1 403.6 Fig. 4. Dependences of the energy pseudogap α gE (α = 104 cm–1) and Urbach energy EU on X-ray irradiation time for Cu5.56P1.66S4.93I0.85 thin films. Dispersion dependences of the refractive index for the X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films at various irradiation time are presented in Fig. 5. In the transparency region, a slight dispersion of the refractive index for the X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films is observed, increasing with approaching to the optical absorption edge. With the irradiation time increase, the nonlinear increase of the refractive index in the X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films is revealed (the X-ray irradiation leads to the refractive index increase from 2.443 to 2.461 for λ = 1 µm). It should be noted that the results of the similar investigations of the optical properties of X-ray irradiated a-Se1−xAsx thin films were recently presented in Ref. [12]. It is shown that as a result of X-ray irradiation, there is an increase in the refractive index and a decrease in the film thickness (increase in its density). Fig. 5. Refractive index dispersions of non-irradiated (1) and X-ray irradiated Cu5.56P1.66S4.93I0.85 thin films at various irradiation times: (2) 30, (3) 90 and (4) 210 min. The inset shows the dependence of refractive index on X-ray irradiation time. Semiconductor Physics, Quantum Electronics & Optoelectronics, 2017. V. 20, N 2. P. 246-249. doi: https://doi.org/10.15407/spqeo20.02.246 © 2017, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine 249 4. Conclusions Cu5.56P1.66S4.93I0.85 thin films were deposited onto silicate glass substrates by using the non-reactive radio- frequency magnetron sputtering. The influence of X-ray irradiation on optical properties of Cu5.56P1.66S4.93I0.85 thin films has been investigated. With the irradiation time increase, the decrease of the energy pseudogap as well as the increase of the Urbach energy and refractive index have been observed. Thus, the X-ray irradiation leads to the thin films darkening and density increase. Besides, the increase of Urbach energy is the evidence of increase in structural disordering contribution, which is caused by X-ray irradiation. Acknowledgements Mykhailo Kutsyk (contract number 51602011) is deeply grateful to the International Visegrad Fund scholarship for the funding of the project. References 1. Kuhs W.F., Nitsche R., Scheunemann K. The argyrodites – a new family of the tetrahedrally close-packed structures. Mat. Res. Bull. 1979. 14. P. 241–248. 2. Studenyak I.P., Kranjčec M. Disordering Effects in Superionic Conductors with Argyrodite Structure. Uzhhorode: Hoverla, 2007, 200 p. (in Ukrainian). 3. Studenyak I., Kranjčec M., Kurik M. Urbach rule in solid state physics. Int. J. Opt. Appl. 2014. 4. P. 76–83. 4. Studenyak I.P., Kúš P. Structural Disorder in Crystalline and Amorphous Superionic Conductors. Uzhhorod: Hoverla, 2016, 200 p. 5. Studenyak I.P., Kranjčec M., Izai V.Yu. et al. Structural and temperature-related disordering studies of Cu6PS5I amorphous thin films. Thin Solid Films. 2012. 520. P. 1729–1733. 6. Studenyak I.P., Kranjčec M., Chomolyak A.A., Vorohta M., Matolin V. Optical absorption and refractometric properties of annealed thin films of Cu6PS5I superionic conductor. Nanosystems, Nanomaterials, Nanotechnologies. 2012. 10. P. 489–496. 7. Studenyak I.P., Bendak A.V., Demko P.Yu. et al. Influence of external factors on optical parameters in Cu6PS5I thin films. Proc. SPIE. 2015. 9816. Op- tical Fibers and Their Applications. P. 98160C-8. 8. Studenyak I.P., Bendak A.V., Izai V.Yu. et al. Electrical and optical parameters of Cu6PS5I-based thin films deposited using magnetron sputtering. Semiconductor Physics, Quantum Electronics & Optoelectronics. 2016. 19. P. 79–83. 9. Swanepoel R. Determination of the thickness and optical constants of amorphous silicon. J. Phys. E: Sci. Instrum. 1983. 16. P. 1214–1222. 10. Urbach F. The long-wavelength edge of photographic sensitivity and of the electronic absorption of solids. Phys. Rev. 1953. 92. P. 1324– 1326. 11. Cody G.D., Tiedje T., Abeles B., Brooks B., Goldstein Y. Disorder and the optical-absorption edge of hydrogenated amorphous silicon. Phys. Rev. Lett. 1981. 47. P. 1480–1483. 12. Jung Y., Güneş O., Belev G., Koughia C., Johanson R., Kasap S. X-ray induced effects in the optical and thermal properties of a-Se1−xAsx (x = 0, 0.005, 0.06) doped with 0–220 ppm Cs. J. Mater. Sci.: Materials in Electronics. 2017. 28. P. 7139–7150.
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institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
issn 1560-8034
language English
last_indexed 2026-03-21T11:33:47Z
publishDate 2017
publisher Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
record_format dspace
spelling Studenyak, I.P.
Kutsyk, M.M.
Bendak, A.V.
Izai, V.Yu.
Kus, P.
Mikula, M.
2026-03-04T12:48:48Z
2017
Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu₆PS₅I-based thin films deposited using magnetron sputtering / I.P. Studenyak, M.M. Kutsyk, A.V. Bendak, V. Yu. Izai, P. Kus, M. Mikula // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2017. — Т. 20, № 2. — С. 246-249. — Бібліогр.: 12 назв. — англ.
1560-8034
PACS: 78.40.Ha, 77.80.Bh
https://nasplib.isofts.kiev.ua/handle/123456789/214924
https://doi.org/10.15407/spqeo20.02.246
Cu₆PS₅I-based thin films were deposited using non-reactive radio-frequency magnetron sputtering. Structural studies of thin films were performed by scanning electron microscopy, and their chemical composition was determined using energy-dispersive X-ray spectroscopy. As-deposited thin films were irradiated with wideband radiation of a Cu-anode X-ray tube at different exposure times. Optical transmission spectra of X-ray irradiated Cu₅.₅₆P1.₆₆S₄.₉₃I₀.₈₅ thin films were measured depending on irradiation time. The Urbach absorption edge and dispersion of refractive index for X-rays irradiated Cu₅.₅₆P1.₆₆S₄.₉₃I₀.₈₅ thin films were studied. It has been revealed that the nonlinear decrease of energy pseudogap and the nonlinear increase of refractive index occur with the increase of X-ray irradiation time.
Mykhailo Kutsyk (contract number 51602011) is deeply grateful to the International Visegrad Fund scholarship for the funding of the project.
en
Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
Semiconductor Physics Quantum Electronics & Optoelectronics
Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu₆PS₅I-based thin films deposited using magnetron sputtering
Article
published earlier
spellingShingle Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu₆PS₅I-based thin films deposited using magnetron sputtering
Studenyak, I.P.
Kutsyk, M.M.
Bendak, A.V.
Izai, V.Yu.
Kus, P.
Mikula, M.
title Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu₆PS₅I-based thin films deposited using magnetron sputtering
title_full Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu₆PS₅I-based thin films deposited using magnetron sputtering
title_fullStr Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu₆PS₅I-based thin films deposited using magnetron sputtering
title_full_unstemmed Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu₆PS₅I-based thin films deposited using magnetron sputtering
title_short Influence of X-ray irradiation on the optical absorption edge and refractive index dispersion in Cu₆PS₅I-based thin films deposited using magnetron sputtering
title_sort influence of x-ray irradiation on the optical absorption edge and refractive index dispersion in cu₆ps₅i-based thin films deposited using magnetron sputtering
url https://nasplib.isofts.kiev.ua/handle/123456789/214924
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