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AgNbO3, with the antiferroelectric ordering and huge polarization (>50 μC/cm2), has potential applications in smart electronic devices, such as energy storage dielectrics, large displacement actuators, and electrocaloric cooling device. Large electro-strain and excellent energy storage properties have been reported in AgNbO3-based ceramics. Nevertheless, the lack of systematic research on the AbNbO3 single crystals increases the difficulty in further understanding their structure-property relationship. In this work, ${\left\langle {001} \right\rangle _c}$ oriented AgNbO3 single crystals with a large size (maximum size 5 mm×4 mm×4 mm) and high quality are successfully grown by the flux method. The phase transition characteristics are studied by the X-ray diffraction, temperature dependence of dielectric data and AC impedance, polarized light microscope photos, and differential scanning calorimetry curves. The electrical and optical properties are studied by the ferroelectric response and electro-strain response, optical absorbance spectrum and photo-dielectric effect.The AgNbO3 single crystals with the M phase exhibit the same domain structure. When the structure changes from M2 to M3, the contrast of the PLM image is darkened. Correspondingly, the conductivity and dielectric loss significantly increase, which relates to the dynamic behaviors of the carriers. Interestingly, neither exothermic peak nor endothermic peak relating to the M2-M3 transition is observed. The active energy for the M3 phase AgNbO3 single crystal is ~1.24 eV. When the structure changes from orthogonal M3 to paraelectric orthogonal O, the domain structure disappears and the contrast becomes darker. The finding indicates that the anisotropy of the crystals disappears. At the same time, an obvious thermal hysteresis observed in the DSC curve reveals that the M3-O transition is first-order. At room temperature, the direct band gap of AgNbO3 single crystal is ~2.73 eV, which is slightly narrower than that of AgNbO3 ceramic. Below the critical electric field, AgNbO3 single crystal shows an electro-strain of 0.076% under Em = 130 kV/cm. The obtained electro-strain value is much higher than that of AgNbO3 ceramic under the same electric field. The relative permittivity increases from 70 to 73 under the green laser irradiation, showing an apparent photo-dielectric effect. We believe that our study can assist in the further understanding of the phase transition characteristics and physical properties in AgNbO3 single crystals. -
Keywords:
- AgNbO3 single crystal /
- flux method /
- phase transition characteristics
[1] Chen X, Jiang P P, Duan Z H, Hu Z G, Chen X F, Wang G S, Dong X L, Chu J H 2013 Appl. Phys. Lett. 103 192910
Google Scholar
[2] Tagantsev A K, Vaideeswaran K, Vakhrushev S B, Filimonov A V, Burkovsky R G, Shaganov A, Andronikova D, Rudskoy A. I, Baron A Q R, Uchiyama H, Chernyshov D, Bosak A, Ujma Z, Roleder K, Majchrowski A, Ko J H, Setter N 2013 Nat. Commun. 4 2229
Google Scholar
[3] Tian Y, Jin L, Zhang H, Xu Z, Wei X Y, Politova E D, Stefanovich S Y, Tarakina Nadezda V, Abrahamsc Isaac, Yan H X 2016 J. Mater. Chem. A. 4 17279
Google Scholar
[4] Rödel J, Jo W, Seifert K T P, Anton E, Granzow T, Damjanovic D 2009 J. Am. Chem. Soc. 92 1153
Google Scholar
[5] Luo N N, Han K, Cabral M, Liao X Z, Zhang S J, Liao C Z, Zhang G Z, Chen X Y, Feng Q, Li J F, Wei Y Z 2020 Nat. Commun. 11 4824
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[6] 田野, 靳立, 冯玉军, 庄永勇, 徐卓, 魏晓勇 2017 物理学进展 37 155
Google Scholar
Tian Y, Jin L, Feng Y J, Zhuang Y Y, Xu Z, Wei X Y 2017 Prog. Phys. 37 155
Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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[17] Sciau P, Kania A, Dkhil B, Suard E, Ratuszna A 2004 J. Phys.: Condens. Matter 16 2795
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Google Scholar
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图 1 利用助溶剂法生长出的AgNbO3单晶块体, 插图为切割抛光后的试样
Figure 1. AgNbO3 single crystals grown by flux method. The inset shows the cut specimen.
图 2 AgNbO3晶体及其粉末XRD图 (a)单晶XRD; (b)粉末XRD(Pbcm)精修; (c)粉末XRD(Pmc21)精修
Figure 2. X-ray diffraction patterns of AgNbO3: (a) Single-crystal XRD pattern; (b) rietveld refined powder XRD data with the Pbcm space group; (c) rietveld refined powder XRD data with the Pmc21 space group.
图 3 AgNbO3的相转变特征 (a)介电常数与温度关系; (b)介电损耗与温度关系; (c)变温XRD图谱; (d) 不同温度下的PLM照片; (e)升降温DSC图谱
Figure 3. Phase transition characteristics of AgNbO3: (a) Temperature dependence of relative permittivity; (b) temperature dependence of loss tangent; (c) XRD patterns at various temperatures; (d) PLM photos at various temperatures; (e) DSC curves on heating and cooling.
图 4 AgNbO3晶体的(a)阻抗实部与虚部关系、 (b) Arrhenius拟合曲线及介电常数与温度的关系
Figure 4. (a) Relationship between the real part and imaginary part of the impedance, and (b) Arrhenius fitting curve, and temperature dependence of relative permittivity in AgNbO3 single crystals.
图 5 在不同场强下AgNbO3晶体的(a)极化电流-电场曲线、(b) 极化强度-电场曲线和(c)应变响应
Figure 5. Loops of (a) polarization current, (b) polarization versus external electric field E and (c) strain response of AgNbO3 crystal under different ac maximum electric field
图 6 AgNbO3晶体的光吸收谱线, 插图(a)为(αhν)2与(hν)的关系, 插图(b)为(αhν)1/2与(hν)的关系
Figure 6. Optical absorbance spectrum of AgNbO3 single crystals, inset (a) shows the relationship of (αhν)2and (hν), inset (b) shows the relationship of (αhν)1/2and (hν)
图 7 AgNbO3晶体在暗光下和绿激光照射下的介电常数与损耗
Figure 7. Light-on (under green light illumination) and light-off values of relative permittivity and dielectric loss in AgNbO3 single crystals.
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[1] Chen X, Jiang P P, Duan Z H, Hu Z G, Chen X F, Wang G S, Dong X L, Chu J H 2013 Appl. Phys. Lett. 103 192910
Google Scholar
[2] Tagantsev A K, Vaideeswaran K, Vakhrushev S B, Filimonov A V, Burkovsky R G, Shaganov A, Andronikova D, Rudskoy A. I, Baron A Q R, Uchiyama H, Chernyshov D, Bosak A, Ujma Z, Roleder K, Majchrowski A, Ko J H, Setter N 2013 Nat. Commun. 4 2229
Google Scholar
[3] Tian Y, Jin L, Zhang H, Xu Z, Wei X Y, Politova E D, Stefanovich S Y, Tarakina Nadezda V, Abrahamsc Isaac, Yan H X 2016 J. Mater. Chem. A. 4 17279
Google Scholar
[4] Rödel J, Jo W, Seifert K T P, Anton E, Granzow T, Damjanovic D 2009 J. Am. Chem. Soc. 92 1153
Google Scholar
[5] Luo N N, Han K, Cabral M, Liao X Z, Zhang S J, Liao C Z, Zhang G Z, Chen X Y, Feng Q, Li J F, Wei Y Z 2020 Nat. Commun. 11 4824
Google Scholar
[6] 田野, 靳立, 冯玉军, 庄永勇, 徐卓, 魏晓勇 2017 物理学进展 37 155
Google Scholar
Tian Y, Jin L, Feng Y J, Zhuang Y Y, Xu Z, Wei X Y 2017 Prog. Phys. 37 155
Google Scholar
[7] Kania A, Roleder K, Kugel G E, Fontana M D 1986 J. Phys. C: Solid State Phys. 19 9
Google Scholar
[8] Fu D, Endo M, Taniguchi H, Taniyama T, Itoh M 2007 Appl. Phys. Lett. 90 252907
Google Scholar
[9] Yashima M, Matsuyama S, Sano R, Itoh M, Tsuda K, Fu D 2011 Chem. Mater. 23 1643
Google Scholar
[10] Lu Z L, Sun D Y, Wang G, Zhao J W, Zhang B, Wang D W 2023 J. Adv. Dielectr. 13 2242006
Google Scholar
[11] 洪元婷, 马江平, 武峥, 应静诗, 尤慧琳, 贾艳敏 2018 物理学报 67 107702
Google Scholar
Hong Y T, Ma J P, Wu Z, Ying J S, You H L, Jia Y M 2018 Acta Phys. Sin. 67 107702
Google Scholar
[12] Łukaszewski M, Kania A, Ratuszna A 1980 J. Crystal Growth 48 493
Google Scholar
[13] Kitanaka Y, Egawa T, Noguchi Y, Miyayama M 2016 Jpn. J. Appl. Phys. 55 10TB03
Google Scholar
[14] Zhao W, Fu Z Q, Deng J M, Li S, Han Y F, Li M R, Wang X Y, Hong J W 2021 Chin. Phys. Lett. 38 037701
Google Scholar
[15] Pawełczyk M 1987 Phase Transitions 8 273
Google Scholar
[16] Verwerft M, Van Dyck D, Brabers V A M, Van Landuyt J, Amelinckx S 1989 Phys. Status Solidi A 112 451
Google Scholar
[17] Sciau P, Kania A, Dkhil B, Suard E, Ratuszna A 2004 J. Phys.: Condens. Matter 16 2795
Google Scholar
[18] Levin I, Krayzman V, Woicik J C, Karapetrova J, Proffen T, Tucker M G, Reaney I M 2009 Phys. Rev. B 79 104113
Google Scholar
[19] Ratuszna A, Pawluk J, Kania A 2003 Phase Transitions. 76 611
Google Scholar
[20] Kania A, Niewiadomski A, Miga S, Sumara I J, Pawlik M, Ujma Z, Koperski J, Suchanicz J 2014 J. Eur. Ceram. Soc. 34 1761
Google Scholar
[21] Sakurai H, Yamazoe S, Wada T 2010 Appl. Phys. Lett. 97 042901
Google Scholar
[22] Yashima M, Matsuyama S 2012 J. Phys. Chem. C 116 24902
Google Scholar
[23] Samantaray C B, Sim H, Hwang H 2005 Microelectronics J. 36 725
Google Scholar
[24] Pandey S K, James A R, Raman R, Chatterjee S N, Goyal A, Prakash C, Goel T C 2005 J. Phys B 369 135
Google Scholar
[25] Burkert F, Kreisel J, Kuntscher C A 2016 Appl. Phys. Lett. 109 182903
Google Scholar
[26] Wei Y X, Jin C Q, Ni R R, Zeng Y M, Gao D, Jian Z Y 2018 J. Eur. Ceram. Soc. 38 4689
Google Scholar
[27] Rubio-Marcos F, Ochoa D A, Campo A D, García M A, Castro G R, Fernández J F, García J E 2018 Nat. Photon. 12 29
Google Scholar
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