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1. Ordering/displacive ferrielectricity in 2D CuInP$_2$S$_6$

Author

Vysochanskii, Yulian, Liubachko, Vitalii, Glukhov, Konstantin, Yevych, Ruslan, Kohutych, Anton, Hryts, Viacheslav, Dziaugys, Andrius, and Banys, Juras

Subjects
Condensed Matter - Materials Science
Abstract

Using DFT-based molecular dynamics simulation of Cu$^+$ cations flipping and In$^{3+}$ cations displacive dynamics, we clarify the dipole ordering of CuInP$_2$S$_6$ ferrielectrics through the second order Jahn-Teller effect which determines the double-well potential for copper cations as well as three-well potential for indium cations inside the structural layers. The temperature dependence of the spatial distribution of Cu$^+$ and In$^{3+}$ cations is also described within the quantum anharmonic oscillators model. In$^{3+}$ cations play a decisive role in the character of the polar ordering: at ambient or for positive pressures, the first order transition occurs; with the rise of negative compression, the ferrielectric transition evolves to the second order. The peculiarities of spontaneous polarization switching are related to the contributions of copper and indium cationic sublattices.

Published
2023

2. Origin of relaxor behavior in barium-titanate based lead-free perovskites

Author

Veerapandiyan, Vignaswaran, Popov, Maxim N., Mayer, Florian, Spitaler, Jürgen, Svirskas, Sarunas, Kalendra, Vidmantas, Lins, Jonas, Canu, Giovanna, Buscaglia, Maria Teresa, Pasciak, Marek, Banys, Juras, Groszewicz, Pedro B., Buscaglia, Vincenzo, Hlinka, Jiri, and Deluca, Marco

Subjects
Condensed Matter - Materials Science
Abstract

It is well known that disordered relaxor ferroelectrics exhibit local polar correlations. The origin of localized fields that disrupt long range polar order for different substitution types, however, is unclear. Currently, it is known that substituents of the same valence as Ti4+ at the B-site of barium titanate lattice produce random disruption of Ti-O-Ti chains that induces relaxor behavior. On the other hand, investigating lattice disruption and relaxor behavior resulting from substituents of different valence at the B-site is more complex due to the simultaneous occurrence of charge imbalances and displacements of the substituent cation. The existence of an effective charge mediated mechanism for relaxor behavior appearing at low (< 10%) substituent contents in heterovalent modified barium titanate ceramics is presented in this work. These results will add credits to the current understanding of relaxor behavior in chemically modified ferroelectric materials and also acknowledge the critical role of defects (such as cation vacancies) in lattice disruption, paving the way for chemistry-based materials design in the field of dielectric and energy storage applications.

Published
2021
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4. Q-band EPR cryoprobe

Author

Kalendra, Vidmantas, Turčak, Justinas, Usevičius, Gediminas, Karas, Hugo, Hülsmann, Miriam, Godt, Adelheid, Jeschke, Gunnar, Banys, Jūras, Morton, John J.L., and Šimėnas, Mantas

Published
2023
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12. Broadband dielectric spectroscopy of a PbHf1-xSnxO3 material.

Author

Haronin, Vadzim, Jankowska-Sumara, Irena, Kadlec, Christelle, Majchrowski, Andrzej, Suvorova, Olga, Grigalaitis, Robertas, and Banys, Juras

Subjects
PHASE transitions, LATTICE dynamics, SOLID solutions, LEAD, TIN, BROADBAND dielectric spectroscopy
Abstract

The combination of PbHfO3 and PbSnO3 in perovskite solid solutions presents valuable opportunities to study the formation mechanisms of incommensurate phases. Crystals of PbHf1-xSnxO3 with 8% Sn were grown and measured using broadband dielectric spectroscopy to investigate the nature of relaxation and the effects of phase transitions. Our findings reveal significant alterations in the dielectric response of the PbHf0.92Sn0.08O3 solid solution, shedding light on the influence of Sn doping on lattice dynamics during the phase transition. [ABSTRACT FROM AUTHOR]

Published
2024
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15. Probing structural and dynamic properties of MAPbCl3 hybrid perovskite using Mn2+ EPR

Author

Usevicius, Gediminas, primary, Turcak, Justinas, additional, Zhang, Yuxuan, additional, Eggeling, Andrea, additional, Einoryte, Zyginta, additional, Hope, Michael A., additional, Svirskas, Sarunas, additional, Klose, Daniel, additional, Kalendra, Vidmantas, additional, Aidas, Kęstutis, additional, Jeschke, Gunnar, additional, Banys, Juras, additional, and Simenas, Mantas, additional

Published
2024
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17. Peculiar Bi-ion dynamics in Na1/2Bi1/2TiO3 from terahertz and microwave dielectric spectroscopy

Author

Petzelt, Jan, Nuzhnyy, Dmitry, Bovtun, Viktor, Pasciak, Marek, Kamba, Stanislav, Dittmer, Robert, Svirskas, Sarunas, Banys, Juras, and Rodel, Jurgen

Subjects
Condensed Matter - Materials Science
Abstract

Dynamics of the main dielectric anomaly in Na1/2Bi1/2TiO3 (NBT) was studied by time-domain THz and microwave spectroscopy, using also previously published data and their new overall fits. Above the dielectric maximum temperature Tm ~ 600 K, the response consists of coupled sub-THz oscillator and a relaxation mode, assigned to strongly anharmonic Bi-ion vibrations and hopping, whose slowing down explains the paraelectric-like permittivity increase to Tm. Below Tm, the main relaxation continues slowing down and additional relaxation, assigned to quasi-Debye losses, appears in the 10^11 Hz range. The oscillator hardens on cooling and takes over the whole oscillator strength. The permittivity decrease below Tm is caused by the reduced strength of the relaxations due to dominance of the rhombohedral phase within the coexistence region with the tetragonal phase. The anharmonic dynamics of Bi is supported by previous structural studies. NBT represents a hybrid between standard and relaxor ferroelectric behaviour.

Published
2014

19. Phase Diagram and Dielectric Response of Hybrid Lead Halide Hollow Perovskites: A Universal Behavior of Molecular Cation Mixing

Author

Rimkus, Gabrielius, Balčiu̅nas, Sergejus, Ptak, Maciej, Smółka, Szymon, Klimavičius, Vytautas, Szewczyk, Daria, Sieradzki, Adam, Kalendra, Vidmantas, Banys, Ju̅ras, Mączka, Mirosław, and Šimėnas, Mantas

Abstract

Mixing of molecular cations in hybrid lead halide perovskites is used to effectively tune the stability and performance of the photovoltaic devices based on these compounds. Upon introduction of bulky molecular cations such as ethylenediammonium (EN), the perovskite framework becomes locally broken resulting in so-called hollow perovskites. Here, we use a set of different experimental techniques to probe the structural phase transitions, molecular cation dynamics, and dielectric response in methylammonium-based MA1–xENxPb1–0.7xI3–0.4xhollow perovskites containing different amounts of EN molecular cations (x≤ 0.26). We determine the temperature–composition phase diagram of this system and show that the introduction of EN results in stabilization of the desirable high-symmetry cubic phase, as the structural phase transitions become partially suppressed. Broadband dielectric spectroscopy experiments are used to study the dynamics of molecular cations for different fractions of EN. For high levels of EN, we observe signatures of a dipolar glass phase formation. Our findings indicate a universal trend of the dielectric response upon molecular cation mixing independent of the size and charge of the incorporated guest cations in MAPbI3.

Published
2024
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20. Mechanism of isosymmetric polar order–disorder phase transition in pyroelectric [CH3CH2NH3]2NaGa(HCOO)6 double perovskite.

Author

Ptak, Maciej, Kabański, Adam, Dziuk, Błażej, Balciunas, Sergejus, Usevicius, Gediminas, Zaręba, Jan K., Banys, Juras, Simenas, Mantas, Sieradzki, Adam, and Stefańska, Dagmara

Abstract

Recently, hybrid double-perovskite structures have attracted attention due to their versatile multifunctional properties originating from the variety of different constituent units in these materials. Here, we report the synthesis and comprehensive multitechnique characterization of a novel hybrid double-perovskite formate-based material [CH3CH2NH3]2NaGa(HCOO)6. The heat capacity measurements indicate that this compound has a structural phase transition at 379 K. In the low-temperature phase, the compound crystallizes in the non-centrosymmetric polar Pn structure, which exhibits a long-range order of ethylammonium (EA+) cations. Surprisingly, the Pn space group is not affected by the transition to the high-temperature disordered phase, which indicates that the transitions are isosymmetric making this compound a unique member of the formate-based double-perovskite family. The presence of the second-harmonic generation response in both phases confirms their non-centrosymmetric nature, while the dielectric spectroscopy experiments reveal that the transitions have a continuous order–disorder character. The observation of the pyroelectric current, but the absence of the electric polarization switching indicate that this compound is not properly ferroelectric. The electron paramagnetic resonance experiments of a compound slightly doped with paramagnetic Fe3+ impurities confirm the continuous character of the transition and allow us to probe the EA+ cation and framework dynamics in this system. The vibrational spectroscopy data confirm that the phase transition is primarily driven by the progressive ordering of EA+ cations and the resulting changes in the hydrogen bond strength. The temperature-dependent luminescence studies show that the [EA]2NaCr0.931Ga0.069(HCOO)6 perovskite is a promising material for noncontact temperature monitoring. [ABSTRACT FROM AUTHOR]

Published
2024
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21. Phase Transitions, Dielectric Response, and Nonlinear Optical Properties of Aziridinium Lead Halide Perovskites

Author

Mączka, Mirosław, primary, Ptak, Maciej, additional, Gągor, Anna, additional, Zaręba, Jan K., additional, Liang, Xia, additional, Balčiu̅nas, Sergejus, additional, Semenikhin, Oleksandr A., additional, Kucheriv, Olesia I., additional, Gural’skiy, Il’ya A., additional, Shova, Sergiu, additional, Walsh, Aron, additional, Banys, Ju̅ras, additional, and Šimėnas, Mantas, additional

Published
2023
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31. Piezoelectric domain walls in van der Waals antiferroelectric CuInP2Se6

Author

Dziaugys, Andrius, Kelley, Kyle, Brehm, John A., Tao, Lei, Puretzky, Alexander, Feng, Tianli, O’Hara, Andrew, Neumayer, Sabine, Chyasnavichyus, Marius, Eliseev, Eugene A., Banys, Juras, Vysochanskii, Yulian, Ye, Feng, Chakoumakos, Bryan C., Susner, Michael A., McGuire, Michael A., Kalinin, Sergei V., Ganesh, Panchapakesan, Balke, Nina, Pantelides, Sokrates T., Morozovska, Anna N., and Maksymovych, Petro

Published
2020
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32. Ordering/displacive ferrielectricity in 2D CuInP2S6.

Author

Vysochanskii, Yulian, Liubachko, Vitalii, Glukhov, Konstantin, Yevych, Ruslan, Kohutych, Anton, Hryts, Viacheslav, Dziaugys, Andrius, and Banys, Juras

Subjects
ANHARMONIC oscillator, MOLECULAR dynamics, COPPER, JAHN-Teller effect
Abstract

Using DFT-based molecular dynamics simulation of Cu+ cations flipping and In3+ cations displacive dynamics, we clarify the dipole ordering of CuInP2S6 ferrielectrics through the second order Jahn-Teller effect which determines the double-well potential for copper cations as well as three-well potential for indium cations inside the structural layers. The temperature dependence of the spatial distribution of Cu+ and In3+ cations is also described within the quantum anharmonic oscillator model. In3+ cations play a decisive role in the character of the polar ordering: at ambient or for positive pressures, the first order transition occurs; with the rise of negative compression, the ferrielectric transition evolves to the second order. The peculiarities of spontaneous polarization switching are related to the contributions of copper and indium cationic sublattices. [ABSTRACT FROM AUTHOR]

Published
2024
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33. Ordering/displacive ferrielectricity in 2D CuInP2S6.

Author

Vysochanskii, Yulian, Liubachko, Vitalii, Glukhov, Konstantin, Yevych, Ruslan, Kohutych, Anton, Hryts, Viacheslav, Dziaugys, Andrius, and Banys, Juras

Abstract

Using DFT-based molecular dynamics simulation of Cu+ cations flipping and In3+ cations displacive dynamics, we clarify the dipole ordering of CuInP2S6 ferrielectrics through the second order Jahn-Teller effect which determines the double-well potential for copper cations as well as three-well potential for indium cations inside the structural layers. The temperature dependence of the spatial distribution of Cu+ and In3+ cations is also described within the quantum anharmonic oscillator model. In3+ cations play a decisive role in the character of the polar ordering: at ambient or for positive pressures, the first order transition occurs; with the rise of negative compression, the ferrielectric transition evolves to the second order. The peculiarities of spontaneous polarization switching are related to the contributions of copper and indium cationic sublattices. [ABSTRACT FROM AUTHOR]

Published
2024
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34. Piezoelectric Nanogenerators Based On BaTiO3/PDMS Composites for High-Frequency Applications

Author

Meisak, Darya, primary, Kinka, Martynas, additional, Plyushch, Artyom, additional, Macutkevič, Jan, additional, Zarkov, Aleksej, additional, Schaefer, Sébastien, additional, Selskis, Algirdas, additional, Samulionis, Vytautas, additional, Kuzhir, Polina, additional, Banys, Ju̅ras, additional, Fierro, Vanessa, additional, and Celzard, Alain, additional

Published
2023
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36. List of contributors

Author

Araujo, Luis A.O., primary, Banys, Juras, additional, Barbier, Antoine, additional, Bastos, Wagner B., additional, Bencan, Andreja, additional, Blaž, Nelu, additional, Bobic, Jelena D., additional, Cilense, Mario, additional, Ciomaga, Cristina E., additional, Cirkovic, Sasa T., additional, Cortés, Johan A., additional, Cvejić, Zeljka, additional, Damnjanović, Mirjana, additional, Djordjevic, Drago M., additional, dos Reis, Idalci Cruvinel, additional, Dzunuzovic, Adis S., additional, Feteira, Antonio, additional, Fortulan, Carlos A., additional, Foschini, Cesar R., additional, Gonzalez, Amador M., additional, González-Abreu, Yuslín, additional, Grigalaitis, Robertas, additional, Guerra, José de los Santos, additional, Hinojosa, Juan, additional, Ianculescu, Adelina-Carmen, additional, Ilic, Nikola I., additional, Ivanov, Maksim, additional, Katiyar, Ram S., additional, Khomyakova, Evgeniya, additional, Kisić, Milica, additional, Kodumudi Venkataraman, Lalitha, additional, Kong, Ling Bing, additional, Koruza, Jurij, additional, Kumar, Ashok, additional, Kumari, Shalini, additional, Kuščer, Danjela, additional, Li, Sean, additional, Liu, Lie, additional, Longo, Elson, additional, Lustosa, Glauco M.M.M., additional, Macutkevic, Jan, additional, Malič, Barbara, additional, Mandic, Dusanka S., additional, Marić, Andrea, additional, Martínez-Viviente, Félix Lorenzo, additional, Milanović, Marija, additional, Mitoseriu, Liliana, additional, Morán, Emilio, additional, Moura, Francisco, additional, Paiva-Santos, Carlos O., additional, Pardo, Lorena, additional, Pascual-Gonzalez, Cristina, additional, Peláiz-Barranco, Aimé, additional, Perazolli, Leinig A., additional, Pintilie, Ioana, additional, Pintilie, Lucian, additional, Pradhan, Dhiren K., additional, Radosavljević, Goran, additional, Rakić, Srdjan, additional, Ramirez, Miguel A., additional, Reyes-Montero, Armando, additional, Rocha, Leandro S.R., additional, Rojac, Tadej, additional, Schileo, Giorgio, additional, Simões, Alexandre Z., additional, Srdić, Vladimir V., additional, Stanciu, Catalina-Andreea, additional, Stojanovic, Biljana D., additional, Stojanović, Goran, additional, Tararam, Ronald, additional, Teixeira, Guilhermina F., additional, Ursic, Hana, additional, Vijatovic Petrovic, Mirjana M., additional, Villafuerte-Castrejón, María E., additional, Vivar-Ocampo, Rodrigo, additional, Vrabelj, Marko, additional, Walker, Julian, additional, Wang, Chuanhu, additional, Yang, Zhihong, additional, Zaghete, Maria A., additional, Zanetti, Sonia M., additional, Zhang, Tianshu, additional, and Živanov, Ljiljana, additional

Published
2018
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38. Ordering/displacive ferrielectricity in 2D MM'P$_2$S$_6$

Author

Vysochanskii, Yulian, Liubachko, Vitalii, Glukhov, Konstantin, Yevych, Ruslan, Kohutych, Anton, Hryts, Viacheslav, Dziaugys, Andrius, and Banys, Juras

Subjects
Materials Science (cond-mat.mtrl-sci), FOS: Physical sciences
Abstract

DFT-based molecular dynamics simulation of the Cu$^+$ cations flipping of and the In$^{3+}$ cations displacive dynamics of, we clarify the dipole ordering of CuInP$_2$S$_6$ ferrielectrics through the second order Jahn-Teller effect which determines the double-well potential for copper cations as well as three-well potential for indium cations inside the structural layers. The temperature dependence of the spatial distribution of Cu$^+$ and In$^{3+}$ cations is also described within the quantum anharmonic oscillators model. In$^{3+}$ cations play a decisive role in the character of the polar ordering: at ambient or for positive pressures, the first order transition occurs; with the rise of negative compression, the ferrielectric transition evolves to the second order. The peculiarities of spontaneous polarization switching are related to the contributions of copper and indium cationic sublattices.

Published
2023
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39. Mixology of MA1–xEAxPbI3 Hybrid Perovskites: Phase Transitions, Cation Dynamics, and Photoluminescence

Author

Šimėnas, Mantas, primary, Balčiu̅nas, Sergejus, additional, Ga̧gor, Anna, additional, Pienia̧żek, Agnieszka, additional, Tolborg, Kasper, additional, Kinka, Martynas, additional, Klimavicius, Vytautas, additional, Svirskas, Šaru̅nas, additional, Kalendra, Vidmantas, additional, Ptak, Maciej, additional, Szewczyk, Daria, additional, Herman, Artur P., additional, Kudrawiec, Robert, additional, Sieradzki, Adam, additional, Grigalaitis, Robertas, additional, Walsh, Aron, additional, Ma̧czka, Mirosław, additional, and Banys, Ju̅ras, additional

Published
2022
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47. Van der Waals Ferroelectrics

Author

Banys, Juras, primary, Dziaugys, Andrius, additional, Glukhov, Konstantin E., additional, Morozovska, Anna N., additional, Morozovsky, Nicholas V., additional, and Vysochanskii, Yulian M., additional

Published
2022
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