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Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties...
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Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications

A special issue of Crystals (ISSN 2073-4352). This special issue belongs to the section "Inorganic Crystalline Materials".

Deadline for manuscript submissions: closed (25 August 2020) | Viewed by 27860

Special Issue Editors

Prof. Dr. Fapeng Yu

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Guest Editor
State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, China
Interests: piezoelectric crystals; nonlinear optical crystals; single crystal growth; structure–property relationships; piezoelectric sensors
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Limei Zheng

E-Mail Website
Guest Editor
School of Physics, Shandong University, Jinan, China
Interests: piezoelectric ceramics; ferroelectric films; ferroelectric single crystals; ferroelectric tunnel junctions
Prof. Bo Wang

E-Mail Website
Guest Editor
Institute of Crystal Materials, Shandong University, Jinan, China

Special Issue Information

Dear Colleagues,

The advances in non-centrosymmetric crystal materials greatly promote the development of multifunctional devices, taking advantage of piezoelectric, ferroelectric, pyroelectric, non-linear optic and electro-optic effects and affect many aspects of industry fields. These crystal materials are capable of achieving the mutual conversion of different energies, including light, electricity, heat, magnetism, mechanical force and so on. Among the non-centrosymmetric crystals, the piezoelectric, ferroelectric and nonlinear optical crystal materials have attracted a lot of attention in recent decades.

Extensive studies have been implemented on designing new non-centrosymmetric crystal materials and/or optimising the opto-electric functions of crystal materials to improve the selectivity of crystal materials for device applications. Crystal growth has also been proposed to enhance the piezoelectric, ferroelectric and nonlinear optical response. Firstly, the absence of grain boundaries in single crystals enables a larger volume of the material, contributing to the electromechanical and nonlinear responses. Secondly, the chemical doping in piezoelectric, ferroelectric and nonlinear optical crystals can manipulate the microscopic polarization, thus improving the macroscopic opto-electric properties. Thirdly, the low-dimensional piezoelectric, ferroelectric and nonlinear optical crystals would be conducive to the findings of interesting electrical and optical behaviours.

This Special Issue aims at covering all the relevant aspects of piezoelectric and nonlinear optical crystal materials. Both well-established, novel, or less common compounds, and micro mechanisms in single crystals will be covered. Therefore, the Issue welcomes original research and review manuscripts on the following main aspects:

  • Development and design of non-centrosymmetric crystal materials
  • Piezoelectric and/or ferroelectric crystals and films
  • Nonlinear optical crystals
  • Piezoelectricity
  • Ferroelectricity
  • Domain engineering
  • Crystal defects
  • Opto-electric property characterization
  • Theoretical study with Ab-initio, DFT, and first principle calculations on non-centrosymmetric crystal materials

Prof. Fapeng Yu
Prof. Limei Zheng
Prof. Bo Wang
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Crystals is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • Piezoelectric and/or ferroelectric crystals and films
  • Nonlinear optical crystals
  • Piezoelectricity
  • Crystal defects

Related Special Issue

Published Papers (11 papers)

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Research

16 pages, 7799 KiB  
Article
Numerical Simulation Study on the Front Shape and Thermal Stresses in Growing Multicrystalline Silicon Ingot: Process and Structural Design
by Chengmin Chen, Guangxia Liu, Lei Zhang, Guodong Wang, Yanjin Hou and Yan Li
Crystals 2020, 10(11), 1053; https://doi.org/10.3390/cryst10111053 - 19 Nov 2020
Cited by 4 | Viewed by 1862
Abstract
In this paper, a transient numerical simulation method is used to investigate the effects of the two furnace configurations on the thermal field: the shape of the melt–crystal (M/C) interface and the thermal stress in the growing multicrystalline ingot. First, four different power [...] Read more.
In this paper, a transient numerical simulation method is used to investigate the effects of the two furnace configurations on the thermal field: the shape of the melt–crystal (M/C) interface and the thermal stress in the growing multicrystalline ingot. First, four different power ratios (top power to side power) are investigated, and then three positions (i.e., the vertical, angled, and horizontal positions) of the insulation block are compared with the conventional setup. The power ratio simulation results show that with a descending power ratio, the M/C interface becomes flatter and the thermal stress in the solidified ingot is lower. In our cases, a power ratio of 1:3–1:4 is more feasible for high-quality ingot. The block’s position simulation results indicate that the horizontal block can more effectively reduce the radial temperature gradient, resulting in a flatter M/C interface and lower thermal stress. Full article
(This article belongs to the Special Issue Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications)
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11 pages, 2704 KiB  
Article
Spectroscopic, Raman, EMPA, Micro-XRF and Micro-XANES Analyses of Sulphur Concentration and Oxidation State of Natural Apatite Crystals
by Bo Xu, Guanyu Kou, Barbara Etschmann, Daiyue Liu and Joël Brugger
Crystals 2020, 10(11), 1032; https://doi.org/10.3390/cryst10111032 - 12 Nov 2020
Cited by 15 | Viewed by 2729
Abstract
Sulphur is the third most abundant volatile element in deep Earth systems. Analytical methods for accurately and efficiently determining the sulphur content and oxidation state in natural minerals are still lacking. Natural apatite is widely distributed in the Earth and incorporates a large [...] Read more.
Sulphur is the third most abundant volatile element in deep Earth systems. Analytical methods for accurately and efficiently determining the sulphur content and oxidation state in natural minerals are still lacking. Natural apatite is widely distributed in the Earth and incorporates a large amount of sulphur. Therefore, apatite is an ideal mineral for performing sulphur measurements. Here, we used spectroscopic, Raman, X-ray diffraction, laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS), electron microprobe (EMPA) and micro-X-ray fluorescence spectrometry (micro-XRF) analysis techniques and developed a new analytical approach (i.e., micro-X-ray absorption near-edge structure (micro-XANES) analysis of the sulphur K-edge) to investigate the chemical characteristics of natural apatite. These multiple methods were developed to measure in situ sulphur concentration and S oxidation states and to assess a potential natural apatite reference material. Apatite contains chemically homogeneous sulphur, with micro-XANES located at the peak energies corresponding to S6+ (sulphate; ~2482 eV), S4+ (sulfite; ~2478 eV), and S2− (sulphide; ~2467, 2470 and 2474 eV). The Durango apatite contains total S presented as SO3 at amount of 0.332 ± 0.012 wt.% (1σ), with a large amount of S6+ and a small contribution of S4+. The Kovdor apatite contains 44–100 ppm of S and is dominated by S6+. These results indicate that the Durango apatite crystallised under relative oxidising conditions, and the Kovdor apatite has a higher oxygen fugacity than Durango. In addition, this study indicates the potential use of the natural apatite reference material with its S composition and S oxidation state. Full article
(This article belongs to the Special Issue Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications)
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14 pages, 3483 KiB  
Article
Molecular Orbital Calculation of Lead-Free Perovskite Compounds for Efficient Use of Alkaline and Alkaline Earth Metals
by Naohisa Takesue and Jun-ichi Saito
Crystals 2020, 10(11), 956; https://doi.org/10.3390/cryst10110956 - 22 Oct 2020
Viewed by 2259
Abstract
The effective ionic charges of lead-free perovskite dielectric complex compounds were investigated with molecular orbital calculation. The base model was a double perovskite cluster that consisted of octahedral oxygen cages with a transition metal ion of titanium, niobium, or zirconium located at each [...] Read more.
The effective ionic charges of lead-free perovskite dielectric complex compounds were investigated with molecular orbital calculation. The base model was a double perovskite cluster that consisted of octahedral oxygen cages with a transition metal ion of titanium, niobium, or zirconium located at each of their centers, and alkali and/or alkaline earth metal ions located at the body center, corners, edge centers, or face centers of the cluster. The results showed significant covalent bonds between the transition metals and the oxygens, and the alkali metals, especially sodium and oxygen. On the other hand, the alkaline earth metals have weak covalency. Calculation was also performed with the replacement of some of the oxygens with chlorine or fluorine; such replacement enhances the covalency of the transition metals. These trends provide good guidelines for the design properties of lead-free perovskite piezoelectrics based on ubiquitous sodium use. Full article
(This article belongs to the Special Issue Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications)
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9 pages, 1912 KiB  
Article
Control of Thermophysical Properties of Langasite-Type La3Ta0.5Ga5.5O14 Crystals for Pressure Sensors
by Haruki Usui, Makoto Tokuda, Kazumasa Sugiyama, Takuya Hoshina, Takaaki Tsurumi, Kheirreddine Lebbou, Ikuo Yanase and Hiroaki Takeda
Crystals 2020, 10(10), 936; https://doi.org/10.3390/cryst10100936 - 14 Oct 2020
Cited by 1 | Viewed by 2033
Abstract
We present a possible method to reduce the anisotropy of the thermal stress generated on langasite-type La3Ta0.5Ga5.5O14 (LTG) piezoelectric crystals arising from the mismatch of the thermal expansion coefficients and Young’s moduli of the crystals and [...] Read more.
We present a possible method to reduce the anisotropy of the thermal stress generated on langasite-type La3Ta0.5Ga5.5O14 (LTG) piezoelectric crystals arising from the mismatch of the thermal expansion coefficients and Young’s moduli of the crystals and metals at high temperatures. To formulate this method, the thermal stresses of order-type langasite crystals, in which each cation site is occupied by one element only, were calculated and compared to each other. Our results suggest that the largest cation site affects the thermal stress. We attempted to replace La3+ in LTG by a larger ion and considered Sr2+. Single crystals of strontium-substituted LTG (Sr-LTG) were grown using the Czochralski method. The thermal stress along the crystallographic c-axis decreased but that perpendicular to the c-axis increased by strontium substitution into the LTG crystal. The anisotropic thermal stress was reduced effectively. The Sr-LTG single crystal is a superior candidate material for pressure sensors usable at high temperatures. Full article
(This article belongs to the Special Issue Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications)
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9 pages, 3952 KiB  
Article
Electro-Optic Intensity Modulation in Fe-Doped KTa0.65Nb0.35O3 Crystals
by Cheng-Kai Yang, Xu-Ping Wang, Fei Zhang, Hua-Di Zhang, Bing Liu, Jing Li, Yuan-Yuan Zhang, Yu-Guo Yang, Xian-Shun Lv and Lei Wei
Crystals 2020, 10(10), 870; https://doi.org/10.3390/cryst10100870 - 26 Sep 2020
Cited by 2 | Viewed by 2158
Abstract
KTa0.65Nb0.35O3 and Fe-doped KTa0.65Nb0.35O3 crystals were grown by the top-seeded solution growth method (TSSG). Fe ion doping significantly improves the electro-optic properties of cubic KTN crystals. We describe their electro-optic modulation theory and [...] Read more.
KTa0.65Nb0.35O3 and Fe-doped KTa0.65Nb0.35O3 crystals were grown by the top-seeded solution growth method (TSSG). Fe ion doping significantly improves the electro-optic properties of cubic KTN crystals. We describe their electro-optic modulation theory and experimental research. The electro-optic modulation waveform deduced by theoretical calculation is basically consistent with the waveform measured in the experiment. We observed the attenuation of light modulation under multiple voltage cycles. The modulation curve of the crystal is inconsistent when the crystal voltage is boosting and bucking. Under the same voltage condition, the higher the incident light power, the faster the modulation depth attenuation. In this experiment, the size of the KTN crystal chip is 6 mm × 5 mm × 2 mm. We obtain the effective electro-optic coefficient as s11 − s12 = 1.34 × 10−15 m2/V2; the half-wave voltage near the Curie temperature is 39 V. Full article
(This article belongs to the Special Issue Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications)
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9 pages, 1548 KiB  
Article
Synthesis, Crystal Structures and Characterization of Two Nonmetal Cation Tetrafluoroborates
by Noura Othman Alzamil, Ghareeba Mussad Al-Enzi, Aishah Hassan Alamri, Insaf Abdi and Amor BenAli
Crystals 2020, 10(9), 812; https://doi.org/10.3390/cryst10090812 - 14 Sep 2020
Cited by 3 | Viewed by 2291
Abstract
Two new nonmetal cation tetrafluoroborate phases [H3tren](BF4)3 (I) and [H3tren](BF4)3 HF (II) were synthesized by microwave-assisted solvothermal and characterized by single crystal X-ray diffraction, IR spectroscopy and thermal analysis DTA-TGA. [H [...] Read more.
Two new nonmetal cation tetrafluoroborate phases [H3tren](BF4)3 (I) and [H3tren](BF4)3 HF (II) were synthesized by microwave-assisted solvothermal and characterized by single crystal X-ray diffraction, IR spectroscopy and thermal analysis DTA-TGA. [H3tren](BF4)3 is cubic (P213) with unit cell parameter a = 11.688(1) Å. [H3tren](BF4)3•HF is trigonal (R3c) with unit cell parameters a = 15.297(6) Å and c = 12.007(2) Å. Both (I) and (II) structures can be described from isolated tetrafluoroborate BF4- anions, triprotonated tris-(2-aminoethyl)amine (tren) [H3tren]3+. Phase (II) contains disordered BF4- tetrahedron and hydrofluoric acid. Full article
(This article belongs to the Special Issue Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications)
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14 pages, 1472 KiB  
Article
Widely Tunable Angular Non-Critical Phase-Matching Wavelengths from 0.72 to 1.42 μm Based on RE1xRE21−xCOB Mixed Crystals
by Ranran Li, Hongwei Qi, Yanqing Liu, Fapeng Yu, Pingzhang Yu, Zhengping Wang, Xinguang Xu and Xian Zhao
Crystals 2020, 10(9), 744; https://doi.org/10.3390/cryst10090744 - 24 Aug 2020
Cited by 3 | Viewed by 1963
Abstract
The angular non-critical phase-matching (A-NCPM) second-harmonic-generation (SHG) properties of RE1xRE21−xCOB (RE1, RE2 = Y, Gd, La, Tm, Sm, and Nd) type mixed crystals including NCPM wavelength and conversion efficiency were detailedly investigated. Theoretical calculations manifest that the A-NCPM SHG [...] Read more.
The angular non-critical phase-matching (A-NCPM) second-harmonic-generation (SHG) properties of RE1xRE21−xCOB (RE1, RE2 = Y, Gd, La, Tm, Sm, and Nd) type mixed crystals including NCPM wavelength and conversion efficiency were detailedly investigated. Theoretical calculations manifest that the A-NCPM SHG scope of these crystals is 0.72~1.42 µm, and in experiments, the A-NCPM SHG waveband of 0.72~1.25 µm has been realized, by changing the ratio of the rare-earth elements RE1 and RE2 in RE1xRE21−xCOB crystals. Comparing to the temperature-dependent A-NCPM SHG of 0.95~1.34 µm in LiB3O5 (LBO) crystal, the composition-dependent A-NCPM SHG of 0.72~0.95 µm in RE1xRE21−xCOB type crystals is unique and has special significance for the frequency conversion of Ti:Sapphire lasers. Relationships between the birefringence and radius of rare-earth ion RE3+ in RE1xRE21−xCOB mixed crystals were discussed. Aiming for the A-NCPM SHG of 0.72~1.42 µm, we supply a clear, completed, and optimized solution on how to select the compositions of RE1xRE21−xCOB mixed crystals. Under focusing light beam conditions, high efficient A-NCPM SHG for both OPO and Ti:sapphire lasers were realized experimentally by using long Y- and Z-cut RE1xRE21−xCOB crystal samples. Full article
(This article belongs to the Special Issue Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications)
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8 pages, 2941 KiB  
Communication
Towards a Large-Area Freestanding Single-Crystal Ferroelectric BaTiO3 Membrane
by Qixiang Wang, Hong Fang, Di Wang, Jie Wang, Nana Zhang, Bin He and Weiming Lü
Crystals 2020, 10(9), 733; https://doi.org/10.3390/cryst10090733 - 21 Aug 2020
Cited by 18 | Viewed by 4184
Abstract
The fabrication and transfer of freestanding single-crystal ferroelectric membranes deserve intensive investigations as to their potential applications in flexible wearable devices, such as flexible data storage devices and varied sensors in E-skin configurations. In this report, we have shown a comprehensive study approach [...] Read more.
The fabrication and transfer of freestanding single-crystal ferroelectric membranes deserve intensive investigations as to their potential applications in flexible wearable devices, such as flexible data storage devices and varied sensors in E-skin configurations. In this report, we have shown a comprehensive study approach to the acquisition of a large-area freestanding single-crystal ferroelectric BaTiO3 by the Sr3Al2O6 scarification layer method. By controlling the thickness of the BaTiO3 and Sr3Al2O6, the exposed area of the Sr3Al2O6 interlayer, and the utilization of an additional electrode La2/3Sr1/3MnO3 layer, the crack density on the freestanding BaTiO3 can be dramatically decreased from 24.53% to almost none; then, a more than 700 × 530 μm2 area high-quality freestanding BaTiO3 membrane can be achieved. Our results offer a clear and repeatable technology routine for the acquisition of a flexible large-area ferroelectric membrane, which should be instructive to other transition metal oxides as well. Our study can confidently boost flexible device fabrication based on single-crystal transition metal oxides. Full article
(This article belongs to the Special Issue Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications)
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8 pages, 2071 KiB  
Article
Structural and Electric Properties of MnO2-Doped KNN-LT Lead-Free Piezoelectric Ceramics
by Yunfeng Deng, Junjun Wang, Chunxiao Zhang, Hui Ma, Chungeng Bai, Danqing Liu, Fengmin Wu and Bin Yang
Crystals 2020, 10(8), 705; https://doi.org/10.3390/cryst10080705 - 15 Aug 2020
Cited by 9 | Viewed by 2742
Abstract
Structural, ferroelectric, dielectric, and piezoelectric properties of K0.5Na0.5NbO3-LiTaO3-xmol%MnO2 lead-free piezoelectric ceramics with 0.0 ≤ x ≤ 0.3 were studied. The ceramic samples were synthesized through the conventional solid-state reaction method. The MnO [...] Read more.
Structural, ferroelectric, dielectric, and piezoelectric properties of K0.5Na0.5NbO3-LiTaO3-xmol%MnO2 lead-free piezoelectric ceramics with 0.0 ≤ x ≤ 0.3 were studied. The ceramic samples were synthesized through the conventional solid-state reaction method. The MnO2 addition can reduce the sintering temperature of KNLNT ceramics. Compared with undoped KNLNT ceramic, the piezoelectric measurements showed that piezoelectric properties of K0.5Na0.5NbO3-LiTaO3-xMnO2 were improved (d33 = 251 pC/N) when x = 0.1. In addition, KNLNT-xMnO2 ceramics have larger Pr(20.59~21.97 μC/cm2) and smaller Ec(10.77~6.95 kV/cm), which indicates MnO2 has excellent softening property, which improves the ferroelectric properties of KNLNT ceramics This work adds relevant information regarding of potassium sodium niobate K0.5Na0.5NbO3 (KNN) when doped Li, Ta, Mn at the B-site. Full article
(This article belongs to the Special Issue Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications)
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10 pages, 3399 KiB  
Article
Spontaneous Growth of CaBi4Ti4O15 Piezoelectric Crystal Using Mixed Flux Agents
by Mengdi Fan, Guangda Wu, Fapeng Yu, Lili Li, Yanlu Li, Xiufeng Cheng and Xian Zhao
Crystals 2020, 10(8), 698; https://doi.org/10.3390/cryst10080698 - 12 Aug 2020
Cited by 3 | Viewed by 2468
Abstract
The bismuth layer-structured ferroelectrics (BLSFs) materials have potential for high-temperature piezoelectric applications. Among these piezoelectric materials, the CaBi4Ti4O15 (CBT) piezoelectric ceramic with a high decomposition temperature of about 1250 °C attracts a lot of attention. Achieving a CBT [...] Read more.
The bismuth layer-structured ferroelectrics (BLSFs) materials have potential for high-temperature piezoelectric applications. Among these piezoelectric materials, the CaBi4Ti4O15 (CBT) piezoelectric ceramic with a high decomposition temperature of about 1250 °C attracts a lot of attention. Achieving a CBT single crystal is a significant way to improve its piezoelectric properties. For this purpose, the flux system for growing CBT crystal was explored in this study. The optimum flux composition ratio was found to be PbO:B2O3:CBT = 3:3:1 in mol%, where the PbO–B2O3 mixtures were used as a flux system. Millimeter size flake-shaped CBT crystals were obtained using the spontaneous growth process for the first time. The relationship between the crystal structure and flake growth habit was analyzed. In addition, the bandgap was evaluated by the combination of transmittance spectrum and first-principle calculations. Besides, the piezoelectric property was predicted from the perspective of polyhedral distortion, which indicated the potential of CBT crystal for piezoelectric applications. Full article
(This article belongs to the Special Issue Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications)
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13 pages, 5614 KiB  
Article
Piezoelectric Resonators Excited by Lateral Electric Fields Based on a LiTaO3 Single Crystal
by Hao Shi, Liang Yan, Yuanzhen Zheng, Tingfeng Ma, Mingfei Wang, Bin Huang, Lili Yuan, Ji Wang, Jianke Du and Han Zhang
Crystals 2020, 10(6), 525; https://doi.org/10.3390/cryst10060525 - 18 Jun 2020
Cited by 1 | Viewed by 2442
Abstract
In the present study, piezoelectric resonators under lateral field excitation (LFE) based on a LiTaO3 single crystal are modeled and analyzed. An electrically forced vibration study is employed to acquire the motional capacitance curve and vibration mode shapes. A finite element approach [...] Read more.
In the present study, piezoelectric resonators under lateral field excitation (LFE) based on a LiTaO3 single crystal are modeled and analyzed. An electrically forced vibration study is employed to acquire the motional capacitance curve and vibration mode shapes. A finite element approach is utilized to investigate the influences of some basic parameters, such as the electrode/plate mass ratio, electrode gap, and electrode width on resonance characteristics. In addition, the design criteria for the gap and width of the electrode of the LiTaO3 LFE resonators are obtained by analyzing the effects of those parameters on vibration strain distributions. The obtained results are essential for designing LFE piezoelectric resonators by using a LiTaO3 single crystal. Full article
(This article belongs to the Special Issue Multifunctional Crystal Materials with Non-centrosymmetry: Piezoelectric and Nonlinear Optical Properties and Their Applications)
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