Nonlinear Optical Borate Crystals: Principals and Applications


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Nonlinear optical NLO materials are the vital components of future photoelectric technologies as they can broaden the tunable wavelength range supplied by common laser sources.

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However, the necessary prerequisites for a practical NLO material are rather strict. Accordingly, considerable efforts have been focused on finding potential NLO materials. The reversible phase transition among two polymorphs was demonstrated by multiple experimental tests. Remarkably, Pna 2 1 -Ba 3 Mg 3 BO 3 3 F 3 has a large laser damage threshold, a deep-ultraviolet cutoff edge, a favorable anisotropic thermal expansion as well as the capacity of insolubility in water.

Nonlinear optical NLO materials applied from ultraviolet UV to infrared spectral ranges are the vital components of future photoelectric technologies 1 — 4. Accordingly, considerable and sustained efforts have been focused on designing and synthesizing new potential NLO materials 5 — 9. Targeting above conditions, until now, the borate system plays a dominant role in UV NLO materials because borates possess wide optical transparency windows, varied acentric structure types, high LDTs, and large polarizabilities 11 — Therefore, a variety of commercial borate-based UV NLO materials have been widely investigated and developed.

Third, the introduction of fluoride-containing flux can effectively decrease the viscosity of the borate systems during the growth of single crystals, which is a desirable choose for growing the large single crystals 20 , 24 , 25 , For us, besides selecting the appropriate system borate and introducing anion fluorine , how to effectively design UV NLO materials with presupposed structures and properties is also critically important.

Second, we use the strategy of chemical cosubstitution to make structural modifications based on the classic NLO materials with the goal of obtaining new molecular structures contain NLO-favorable layered structures 32 , Motivated by these, considering that s -block elements Be and Mg, Sr and Ba appear tightly clustered in the periodic table with the similar electronic configurations, sharing many common physicochemical properties.

Based on the top designing molecule structures, large-size single crystals of Pna 2 1 -BMBF were also grown through finding the suitable flux system. Single crystal X-ray diffraction reveals that two new borates crystallize into the asymmetric space group of Pna 2 1 No. And the relatively low temperature factors and residual factors verify the correctness of those two crystal models, which also indicates the existence of two polymorphs.

Furthermore, the BMBF polymorphs and phase transitions are further confirmed by high-temperature in situ powder X-ray diffraction and thermal expansion coefficients experiment: based on the results of thermal gravimetric and differential scanning calorimetry analysis Fig. Endo means the endothermic direction. There are two remarkable endothermic peaks As shown in Fig.

Nonlinear optics

The Mg atoms in both polymorphs are six-coordinated into the MgO 4 F 2 octahedra with four O and two F atoms locating in the equatorial and axial positions, respectively. Pna 2 1 -BMBF crystal has never cracked during cutting and polishing into , , and wafers Fig. The crystallization quality of the as-grown crystal was checked by the X-ray rocking curve.

The conoscopic interference pattern Fig. When taken together, Pna 2 1 -BMBF crystal shows high optical quality, and the optical measurements based on this crystal are reliable. All the images and elements of them were created by ourselves. Pna 2 1 -BMBF was subjected to physicochemical property characterizations based on the single-crystal level. Thermal expansion coefficients are vital parameters for crystal growth and application in devices.

As can be seen in Fig. Therefore, Pna 2 1 -BMBF crystal exhibits a more favorable anisotropic thermal expansion, which will effectively protect the crystals from cracking caused by thermal expansion during crystal growth and optical devices fabrication.

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As plotted in Fig. According to the results, the SHG efficiency increases with the raising particle sizes, indicating that both BMBF polymorphs exhibit type I phase-matching behavior in nm incident lasers. In order to verify the results, large sizes of single crystals should be grown and cut to evaluate the SHG coefficients based on the crystal level, which is discussed in detail in the following parts. The as-grown crystals were cut and optically polished to 1 mm thickness for the spectrum measurement.

As presented in Fig. The short cutoff edge is beneficial to obtain high LDT, therefore, LDT measurements were carried out using a pulsed nanosecond laser nm, 10 ns, and 10 Hz. The curves are drawn to guide the eyes, and are not fit to the data. Transmittance curve black line between and nm was collected by a Shimadzu IRAffinity-1 spectrometer. A least-square method was used to fit the dispersion parameters of the refractive indices, n i , using the Sellmeier Eq.

The Sellmeier Eq. The calculated values are consistent with experimental ones to the fourth decimal place, which indicates that the fitted Sellmeier equations based on the current data are reliable Fig. Therefore, the Pna 2 1 -BMBF crystal can generate and nm light by direct second and third harmonic generation from a nm laser. The schematic of the Maker fringe measurement system is shown in Fig.

However, the Maker fringe for d 31 is too weak to be observed. As d 36 coefficient of KDP is 0. A Q-switched Nd:YVO 4 laser system was adopted as fundamental light source with the following experimental conditions: fundamental wavelength: nm; repetition frequency: 10 kHz; and pulse width: 10 ns. The second-harmonic signal, which changed with rotation angle of Pna 2 1 -Ba 3 Mg 3 BO 3 3 F 3 crystal, was detected by a photomultiplier tube, averaged by a fast-gated integrator and boxcar integrator, and then recorded by computer system.

The data were fitted according to the Maker fringe theory and the detailed fitting procedure is available in the Methods section. In order to achieve a deep investigation about the structure-property relationship, theoretical calculations based on density functional theory methods were performed 42 — The total and partial density of states projected on the constitutional atoms of Pna 2 1 -BMBF crystal are given in Fig.

The Design of Organic Molecules and Materials for Nonlinear Optical Applications

Clearly, the energy bands can be divided into several regions. While the bottom of the conduction band is essentially composed of Ba 5 d , Ba 5 s , B 2 p , and O 2 p orbitals. In principle, the optical properties are mainly determined by the electronic transitions among the states near Fermi level, which are mainly occupied by the O 2 p nonbonding orbitals, B—O hybridization states and Ba 5 d states in Pna 2 1 -BMBF.

Besides, the interatomic interactions within the BO 3 units and MgO 4 F 2 octahedra can be clearly visualized by the electron localization function diagrams. Through the Mulliken population analysis, the same conclusions can also be substantiated by the calculated overlap populations for Mg—F, Mg—O and B—O, which are 0. Isovalue increases from blue to red, and the maximum electron localization function value is scaled to 4. And the SHG process is denoted by two virtual transition processes, namely virtual electron VE and virtual hole processes. Both occupied and unoccupied states of the Ba cations, in analogy to alkali metal and alkali earth metal ions in other NLO crystals, have very little contribution on the SHG effect, which agrees well with the anionic group theory Isovalue increases from blue to red, and the maximum electron localization function values are scaled to 5.

In summary, by starting from the SBBO structure, we designed and synthesized two beryllium-free SBBO-like borates through chemical cosubstitution strategy. All the reagents were mixed homogeneously and transferred to a platinum crucible. The selected single crystals with dimensions up to 0. The Bruker Suite software package was used to reduce the collected data. The original structures were established by the direct method and refined by the full-matrix least-squares program on SHELXL The PLATON program was used for checking the possible missing symmetry elements, but no higher symmetries were found The sample of 6.

The measurements were carried out in an atmosphere of flowing N 2. The microcrystalline KDP samples with the same particle sizes were used as references. A Q-switched Nd:YAG laser with a pulse width of 10 ns and repetition frequency of 10 kHz was employed as the fundamental light source nm.

The second-harmonic signal generated from the sample wafer was detected by a side window photomultiplier tube, averaged by a fast-gated integrator and boxcar average, and then automatically recorded by a computer. A cut-KDP wafer was used as a reference. Maker fringe measurements of Pna 2 1 -BMBF were performed on two crystal wafers cut perpendicular to the a - and b -crystallographic axes in order to measure d 31 , d 32 , and d 33 NLO coefficients. Then, the data were fitted according to the Maker fringe theory.

The exchange and correlation effects were treated by Perdew—Burke—Ernzerhof in the generalized gradient approximation The interactions between the ionic cores and electrons were described by norm-conserving pseudopotentials The authors declare that the data supporting the findings of this study are available within the article and Supplementary Information files, or from the corresponding authors upon reasonable request. All the authors discussed the results and commented on the manuscript. Publisher's note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Junliang Sun, Email: nc. Shilie Pan, Email: nc. Supplementary Information accompanies this paper at Europe PMC requires Javascript to function effectively. Recent Activity. Remarkably, PnaBa3Mg3 BO3 3F3 has a large laser damage threshold, a deep-ultraviolet cutoff edge, a favorable anisotropic thermal expansion as well as the capacity of insolubility in water.

The snippet could not be located in the article text. This may be because the snippet appears in a figure legend, contains special characters or spans different sections of the article. Nat Commun. These crystals are grown by flux techniques and are mainly employed in SFD purposes. Later intense work on the growth and characterization of this family of crystals with various rare-earth elements such as La, Nd, Gd, Er, and Y were carried out and reported. The RECOB crystals with the rare-earth ions with electronic configurations 4 , give rise to electronic transitions in the visible region that would interfere with the expected NLO properties.

The melting temperatures of the RECOB crystals increase with a decrease in the ionic radii of the rare-earth ion present in it [ 26 ]. They are biaxial crystals. The flux growth of yttrium calcium oxy borate YCOB single crystals by flux technique was also carried out by our group earlier and reported [ 30 ]. Another emerging borate-based crystal family is rare-earth calcium borate RCB crystals, with the general chemical formula R 2 CaB 10 O 19 R represents rare-earth element.

In this series of crystals, only crystal growth of pure and doped lanthanum calcium borate LCB are performed and reported in literature.

Nonlinear optical borate crystals : principles and applications

There are no reports available on any other materials in the RCB family of crystals. The LCB crystal is reported to be insensitive to moisture, has high hardness 6. Growth and material characteristics of several borate-based single crystals were discussed. Borate crystals are grown from melt and flux techniques. Anionic group theory plays an essential theory for selecting borate materials for nonlinear optical applications. Several borate-based crystals act as desirable host materials for fabricating lasers. Borate crystals offer themselves as suitable candidates for both nonlinear optical and laser applications.


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Journal of Chemistry. Indexed in Science Citation Index Expanded. Journal Menu. Special Issues Menu. Subscribe to Table of Contents Alerts. Table of Contents Alerts. Abstract The development of borate-based single crystals for laser and frequency conversion applications is reviewed. Introduction 1. Demand for UV and Visible Radiations The development of lasers has played a key role in the past five decades for the development of mankind in various fields and to reach several technological advancements.

Emphasis of the Present Review The recent developments in NLO borate crystals for the generation of high power visible and ultraviolet laser radiations are reviewed. Nonlinear Optics and Borate Crystals 2. Basic Principles of Nonlinear Optics The successful demonstration of lasers by Maiman and his coworkers in the year paved way for various scientific and technological advancements in the twentieth century [ 1 ]. Nonlinear Optical Borate Crystals The large family of borate compounds is a suitable chemical playground now adopted by many materials scientists, because the extremely wide variability of borate crystal chemistry allows the creation of various different structure types [ 2 ].

Figure 1: Basic structure units of a BO 3 b B 3 O 6 c B 3 O 7 borates dark circles represent boron and bright circles represent oxygen atoms. References T. Xue, K. Betzler, H. Hesse, and D. Aka and A. Dewey, W. Cook, R. Hodgson, and J. Adamiv, Y. Burak, I. Kityk, J. Kasperczyk, R. Smok, and M. Majchrowski, I.

Nonlinear Optical Borate Crystals | Wiley Online Books

Kityk, and J. Ghotbi, M. Ebrahim-Zadeh, A. Majchrowski, E. Michalski, and I. Ghotbi, Z. Sun, A. Petrov, M. Ghotbi, O. Kokabee et al. Kityk and A. Sasaki, Y. Mori, M. Yoshimura, Y. Yap, and T. Chen, Y. Wang, B. Wu, K. Wu, W. Zeng, and L. Hu, T. Higashiyama, M. Yap, Y. Mori, and T.

Zhang, J. Wang, X. Cheng et al. Reshak, S. Auluck, A. Majchrowski, and I. Jaque, J. Capmany, and S. Majchrowski, J. Fuks-Janczarek, M. Makowska-Janusik, B. Sahraoui, and I. Dominiak-Dzik, W. Ryba-Romanowski, L. You, Y. Lin, Y. Chen, Z. Luo, and Y. Capmany, F. Molero, Z. Luo, and J. Li, J. Cheng, X. Hu, X. Wang, and S.


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