CN112442738A - Nonlinear optical application of two alkaline earth metal hydroxy borate crystals - Google Patents

Nonlinear optical application of two alkaline earth metal hydroxy borate crystals Download PDF

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CN112442738A
CN112442738A CN201910812661.7A CN201910812661A CN112442738A CN 112442738 A CN112442738 A CN 112442738A CN 201910812661 A CN201910812661 A CN 201910812661A CN 112442738 A CN112442738 A CN 112442738A
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康雷
林哲帅
黄兵
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Abstract

The invention provides application of two alkaline earth metal hydroxyl borate crystals as nonlinear optical materials in preparation of nonlinear optical devices, and results show that the two alkaline earth metal hydroxyl borate crystals provided by the invention are used as nonlinear optical materials, and the frequency multiplication coefficients of the two alkaline earth metal hydroxyl borate crystals are matched with that of KBe2BO3F2The crystals are equivalent. Their ultraviolet absorption edges are less than 170 nm and 180 nm, respectively. Their optical birefringence is about 0.08 to 0.10. The shortest phase matching frequency multiplication output wavelengths of the two are respectively less than 175 nanometers and 190 nanometers, and 177.3 nanometers and 193.7 nanometers of deep ultraviolet coherent light frequency multiplication output and 266 nanometers of ultraviolet coherent light frequency multiplication output can be respectively realized. Therefore, the two alkaline earth metal hydroxy borate crystals CaB provided by the invention8O11(OH)4And SrB8O11(OH)4The optical material has good second-order nonlinear optical effect, can be used as a good deep ultraviolet nonlinear optical material and a deep ultraviolet birefringent material, and can be widely applied to various nonlinear optical fields, especially to the nonlinear optical application in ultraviolet and deep ultraviolet wave bands.

Description

Nonlinear optical application of two alkaline earth metal hydroxy borate crystals
Technical Field
The invention relates to the field of optical materials, in particular to two alkaline earth metal hydroxy borate nonlinear optical crystals and a preparation method and application thereof.
Background
The nonlinear optical material is an important element of the all-solid-state laser technology, can expand the spectral range of laser output in a frequency conversion mode, can span a wide range from deep ultraviolet to mid-infrared, and has great application potential in various aspects such as national defense, military and industrial production. To date, commercially practical nonlinear optical materials have covered the spectral region from ultraviolet to near infrared (0.2-2 microns). However, in the deep ultraviolet region, there is no commercially available crystalline material so far, although it is important in practical application of deep ultraviolet all-solid-state laser technology. Deep ultraviolet nonlinear optical materials can convert laser light with specific wavelength of practical lasers (such as Nd: YAG 1064 nm lasers) into harmonic light in the deep ultraviolet spectral region (less than 200 nm) by means of multiple frequency multiplication.
In the deep ultraviolet band, potassium fluoroberyllinate (KBe)2BO3F2KBBF), which successfully converts practical Nd: the conversion of 1064 nm near-infrared laser of YAG laser into 177.3 nm deep-ultraviolet laser has greatly promoted the development of deep-ultraviolet all-solid-state laser technology and the research of basic science. Although many nonlinear optical materials are synthesized and discovered at present, most of them cannot realize phase matching in the deep ultraviolet region, and therefore cannot replace KBBF crystals to realize effective deep ultraviolet frequency doubling output.
However, the structure of KBBF crystal is stacked layer by layer, and isolated cation K is embedded between layers+The interaction between layers belongs to ion interaction and has no directionality, so that slippage is easy to occur between the layers; meanwhile, the distance between layers is large, and the interaction between layers along the direction vertical to the layers is weak, so that the interlayer combination is not firm, the layer habit is serious, a block material with large thickness is difficult to grow, and a crystal material with the thickness of more than 4 mm and high optical quality is not reported so far.
Disclosure of Invention
In view of the above, the technical problem to be solved by the present invention is to provide a nonlinear optical application of two alkaline earth metal hydroxy borate crystals in a deep ultraviolet region, the two alkaline earth metal hydroxy borate crystals provided by the present invention are used as a nonlinear optical material, the shortest phase matching frequency doubling output wavelength of the two alkaline earth metal hydroxy borate crystals is respectively less than 175 nm and 190 nm, the frequency doubling output of 177.3 nm and 193.7 nm deep ultraviolet coherent light and the frequency doubling output of 266 nm ultraviolet coherent light can be realized, the frequency doubling effect is large, and the deep ultraviolet phase matching output performance is equivalent to that of a KBBF crystal. And the material is a framework structure, has stronger covalent linkage than a KBBF (KbF) laminated structure, and can show better crystal growth performance, mechanical property and machining performance.
The invention provides application of two alkaline earth metal hydroxyl borate crystals as nonlinear optical materials in preparation of nonlinear optical devices.
Preferably, the chemical compositions of the alkaline earth metal hydroxy borate crystals are CaB8O11(OH)4And SrB8O11(OH)4。
Preferably, the alkaline earth metal hydroxyborate crystal is monoclinic.
Preferably, the space group of the alkaline earth metal hydroxy borate crystal is P21The cell parameters are respectively: for CaB8O11(OH)4，
Figure BSA0000189160730000021
α ═ γ ═ 90 °, β ═ 108.8 °, z ═ 2, and the unit cell volume is
Figure BSA0000189160730000022
For SrB8O11(OH)4，
Figure BSA0000189160730000023
Figure BSA0000189160730000024
α ═ γ ═ 90 °, β ═ 108.4 °, z ═ 2, and the unit cell volume is
Figure BSA0000189160730000025
Preferably, the laser frequency conversion device is a frequency doubling device, a frequency tripling device, a frequency quadrupling device, a frequency quintuplet device or a frequency sextuple device.
Preferably, the laser frequency conversion device is a harmonic generator of ultraviolet and deep ultraviolet regions or an optical parametric device of ultraviolet and deep ultraviolet regions.
Compared with the prior art, the invention provides the application of two alkaline earth metal hydroxyl borate crystals as nonlinear optical materials in the preparation of nonlinear optical devices, and available experimental data and systematic theoretical calculation show that the frequency multiplication coefficients of the alkaline earth metal hydroxyl borate crystals provided by the invention are equivalent to KBBF crystals in the application of the alkaline earth metal hydroxyl borate crystals as the nonlinear optical materials in the preparation of the nonlinear optical devices. Their ultraviolet absorption edges are less than 170 nanometers and 180 nanometers, respectively. Their optical birefringence is about 0.08 to 0.10. The shortest phase matching frequency multiplication output wavelengths of the two are respectively less than 175 nanometers and 190 nanometers, and 177.3 nanometers and 193.7 nanometers of deep ultraviolet coherent light frequency multiplication output and 266 nanometers of ultraviolet coherent light frequency multiplication output can be respectively realized. Therefore, the two alkaline earth metal hydroxy borate crystals provided by the invention have good second-order nonlinear optical effects, can be used as good deep ultraviolet nonlinear optical materials and deep ultraviolet birefringent materials, and can be widely applied to various nonlinear optical fields, especially to nonlinear optical applications in ultraviolet and deep ultraviolet bands. Meanwhile, the alkaline earth metal hydroxy borate crystal has better crystal growth and mechanical and thermal processing performance, and has better application value in practical use.
Drawings
FIG. 1 shows two alkaline earth metal hydroxy borate crystals CaB according to the invention8O11(OH)4And SrB8O11(OH)4The crystal structure of (1).
Detailed Description
The invention provides application of two alkaline earth metal hydroxyl borate crystals as nonlinear optical materials in preparation of nonlinear optical devices, wherein the alkaline earth metal hydroxyl borate crystals are goldThe chemical composition of the crystal belongs to hydroxy borate, and is CaB8O11(OH)4And SrB8O11(OH)4The alkaline earth metal hydroxy borate crystal is monoclinic system, and the space group is P21Cell parameters for CaB8O11(OH)4And SrB8O11(OH)4Are respectively as
Figure BSA0000189160730000031
α＝γ＝90°，β＝108.8°，z＝2，
Figure BSA0000189160730000032
And
Figure BSA0000189160730000033
α＝γ＝90°，β＝108.4°，z＝2，
Figure BSA0000189160730000034
specifically, the alkaline earth metal hydroxyborate crystal CaB8O11(OH)4And SrB8O11(OH)4The crystal structure of (a) is shown in FIG. 1; the invention relates to alkaline earth metal hydroxy borate crystal CaB8O11(OH)4And SrB8O11(OH)4The source of the compound has no special requirements, and the compound can be mined, purchased or self-made according to the existing preparation method; the nonlinear optical device is preferably a laser frequency conversion device, and the laser frequency conversion device is preferably a frequency doubling device, a frequency tripling device, a frequency quadrupling device, a frequency quintupler device or a frequency sextupler device; the laser frequency conversion device is preferably a harmonic generator in the deep ultraviolet region or an optical parametric device in the deep ultraviolet region.
The invention provides application of two alkaline earth metal hydroxyl borate crystals as nonlinear optical materials in preparation of nonlinear optical devices, and available experimental data and theoretical calculation results of a system show that the alkaline earth metal hydroxyl borate crystal CaB provided by the invention8O11(OH)4And SrB8O11(OH)4As non-linear opticsIn the application of the material in preparing nonlinear optical devices, the frequency multiplication coefficient of the material is equivalent to that of KBBF crystals. Their ultraviolet absorption edges are less than 170 nm and 180 nm, respectively. Their optical birefringence is about 0.08 to 0.10, comparable to that of KBBF crystals. The shortest phase matching frequency multiplication output wavelengths of the two are respectively less than 175 nanometers and 190 nanometers, and 177.3 nanometers and 193.7 nanometers of deep ultraviolet coherent light frequency multiplication output and 266 nanometers of ultraviolet coherent light frequency multiplication output can be respectively realized. It can be seen that the alkaline earth metal hydroxyborate crystal CaB8O11(OH)4And SrB8O11(OH)4Has good nonlinear optical effect, can be used as good deep ultraviolet nonlinear optical material and deep ultraviolet birefringent material, and can be widely applied in various nonlinear optical fields, in particular to nonlinear optical application in ultraviolet and deep ultraviolet wave bands.
Interpretation of related terms
Nonlinear optical effects: the optical effect related to the higher order term of the optical electric field by the laser light generally refers to an effect in which the optical frequency changes.
Nonlinear optical material: crystalline material having a nonlinear optical effect.
Frequency doubling effect: the second-order nonlinear optical effect refers to the phenomenon that the frequency of laser with a certain frequency is doubled or the wavelength is halved under the action of a second-order nonlinear optical material. Such as Nd: the 1064 nm laser of the YAG laser is changed into 532 nm laser through the LBO crystal. In addition, frequency tripled, quadrupled, quintuple, sextuple, etc. are available. For example, the frequency tripling of the 1064 nm laser can be realized by summing (i.e., adding) 532 nm frequency doubled light and 1064 nm fundamental light to 354.7 nm. The six-frequency doubling can re-frequency the 357.4 nm laser to generate 177.3 nm laser, which is the most practical way to generate deep ultraviolet light nowadays.
Birefringence: the phenomenon that one incident ray is emitted into an anisotropic crystal and is decomposed into two refracted rays along different directions is very important for realizing angle phase matching of a deep ultraviolet region.
Deep ultraviolet laser: refers to coherent light having a wavelength of less than 200 nanometers.
Experimental testing and characterization: the test and characterization of the current nonlinear optical material mainly comprise a transmission or absorption spectrum test, a refractive index measurement, a powder frequency doubling effect test, a frequency doubling coefficient Mike stripe test method, a phase matching test and the like.
The following will clearly and completely describe the technical solutions of the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Example 1
Alkaline earth metal hydroxyborate crystal SrB8O11(OH)4It is a mineral known as borostrontianite, produced in carbonate rock and often coexists with borocalcite, boracite, and rhombohedral boromagnesite. The crystal is colorless and transparent, biaxial crystal and has birefringence of about 0.11. The crystal can be obtained by mining or direct purchase, and can also be synthesized and subjected to single crystal growth in a laboratory. CaB8O11(OH)4It is a calcium compound with a structure similar to that of boron strontium stone, and has been synthesized experimentally in 2005 (refer to Crystallography Report, 2005, 50, 766-.
The synthesis method can adopt a hydrothermal method to prepare the alkaline earth metal hydroxy borate CaB according to the following chemical reaction formula8O11(OH)4And SrB8O11(OH)4A compound:
(1)2CaCl2+2Rb2CO3+4B2O3+3H2O＝CaB8O11(OH)4+Ca(OH)2+4RbCl+2CO2
(2)2SrCl2+2Rb2CO3+4B2O3+3H2O＝SrB8O11(OH)4+Sr(OH)2+4RbCl+2CO2
the structures of the two obtained alkaline earth metal hydroxy borate are detected, the crystal structures belong to a monoclinic system, and the space group is P21The cell parameters are respectively: for CaB8O11(OH)4，
Figure BSA0000189160730000051
Figure BSA0000189160730000052
α ═ γ ═ 90 °, β ═ 108.8 °, z ═ 2, and the unit cell volume is
Figure BSA0000189160730000053
For SrB8O11(OH)4，
Figure BSA0000189160730000054
α ═ γ ═ 90 °, β ═ 108.4 °, z ═ 2, and the unit cell volume is
Figure BSA0000189160730000055
The optical properties of the obtained two alkaline earth metal hydroxy borate are tested and accurately calculated theoretically, and the frequency multiplication coefficients of the two alkaline earth metal hydroxy borate and the KBe are obtained2BO3F2The crystals are equivalent. Their ultraviolet absorption edges are less than 170 nm and 180 nm, respectively. They have optical birefringence of about 0.08 to 0.10, comparable to KBBF. The shortest phase matching frequency multiplication output wavelengths of the two are respectively less than 175 nanometers and 190 nanometers, and 177.3 nanometers and 193.7 nanometers of deep ultraviolet coherent light frequency multiplication output and 266 nanometers of ultraviolet coherent light frequency multiplication output can be respectively realized.
The theoretical calculation method adopted by the invention is a first principle density functional theoretical method based on high-performance calculation, and has reliable theoretical basis and wide accuracy in the research of numerous properties of physics, chemistry and materials, including optical properties. In order to prove the referability of the theoretical calculation result, the invention adopts the calculation method for obtaining the crystal data to carry out calculation on the existing known deep ultraviolet nonlinear optical crystal compoundLine calculation; the results are shown in Table 1, where KBe is shown in Table 12BO3F2And KB5O8·4H2The nonlinear optical properties of O and the optical performance results of the two alkaline earth metal hydroxyborate crystals of the present invention. Wherein the experimental data of the strontianite is derived from relevant mineralogy information of a national rock and ore fossil sample resource sharing platform system.
TABLE 1
Figure BSA0000189160730000056
As can be seen from Table 1, the optical properties of the crystal obtained by the theoretical calculation method provided by the invention are almost consistent with the experimental values, so that the data results of the optical properties obtained by the theoretical calculation method provided by the invention are real and effective and have referential property. Meanwhile, as shown in the table, the alkaline earth metal hydroxy borate crystal CaB8O11(OH)4And SrB8O11(OH)4Compared with KBBF crystal, the crystal has similar frequency doubling effect, birefringence and shortest frequency doubling output wavelength, and the crystal growth performance of the framework structure is superior to that of the KBBF crystal with a laminated structure. Therefore, the alkaline earth metal hydroxyborate crystal CaB of the present invention8O11(OH)4And SrB8O11(OH)4The optical material is two deep ultraviolet nonlinear optical materials which can be compared with KBBF crystal, and has better practicability, and the nonlinear optical device prepared by the optical material has good performance.
The above description of the embodiments is only intended to facilitate the understanding of the method of the invention and its core idea. It should be noted that, for those skilled in the art, it is possible to make various improvements and modifications to the present invention without departing from the principle of the present invention, and those improvements and modifications also fall within the scope of the claims of the present invention. For example, strontium or calcium may be substituted with other alkaline earth metals (magnesium or barium) to form alkaline earth metal hydroxy borate crystals of similar structure.

Claims (7)

1. The two alkaline earth metal hydroxyl borate crystals are used as nonlinear optical materials in the preparation of nonlinear optical devices.
2. Use according to claim 1, wherein the chemical composition of the alkaline earth metal hydroxyborate crystals is CaB8O11(OH)4And SrB8O11(OH)4。
3. Use according to claim 1, characterized in that the alkaline earth metal hydroxyborate crystals are monoclinic.
4. Use according to claim 1, wherein the alkaline earth metal hydroxyborate crystal has a space group of P21，CaB8O11(OH)4And SrB8O11(OH)4Respectively has unit cell parameters of
Figure FSA0000189160720000011
α ═ γ ═ 90 °, β ═ 108.8 °, z ═ 2, unit cell volume
Figure FSA0000189160720000012
Figure FSA0000189160720000013
And
Figure FSA0000189160720000014
α ═ γ ═ 90 °, β ═ 108.4 °, z ═ 2, unit cell volume
Figure FSA0000189160720000015
5. Use according to claim 1, wherein the non-linear optical device is a laser frequency conversion device.
6. Use according to claim 5, wherein the laser frequency conversion device is a frequency doubling device, a frequency tripling device, a frequency quadrupling device, a frequency quintuplet device or a frequency sextuplet device.
7. Use according to claim 5, wherein the laser frequency conversion device is a harmonic generator in the ultraviolet and deep ultraviolet region or an optical parametric device in the ultraviolet and deep ultraviolet region.
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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115044976A (en) * 2021-03-09 2022-09-13 中国科学院理化技术研究所 Second-order nonlinear optical crystal and preparation method and application thereof

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115044976A (en) * 2021-03-09 2022-09-13 中国科学院理化技术研究所 Second-order nonlinear optical crystal and preparation method and application thereof
CN115044976B (en) * 2021-03-09 2024-04-12 中国科学院理化技术研究所 Second-order nonlinear optical crystal and preparation method and application thereof

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