CN112670402B - Three-dimensional polarization method and device for single-domain tetragonal phase relaxor ferroelectric single crystal - Google Patents

Three-dimensional polarization method and device for single-domain tetragonal phase relaxor ferroelectric single crystal Download PDF

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CN112670402B
CN112670402B CN202011419028.0A CN202011419028A CN112670402B CN 112670402 B CN112670402 B CN 112670402B CN 202011419028 A CN202011419028 A CN 202011419028A CN 112670402 B CN112670402 B CN 112670402B
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relaxor ferroelectric
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陈鑫
王军利
魏志义
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Xidian University
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Xidian University
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Abstract

The invention discloses a three-dimensional polarization method and a device of a single-domain tetragonal phase relaxor ferroelectric single crystal, which comprise the following steps: a first laser beam emitted by a laser device is irradiated to a beam energy attenuator through a shutter to obtain a second laser beam; irradiating the second laser beam to the beam splitter for splitting to obtain a third laser beam and a fourth laser beam; the third laser beam irradiates the imaging system to be filtered; irradiating the fourth laser beam to the direct-writing objective lens to obtain a focused beam; adjusting a shutter and a three-dimensional platform and simultaneously obtaining a target three-dimensional reverse domain structure by using a focused light beam; and monitoring the image of the crystal focusing area in real time by using an imaging system. The polarization period and the period number can be flexibly controlled by adjusting the shutter and the three-dimensional platform, and meanwhile, the single-domain relaxor ferroelectric crystal has high transmittance in the wave band of a laser beam and can be focused to different depths and positions, so that the three-dimensional polarization of the single-domain relaxor ferroelectric crystal is realized.

Description

Three-dimensional polarization method and device for single-domain tetragonal phase relaxor ferroelectric single crystal
Technical Field
The invention belongs to the technical field of ferroelectric material processing, and particularly relates to a three-dimensional polarization method and a three-dimensional polarization device for a single-domain tetragonal phase relaxor ferroelectric single crystal.
Background
Since the last 90 s, relaxor ferroelectric single crystals (PMN-PT) have been extensively studied and applied with their ultra-high piezoelectric constant and electromechanical coupling coefficientRepresentative examples thereof include lead magnesium niobate-lead titanate (PMN-PT), lead zinc niobate-lead titanate (PZN-PT), lead indium niobate-lead titanate (PIN-PT), lead indium niobate-lead magnesium niobate-lead titanate (PIN-PMN-PT), and doped modified materials thereof. In recent years, thanks to the progress of crystal growth and processing technology, the excellent optical properties of the relaxor ferroelectric single crystal are increasingly emphasized, and particularly, the maturation of the single domain technology is combined with the high second-order nonlinear coefficient of the relaxor ferroelectric single crystal, so that the relaxor ferroelectric single crystal becomes an excellent material for preparing a periodic ferroelectric domain structure. Taking tetragonal phase PMN-0.38PT (lead titanate content 38%) as an example, the ferroelectric phase PMN-0.38PT has wide light-passing range (0.45-6 μm), high nonlinear coefficient, low Curie temperature (180 ℃) and extremely low coercive field (0.4 kV/mm), theoretically, the ferroelectric domain of PMN-0.38PT can be reversed by using an external electric field less than 1kV/mm under the room temperature condition, and compared with the traditional nonlinear crystal requiring high external voltage polarization, such as lithium niobate (LiNbO) 3 ) And potassium titanyl phosphate (KTiOPO) 4 ) And the relaxor ferroelectric crystal has more advantages when being used for preparing a functional ferroelectric domain structure, so that the relaxor ferroelectric crystal has wide application prospects in the fields of nonlinear optical frequency conversion, quantum communication and the like.
The traditional external electric field polarization method is easy to cause cracking of crystals in the polarization process. There are reports in the literature of the use of nanocomposite electrodes (including MnO) x Semiconductor nanogrid and Ti/Au conductive layer) to periodically polarize the PMN-0.3PT single crystal, but this method requires a crystal thickness of less than 200 μm. There are other documents reporting that the preparation of the periodically inverted domain structure is achieved in the tetragonal phase PMN-0.39PT by means of electron beam scanning, but the obtained inverted domain structure can only maintain the shape defined by the electron beam scanning path within a limited depth. After a depth of more than 30 μm, the inverse ferroelectric domain of the electron beam polarization may be deformed and even decomposed into discrete small domains, resulting in that the periodic structure defined by the electron beam scanning no longer exists. More importantly, neither the improved electric field polarization method nor the electron beam scanning polarization method (which requires a back electrode) can be eliminated from the pattern electrode, so that the obtained inversion domain structure can only be limited to a one-dimensional or two-dimensional structure, thereby limiting the application of the polarization structure in aspects such as nonlinear frequency conversion. Take the simplest frequency multiplication conversion example, threeThe dimensional ferroelectric domain structure can provide an inverted format in three dimensions, and theoretically can compensate phase adaptation for fundamental frequency light with any wavelength and any incident angle, so that high-efficiency frequency multiplication output is obtained.
However, at present, the relaxor ferroelectric single crystal still lacks an effective periodic polarization technology, especially a polarization technology capable of realizing a three-dimensional ferroelectric domain structure, so that the application of the single-domain relaxor ferroelectric single crystal in the field of nonlinear optics is greatly hindered.
Disclosure of Invention
In order to solve the above-mentioned problems in the prior art, the present invention provides a three-dimensional polarization method and apparatus of a single-domain tetragonal relaxor ferroelectric single crystal. The technical problem to be solved by the invention is realized by the following technical scheme:
a three-dimensional polarization method of a single-domain tetragonal relaxor ferroelectric single crystal, comprising:
emitting a first laser beam by a laser;
the first laser beam irradiates a beam energy attenuator through a shutter, and the beam energy attenuator attenuates and adjusts the first laser beam to obtain a second laser beam;
the second laser beam irradiates to a beam splitter, and the beam splitter splits the second laser beam to obtain a third laser beam and a fourth laser beam;
the third laser beam irradiates an imaging system, and the imaging system filters the third laser beam;
the fourth laser beam irradiates a direct-writing objective lens, and the direct-writing objective lens focuses the fourth laser beam on a to-be-polarized area of the single-domain relaxor ferroelectric crystal to obtain a focused beam;
adjusting the shutter and the three-dimensional platform, and simultaneously performing laser direct writing on the to-be-polarized region of the single-domain relaxor ferroelectric crystal by using the focused light beam to obtain a target three-dimensional inversion domain structure;
and imaging the target three-dimensional inversion domain structure in the focusing area of the single domain relaxor ferroelectric crystal to the imaging system by using the imaging system to obtain an image of the focusing area of the single domain relaxor ferroelectric crystal.
In one embodiment of the present invention, the beam directions of the first laser beam, the second laser beam, and the fourth laser beam are perpendicular to the (001) plane of the single-domain relaxor ferroelectric crystal.
In one embodiment of the invention, the power of the fourth laser beam is less than the crystal damage threshold power by 30-50mW.
In one embodiment of the invention, the first laser beam is a femtosecond laser, wherein,
the wavelength of the femtosecond laser is 780 to 800nm, the pulse width is less than 200fs, and the repetition frequency is 76MHz.
In one embodiment of the present invention, the beam energy attenuator comprises: a half-wave plate and a polarizing plate, wherein,
the half-wave plate and the polaroid are sequentially arranged along the optical path of the first laser beam.
In an embodiment of the present invention, adjusting the shutter and the three-dimensional platform, and performing laser direct writing on the to-be-polarized region of the single-domain relaxor ferroelectric crystal by using the focused beam to obtain a target three-dimensional inverted domain structure, includes:
keeping a shutter closed, and moving the three-dimensional platform to an nth target position, wherein the target position is determined by an x axis, a y axis and a z axis, and n is greater than 0;
and opening a shutter, moving the three-dimensional platform according to a preset polarization pattern, and simultaneously carrying out laser direct writing on the preset polarization pattern by the focused light beam along the moving track of the three-dimensional platform to obtain an nth target polarization structure, wherein the target three-dimensional inversion domain structure is formed by the n target polarization structures.
In one embodiment of the invention, the imaging system comprises: a first illumination objective, a second illumination objective, an LED lamp, an optical filter, a focusing lens, and a CCD camera, wherein,
the first illumination objective lens, the second illumination objective lens and the LED lamp are sequentially arranged along the light path of the illumination blue light beam emitted by the LED lamp;
the optical filter, the focusing lens and the CCD camera are sequentially arranged along the light path of the third laser beam.
In one embodiment of the present invention, the monitoring of the focus area image of the single domain relaxor ferroelectric crystal in real time by the imaging system includes:
the illumination blue light beam emitted by the LED lamp is focused on the single-domain relaxor ferroelectric crystal through the second illumination objective lens and the first illumination objective lens to obtain an illumination focused light beam;
the illumination focusing light beam irradiates a focusing area of the single-domain relaxor ferroelectric crystal to obtain a first illumination light beam;
the first illumination light beam is irradiated on the direct writing objective lens and then amplified to obtain a second illumination light beam;
and the second illumination light beam is reflected by the beam splitter and then imaged to the CCD camera through the optical filter and the focusing lens to obtain an image of the focusing area of the single-domain relaxor ferroelectric crystal.
In one embodiment of the present invention, the target three-dimensional inversion domain structure includes a periodic three-dimensional inversion domain structure and an aperiodic three-dimensional inversion domain structure.
A three-dimensional polarization device of a single-domain tetragonal relaxor ferroelectric single crystal is prepared by using a three-dimensional polarization method of the single-domain tetragonal relaxor ferroelectric single crystal, and comprises the following steps: the laser, the shutter, the beam energy attenuator, the beam splitter, the direct-writing objective lens, the single-domain relaxor ferroelectric crystal, the three-dimensional platform and the imaging system are sequentially arranged along the light path of a first laser beam, wherein,
the laser is used for emitting the first laser beam;
the shutter is used for controlling the first laser beam to pass through;
the beam energy attenuator is used for carrying out attenuation adjustment on the first laser beam to obtain a second laser beam;
the beam splitter is used for splitting the second laser beam to obtain a third laser beam and a fourth laser beam;
the direct-write objective lens is used for focusing the fourth laser beam to a region to be polarized of the single-domain relaxor ferroelectric crystal to obtain a focused beam;
the single-domain relaxor ferroelectric crystal is used for performing laser direct writing on the focused light beam in a to-be-polarized area of the single-domain relaxor ferroelectric crystal to obtain a target three-dimensional inversion domain structure;
the three-dimensional platform is used for adjusting the position movement of the single-domain relaxor ferroelectric crystal in a three-dimensional space;
the imaging system is used for imaging the target three-dimensional inverse domain structure in the focusing area of the single-domain relaxor ferroelectric crystal to the imaging system to obtain an image of the focusing area of the single-domain relaxor ferroelectric crystal.
The invention has the beneficial effects that:
the invention discloses a three-dimensional polarization method and a three-dimensional polarization device for a single-domain tetragonal phase relaxor ferroelectric single crystal, aiming at the problem that the relaxor ferroelectric single crystal still lacks an effective three-dimensional periodic polarization technology at the present stage. Compared with electric field polarization and electron beam scanning polarization, the three-dimensional polarization method completely gets rid of the limitation of a pattern electrode, and the polarization period and the period number can be flexibly controlled by adjusting the shutter and the three-dimensional platform; meanwhile, the single-domain relaxor ferroelectric crystal has high transmittance in the wave band of the laser beam and can be focused to different depths and positions, so that the nonlinear three-dimensional polarization of the single-domain relaxor ferroelectric crystal is realized.
The present invention will be described in further detail with reference to the drawings and examples.
Drawings
FIG. 1 is a flow chart of a three-dimensional polarization method of a single-domain tetragonal relaxor ferroelectric single crystal according to an embodiment of the present invention;
FIG. 2 is a structural view of a three-dimensional polarization apparatus of a single-domain tetragonal relaxor ferroelectric single crystal according to an embodiment of the present invention;
FIG. 3 is a Cerenkov frequency doubling microscope (CSHM) diagram for preparing a three-dimensional lattice domain structure in a single-domain tetragonal phase PMN-0.38PT provided by an embodiment of the present invention.
Detailed Description
The present invention will be described in further detail with reference to specific examples, but the embodiments of the present invention are not limited thereto.
Example one
Referring to fig. 1, fig. 1 is a flowchart of a three-dimensional polarization method of a single-domain tetragonal relaxor ferroelectric single crystal according to an embodiment of the present invention, and this embodiment discloses a three-dimensional polarization method of a single-domain tetragonal relaxor ferroelectric single crystal, including:
first, the single-domain relaxor ferroelectric crystal 6 is fixed on the three-dimensional stage 7.
Step 1, emitting a first laser beam through a laser 1.
Further, the first laser beam is a femtosecond laser, wherein the wavelength of the femtosecond laser is 780 to 800nm, the pulse width is less than 200fs, and the repetition frequency is 76MHz.
In the present embodiment, the beam direction of the first laser beam is perpendicular to the (001) plane of the single-domain relaxor ferroelectric crystal 6. The laser 1 may be, for example, a Coherent Mira 900 model.
And 2, irradiating the first laser beam to a beam energy attenuator 3 through the shutter 2, and performing attenuation adjustment on the first laser beam by the beam energy attenuator 3 to obtain a second laser beam.
The beam energy attenuator 3 includes: a half-wave plate 31 and a polarizing plate 32, wherein the half-wave plate 31 and the polarizing plate 32 are arranged in sequence along the optical path of the first laser beam.
Half-wave plate 31 may be of the type Thorlabs WPHSM05-808, for example, and polarizer plate 32 may be of the type Thorlabs GL10-C, for example.
And 3, irradiating the second laser beam to the beam splitter 4, and splitting the second laser beam by the beam splitter 4 to obtain a third laser beam and a fourth laser beam.
In this embodiment, the beam splitter 4 is used to split the laser beam for laser direct writing, that is, the fourth laser beam is a laser beam required by laser direct writing, the energy value of the fourth laser beam is 92% of the energy value of the second laser beam, and the model of the beam splitter 4 may be Thorlabs BP058, for example.
And 4, irradiating the third laser beam to the imaging system 8, and filtering the third laser beam by the imaging system 8.
Further, the imaging system 8 includes: a first illumination objective 81, a second illumination objective 82, an LED lamp 83, an optical filter 84, a focusing lens 85 and a CCD camera 86, wherein,
the first illumination objective 81, the second illumination objective 82 and the LED lamp 83 are sequentially disposed along the optical path of the blue illumination light beam emitted from the LED lamp 83;
the filter 84, the focusing lens 85, and the CCD camera 86 are sequentially disposed along the optical path of the third laser beam.
In this embodiment, the third laser beam irradiates the filter 84 and cannot pass through the filter 84, and is filtered by the filter 84.
And 5, irradiating the fourth laser beam to the direct-writing objective lens 5, and focusing the fourth laser beam to a to-be-polarized area of the single-domain relaxor ferroelectric crystal 6 by the direct-writing objective lens 5 to obtain a focused beam.
Further, the power of the fourth laser beam is less than the crystal damage threshold power by 30 to 50mW.
In the present embodiment, the numerical aperture of the direct-write objective 5 is 0.45, which may be of the type Olympus LCPLN20XIR, for example.
And 6, adjusting the shutter 2 and the three-dimensional platform 7, and simultaneously performing laser direct writing on the to-be-polarized area of the single-domain relaxor ferroelectric crystal 6 by using the focused light beam to obtain a target three-dimensional inversion domain structure.
The target three-dimensional inversion domain structure includes a periodic three-dimensional inversion domain structure and an aperiodic three-dimensional inversion domain structure.
Further, step 6 comprises:
and 6.1, keeping the shutter 2 closed, and moving the three-dimensional platform 7 to an nth target position, wherein the target position is determined by an x axis, a y axis and a z axis, and n is greater than 0.
And 6.2, opening the shutter 2, moving the three-dimensional platform 7 according to a preset polarization pattern, and simultaneously carrying out laser direct writing on the preset polarization pattern by the focused light beam along the moving track of the three-dimensional platform 7 to obtain an nth target polarization structure, wherein the n target polarization structures form a target three-dimensional reverse domain structure.
Specifically, the shutter 2 is closed, the speed and the acceleration of the three-dimensional platform 7 are respectively adjusted to a first speed and a first acceleration to control the movement of the single-domain relaxor ferroelectric crystal 6 to enable the focused light beam to reach a 1 st target position, namely the initial position of a first preset polarization pattern, then the shutter 2 is opened, the first laser beam irradiates into the shutter 2 and reaches a to-be-polarized area of the single-domain relaxor ferroelectric crystal 6 through the beam energy attenuator 3, the beam splitter 4 and the direct writing objective lens 5, and then the speed and the acceleration of the three-dimensional platform 7 are respectively adjusted to a second speed and a second acceleration to enable the focused light beam to carry out laser direct writing in the to-be-polarized area to obtain a 1 st target polarization structure; closing the shutter 2, adjusting the speed and the acceleration of the three-dimensional platform 7 to be the first speed and the first acceleration respectively, enabling the focused light beam to reach the 2 nd target position, opening the shutter 2, adjusting the speed and the acceleration of the three-dimensional platform 7 to be the second speed and the second acceleration respectively again, enabling the focused light beam to perform laser direct writing in the region to be polarized to obtain the 2 nd target polarization structure, and so on, obtaining the nth target polarization structure at the nth target position, wherein the n target polarization structures form a target three-dimensional inversion domain structure.
When the distances among the n target polarized structures are equal, the target three-dimensional reverse domain structure is a periodic three-dimensional reverse domain structure; and when the distances among the n target polarized structures are not equal, the target three-dimensional reverse domain structure is a non-periodic three-dimensional reverse domain structure.
In the present embodiment, the shutter 2 may be, for example, a Thorlabs SH05 model, and the three-dimensional platform 7 may be, for example, a Thorlabs MAX383 model.
And 7, imaging the target three-dimensional inversion domain structure in the focusing area of the single domain relaxor ferroelectric crystal 6 to an imaging system 8 by using the imaging system 8 to obtain an image of the focusing area of the single domain relaxor ferroelectric crystal 6.
Further, step 7 comprises:
and 7.1, focusing the blue illumination light beam emitted by the LED lamp 83 on the single-domain relaxor ferroelectric crystal 6 through the second illumination objective 82 and the first illumination objective 81 to obtain an illumination focused light beam.
And 7.2, irradiating the target three-dimensional reverse domain structure by the illumination focused light beam to obtain a first illumination light beam in a focusing area of the single-domain relaxor ferroelectric crystal 6.
And 7.3, the first illumination light beam is irradiated on the direct-writing objective lens 5 and then is amplified to obtain a second illumination light beam.
And 7.4, the second illumination light beam is reflected by the beam splitter 4, then is imaged to the CCD camera 86 through the optical filter 84 and the focusing lens 85, and an image of the focusing area of the single-domain relaxor ferroelectric crystal 6 is obtained.
In the present embodiment, the imaging system 8 is used to image the target three-dimensional inverted domain structure on the focus area of the single domain relaxor ferroelectric crystal 6 to the CCD camera to monitor whether the target area is suitable for polarization and the refractive index change after polarization.
The first illumination objective 81 may be, for example, of the type Olympus MPLN10x, the second illumination objective 82 may be, for example, of the type Olympus MPLN10x, the LED lamp 83 may be, for example, of the type Thorlabs M470F3, the optical filter 84 may be, for example, of the type Thorlabs FGS900-a, the focusing lens 85 may be, for example, of the type Thorlabs LB1945, and the CCD camera 86 may be, for example, of the type Thorlabs DCU223C.
In summary, in the three-dimensional polarization method of the single-domain tetragonal phase relaxor ferroelectric single crystal, the target unit inverse domain structure is obtained by focusing the first laser beam on the to-be-polarized region of the single-domain relaxor ferroelectric crystal 6 and performing laser direct writing on the to-be-polarized region of the single-domain relaxor ferroelectric crystal 6 by using the focused laser beam in combination with the adjustment of the shutter 2 and the three-dimensional platform 7. Compared with electric field polarization and electron beam scanning polarization, the three-dimensional polarization method completely gets rid of the limitation of a pattern electrode, and the polarization period and the period number can be flexibly controlled by adjusting the shutter 2 and the three-dimensional platform 7; meanwhile, the single-domain relaxor ferroelectric crystal 6 has high transmittance in the wave band of the laser beam, and can be focused to different depths and positions, thereby realizing the nonlinear three-dimensional polarization of the single-domain relaxor ferroelectric crystal 6.
Example two
Referring to fig. 2, fig. 2 is a structural diagram of a three-dimensional polarization apparatus for a single-domain tetragonal relaxor ferroelectric single crystal according to a first embodiment of the present invention. The embodiment discloses a three-dimensional polarization device of a single-domain tetragonal phase relaxor ferroelectric single crystal, which is prepared by a three-dimensional polarization method of the single-domain tetragonal phase relaxor ferroelectric single crystal, and comprises the following steps: the laser 1, the shutter 2, the beam energy attenuator 3, the beam splitter 4, the direct-write objective lens 5, the single-domain relaxor ferroelectric crystal 6, the three-dimensional platform 7 and the imaging system 8 are sequentially arranged along the optical path of the first laser beam, wherein,
a laser 1 for emitting a first laser beam;
a shutter 2 for controlling the first laser beam to pass through;
the beam energy attenuator 3 is used for carrying out attenuation adjustment on the first laser beam to obtain a second laser beam;
the beam splitter 4 is used for splitting the second laser beam to obtain a third laser beam and a fourth laser beam;
the direct-writing objective lens 5 is used for focusing the fourth laser beam to a to-be-polarized area of the single-domain relaxor ferroelectric crystal 6 to obtain a focused beam;
the single-domain relaxor ferroelectric crystal 6 is used for focusing a light beam to perform laser direct writing on a to-be-polarized area of the single-domain relaxor ferroelectric crystal to obtain a target three-dimensional inversion domain structure;
the three-dimensional platform 7 is used for adjusting the position movement of the single-domain relaxor ferroelectric crystal 6 in a three-dimensional space;
and the imaging system 8 is used for imaging the target three-dimensional inverted domain structure in the focusing area of the single-domain relaxor ferroelectric crystal 6 to the imaging system to obtain an image of the focusing area of the single-domain relaxor ferroelectric crystal 6.
Further, the beam energy attenuator 3 includes: a half-wave plate 31 and a polarizing plate 32.
The imaging system 8 includes: a first illumination objective 81, a second illumination objective 82, an LED lamp 83, an optical filter 84, a focusing lens 85, and a CCD camera 86.
In the embodiment, firstly, a single-domain relaxor ferroelectric crystal 6 is fixed on a three-dimensional platform 7, a power meter is placed in front of a direct writing objective lens 5, a laser 1 emits a first laser beam, a shutter 2 is opened, the first laser beam is attenuated and adjusted through a beam energy attenuator 3 to obtain a second laser beam, a beam splitter 4 splits the second laser beam to obtain a third laser beam and a fourth laser beam, the third laser beam irradiates an imaging system 8 and is filtered by the imaging system 8, the fourth laser beam is focused to a to-be-polarized area of the single-domain relaxor ferroelectric crystal 6 by the direct writing objective lens 5 to obtain a focused beam, the beam energy attenuator 3 is adjusted to enable the power of the fourth laser beam to be 30 to 50mw lower than a crystal damage threshold value, the shutter 2 is closed, and the power meter is removed. Moving the position of the three-dimensional platform 7 to a 1 st target position, opening the shutter 2, irradiating the focused light beam to a to-be-polarized region of the single-domain relaxor ferroelectric crystal 6, and further controlling the focused light beam to perform laser direct writing on the to-be-polarized region of the single-domain relaxor ferroelectric crystal 6 to obtain a 1 st target polarized structure; then closing the shutter 2, moving the position of the three-dimensional platform 7 to a 2 nd target position, then opening the shutter 2, enabling the laser 1 to emit a fifth laser beam, enabling the fifth laser beam to be attenuated and adjusted through the beam energy attenuator 3 to obtain a sixth laser beam, enabling the beam splitter 4 to split the sixth laser beam to obtain a seventh laser beam and an eighth laser beam, enabling the seventh laser beam to irradiate the imaging system 8 and be filtered by the imaging system 8, enabling the eighth laser beam to be focused to a to-be-polarized area of the single-domain relaxor ferroelectric crystal 6 by the direct writing objective lens 5 to obtain a focused beam, enabling the focused beam to irradiate the to-be-polarized area of the single-domain relaxor ferroelectric crystal 6, moving the position of the three-dimensional platform 7, further controlling the focused beam to perform laser direct writing in the to-be-polarized area of the single-domain relaxor ferroelectric crystal 6 to obtain a 2 nd target polarized structure, and then closing the shutter 2; and by analogy, obtaining an nth target polarized structure, wherein the n target polarized structures form a target three-dimensional reverse domain structure.
EXAMPLE III
Referring to fig. 1 and 3, fig. 1 is a flowchart of a three-dimensional polarization method of a single-domain tetragonal relaxor ferroelectric single crystal according to an embodiment of the present invention, and fig. 3 is a cerenkov frequency multiplication microscope (CSHM) diagram of a three-dimensional lattice domain structure prepared in a single-domain tetragonal PMN-0.38PT according to an embodiment of the present invention. The embodiment discloses a three-dimensional polarization method of a single-domain tetragonal phase relaxor ferroelectric single crystal, which comprises the following steps:
firstly, fixing a single-domain relaxor ferroelectric crystal 6 on a three-dimensional platform 7, in particular to a three-dimensional lattice domain structure in a single-domain tetragonal phase PMN-0.38PT relaxor ferroelectric single crystal.
Step 1, emitting a first laser beam through a laser 1.
Specifically, the first laser beam is a femtosecond laser having a wavelength of 800nm, a pulse width of 180fs, and a repetition frequency of 76MHz, and is perpendicularly incident to the (001) plane of the single-domain relaxor ferroelectric crystal 6 along the polar axis direction of the single-domain relaxor ferroelectric crystal 6.
And 2, irradiating the first laser beam to a beam energy attenuator 3 through a shutter 2, and performing attenuation adjustment on the first laser beam by the beam energy attenuator 3 to obtain a second laser beam.
The beam energy attenuator 3 includes: a half-wave plate 31 and a polarizing plate 32, wherein the half-wave plate 31 and the polarizing plate 32 are arranged in sequence along the optical path of the first laser beam.
And 3, irradiating the second laser beam to the beam splitter 4, and splitting the second laser beam by the beam splitter 4 to obtain a third laser beam and a fourth laser beam.
And 4, irradiating the third laser beam to the imaging system 8, and filtering the third laser beam by the imaging system 8.
Further, the imaging system 8 includes: a first illumination objective 81, a second illumination objective 82, an LED lamp 83, an optical filter 84, a focusing lens 85, and a CCD camera 86, wherein,
the first illumination objective 81, the second illumination objective 82 and the LED lamp 83 are sequentially disposed along the optical path of the blue illumination light beam emitted from the LED lamp 83;
the filter 84, the focusing lens 85, and the CCD camera 86 are sequentially disposed along the optical path of the third laser beam.
And 5, irradiating the direct-write objective lens 5 with the fourth laser beam, and focusing the fourth laser beam to a to-be-polarized area of the single-domain relaxor ferroelectric crystal 6 by the direct-write objective lens 5 to obtain a focused beam.
Further, the power of the fourth laser beam is less than the crystal damage threshold power by 30 to 50mW.
Specifically, the average power of the fourth laser beam was adjusted to 230mW with the beam energy attenuator 3. Specifically, a direct write objective lens 5 having a numerical aperture of 0.45 is employed.
And 6, adjusting the shutter 2 and the three-dimensional platform 7, and simultaneously performing laser direct writing on the to-be-polarized area of the single-domain relaxor ferroelectric crystal 6 by using the focused light beam to obtain a target three-dimensional inversion domain structure.
Further, step 6 comprises:
and 6.1, keeping the shutter 2 closed, and moving the three-dimensional platform 7 to an nth target position, wherein the target position is determined by an x axis, a y axis and a z axis, and n is greater than 0.
And 6.2, opening the shutter 2, moving the three-dimensional platform 7 according to a preset polarization pattern, and simultaneously carrying out laser direct writing on the preset polarization pattern by the focused light beam along the moving track of the three-dimensional platform 7 to obtain an nth target polarization structure, wherein the n target polarization structures form a target three-dimensional reverse domain structure.
Specifically, the first speed and the second speed of the three-dimensional platform 7 are both set to 2.5mm/s, and the first acceleration and the second acceleration are both set to 2.5mm/s 2 The single domain relaxor ferroelectric crystal 6 was moved to (0 mm, 0.17mm) position, and laser direct writing was started with a focused light beam to a three-dimensional periodic lattice domain structure of 5 layers in which the periods of the inversion domains in the x, y, and z directions were 5 μm, and 72 μm, respectively, and each layer contained 10 × 10 inversion domains. Open shutter 2, stop t 1 =0.5s, and then the shutter 2 is closed, i.e. laser direct writing of the 1 st target polarization structure is completed.
And moving the single-domain relaxor ferroelectric crystal 6 in the xoy plane according to the x and y directions and the period interval of 5 mu m, opening the shutter 2 for 0.5s after moving to a new position, closing the shutter 2, and moving to the next position to repeat the laser direct writing process until the layer of 100 target polarization structures is completed.
The shutter 2 was kept closed, and the single-domain relaxor ferroelectric crystal 6 was moved to the (0 mm, 0.14mm) position, and the laser direct writing process in the above-described step 6 was started to complete the 100 target polarization structures of the second layer. Then, the single domain relaxor ferroelectric crystal 6 was sequentially moved to (0mm, 0.11mm), (0mm, 0.08mm), and (0mm, 0.05mm) equal-depth positions, and the target polarization structure of the remaining several layers was completed. And finally, closing the shutter 2, namely obtaining the target three-dimensional inversion domain structure in the sample.
And 7, imaging the target three-dimensional reverse domain structure in the focusing area of the single-domain relaxor ferroelectric crystal 6 to the imaging system 8 by using the imaging system 8 to obtain an image of the focusing area of the single-domain relaxor ferroelectric crystal 6.
Further, step 7 comprises:
and 7.1, focusing the illumination blue light beams emitted by the LED lamp 83 on the single-domain relaxor ferroelectric crystal 6 through the second illumination objective 82 and the first illumination objective 81 to obtain illumination focused light beams.
And 7.2, irradiating the target three-dimensional reverse domain structure by the illumination focused light beam to obtain a first illumination light beam in a focusing area of the single-domain relaxor ferroelectric crystal 6.
And 7.3, the first illumination light beam is irradiated on the direct-writing objective lens 5 and then amplified to obtain a second illumination light beam.
And 7.4, the second illumination light beam is reflected by the beam splitter 4, then is imaged to the CCD camera 86 through the optical filter 84 and the focusing lens 85, and an image of the focusing area of the single-domain relaxor ferroelectric crystal 6 is obtained.
In this embodiment, the imaging system 8 is configured to image the target three-dimensional inverted domain structure onto a CCD camera in a focusing area of the single domain relaxor ferroelectric crystal 6, and perform imaging characterization on the single domain relaxor ferroelectric crystal 6 before and after laser polarization, so as to verify the polarization effect of the method of the present invention.
Example four
Referring to fig. 1 and 3, fig. 1 is a flow chart of a three-dimensional polarization method of a single-domain tetragonal relaxor ferroelectric single crystal according to an embodiment of the present invention, and fig. 3 is a drawing of a cerenkov frequency multiplication microscope (CSHM) for preparing a three-dimensional lattice domain structure in a single-domain tetragonal PMN-0.38PT according to an embodiment of the present invention. The embodiment discloses a three-dimensional polarization method of a single-domain tetragonal phase relaxor ferroelectric single crystal, which comprises the following steps:
firstly, a single-domain relaxor ferroelectric crystal 6 is fixed on a three-dimensional platform 7, in particular to a linear periodic domain structure in a single-domain tetragonal phase PMN-0.38PT relaxor ferroelectric single crystal.
Step 1, emitting a first laser beam through a laser 1.
Specifically, the first laser beam is a femtosecond laser having a wavelength of 800nm, a pulse width of 180fs, and a repetition frequency of 76MHz, and is perpendicularly incident to the (001) plane of the single-domain relaxor ferroelectric crystal 6 along the polar axis direction of the single-domain relaxor ferroelectric crystal 6.
And 2, irradiating the first laser beam to a beam energy attenuator 3 through the shutter 2, and performing attenuation adjustment on the first laser beam by the beam energy attenuator 3 to obtain a second laser beam.
The beam energy attenuator 3 includes: a half-wave plate 31 and a polarizing plate 32, wherein the half-wave plate 31 and the polarizing plate 32 are arranged in sequence along the optical path of the first laser beam.
And 3, irradiating the second laser beam to the beam splitter 4, and splitting the second laser beam by the beam splitter 4 to obtain a third laser beam and a fourth laser beam.
And 4, irradiating the third laser beam to the imaging system 8, and filtering the third laser beam by the imaging system 8.
Further, the imaging system 8 includes: a first illumination objective 81, a second illumination objective 82, an LED lamp 83, an optical filter 84, a focusing lens 85 and a CCD camera 86, wherein,
the first illumination objective 81, the second illumination objective 82 and the LED lamp 83 are sequentially disposed along the optical path of the blue illumination light beam emitted from the LED lamp 83;
the optical filter 84, the focusing lens 85, and the CCD camera 86 are sequentially disposed along the optical path of the third laser beam.
And 5, irradiating the fourth laser beam to the direct-writing objective lens 5, and focusing the fourth laser beam to a to-be-polarized area of the single-domain relaxor ferroelectric crystal 6 by the direct-writing objective lens 5 to obtain a focused beam.
Further, the power of the fourth laser beam is less than the crystal damage threshold power by 30 to 50mW.
Specifically, the average power of the fourth laser beam was adjusted to 230mW using the beam energy attenuator 3.
Specifically, a direct write objective lens 5 having a numerical aperture of 0.45 is employed.
And 6, adjusting the shutter 2 and the three-dimensional platform 7, and simultaneously performing laser direct writing on the to-be-polarized region of the single-domain relaxor ferroelectric crystal 6 by using the focused light beam to obtain a target three-dimensional inversion domain structure.
Further, step 6 comprises:
and 6.1, keeping the shutter 2 closed, and moving the three-dimensional platform 7 to an nth target position, wherein the target position is determined by an x axis, a y axis and a z axis, and n is greater than 0.
And 6.2, opening the shutter 2, moving the three-dimensional platform 7 according to a preset polarization pattern, and simultaneously carrying out laser direct writing on the preset polarization pattern by the focused light beam along the moving track of the three-dimensional platform 7 to obtain an nth target polarization structure, wherein the n target polarization structures form a target three-dimensional reverse domain structure.
Specifically, the first velocity of the three-dimensional stage 7 is set to 2.5mm/s, and the first acceleration is set to 2.5mm/s 2 The single domain relaxor ferroelectric crystal 6 was moved to the (0 mm, 0.05mm) position, and then the second velocity of the three-dimensional platform 7 was set to 0.01mm/s and the second acceleration was set to 0.01mm/s 2 The direct writing of 5 linear inverted domain structures along the x-direction, each having a length of 100 μm and an inverted domain period of 5 μm in the y-direction, using a focused beam laser was started. And opening the shutter 2 to enable the single-domain relaxor ferroelectric crystal 6 to move 100 microns along the x-axis direction, and then closing the shutter 2, namely completing the laser direct writing of the 1 st target polarization structure. The shutter 2 is closed.
The first speed of the three-dimensional platform 7 is set to 2.5mm/s and the first acceleration is set to 2.5mm/s 2 The sample was moved to a (0 mm,0.005mm, 0.05mm) position, and the second velocity of the three-dimensional stage 7 was set to 0.01mm/s and the second acceleration was set to 0.01mm/s 2 The laser writing of a second inversion domain is started. The shutter is opened to move the single-domain relaxor ferroelectric crystal 6 by 100 μm in the x-axis direction, and then the shutter 2 is closed, thereby completing the laser direct writing of the item 2 standard polarization structure. Then using the same methodThe method completes the laser direct writing of the remaining three target polarization structures.
And 7, imaging the target three-dimensional reverse domain structure in the focusing area of the single-domain relaxor ferroelectric crystal 6 to the imaging system 8 by using the imaging system 8 to obtain an image of the focusing area of the single-domain relaxor ferroelectric crystal 6.
Further, step 7 comprises:
and 7.1, focusing the blue illumination light beam emitted by the LED lamp 83 on the single-domain relaxor ferroelectric crystal 6 through the second illumination objective 82 and the first illumination objective 81 to obtain an illumination focused light beam.
And 7.2, irradiating the target three-dimensional inversion domain structure by the illumination focused light beam to obtain a first illumination light beam in the focusing area of the single-domain relaxor ferroelectric crystal 6.
And 7.3, the first illumination light beam is irradiated on the direct-writing objective lens 5 and then is amplified to obtain a second illumination light beam.
And 7.4, the second illumination light beam is reflected by the beam splitter 4, then is imaged to the CCD camera 86 through the optical filter 84 and the focusing lens 85, and an image of the focusing area of the single-domain relaxor ferroelectric crystal 6 is obtained.
In this embodiment, the imaging system 8 is configured to image the target three-dimensional inverted domain structure onto a CCD camera in a focusing area of the single domain relaxor ferroelectric crystal 6, and perform imaging characterization on the single domain relaxor ferroelectric crystal 6 before and after laser polarization, so as to verify the polarization effect of the method of the present invention.
It should be noted that the terms "first" and "second" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more features. In the description of the present invention, "a plurality" means two or more unless specifically defined otherwise.
In the description of the specification, reference to the description of the term "one embodiment", "some embodiments", "an example", "a specific example", or "some examples", etc., means that a particular feature or characteristic described in connection with the embodiment or example is included in at least one embodiment or example of the invention. In this specification, the schematic representations of the terms used above are not necessarily intended to refer to the same embodiment or example. Furthermore, the particular features or characteristics described may be combined in any suitable manner in any one or more embodiments or examples. Furthermore, various embodiments or examples described in this specification can be combined and combined by those skilled in the art.
While the present application has been described in connection with various embodiments, other variations to the disclosed embodiments can be understood and effected by those skilled in the art in practicing the claimed application, from a review of the drawings, the disclosure, and the appended claims.
The foregoing is a more detailed description of the invention in connection with specific preferred embodiments and it is not intended that the invention be limited to these specific details. For those skilled in the art to which the invention pertains, numerous simple deductions or substitutions may be made without departing from the spirit of the invention, which shall be deemed to belong to the scope of the invention.

Claims (4)

1. A three-dimensional polarization method of a single-domain tetragonal phase relaxor ferroelectric single crystal, comprising:
emitting a first laser beam by a laser (1);
the first laser beam irradiates a beam energy attenuator (3) through a shutter (2), and the beam energy attenuator (3) attenuates and adjusts the first laser beam to obtain a second laser beam;
the second laser beam irradiates to a beam splitter (4), and the beam splitter (4) splits the second laser beam to obtain a third laser beam and a fourth laser beam;
the third laser beam irradiates an imaging system (8), and the imaging system (8) filters the third laser beam;
the fourth laser beam irradiates a direct writing objective lens (5), the direct writing objective lens (5) focuses the fourth laser beam to a to-be-polarized area of a single-domain relaxor ferroelectric crystal (6) to obtain a focused beam, wherein the single-domain relaxor ferroelectric crystal (6) is a single-domain tetragonal phase PMN-0.38PT relaxor ferroelectric single crystal, the beam directions of the first laser beam, the second laser beam and the fourth laser beam are perpendicular to a (001) surface of the single-domain relaxor ferroelectric crystal (6), the power of the fourth laser beam is smaller than a crystal damage threshold power by 30 to 50mW, and the numerical aperture of the direct writing objective lens (5) is 0.45;
adjusting the shutter (2) and the three-dimensional platform (7), and simultaneously performing laser direct writing on a to-be-polarized region of the single-domain relaxor ferroelectric crystal (6) by using the focused light beam to obtain a target three-dimensional inversion domain structure;
and monitoring the focus area image of the single-domain relaxor ferroelectric crystal (6) in real time by using the imaging system (8).
2. The three-dimensional polarization method of a single-domain tetragonal relaxor ferroelectric single crystal according to claim 1, wherein the first laser beam is a femtosecond laser, wherein,
the wavelength of the femtosecond laser is 780 to 800nm, the pulse width is less than 200fs, and the repetition frequency is 76MHz.
3. The three-dimensional polarization method of a single-domain tetragonal relaxor ferroelectric single crystal according to claim 1, wherein adjusting the shutter (2) and the three-dimensional platform (7) while performing laser direct writing on the to-be-polarized region of the single-domain relaxor ferroelectric crystal (6) with the focused beam to obtain a target three-dimensional inverted domain structure comprises:
keeping the shutter (2) closed, and moving the three-dimensional platform (7) to an nth target position, wherein the target position is determined by an x axis, a y axis and a z axis, and n is greater than 0;
and opening the shutter (2), moving the three-dimensional platform (7) according to a preset polarization pattern, and simultaneously carrying out laser direct writing on the preset polarization pattern by the focused light beam along the moving track of the three-dimensional platform (7) to obtain an nth target polarization structure, wherein the target three-dimensional inversion domain structure is formed by the n target polarization structures.
4. The three-dimensional poling method of a single-domain tetragonal relaxor ferroelectric single crystal according to claim 1, wherein the target three-dimensional inversion domain structure includes a periodic three-dimensional inversion domain structure and an aperiodic three-dimensional inversion domain structure.
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