CN113745400B - Fe intercalated graphene oxide two-dimensional adjustable ferroelectric polarization material structure design method - Google Patents
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Abstract
The invention discloses a two-dimensional adjustable ferroelectric polarization material structural design based on Fe intercalation graphene oxide, which comprises the following design scheme: the method comprises the steps of selecting a base material, designing an intercalation polarization structure, using energy-strain required by polarization inversion, and carrying out polarization treatment, wherein graphene oxide realizes a simple structure for storing ferroelectric information, and has low dimension and small scale, and an external electric field required by inversion polarization is small; the ferroelectric polarization of the structure is vertical to the surface of the single-layer film, and the data can be easily read and written by an external electric field; the invention has the advantages of simple structural design, convenient operation, easy processing, greatly improved integration level and the like, and along with the increase of a certain range of strain, the external electric field required for realizing the ferroelectric information storage can be smaller, thereby having considerable application prospect.
Description
Technical Field
The invention belongs to the field of dielectric material application, and particularly relates to a structural design method of a Fe intercalated graphene oxide two-dimensional adjustable ferroelectric polarization material.
Background
The dielectric material with ferroelectric property has extremely wide development prospect in the application fields of sensing, information storage, photoelectricity and other multifunctional devices due to the characteristic that the electric polarization of the dielectric material can be regulated and controlled by an external electric field. Meanwhile, with the development of modern science, the electronic devices tend to be miniaturized, integrated and multifunctional with the rapid development of microelectronic integration technology, but the traditional ferroelectric materials are difficult to meet the increasingly developed demands of the modern technology due to the characteristics of the bulk materials, the size limitation and the surface depolarization effect, so that the ferroelectric materials with proper and excellent properties and structures with adjustable ferroelectric properties are searched and designed in the field of low-dimensional materials to form new research hotspots.
In recent years, using the first principles and other theoretical tools, one has successfully predicted and designed two-dimensional materials and structures with good ferroelectric properties, such as: in single layer MX (m=ge, sn; x=s, se), in 2 Se 3 Reversible in-plane ferroelectric polarization in the material; 1T-MoS 2 Layered CuIn 2 P 6 The stable out-of-plane ferroelectricity can exist at room temperature; while single layer VOX 2 (X=F,Cl,Br,I)、Hf 2 VC 2 F 2 Then the two-dimensional multiferroic material with coexisting magnetism and in-plane ferroelectricity is adopted; meanwhile, two-dimensional ferroelectric materials which exist stably at room temperature have been successfully prepared from experimental technology, such as Chang et al, successfully prepare SnTe thin films with stable performance by using a molecular beam epitaxy technology, and the existence of ferroelectricity is proved.
Graphene is the thinnest two-dimensional nanomaterial in the world, which is composed of single-layer carbon atoms and has excellent optical, electrical, mechanical and other properties which are not possessed by common carbon materials, and the properties of the graphene can be effectively regulated and modified by modifying the graphene, magic angle, doping, strain, intercalation method and the like. For example, it is found that graphene modified by hydroxyl is a two-dimensional organic material with multiferroics, and ferroelectric polarization of the graphene is perpendicular to the surface of the graphene due to the structural transformation from a central symmetrical structure to a space inversion symmetry break.
Graphene oxide has a large amount of oxygen-containing functional groups on the surface, so that the carbon layer is negatively charged, cations are easily attracted into the interlayer, the interlayer distance is enlarged, and favorable conditions are provided for loading of polymers and inorganic nanoparticles. Fe ions have the characteristics of larger spontaneous magnetic dipole moment, larger spin coupling between magnetic moments, ion chargeability and the like, and have wide application in practical production, and the structure symmetry of the Fe ions is changed through intercalation graphene oxide, and the external strain is combined to regulate and control the two-dimensional ferroelectric polarization and magnetism of the structure.
Disclosure of Invention
The invention aims to solve the problems and provide a microstructure for realizing ferroelectric information storage and regulation through Fe intercalation and external strain; the structure not only has the smallest information storage unit, but also has the characteristics of large polarization intensity, polarization vertical to the surface of the film, low polarization flip barrier, easy regulation and control by an external electric field and the like.
In order to achieve the above purpose, the technical scheme of the invention is realized as follows:
the design method of the Fe intercalated graphene oxide two-dimensional adjustable ferroelectric polarization material structure comprises the following steps:
step one, selecting a base material:
selecting two-dimensional graphene oxide as a base material, wherein the graphene oxide is obtained by covalent bonding of O and C in the graphene, and the graphene is C to form a hexagonal honeycomb structure; in the graphene oxide, an O layer is distributed in plane inversion symmetry about a C atomic layer, namely in a C atomic hexagonal honeycomb structure, C atoms in the next neighbor form a covalent bond with O on the same side, namely O and C atoms form a central symmetry structure about a C six-ring, and the system is unpolarized;
step two, designing an intercalation polarization structure:
simulating and constructing an Fe intercalated graphene oxide crystal structure by utilizing material Studio 2019 and VESTA visual structure drawing software, performing preliminary structure optimization after intercalation by utilizing a VASP software program package, and calculating to obtain an optimal adsorption position of Fe;
step three, energy required by polarization inversion:
adopting the method that Fe atoms move up and down along the direction of a c-axis, wherein the direction of the c-axis is perpendicular to the plane direction, calculating and determining the energy barrier which needs to be overcome by polarization inversion due to Fe ions moving in the whole process of moving Fe ions from above the plane to below the plane, and primarily judging the possibility of iron polarization inversion in the two-dimensional material;
and step four, strain application:
the Fe intercalated graphene oxide film is fixed on a lattice matched substrate, and strain is applied to the film by applying two-dimensional mechanical stress to the substrate.
Step five, polarization treatment:
since the stable adsorption positions of Fe ion intercalation are symmetrical about a C atomic layer, the Fe ions are randomly distributed at the positions during intercalation, so that the two-dimensional structure of the intercalation is possibly free of macroscopic ferroelectric polarization, and therefore, the iron intercalation graphene oxide film fixed on a substrate is subjected to single domain treatment during actual application; and (3) placing the film in a stronger constant external electric field to carry out initial polarization, so as to obtain a single-phase single crystal of the single-layer film.
Further, the optimal adsorption position of Fe is calculated in the second step: the Fe ions are positioned above the center of the C six-ring, and below the centers of three O atoms adjacent to each other above the C plane, and the structure breaks through the spatial symmetry of the graphene oxide and has intrinsic spontaneous polarization.
Furthermore, in the third step, as the radius of Fe ions is far larger than that of C atoms and the ionic combination between Fe and O ions, the energy barrier which is required to be overcome when Fe ions pass through the center of the C ring is calculated and found to be far higher than the field intensity range of a common external electric field.
Further, in the fourth step, it was found that when the two-dimensional biaxial tensile strain reached 30%, the single layer C was calculated 2 O 2 The potential barrier height corresponding to single Fe ion inversion in Fe is only 0.32eV, and the potential barrier height is obviously reduced along with the increase of tensile strain, namely, the ferroelectric polarization inversion in the Fe intercalated graphene oxide film can be realized through a small external electric field, and the monolayer film cannot be broken down due to the over-strong external electric field.
Further, the fifth step is to conduct single domain treatment on the film, gradually increase the electric field in the direction perpendicular to the surface of the film, and measure the polarization intensity of the film in situ in real time until the polarization intensity of the film along the direction of the electric field is not increased any more; changing the direction of the electric field, gradually increasing the reverse electric field intensity, measuring the polarization intensity in real time, recording the relation between the electric field intensity and the polarization intensity, and drawing a hysteresis loop.
The invention provides a two-dimensional adjustable ferroelectric polarization material structural design based on Fe intercalated graphene oxide, which enables the graphene oxide to realize a simple structure for storing ferroelectric information, and has the advantages of low dimension, small scale and small external electric field required by inversion polarization; the ferroelectric polarization of the structure is vertical to the surface of the single-layer film, and the data can be easily read and written by an external electric field; the invention has the advantages of simple structural design, convenient operation, easy processing, greatly improved integration level and the like, and along with the increase of the strain in a certain range, the required external electric field for realizing the ferroelectric information storage can be smaller, thereby having considerable application prospect.
Drawings
FIG. 1 is a block diagram of different sides of Fe intercalated graphene oxide; wherein (a) is a top view, and B-D is a side view, (B) ferroelectric polarization is upward, (c) no-iron polarization, (D) ferroelectric polarization is downward;
FIG. 2 is a graph of barrier height (inversion containing a single Fe ion) of a cell under different strains;
FIG. 3 is an energy plot as a function of Fe atomic position at 30% strain.
Detailed Description
The present invention will be described in further detail with reference to the accompanying drawings and examples.
The design method of the Fe intercalated graphene oxide two-dimensional adjustable ferroelectric polarization material structure comprises the following steps:
step one, selecting a base material:
in order to meet the design requirements of a nano multifunctional device on a ferroelectric memory cell, which has low necessary dimension and small dimension, two-dimensional graphene oxide is selected as a base material, C in the graphene oxide forms a hexagonal honeycomb structure, O and C are covalently combined, O and C are symmetrically distributed about the center of a C six-ring, namely, in the C-atom hexagonal honeycomb structure, C atoms in the next nearest neighbor form covalent bonds with O on the same side, namely, an O layer forms a symmetrical structure about the C-atom layer surface, and the system is unpolarized;
step two, designing an intercalation polarization structure:
the Fe intercalated graphene oxide crystal structure is simulated and constructed by utilizing material Studio 2019 and VESTA visual structure drawing software, the initial structural optimization is carried out after intercalation by utilizing a VASP software program package, the optimal adsorption position of Fe is obtained by calculation, fe ions are found to be positioned above the center of a C six ring and below the centers of three O atoms adjacent to each other above a C plane, and the structure breaks through the spatial symmetry of graphene oxide and has intrinsic spontaneous polarization as shown in figure 1;
step three, energy required by polarization inversion:
and (3) adopting the position of the Fe atom to move up and down along the direction of the c-axis (perpendicular to the plane), calculating and determining the energy barrier which needs to be overcome by polarization inversion due to the movement of the Fe ion in the whole process of moving Fe ions from above the plane to below the plane, and primarily judging the possibility of the iron polarization inversion in the two-dimensional material. Since the radius of Fe ion is far larger than that of C atom and the ionic combination between Fe and O ion, the energy barrier to be overcome when Fe ion passes through C ring center is far higher than the field intensity range of general external electric field.
And step four, strain application:
and fixing the Fe intercalated graphene oxide film on the substrate, and applying strain to the graphene oxide by applying two-dimensional mechanical stress to the substrate. Calculations found that when the two-dimensional biaxial tensile strain reached 30%, monolayer C 2 O 2 The barrier height corresponding to the inversion of a single Fe ion in Fe is only 0.32eV (figures 2 and 3), which is comparable with that in bulk material PaTiO3, and the barrier height is obviously reduced along with the increase of tensile strain (figure 2), namely the ferroelectric polarization inversion in the graphene oxide film can be realized through a small external electric field, and the single-layer film cannot be broken down due to the over-strong external electric field.
Step five, polarization treatment:
since the stable adsorption positions of Fe ion intercalation are symmetrical about C atomic layer, fe ions can be randomly distributed at the positions during intercalation, so that the two-dimensional structure of the intercalation is probably free of macroscopic ferroelectric polarization, and the film should be subjected to single-domain treatment before practical application. The film can be placed in a stronger constant external electric field for initial polarization, so that the obtained single-layer film can be ensured to be single-phase single crystal.
Fig. 1 is a schematic diagram showing different sides of Fe intercalated graphene oxide. In the figure, the atom with the smallest diameter is a C atom, the atom with the largest diameter is a Fe atom, the atom with the diameter between the C atom and the Fe atom is an O atom, and in the C six-ring, one O above the C atom with the next neighbor coordinates with the C atom to form a covalent bond, the O forms a planar regular triangle lattice, the other three C atoms with the next neighbor coordinate with the O atom below the C atom in a covalent bond, and the O below the C six-ring also forms the planar regular triangle lattice. In the polarized structure, all the Fe ions are located above the center of the C six rings but below the center of the upper O-ion regular triangle lattice. The ferroelectric polarization in the intercalated two-dimensional structure is upward due to the insertion of Fe ions.
According to the theoretical calculation result, when the Fe ions move from above the plane to a symmetrical position below the plane without the applied strain, the required energy is too large, as shown in fig. 2, and the ferroelectric polarization is difficult to turn over. In order to reduce the energy required for ferroelectric inversion, the energy barrier can be effectively reduced by applying strain, and as can be seen from fig. 3, when the tensile strain reaches about 30%, the energy required for single electric dipole inversion is only 0.32eV, and the maximum polarization intensity of the stable state is 1.6x10 -10 C/m, that is, the inversion of the larger ferroelectric polarization can be achieved by a smaller applied electric field.
While the embodiments and effects of the present invention have been shown and described, it should be noted that it will be apparent to those skilled in the art that various modifications and adaptations can be made without departing from the principles of the present invention, and such modifications and adaptations should and are intended to be comprehended within the scope of the invention.
Claims (2)
1. A structural design method of a Fe intercalated graphene oxide two-dimensional adjustable ferroelectric polarization material is characterized by comprising the following steps of: the design method comprises the following steps:
step one, selecting a base material:
selecting two-dimensional graphene oxide as a base material, wherein the graphene oxide is obtained by covalent bonding of O and C in the graphene, and the graphene is C to form a hexagonal honeycomb structure; in the graphene oxide, an O layer is distributed in plane inversion symmetry about a C atomic layer, namely in a C atomic hexagonal honeycomb structure, C atoms in the next neighbor form a covalent bond with O on the same side, namely O and C atoms form a central symmetry structure about a C six-ring, and the system is unpolarized;
step two, designing an intercalation polarization structure:
simulating and constructing an Fe intercalated graphene oxide crystal structure by utilizing material Studio 2019 and VESTA visual structure drawing software, performing preliminary structure optimization after intercalation by utilizing a VASP software program package, and calculating to obtain an optimal adsorption position of Fe;
step three, energy required by polarization inversion:
adopting the method that Fe atoms move up and down along the direction of a c-axis, wherein the direction of the c-axis is perpendicular to the plane direction, calculating and determining the energy barrier which needs to be overcome by polarization inversion due to Fe ions moving in the whole process of moving Fe ions from above the plane to below the plane, and primarily judging the possibility of iron polarization inversion in the two-dimensional material;
and step four, strain application:
fixing the Fe intercalated graphene oxide film on a lattice matched substrate, and applying strain to the film by applying two-dimensional mechanical stress to the substrate;
step five, polarization treatment:
since the stable adsorption positions of Fe ion intercalation are symmetrical about a C atomic layer, the Fe ions are randomly distributed at the positions during intercalation, so that the two-dimensional structure of the intercalation has no macroscopic ferroelectric polarization, and the iron intercalation graphene oxide film fixed on a substrate is subjected to single domain treatment during actual application; placing the film in a stronger constant external electric field for initial polarization to obtain a single-phase single crystal of the single-layer film;
wherein, the optimal adsorption position of Fe is calculated in the second step: the Fe ions are positioned above the center of the C six-ring, and below the centers of three O atoms adjacent to each other above the C plane, and the structure breaks through the spatial symmetry of the graphene oxide and has intrinsic spontaneous polarization;
wherein in the fourth step, the calculation finds that when the two-dimensional biaxial tensile strain reaches 30%, the single layer C 2 O 2 The potential barrier height corresponding to the inversion of a single Fe ion in Fe is only 0.32eV, and the potential barrier height is obviously reduced along with the increase of tensile strain,namely, ferroelectric polarization inversion in the Fe intercalated graphene oxide film can be realized through a small external electric field, and the monolayer film cannot be broken down due to the fact that the external electric field is too strong.
2. The structural design method of the Fe-intercalated graphene oxide two-dimensional adjustable ferroelectric polarization material according to claim 1, which is characterized by comprising the following steps: step five, performing single domain treatment on the film, gradually increasing an electric field in the direction vertical to the surface of the film, and measuring the polarization intensity of the film in situ in real time until the polarization intensity of the film along the direction of the electric field is not increased any more; changing the direction of the electric field, gradually increasing the reverse electric field intensity, measuring the polarization intensity in real time, recording the relation between the electric field intensity and the polarization intensity, and drawing a hysteresis loop.
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