CN113745400A - Structural design of two-dimensional adjustable ferroelectric polarization material based on Fe intercalated graphene oxide - Google Patents
Structural design of two-dimensional adjustable ferroelectric polarization material based on Fe intercalated graphene oxide Download PDFInfo
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Abstract
The invention discloses a structural design of a two-dimensional adjustable ferroelectric polarization material based on Fe intercalated graphene oxide, which comprises the following design schemes: the method comprises the following steps of selecting a base material, designing an intercalation polarization structure, using energy required by polarization inversion, and performing polarization treatment, wherein the graphene oxide realizes a simple structure of ferroelectric information storage, and has the advantages of low dimensionality, small size and small applied electric field required by the inversion polarization; different from the ferroelectric polarization in other two-dimensional materials lying in a plane, the ferroelectric polarization of the structure is vertical to the surface of the single-layer film, and an external electric field is easy to read and write data; the invention has the advantages of simple structural design, convenient operation, easy processing, greatly improved integration level and the like, and can reduce the external electric field required for realizing the ferroelectric information storage along with the increase of the strain within a certain range, thereby having very considerable application prospect.
Description
Technical Field
The invention belongs to the field of dielectric material application, and particularly relates to a structural design of a two-dimensional adjustable ferroelectric polarization material based on Fe intercalated graphene oxide.
Background
The dielectric material with ferroelectric property has very wide development prospect in the application aspect of multifunctional devices such as sensing, information storage, photoelectricity and the like 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 and the rapid development of microelectronic integration technology, electronic devices tend to be miniaturized, integrated and multifunctional more and more, but the traditional ferroelectric materials are affected by size limitation and surface depolarization effect due to the characteristics of bulk materials, and are difficult to meet the increasingly developed requirements of modern technology, so that a new research hotspot is formed by searching and designing suitable ferroelectric materials with excellent properties and junctions with adjustable and controllable ferroelectric properties in the field of low-dimensional materials.
In recent years, with the first principles and other theoretical tools, we have succeeded in predicting and designing some two-dimensional materials and structures with excellent ferroelectric properties, such as: in a single layer of MX (M = Ge, Sn; X = S, Se), In2Se3Reversible in-plane ferroelectric polarization in the material; 1T-MoS2Lamellar CuIn2P6Out-of-plane ferroelectricity which can exist stably at room temperature; while a single layer VOX2（X=F, Cl, Br, I）、Hf2VC2F2The material is a two-dimensional multiferroic material with magnetism and in-plane ferroelectricity coexisting; meanwhile, two-dimensional ferroelectric materials which exist stably at room temperature have also been successfully prepared from experimental techniques, for example, Chang et al successfully prepare SnTe thin films with stable performance by using molecular beam epitaxy technique, and prove the existence of ferroelectricity.
Graphene is the thinnest two-dimensional nanomaterial in the world composed of single-layer carbon atoms, which is discovered so far, has excellent optical, electrical and mechanical properties which are not possessed by common carbon materials, and the properties of graphene can be effectively regulated and modified by modification, magic angle, doping, strain, intercalation methods and the like. For example, researches find that graphene modified by hydroxyl is a two-dimensional organic material with multiferroic property, and ferroelectric polarization of the graphene is perpendicular to the surface of the graphene due to structural transformation from a central symmetric structure to a space inversion symmetry-breaking structure.
The graphene oxide has a large number of oxygen-containing functional groups on the surface, so that the carbon layer has negative charges, cations are easily attracted into the interlayer, and the interlayer spacing is enlarged, which provides favorable conditions for loading of polymers and inorganic nanoparticles. Fe ions have the characteristics of large spontaneous magnetic dipole moment, large spin coupling among magnetic moments, ion charge performance and the like, and have wide application in practical production.
Disclosure of Invention
The invention aims to solve the problems and provides a microstructure for realizing ferroelectric information storage and regulation through Fe intercalation and external strain; the structure not only has the minimum information storage unit, but also has the characteristics of large polarization intensity, polarization vertical to the surface of the film, low polarization overturning potential barrier, easy regulation and control through an external electric field and the like.
In order to achieve the purpose, the technical scheme of the invention is realized as follows:
a structural design of a two-dimensional adjustable ferroelectric polarization material based on Fe intercalated graphene oxide 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 covalently bonding O and C in the graphene, and the graphene is C to form a hexagonal honeycomb structure; the O layers in the graphene oxide are distributed in plane inversion symmetry relative to the C atomic layer, namely in a C atom hexagonal honeycomb structure, the next adjacent C atoms and O form covalent bonds at the same side, namely the O and C atoms form a central symmetry structure relative to a C six-ring, and the system is nonpolarized;
step two, designing an intercalation polarization structure:
simulating and constructing a Fe intercalation graphene oxide crystal structure by using Materials Studio 2019 and VESTA visual structure drawing software, carrying out primary structure optimization after intercalation by using a VASP software program package, and calculating to obtain the optimal adsorption position of Fe;
step three, polarizing the energy required for turning over:
the method comprises the steps that the position of an Fe atom is moved up and down along a c-axis direction, the c-axis direction is perpendicular to a plane direction, the energy barrier which needs to be overcome due to polarization overturning caused by Fe ion movement in the whole process that the Fe ion moves from the upper side to the lower side of the plane is calculated and determined, and the possibility of iron polarization overturning in the two-dimensional material is preliminarily judged;
step four, strain application:
the Fe intercalated graphene oxide film is fixed on a substrate matched with a crystal lattice, and a strain is applied to the film by applying a two-dimensional mechanical stress to the substrate.
Step five, polarization treatment:
because the positions of stable adsorption of the Fe ion intercalation are symmetrical about the C atomic layer, the Fe ion is randomly distributed at the positions during the intercalation, so that the two-dimensional structure of the intercalation is probably free from macroscopic ferroelectric polarization, and the iron intercalation graphene oxide film fixed on the substrate is subjected to single domain treatment during practical application; the film is put in a strong constant external electric field for initial polarization, and the obtained single-layer film is single-phase single crystal.
Further, the optimal adsorption position of Fe is calculated in the second step: the Fe ions are located above the center of the C-shaped six-ring and below the centers of three adjacent O atoms above the C plane, and the structure breaks the space symmetry of the graphene oxide and has intrinsic spontaneous polarization.
Further, in the third step, because the radius of the Fe ion is far greater than the radius of the C atom, and the ionic combination between the Fe ion and the O ion, it is found through calculation that the energy barrier to be overcome when the Fe ion crosses the center of the C ring is far higher than the field intensity range of a general external electric field.
Further, in the fourth step, it was found by calculation that the monolayer C was formed when the biaxial tensile strain in two dimensions reached 30%2O2In FeThe potential barrier height corresponding to the Fe ion overturn is only 0.32 eV, and the potential barrier height is obviously reduced along with the increase of tensile strain, namely, the ferroelectric polarization overturn in the Fe intercalation graphene oxide film can be realized through a very small external electric field, and the single-layer film cannot be broken down due to the fact that the external electric field is too strong.
Further, the fifth step is to perform single domain processing on the film, gradually increase the electric field in the direction perpendicular to the surface of the film, and measure the polarization strength of the film in real time in situ until the polarization strength of the film along the electric field direction is not increased any more; and changing the direction of the electric field, gradually increasing the strength of the reversed electric field, measuring the magnitude of the polarization intensity in real time, recording the relation between the magnitude of the electric field and the polarization intensity, and drawing the hysteresis loop.
The invention provides a structural design of a two-dimensional adjustable ferroelectric polarization material based on Fe intercalated graphene oxide, which enables the graphene oxide to realize a simple structure of ferroelectric information storage, and has the advantages of low dimensionality, small size and small external electric field required by reversal polarization; different from the ferroelectric polarization in other two-dimensional materials lying in a plane, the ferroelectric polarization of the structure is vertical to the surface of the single-layer film, and an external electric field is easy to read and write data; the invention has the advantages of simple structural design, convenient operation, easy processing, greatly improved integration level and the like, and can reduce the external electric field required for realizing the ferroelectric information storage along with the increase of the strain in a certain range, thereby having very considerable application prospect.
Drawings
FIG. 1 is a structural diagram of different sides of an Fe intercalated graphene oxide; wherein (a) is a top view, B-D is a side view, (B) is ferroelectric polarized upwards, (c) is no ferroelectric polarized, and (D) is ferroelectric polarized downwards;
FIG. 2 is a graph of the barrier height (including the inversion of a single Fe ion) of the cell under different strains;
FIG. 3 is a graph of energy versus position of Fe atoms at 30% strain.
Detailed Description
The present invention will be described in further detail with reference to the accompanying drawings and examples.
A structural design of a two-dimensional adjustable ferroelectric polarization material based on Fe intercalated graphene oxide 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 unit, which is low in dimension and small in size, 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 bonded, and O is symmetrically distributed about the center of a C six ring, namely in the C atom hexagonal honeycomb structure, C atoms next to each other and O form covalent bonds on the same side, namely an O layer forms a symmetrical structure about the C atom layer, and the system is free of polarization;
step two, designing an intercalation polarization structure:
the method comprises the steps of simulating and constructing a Fe intercalation graphene oxide crystal structure by using Materials Studio 2019 and VESTA visual structure drawing software, carrying out preliminary structure optimization after intercalation by using a VASP software program package, calculating to obtain the optimal adsorption position of Fe, and finding that Fe ions are located above the center of a C six-ring and below the centers of three adjacent O atoms above a C plane, wherein the structure breaks the space symmetry of graphene oxide and has intrinsic spontaneous polarization as shown in figure 1 specifically;
step three, polarizing the energy required for turning over:
and (3) moving the position of the Fe atom up and down along the direction of a c axis (vertical to a plane), calculating and determining the energy barrier which needs to be overcome due to the polarization overturning caused by the movement of the Fe ion in the whole process of moving the Fe ion from the upper part of the plane to the lower part of the plane, and preliminarily judging the possibility of the polarization overturning of the iron electrode in the two-dimensional material. As the radius of the Fe ions is far larger than that of the C atoms and the ionic combination between the Fe ions and the O ions, the calculation finds that the energy barrier to be overcome when the Fe ions pass through the center of the C ring is far higher than the field intensity range of a common external electric field.
Step four, strain application:
and fixing the graphene oxide film with the Fe intercalation on the substrate, and applying strain to the graphene oxide by applying two-dimensional mechanical stress to the substrate. It was found by calculation that when the two-dimensional biaxial tensile strain reached 30%, the monolayer C2O2Single Fe ion reversal pair in FeThe barrier height should be only 0.32 eV (fig. 2 and 3), which is comparable to the barrier in bulk material PaTiO3, and the barrier height is significantly reduced with increasing tensile strain (fig. 2), i.e. the ferroelectric polarization in the graphene oxide thin film can be switched by a small applied electric field, and the single layer thin film is not broken down due to too strong external electric field.
Step five, polarization treatment:
because the stable adsorption positions of the Fe ion intercalation are symmetrical about the C atomic layer, the Fe ion can be randomly distributed at the positions during the intercalation, so that the two-dimensional structure of the intercalation is probably free from macroscopic ferroelectric polarization, and the film is subjected to single domain treatment before practical application. The film can be placed in a strong constant external electric field for initial polarization, so that the obtained single-layer film is ensured to be single-phase single crystal.
Fig. 1 is a simplified diagram showing the structure of different sides of the Fe intercalated graphene oxide. In the figure, the atom with the smallest diameter is a C atom, the atom with the largest diameter is an Fe atom, the atom with the diameter between the two atoms is an O atom, and as can be seen from the figure, in the six rings of C, one O atom is coordinated above the next adjacent C atom to form a covalent bond, the O forms a planar regular triangular lattice, the other three next adjacent C atoms are covalently coordinated with the O atom below the next adjacent C atom, and the lower O also forms the planar regular triangular lattice. In the poled structure, all Fe ions are located above the center of the C-six ring but below the center of the upper O-ion regular triangular 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 the upper part of the plane to the symmetrical position below the plane without external strain, the required energy is too large, as shown in FIG. 2, the ferroelectric polarization is difficult to turn over. In order to reduce the energy required for ferroelectric switching, 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 switching is only 0.32 eV, and the maximum polarization intensity of the stable state is 1.6 x 10-10C/m, that is, a larger reversal of ferroelectric polarization can be achieved by a smaller applied electric field.
While the foregoing is directed to embodiments and effects of the present invention, it will be appreciated by those skilled in the art that various changes and modifications may be made without departing from the principles of the invention, and it is intended that all such changes and modifications be considered as within the scope of the invention.
Claims (5)
1. A two-dimensional adjustable ferroelectric polarization material structure design based on Fe intercalation graphene oxide is characterized in that: the design scheme 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 covalently bonding O and C in the graphene, and the graphene is C to form a hexagonal honeycomb structure; the O layers in the graphene oxide are distributed in plane inversion symmetry relative to the C atomic layer, namely in a C atom hexagonal honeycomb structure, the next adjacent C atoms and O form covalent bonds at the same side, namely the O and C atoms form a central symmetry structure relative to a C six-ring, and the system is nonpolarized;
step two, designing an intercalation polarization structure:
simulating and constructing a Fe intercalation graphene oxide crystal structure by using Materials Studio 2019 and VESTA visual structure drawing software, carrying out primary structure optimization after intercalation by using a VASP software program package, and calculating to obtain the optimal adsorption position of Fe;
step three, polarizing the energy required for turning over:
the method comprises the steps that the position of an Fe atom is moved up and down along a c-axis direction, the c-axis direction is perpendicular to a plane direction, the energy barrier which needs to be overcome due to polarization overturning caused by Fe ion movement in the whole process that the Fe ion moves from the upper side to the lower side of the plane is calculated and determined, and the possibility of iron polarization overturning in the two-dimensional material is preliminarily judged;
step four, strain application:
fixing the Fe intercalated graphene oxide film on a substrate matched with a crystal lattice, and applying strain to the film by applying two-dimensional mechanical stress to the substrate;
step five, polarization treatment:
because the positions of stable adsorption of the Fe ion intercalation are symmetrical about the C atomic layer, the Fe ion is randomly distributed at the positions during the intercalation, so that the two-dimensional structure of the intercalation is probably free from macroscopic ferroelectric polarization, and the iron intercalation graphene oxide film fixed on the substrate is subjected to single domain treatment during practical application; the film is put in a strong constant external electric field for initial polarization, and the obtained single-layer film is single-phase single crystal.
2. The structural design of the Fe intercalated graphene oxide based two-dimensional adjustable ferroelectric polarization material as claimed in claim 1, wherein: calculating the optimal adsorption position of Fe in the step two: the Fe ions are located above the center of the C-shaped six-ring and below the centers of three adjacent O atoms above the C plane, and the structure breaks the space symmetry of the graphene oxide and has intrinsic spontaneous polarization.
3. The structural design of the Fe intercalated graphene oxide based two-dimensional adjustable ferroelectric polarization material as claimed in claim 1, wherein: in the third step, because the radius of the Fe ions is far larger than that of the C atoms and the ionic combination between the Fe ions and the O ions, the calculation finds that the energy barrier to be overcome when the Fe ions pass through the center of the C ring is far higher than the field intensity range of a common external electric field.
4. The structural design of the Fe intercalated graphene oxide based two-dimensional adjustable ferroelectric polarization material as claimed in claim 1, wherein: in the fourth step, the calculation shows that when the two-dimensional biaxial tensile strain reaches 30%, the single layer C2O2The potential barrier height corresponding to the turnover of a single Fe ion in Fe is only 0.32 eV, and the potential barrier height is obviously reduced along with the increase of tensile strain, namely, the ferroelectric polarization turnover in the Fe intercalation graphene oxide film can be realized through a very small external electric field, and the single-layer film cannot be broken down due to the fact that the external electric field is too strong.
5. The structural design of the Fe intercalated graphene oxide based two-dimensional adjustable ferroelectric polarization material as claimed in claim 1, wherein: performing single domain treatment on the film, gradually increasing the electric field in the direction vertical to the surface of the film, and measuring the polarization strength of the film in real time in situ until the polarization strength of the film in the direction of the electric field is not increased any more; and changing the direction of the electric field, gradually increasing the strength of the reversed electric field, measuring the magnitude of the polarization intensity in real time, recording the relation between the magnitude of the electric field and the polarization intensity, and drawing the hysteresis loop.
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| US20110170330A1 (en) * | 2008-09-23 | 2011-07-14 | National University Of Singapore | Graphene Memory Cell and Fabrication Methods Thereof |
| WO2013029094A1 (en) * | 2011-08-29 | 2013-03-07 | Monash University | High performance graphene oxide electromechanical actuators |
| CN104718246A (en) * | 2012-10-09 | 2015-06-17 | 沙特基础工业公司 | Graphene-based composite materials, method of manufacture and applications thereof |
| CN110155989A (en) * | 2019-05-28 | 2019-08-23 | 淮阴师范学院 | A kind of batch large area preparation method of two-dimensional material film |
| US20210111401A1 (en) * | 2018-04-18 | 2021-04-15 | Brno University of Technology | Alkali and/or alkaline earth ion- sulfur battery |
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| US20110170330A1 (en) * | 2008-09-23 | 2011-07-14 | National University Of Singapore | Graphene Memory Cell and Fabrication Methods Thereof |
| WO2013029094A1 (en) * | 2011-08-29 | 2013-03-07 | Monash University | High performance graphene oxide electromechanical actuators |
| CN104718246A (en) * | 2012-10-09 | 2015-06-17 | 沙特基础工业公司 | Graphene-based composite materials, method of manufacture and applications thereof |
| US20210111401A1 (en) * | 2018-04-18 | 2021-04-15 | Brno University of Technology | Alkali and/or alkaline earth ion- sulfur battery |
| CN110155989A (en) * | 2019-05-28 | 2019-08-23 | 淮阴师范学院 | A kind of batch large area preparation method of two-dimensional material film |
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