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The paper presents the results of quantum chemical calculations of the change in the lattice energy and the energy parameters of internal motion in a LaF3 nanocrystal during a phase transition from a dielectric state to a highly conducting phase.

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ISSN(P): 2319-4014; ISSN(E): 2319-4022

Vol. 8, Issue 3, Apr - May 2019; 109-116

© IASET

SUPERIONIC LaF3 NANOCRYSTAL

Research Scholar, Institute of Ion-Plasma and Laser Technologies, Tashkent, Uzbekistan, Asia

ABSTRACT

The paper presents the results of quantum chemical calculations of the change in the lattice energy and the

energy parameters of internal motion in a LaF3 nanocrystal during a phase transition from a dielectric state to a highly

conducting phase. Quantum-chemical calculations were done for three nanogrids with linear dimensions of 2.1 × 2.0 ×

2.2 nm, 2.9 × 2.0 × 2.2 nm and 3.5 × 2.0 × 2.2 nm. It has been established that the increment in the magnitude of the

lattice energy in all nanolattices decreases with an increase in the number of disordered fluorine ions in them. It was also

established that the increment of the lattice energy (with an equal number of disordered fluorine ions) is more significant

for nanogrids with a larger number of ions. It is shown that, for all nanogratings, the energy Ea of a single act of

disordering of the anion sublattice with an increasing number of disordered ions decreases from 0.16–0.17 eV in the

dielectric phase to 0.02–0.04 eV in the superionic state.

Article History

Received: 17 Apr 2019 | Revised: 26 Apr 2019 | Accepted: 07 Apr 2019

INTRODUCTION

Superionic (SI) materials form a special class of substances, attracting the attention of a wide range of researchers

for their unusual properties, which are extremely interesting both from the standpoint of the fundamental problems of solid

state physics and physical chemistry and in connection with purely applied aspects [1–3]. In most cases, the conductivity of

typical SI conductors is close to the values characteristic of melts and concentrated solutions of strong electrolytes. So, if

the conductivity of ordinary ionic crystals at temperatures sufficiently far from the melting point, as a rule, does not exceed

σi ≈ 10- 9 S / cm, then the ionic conductivity of good SI conductors is σi ≈ 10–1 - 100 S / cm. Thus, SI materials have mixed

properties: the conductivity of a melt or electrolyte solution on the one hand, and the mechanical strength and elasticity of

a solid body on the other. For this reason, SI materials are often called solid electrolytes. In some respects, these are

materials that fill the gap between liquids and crystals, and the measure of the disorder of the SI lattice of materials can be

controlled with the help of temperature.

In addition to the practical significance of the SI materials, their comprehensive study is a logical continuation of

a number of objects that are becoming increasingly complex to study. From the point of view of physical chemistry, SI

conductors represent an important link in a vast array of electrically conductive materials. Moreover, for a large class of SI

conductors, the transition from the dielectric (DE) state to the highly conducting state often has the character of a phase

transition (PT), which is diffuse in a certain temperature range. The interest of specialists in the study of transport

processes in solids to fluoride-conducting ionic conductors, in particular, to LnF3 (Ln-La, Ce, Pr) crystals, is primarily

www.iaset.us editor@iaset.us

110 V. F. Krivorotov, G. S. Nuzhdov, V. N. Avdievich, B. A. Allaev & F. Hamidov

determined by the wide possibilities of their application in various technical fields. In particular, the SI LnF3 crystals are

extremely perspective as a material for working modules in high-capacity solid-state batteries, electrochromic displays,

gas-analytical sensors, and various micro-ion devices.

The use of modern film technologies allows changing and improving the physicochemical properties of ion-

conducting materials, as well as significantly expanding the field of application of such materials. In this case, an important

factor in various technical applications is the fact that LnF3 crystals possess a sufficiently high specific conductivity in the

region of room temperature. The anion sublattice of LnF3 crystals consists of three types of structurally nonequivalent

fluorine ions, called F1, F2, and F3. The process of active disordering of the anion sublattice, for example, in a LaF3 crystal,

is observed in the range of 240–540 K and continues until the melting point of the material. Moreover, in the range of 240–

320 K, the lattice disordering is determined by active motion in the F1 sublattice. The remaining fluorine ions F2 and F3

together with metal cations form anion – cation (base) planes in the lattice structure. The sublattices of these ions are more

conservative and disordered at temperatures in excess of 360–420 K.

An analysis of recent work has shown that directly describing the dependence of the energy parameters of internal

motion on the degree of disordering of the SI lattice of materials in the framework of classical thermodynamics is rather

difficult [4]. As a rule, the physical approaches and mathematical methods used in this case lead, on the one hand, too

complex mathematical calculations related to the thermally activated nature of the lattice disordering process, and, on the

other hand, to a significant increase in computer simulation time.

At the same time, the problem of describing the magnitude of the energy parameters of intracellular motion

depending on the degree of disordering of one of the sublattices can be largely successfully solved nowadays on the basis

of modern software. We note in particular the fact that modern computer simulation makes it possible at the microscopic

(atomic) level to investigate and describe in detail the features of the motion of individual ions in a wide temperature range

(both in the DE phase and in the SI state). Moreover, quantum – chemical modeling of the process of moving ions in a

disordered sublattice in some cases can provide new, more detailed information about the intracellular movement of ions,

which is very difficult or impossible in laboratory experiments. For this reason, the data obtained by means of the quantum

chemical simulation are, as a rule, original, describing in detail the atomic picture of internal motion in the lattice of the

conductor under investigation.

For quantum – chemical calculations of the energy parameters of intracellular motion of fluoride ions for

nanoscale LaF3 lattices, we used the package of quantum – chemical programs MOPAC 2016 [5]. For calculating the

lattice energy of bonds and the energy parameters of the internal motion we used the semi-empirical method PM7 with an

extended set of elements, including the elements lanthanum and fluorine. In the process of calculations using quantum –

chemical programs, the bond energy of a system of particles (ions) was determined by a large number of “energy”

members, which are determined by interactions of various types (core – core, electron shell – core, etc.) taking into account

both long-range and short-range potentials . Thus, the energy of interparticle bonds in LaF3 nano-lattices, in solid-state

physics called the lattice energy of cohesion, was calculated in a physically sufficiently adequate approximation. The

methodology for such model calculations is described in detail, for example, in [6].

As already noted, the unusual physicochemical properties of SI materials make them attractive objects for

widespread use in a wide variety of applied fields of physics, chemistry, and technology. For example, instrument

electronics is characterized by the complexity and miniaturization of working modules using modern film technologies.

Energy Parameters of Intracellular Movement of Fluoride Ions in a Superionic LaF3 Nanocrystal 111

Therefore, electronic instrument-making is actively expanding its functionality with new technical devices based on

unconventional physical approaches and principles. However, it is obvious that the problem of a significant reduction in

the size and mass of such devices can be solved through the use of both new technological methods and new materials, in

particular, solid electrolytes as a functional material with a wide range of unusual properties [7, 8]. It is also obvious that

further expansion of the applied use of SI materials is possible only on the basis of a deep and successful study of physical

phenomena that determine the patterns of high internal mobility and the atomic picture of internal motion in the lattice of a

solid body. In terms of the practical use of SI conductors, it should also be noted that the processes occurring in nanoscale

systems form the basis of modern and promising solid-state nanotechnologies. In the context of the above, it is interesting

to study and predict the properties of nanostructured materials based on the study of some characteristic parameters in

nanoscale SI conductors with the number of particles from several tens to 1100-1200.

In the present work, based on the data of computer simulation of structural disorder in a nanosized LaF3 crystal in

a wide temperature range, including a phase transformation region, the change in some energy parameters determining the

efficiency of intracellular movement of fluorine ions is investigated. In particular, the dependence of the magnitude of

these parameters on the degree of disordering of the anion sublattice during the transition from the DE to superion state is

described and analyzed.

For model calculations and a detailed description of the physical picture of changes in the lattice binding energy

and the specific energy Ea of the disordering of the anion sublattice, three SI nanogrids of LaF3 crystals with linear

dimensions of 2.1 × 2.0 × 2.2 nm (720 ions), 2.9 × 2.0 × 2.2 nm (960 ions) and 3.5 × 2.0 × 2.2 nm (1200 ions). Quantum-

chemical calculations of the features of the disordering process of the LaF3 anion sublattice were carried out for the case of

gradual (step-by-step) disordering of the F1 sublattice in the studied nanolattices. The process of thermal disordering of the

anion sublattice was simulated on the F1 sublattice, whose ions make up ~ 70% of the total number of fluoride ions.

Quantum-chemical calculations were carried out for all nanolattices with a consistent increase in the number of F1

ions transferred to the nearest interstices. When modeling the process of thermal disordering of the anion sublattice, the

number of ions transferred to the internode increased with each successive step for all nanogrids in the same way - by ten

disordered F1 ions. At the same time, all ten fluorine ions moved in the interstices shifting in the XY plane. An increase in

the “quasi-liquid” array of ions in the F1 sublattice was carried out by attaching to it (at the next quantum chemical

calculation) ten more disordered ions. In Figure Figure 1 shows the dependences of the change (increments along the

ordinate axis) of the ∆E value of the lattice binding energy for three LaF3 nanolattices, due to the sequential increase in the

number of disordered F1. The abscissa axis shows the numbers of such disordered ions. The zero value of the lattice energy

on the ordinate axis corresponds to a fully ordered lattice when all the ions are located in their site positions. The

increments ∆E of the bond energy in such a nanolattice are absent. The first step corresponds to the formation of arrays of

ten disordered F1 ions in all nano-lattices. In this case, the bonding energy in nanolattices increases by ~ 1.7–1.8 eV

(Figure 1). The second step is associated with the formation of ten more disordered F1 ions in each nanolattice, which

doubles the already existing arrays of point defects. In this case, the total increment of the lattice energies in the three

nanolattices lies in the interval ~ 3.1–3.3 eV. The numbers 1, 2, and 3 with the curves of variation of the lattice energies

correspond to those containing 720, 960, and 1200 ions.

www.iaset.us editor@iaset.us

112 V. F. Krivorotov, G. S. Nuzhdov, V. N. Avdievich, B. A. Allaev & F. Hamidov

Figure 1: Changes in the Lattice Energy in the SI Nano-Lattices of the LaF3 Conductor Depending on the Number

of Disordered Ions F1

It can be clearly seen that each next step inside any of the three curves increases the energy of the nanogrids by an

ever smaller value. Moreover, the increment of the lattice energy ∆E is most significant for nano-grids with a larger

number of ions. So, for a nanolattice with the number of ions 1200 (curve 3), the increments of its energy ∆Е3 from pitch

to pitch significantly exceed the corresponding increments of energy ∆Е1 and ∆Е2 for nano-grids containing 720 and 960

ions. Thus, the lattice binding energy (as expected) is the largest for a nano-lattice with the largest number of ions. From

which it follows that in the studied nano-lattices with the corresponding changes in the number of disordered ions, the

∆E3> ∆E2> ∆E1 ratios are fulfilled.

It is equally interesting to consider the change in the specific energy Ea of the disordering of the F1 sublattice as a

function of the number of disordered fluorine ions and the number of ions in the nano-lattice. Figure 2 shows such changes

in the energy Ea for the three LaF3 nano-grids. Analysis of curves 1, 2, and 3, which (as before) correspond to nano-lattices

with the number of ions 720, 960 and 1200, allows us to draw the following conclusion. The specific energy Еа of

disordering of one F1 ion with an increasing number of disordered F1 ions gradually decreases in all nanolattices from ~

0.16–0.17 eV in the DE phase (when the fraction of disordered F1 is minimal and not more than ten) to 0.02–0.04 eV in the

SI state, when the number of disordered fluorine ions is tens. Moreover, the smallest energy value of Ea = 0.02 eV was

obtained for a lattice of 1200 ions, containing the largest number of disordered F1 ions (90 ions of this type). Accordingly,

the “highest” energy value Ea = 0.04 eV was obtained in the SI phase for curve 1, corresponding to the lattice with the total

number of ions 720, in which 50 F1 ions are disordered (Figure 2).

Energy Parameters of Intracellular Movement of Fluoride Ions in a Superionic LaF3 Nanocrystal 113

0.18

0.16

0.14

0.12

Energy, eV

0.10

0.08

0.06

0.04 1

0.02 2

3

0.00

0 20 40 60 80 100

Number of disordered ions of fluorine

Figure 2: Change in the Specific Energy Ea of Disordering of the F1 Sublattice as a Function of the Number of

Disordered Fluoride Ions in the LaF3 Nano-Lattices

Such a decrease in the specific energy Ea is determined by the fact that when a disordered ion is formed in an

array of already existing interstitial anion – anion vacancy defects, the effect on the energy parameters of the so-called

collective interactions in the quasi-liquid sublattice should be taken into account [4]. Such collective interactions determine

the characteristics of the process of disordering of one of the SI sublattices of the conductor; in particular, they

significantly reduce the value of energy parameters in certain crystallographic directions. Thus, an analysis of the results of

quantum chemical calculations for MOPAC 2016 shows that when there is a relatively large number of disordered fluorine

ions in the F1 sublattice (SI phase), the energy parameters in some crystallographic directions decrease by 4–8 times

compared to their values in DE phase.

From Figure 2 it also follows that with an increase in the fraction of disordered fluorine ions and a decrease, in

this connection, of the energy parameters, in particular, the activation parameter Ea, these parameters take a number of

intermediate values: 0.16, 0.14, 0.12, 0.10, 0.08 and 0.06 eV. This series of Ea values, converging in the SI phase to the

minimum values of three grades of 0.04 eV (curve 1), 0.03 eV (curve 2) and 0.02 eV (curve 3), were obtained for the first

time for the SI crystal of LaF3.

Moreover, the parameter Ea varies from ~ 0.14 eV (curve 1), ~ 0.16 eV (curve 2) and ~ 0.17 eV (curve 3) in the

DE phase to values ~ 0.02 - 0.04 eV in the SI state is almost linear. From this circumstance, it can be concluded that if the

increase in the number of disordered ions in the crystal lattice of the crystal occurs in a linear fashion, then the change in

the activation energy Ea will correspond to a certain linear function. It can also be expected that if the change in the number

of disordered ions with increasing temperature is described by another more complex function (for example, as in Figure 3

taken from [9]), then the change in the energy Ea in the FP region will follow a more complex law.

It should be noted that the obtained values of the activation parameter Ea are well correlated with the values of the

energy Ea of the single act of disordering of the F1 sublattice obtained in a completely different way - for example, from

experimental data on Raman scattering [10] or direct quantum chemical calculations of the parameter Ea - single act

disordering of the F1 sublattice in the DE and SI phases (the results of such calculations are shown in Figure 4 of [11]).

Figure 4 shows that the parameter Еа, which determines the change in the energy of the lattice when the F1 ion moves to

www.iaset.us editor@iaset.us

114 V. F. Krivorotov, G. S. Nuzhdov, V. N. Avdievich, B. A. Allaev & F. Hamidov

Figure 3: Temperature Dependence of the Concentration of Disordered F1 Ions in the Region of Phase

Transformations in LaF3

Figure 4: Profiles of Potential Reliefs in the LaF3 Nano-Lattice of 1200 Ions with a Thermally Activated

Displacement of the F1 Ion From the Node To the Nearest Interstitial Site: Curve 1 - Dielectric Phase (T <Tc),

Curve 2 - Superionic Phase (T ≥Tc).and 0.03 eV (curve 2 for the SI phase). It is clearly seen that these values almost

coincide with the values of Ea for the nano-grids in the DE and SI phases, shown above in Figure 2

CONCLUSIONS

In the work, quantum chemical calculations based on the MOPAC 2016 software package show a consistent

change in the energy parameters that determine the efficiency of fluoride ion transfer in the SI nano-lattice of the LaF3

crystal, depending on the degree of disordering of the anion sublattice. It should be particularly noted that the new data

obtained through quantum – chemical calculations, as a rule, reveal and describe the microscopic picture of the features of

thermally activated processes, in particular, the processes of mass transfer of fluoride ions in the SI lattice of the LaF3

conductor.

Energy Parameters of Intracellular Movement of Fluoride Ions in a Superionic LaF3 Nanocrystal 115

It is also obvious that the conclusions obtained in the work can be attributed to the entire SI series of LnF3 crystals

with a slight change in the numerical values of the corresponding energy parameters due to the so-called lanthanoid

compression of the lattice parameters.

The model schemes developed by the authors for obtaining microscopically small values (on the order of

hundredths of eV) of energy parameters are based on positions widely known in crystal physics. Therefore, the model

approaches used in the work are applicable to the description of the energy characteristics of internal motion in an

extensive SI class of conductors with diffuse phase transitions.

The authors are grateful to professor E.V. Charnaya at the Research Institute of Physics. St. Petersburg State

University and professor S.Z.Mirzaev for the useful discussion of the results. The research was supported by the State

Program for Fundamental Research of the Republic of Uzbekistan (Grant OT-F2-56)

REFERENCES

1. Physics of Superionic Conductors / Ed. M.B. Salamon. Springer–Verlag, Berlin–Heidelberg–New York. 1979. 255

p.

2. Fast Ion Transport in Solids. Electrodes and Electrolites / Eds. P. Vaschishta, J.N. Mundy, G.K. Shenoy – New

York, Amsterdam, Oxford: North Holland. 1979. 744 p.

3. Solid ionic / Ivanov-Shits, A.K., Murin. I.V. / St. Petersburg University/ 2000. V. 1. 615 p.

4. Superionic conductros / Yu.Y. Gurevich, Yu.I. Charcats. / Moscow: Science. 1992. 244 p.

5. MOPAC 2016, James J. P. Stewart, Stewart Computational Chemistry, Colorado Springs, CO, USA,

http://openmopac.net.

7. Nanotechnology: physical chemistry of nanoclusters, nanostructures and nanomaterials / I.P. Suzdalev / Moscow:

KomKniga. 2006. 592 p.

Precursor,International Journal of Applied and Natural Sciences(IJANS),Volume 2, Issue 1, February-March

2013, Pp 9-16.

10. V.F. Krivorotov, P.K. Habibulaev, А.А. Frdman and other //Inorganic materials. 2010. V. 46, № 11. p. 1387–

1391.

11. V.F. Krivorotov, P.K. Habibulaev, А.А. Fridman and other // Inorganic materials. 2010. V. 46. № 7. p. 875 – 879.

12. V.F. Krivorotov, G.S. Nuzhdov, А.А. Fridman and other // Electrochemistry. 2013, V. 49. № 12. p. 1286-1291.

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