First-principles calculations of physical properties of crystals
Prediction of physical properties of materials based only on their chemical
composition has long been an intriguing task. In 1929 Paul Dirac wrote:
"The fundamental laws necessary for the mathematical treatment of a large
part of physics and the whole of chemistry are thus completely known, and
the difficulty lies only in the fact that application of these laws leads to
equations that are too complex to be solved".
Unprecedental success in the development of computer hardware and software
enables now to perform the first-principles (ab initio) calculations
with an accuracy comparable with that obtained in experiment. These approaches
enable also to predict the behavior of materials in extreme conditions (for
example, at very high pressures inaccessible in laboratory conditions), to
study dangerous (radioactive, explosive) materials. They are very useful in
predicting new materials with interesting properties, which have never been
synthesized. Moreover, the first-principles calculations enable to improve
our understanding of physical phenomena occurring in known materials. The
Nobel Prizes awarded to Robert S. Mulliken (1966), Walter Kohn and John Pople
(1998) can be regarded as acknowledgment of their seminal contribution to
the development of first-principles methods in physics, chemistry, and
materials science.
The main interests of Prof. Lebedev's
group are physical properties of crystals exhibiting structural instability,
in which different phase transitions (including the ferroelectric one) can
appear. Crystals of the perovskite family are the examples. One of the goal
of these studies is the search for new off-center
impurities, which can induce phase transitions in incipient
ferroelectrics. Another very interesting objects for investigations, which
are studied now, are the ferroelectric superlattices.
The calculations performed in our laboratory are based on the density
functional theory (DFT) and use the plain-wave basis and atomic structure
described with pseudopotentials. The calculations include finding of the
equilibrium structure (the unit cell parameters, atomic positions),
calculations of the lattice dynamics, the band structure and density of
states, comparison of energies of different phases, computation of spontaneous
polarization, the dielectric, piezoelectric, and elastic tensors, the
second-order nonlinear optical susceptibilities, the mixing enthalpies
of solid solutions. The pressure effect on the phase transitions is also
studied.
As any first-principles calculations are extremely time-consuming, to
perform these calculations it is advantageous to use parallel computing,
in which calculations of the electronic structure at different k
points of the Brillouin zone are executed independently and on different
cores of a computer cluster. This speeds up the calculations considerably.
The times when first-principles calculations were carried out on personal
computers probably have gone away.
The computer cluster, which works under 64-bit Linux operating system and
has 10 nodes with dual-core Intel E8200, E8400, and quad-core Intel i5-760
processors (48 Gbytes of
distributed RAM, 2 TByte of disk memory, peak performance of 270 Gflops),
is used in our laboratory to perform first-principles calculations. OpenMPI
protocol and Gigabit Ethernet are used to organize the communications in
the cluster. The most time-consuming calculations are performed on two
largest supercomputers in Russia,
SKIF-MGU supercomputer
("Chebyshev") and
Lomonosov
supercomputer.
Selected publications:
- A.I. Lebedev. Ab initio calculations of phonon spectra in ATiO3
perovskite crystals (A = Ca, Sr, Ba, Ra, Cd, Zn, Mg, Ge, Sn, Pb). --
Physics of the Solid
State 51, 362 (2009);
e-print arXiv:1305.0240 (2013);
[local copy].
- A.I. Lebedev. Ferroelectric phase transition in orthorhombic
CdTiO3: first-principles studies. --
Physics of the Solid
State 51, 802 (2009);
e-print arXiv:1507.06658 (2015);
[local copy].
- A.I. Lebedev. Ferroelectric phenomena in CdSnO3:
A first-principles study. --
Physics of the Solid
State 51, 1875 (2009);
e-print arXiv:1601.01472 (2016);
[local copy].
- A.I. Lebedev. Ab initio study of dielectric, piezoelectric, and elastic
properties of BaTiO3/SrTiO3 ferroelectric
superlattices. --
Physics of the Solid
State 51, 2324 (2009);
[local copy].
- A.I. Lebedev. Ground state and properties of ferroelectric superlattices
based on crystals of the perovskite family. --
Physics of the Solid
State 52, 1448 (2010);
[local copy].
- A.I. Lebedev. Ground-state structure of KNbO3/KTaO3
superlattices: Array of nearly independent ferroelectrically ordered planes. --
Physica Status Solidi B
249, 789 (2012);
e-print arXiv:1102.1001 (2011);
[local copy].
- A.I. Lebedev. Dielectric, piezoelectric, and elastic properties of
BaTiO3/SrTiO3 ferroelectric superlattices from first
principles. -- J. Adv.
Dielectrics 2, 1250003 (2012);
e-print arXiv:1105.5828 (2011);
[local copy].
- A.I. Lebedev. Quasi-two-dimensional ferroelectricity in
KNbO3/KTaO3 superlattices. --
Physics of the Solid
State 53, 2463 (2011);
[local copy].
- A.I. Lebedev. Ferroelectricity and pressure-induced phase transitions in
HgTiO3. --
Physics of the Solid
State 54, 1663 (2012);
[local copy].
- A.I. Lebedev. First-principles study of ferroelectricity and pressure-induced
phase transitions in HgTiO3. --
Phase Transitions
86, 442 (2013);
e-print arXiv:1203.2370 (2012).
- A.I. Lebedev. Crystal structure and properties of barium thorate BaThO3
from first principles. --
J. Alloys and Compounds
580, 487 (2013);
e-print arXiv:1302.5614 (2013).
- A.I. Lebedev. Properties of BaTiO3/BaZrO3 ferroelectric
superlattices with competing instabilities. --
Physics of the Solid
State 55, 1198 (2013);
e-print arXiv:1304.7596 (2013);
[local copy].
- A.I. Lebedev, I.A. Sluchinskaya. Combined first-principles and EXAFS study of
structural instability in BaZrO3. --
Physics of the Solid
State 55, 1941 (2013);
e-print arXiv:1304.6359 (2013);
[local copy].
- A.I. Lebedev. Band offsets in heterojunctions between cubic perovskite oxides. --
Physics of the Solid State
56, 1039 (2014);
e-print arXiv:1401.1157 (2014);
[local copy].
- A.I. Lebedev. Ferroelectric properties of RbNbO3 and RbTaO3. --
Physics of the Solid State
57, 331 (2015);
e-print arXiv:1501.00670 (2015);
[local copy].
- M.A. Terekhin, V.N. Makhov, A.I. Lebedev, I.A. Sluchinskaya. Effect of local
environment on crossluminescence kinetics in SrF2:Ba and CaF2:Ba solid solutions. --
Journal of Luminescence 166,
137 (2015);
e-print arXiv:1506.02325 (2015).
- A.I. Lebedev. Phase transitions and metastable states in stressed SrTiO3 films. --
Physics of the Solid State
58, 300 (2016).
- A.I. Lebedev. Metastability effects in strained and stressed SrTiO3 films. --
J. Adv. Dielectrics 6, 1650016
(2016);
e-print arXiv:1509.00902 (2015).
- A.I. Lebedev. Nonlinear optical properties of undoped and doped with Zr and Nb
KTiOPO4 crystals. --
Bulletin of the Russian Academy
of Science: Physics 80, 1038 (2016);
e-print arXiv:1610.02654 (2016).
- I.A. Sluchinskaya, A.I. Lebedev. An experimental and theoretical study of Ni impurity
centers in Ba0.8Sr0.2TiO3. --
Physics of the Solid State 59,
1512 (2017);
e-print arXiv:1708.03016 (2017).
- A.I. Lebedev. Lattice dynamics of quasi-two-dimensional CdSe nanoplatelets and their
Raman and infrared spectra. --
Phys. Rev. B 96, 184306 (2017);
e-print arXiv:1707.05444 (2017).
- A.I. Lebedev. Ferroelectricity and piezoelectricity in monolayers and nanoplatelets of SnS. --
J. Appl. Phys. 124, 164302 (2018);
e-print arXiv:1805.08437 (2018).
- A.I. Lebedev. Negative thermal expansion in CdSe quasi-two-dimensional nanoplatelets. --
Phys. Rev. B 100, 035432 (2019);
e-print arXiv:1908.04581 (2019).
- I.A. Sluchinskaya, A.I. Lebedev. Electronic and magnetic properties of structural defects in SrTiO3(Co). --
J. Alloys and Compounds 820, 153243 (2020);
e-print arXiv:1912.10711 (2019).
- A.I. Lebedev. Piezoelectric properties of II-IV/I-V and II-IV/III-III ferroelectric perovskite superlattices. --
Ferroelectrics 567, 89 (2020).
- A.I. Lebedev. Piezoelectric properties of ferroelectric perovskite superlattices with polar discontinuity. --
Computational Materials Science 188,
110113 (2021);
e-print arXiv:2012.08817 (2020).
- A.I. Lebedev, B.M. Saidzhonov, K.A. Drozdov, A.A. Khomich, R.B. Vasiliev. Raman and infrared studies of CdSe/CdS
core/shell nanoplatelets. --
Journal of Physical Chemistry C 125, 6758 (2021).
- A.I. Lebedev. First-principles calculations of vibrational spectra of CdSe/CdS superlattices. --
Physics of the Solid State 64, 2312 (2022);
e-print arXiv:2110.14760 (2021).
- I.A. Sluchinskaya, A.I. Lebedev. On the possibility of incorporation of the iron impurity into A sites in SrTiO3. --
Physics of the Solid State 64, 345 (2022);
e-print arXiv:2204.12775 (2022).
- A.I. Lebedev. Spontaneous strain in quasi-two-dimensional Janus CdSe nanoplatelets and its microscopic mechanisms. --
Journal of Physical Chemistry C 127, 9911 (2023);
e-print arXiv:2405.11679 (2024).
- A.I. Lebedev. A new approach to analyzing the spinor wave functions: Effect of strain on the electronic
structure and optical transitions in bulk CdSe. -- e-print
arXiv:2307.15534 (2023).
Physics of Semiconductors division