Imperial College, Department of Materials

Literature Review: The Metal-Insulator

Transition in Iridium Oxides
Gabriel Sonnet
(Dated: February 13th, 2013)

Introduction

symmetry, dxy dxz and dyz orbitals experience less

Iridates are 5d transition metal oxides (TMOs that

repulsion than the dz2 and dx2-y2 and are thus lower in

exhibit metal-insulator transitions. The 4+ oxidation

energy. The former make up the t2g band, whilst the

state

electron

latter become the eg band and are separated by an

configuration is dominant in the iridates although

energy gap. The strong SOC described by Kim et al.,

there have been some reported instances of mixed

causes a t2g band split (fig. 1c). The narrow Jeff =

valency1. The metal-insulator transition observed in

band is further split by a low on-site Coulombic

the iridium oxides has been rationalised by

repulsion between the electrons. The result is the

consideration of Mott physics and the Hubbard

formation of a Mott gap between the Jeff = Upper

Hamiltonian2. The criterion for the formation of a

and Lower Hubbard bands (fig .1d) - a Mott

Mott insulating state is for the on-site Coulombic

insulator2. Arita et al. preferred in a recent paper to

repulsion U in the system to be much greater than

classify Sr2IrO4 (and Ba2IrO4) as Slater insulators,

the band width W (U>>W).

due

associated

with

d5

valence

the

paramagnetic

metal

transitions

they

undergo above their Nel temperatures .

5

U is reduced in 5d TMOs in comparison to their 3d

analogues3, so it could be deduced that a 5d TMO
such as Sr2IrO4, should be metallic. However, this
has been shown not to be the case resistivity
measurements by Crawford et al. indicated that
Sr2IrO4 is an insulator4. This discrepancy between
theory and experiment was resolved by Kim et al.2.
In their paper, they attribute this nonconcurrence to
a novel, competing interaction: strong, relativistic
spin-orbit coupling (SOC) of the t2g band comprising
the 5d states, causes this band to split into half-filled
Jeff = and filled Jeff = 3/2 bands (fig. 1c), where J eff is
the effective angular momentum quantum number2.
Before explaining how this contributes to an
insulating state, some crystal field theory will be
rationalised.
In Sr2IrO4, crystal field splitting of the 5d subshell
into non-degenerate eg and t2g levels occurs, due to
the varying repulsion of the 5d orbitals with respect
to the oxygen ligands in the IrO6 octahedra. In Oh

Figure 1: Kim et. al. provide this figure in their paper2 to

illustrate the band formation leading to a Mott insulating
state in Sr2IrO4.

Imperial College, Department of Materials

from this type of pressure based metal-insulator

transition.
To contrast with Sr2IrO4, a Mott insulator, IrO2 is
considered. A recent paper by Kahk et al. concludes
that IrO2 is a metal, even though strong spin-orbit
coupling and on-site electron-electron repulsion
occur. However, because of the deviation from Oh
symmetry to D2h symmetry in rutile IrO2 (space
group P42/mnm, see table 3) there are strong orbitaloverlap effects. This, along with crystal field
splitting dominate over the on-site Coulombic
repulsion and SOC, which therefore results in this
iridates metallicity and emphasises the different
phenomena competing with each other6. Thus, the
conduction property an iridate exhibits can vary
according to its space group, as evidenced by IrO2.
Due to the variety and similarity in strength of
competing phenomena, the iridates exhibit metallic
and insulating states and thus transitions between
these two states occur in this family of compounds.
These transitions can be a function of the presence of
different secondary cations, as well as space group,
temperature and pressure. In the subsequent
sections, trends in the metallicities or insulating
states of the following groups of iridates will be
analysed as a function of the aforementioned
variables: alkali and alkaline earth metal iridates,
pyrochlore iridates and other iridates.

Figure 2: 9H BaIrO3 unit cell. This is the ambient phase,

with space group C2/m. Lattice data obtained from
MatNavi online database. Data published by Lazarev et
al.10. IrO6 tetrahedra form face-sharing triplets connected
along the c-axis, with each triplet linked along its vertices
ends. Plotted using CrystalMaker software.

At ambient conditions SrIrO3 has a monoclinic C2/c

space group11 whereas at high pressure and
temperature, when synthesised via epitaxial thin
film growth, an orthorhombic perovskite structure is
obtained12,13. Both these phases are metallic.12,14 This
is contrast to Sr2IrO4 a Mott insulator as previously
detailed and Sr3Ir2O7, a bad insulator, with the
bandwidths of the Jeff = Lower and Upper
Hubbard Bands being such that the gap between
them is very narrow12.

Alkali and Alkaline Earth Metal Iridates

BaIrO3 consists of 9H and 6H polymorphs. 9H is the
ambient phase structure (fig. 2) and is insulating3 7,
whilst the 6H polymorph is metastable (synthesised
above 5GPa and quenched8) and is metallic9.
Although both polymorphs are monoclinic, a metalinsulator transition occurs. This may be attributed to
the subtle change in space group from C2/m to C2/c
respectively for the 9H and 6H forms. One can
envision an ultra-high pressure sensor developing

There is debate in literature as to the space group of

Li2IrO3 OMalley et al.15 argue for a C2/m
description while Kobayashi et al.16 refine the
structure with C2/c space group. Electronic DOS
plots reveal that the Fermi level cuts through the t2g
Li2IrO3 band, indicating metallic behaviour, which is
confirmed by electrical measurements15.

Imperial College, Department of Materials

Na2IrO3 exhibits a honeycomb lattice of the Ir atoms

with deviation of the IrO6 octahedra from their cubic
environment. The edge-sharing IrO6 octahedra (fig.
3) are compressed in the direction of honeycomb
layer

17

stacking .

Predictions

indicate

that

honeycomb lattice Na2IrO3 is a topological insulator,

that is, it exhibits conductivity of its edges or
18

surfaces, but the bulk of the material is insulating .

Figure 4: CaIrO3 crystal structure. IrO6 octahedra arranged

in corner and edge-sharing layers, stacked along the b axis
with the Ca atoms in between, arranged in rows along the
a
direction.
Lattice
data
obtained
from
the
Crystallographic Open Database. Data published by
Martin et. al.19. Plotted using CrystalMaker software.

Figure 3: Crystal structure of Na2IrO3 with space group

C2/m. Figure is from paper by Ye et al17. The honeycomb
lattice is formed by the Ir atoms in the illustrated
octahedra.

CaIrO3 is a post-perovskite (space group Cmcm) and

consists of IrO6 octahedra layers perpendicular to
the b axis sharing edges and corners along the a axis
and c axis respectively (fig. 4). This is a rare structure
and CaIrO3 is the only oxide to exhibit at ambient
19

conditions . CaIrO3 is a Jeff = Mott insulator the

splitting of the t2g band into half-filled Jeff = and
filled Jeff = 3/2 bands due to SOC along with
moderate onsite Coulomb repulsion results in a
20

Mott insulating state .

Imperial College, Department of Materials

Table 1: selected properties of alkali and alkali earth metal

iridates.

topologically insulating states and topological Weyl

Iridate

dimensional system with valence and conduction

Crystal
family
Monoclinic

Li2IrO316

Space group
C2/c

Lattice
Parameters
a =5.16641(17)
b =8.9330(3)
c =9.7804(2)
=100.016(3)

Conduction
Property

semimetals28.

The

latter

is

essentially

3-

bands that just intersect at certain points in k-space,

similarly to graphene (2D)29. Additionally, a giant
magnetoresistance (GMR) effect is observed in
Nd2Ir2O7, of relevance in the relatively recent field of

Li2IrO315

Monoclinic

Na2IrO317

Monoclinic

C2/m

C2/m

CaIrO320

Orthorhombic

Cmcm (postperovskite)

SrIrO314 11

Monoclinic

C2/c

SrIrO3 *12
9H
BaIrO31 7

Orthorhombic
Monoclinic

Pnma (perovskite)
C2/m

6H
BaIrO38

Monoclinic

C2/c

Sr2IrO45 2

Tetragonal

I41 /acd

Sr3Ir2O726

Tetragonal

I4/mmm

22

24 25

27

a =5.1633(2)
b = 8.9294(3)
c = 5.1219(2)
= 109.759(3)

Metallic

a =5.139(1)
b = 9.215(2)
c = 5.536(1)
= 108.67(1)
(measured at
125K)
a = 3.146(1)23
b = 9.867(2)
c = 7.298(2)
a=5.60401(29)14
b =9.6256(4)
c =14.1834(7)
= 93.202(4)

Insulator17,21

a = 10.0052(4)3
b = 5.7514(2)
c = 15.1742(7)
= 103.274(5)
a = 5.7483(2)
b = 9.9390(3)
c = 14.3582(5)
= 91.319(2)
a = 5.4979(2)4
c = 25.798(1)
a = 3.897(5)
b = 20.892(5)

spintronics.

This is a phenomenon whereby a

material consisting of ferromagnetic layers will

exhibit a high resistance with parallel alignment of
spins between the layers. Conversely, when the
alignment between alternating layers is antiparallel,
a low resistance is observed. This effect has been
utilised in the magnetic field sensors of hard disk
Insulator

drives. Cooling Nd2Ir2O7 below its metal-insulator

transition temperature TMI = 33K causes the

Metallic

emergence of a large GMR effect30.

Metallic
Insulator

Metallic9

Insulator

Bad
Insulator12

Pyrochlore Iridates A2Ir2O7

The pyrochlore iridates have the cubic Fd m space
group and consist of corner sharing tetrahedra

Figure 5: Unit cells of Bi2Ir2O7 illustrating the

connectivity of the tetrahedra network in pyrochlore
iridates. Lattice data is from a paper by Sardar et al.31
Plotted using CrystalMaker software.

networks with spin occupied vertices (fig. 5). The

Matsuhira et al. have found the iridates with A = Pr,

geometrical frustration of the magnetic ordering of

Nd, Sm and Eu to exhibit metallic conductivities,

the spins occupying these tetrahedral vertices can

whilst those with A = Gd, Tb, Dy, Ho, Yb to exhibit

result in metallic spin liquid behaviour. The interest

semiconductivity, where the A cation is a lanthanoid

generated by this phenomenon has catalysed

rare earth element32. As we move along the periodic

investigations into the pyrochlore iridates. Further

table in the lanthanoid series, the radii of the ions

interest has been sparked by the observance of

decrease. Consequentially, the Ir-O-Ir bond angles

Imperial College, Department of Materials

become smaller. This results in a lower bandwidth

of the 5d5 t2g band of the Ir4+. The decreased width of
the band means a band gap eventually forms and
grows. This rationalises the decrease in conductivity
observed with increasing atomic number32,33.
Table 2 illustrates this information with decreasing

Table 2: selected properties of the pyrochlore iridates with space

group Fd m. Double line separates lanthanide iridates
investigated by Matsuhira et al.32,33 from other pyrochlore
iridates.
Pyrochlore
Iridate

A
cation
Z

Lattice
constant a

Conduction
Property32,33

TMI32 33 (K)

Pr2Ir2O7

59

10.3940(4)34

Metallic

Nd2Ir2O7

60

10.3647(9)36

Metallic

None
observed
down to
0.335
33

Sm2Ir2O7

62

10.311(2)37

Metallic

117

Eu2Ir2O7

63

10.3020.00138
10.274(3)34

Metallic

120

Gd2Ir2O7

64

10.26610

Semiconductor

127

Tb2Ir2O7

65

10.22210

Semiconductor

132

Dy2Ir2O7

66

10.20610

Semiconductor

134

Ho2Ir2O7

67

10.18310

Semiconductor

141

Yb2Ir2O7

70

10.1015(5)39

Semiconductor

Y2Ir2O7

39

Insulator41 42

Lu2Ir2O7

71

10.10 580(7)40
10.1794(4)37
10.104(2)37

Pb2Ir2O6.543

82

10.2840.002
10.27644

Metallic

Bi2Ir2O728

83

10.314(3)

Metallic

ionic radius of the A cation, the lattice constant

decreases. From Eu to Gd there is a metalsemiconductor transition where the conductivity of
the lanthanide pyrochlore becomes that of a
semiconductor. So changing the A cation from Eu to
Gd results in a critical decrease of ionic radius; a
band gap is formed.
Furthermore, for each lanthanoid iridate (excluding
Yb and Pr), there is a temperature (TMI) at which a
2nd order metal-insulator transition occurs, which
also speculated to be dependent on the t2g
bandwidth

32,33

. For example, if Ho2Ir2O7 is cooled

below 141 K, there is a subtle, but non-trivial

decrease in gradient of the resistivity v. temperature
curve, indicating a 2nd order transition to an
insulating state.

Imperial College, Department of Materials

Other Iridates

Conclusion

Immediately, it can be seen from table 3 that there is

In conclusion, metal-insulator transitions in a large

a metal insulator-transition between tetragonal IrO2

sample of iridium oxides has been compiled,

(fig. 6) and cubic Ir2O4, even though the constituent

identified and rationalised. We have seen how this

atoms are identical. The insulating state of Ir2O4 can

transition can be a function of space group, e.g. in

be attributed to the dominating interactions of on-

the different strontium iridate compounds SrIrO3,

site Coulombic repulsion and SOC, analogously to

Sr2IrO4 and Sr2Ir2O7. Metastable, non-ambient phases

insulating state observed in Sr2IrO4, characterised by

formed at high pressure and temperature can

Kim et al. As was described earlier in this review,

transition to different conductive states than there

Kahk et al. have concluded that dominant crystal

equilibrium counterparts, such as in the various

field

polymorphs of BaIrO3. Keeping the space group

45

splitting

and

effective

orbital

interactions rationalise metallicity of IrO

overlap

constant

26.

and

varying

the

secondary

cation,

beautifully illustrated in the pyrochlore iridates, has

yielded the identification of a metal-semiconductor
transition between Eu2Ir2O7 and Gd2Ir2O7. Looking at
how the effects of temperature can be accounted for,
a metal-insulator transition temperature (TMI) has
been identified by Matsuhira et al.30,32,33 for the
lanthanoid iridates. The trends observed, can be
largely accounted for by consideration of the
competing

interactions

of

on-site

Coulombic

repulsion, crystal field splitting, spin-orbit coupling

and orbital overlap on the Ir4+ 5d5 electrons.
Understanding these interactions and their effects
on metal-insulator transitions are vital to their
application as topological insulators, pressure and
Figure 6: IrO2 unit cell. Lattice data obtained from
MatNavi online database. Data published by Huang et
al46. Plotted using CrystalMaker software.

magnetic field sensors and in the field of spintronics,

where the spin as well as the charge of the electrons
transferred contributes to data transmission. There is

Table 1: selected properties of other iridates.

Iridate
IrO26

Ir2O4

45

Crystal
family
Tetragonal

Cubic

Space group
P42/mnm (rutile)

-Isostructural to
-MnO245,
-Fd3m space
group48.
-Spinel (AB2O4),
without A cation
in octahedral
site45.

Lattice
Parameters
a=
4.5051(3)47
b=
3.1586(2)

room for further investigation in rationalising the

Conduction
property
Metal

band behaviour of several iridates including Na2IrO3

and Li2IrO3 and characterising the unit cell of Ir2O4
whose lattice parameters are not readily available in
the literature.

Insulator

Imperial College, Department of Materials

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