PbI2 Pb1xCdxI2

1994 3


PbI2

Pb1x Cdx I2
PbI2

1.1 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

1.2 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

PbI2 CdI2 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

1.3.1

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

1.3.2

PbI2 CdI2 . . . . . . . . . . . . . . . . .

1.3.3

PbI2 . . . . . . . . . . . . . . . . .

1.3.4

PbI2 . . . . . . . . . . . . . . . . . 10

1.3.5

. . . . . . . . . . . . . . . . . . . . . 10

1.3

2.1

12

PbI2 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
2.1.1

PbI2 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12

2.1.2

Pb1x Cdx I2

. . . . . . . . . . . . . . . . . . . . . . . . 12

2.2 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
2.2.1

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13

2.2.2

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13

2.3 . . . . . . . . . . . . . . . . . . . . . . . . 14
3 PbI2

15

3.1 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
3.2 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22
3.2.1

. . . . . . . . . . . . . . . . . . . . 22

3.2.2

3.2.3

. . . . . . . . . . . . . . . . . . . . 25

. 22

3.3

PbI2 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28

4 Pb1x Cdx I2

4.1 ()

29

. . . . . . . . . . . . . . . . . . . . . . . . . . 29

4.2 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32
4.2.1

Pb1x Cdx I2 (x = 0.03) . . . . . . . . . . . . . . . . . . 32

4.2.2

Pb1x Cdx I2 (x = 0.05) . . . . . . . . . . . . . . . . . . 37

4.3 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43
4.3.1

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43

4.3.2

4.3.3

. . . . . . . . . . . . . . . 45

4.3.4

x = 0.05 2 . . . . . . . . . . . 46

. 43

4.4 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 48
5

49

. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 51

ii

1.1

()
k
h
k
[1]

ck

)2

= ()
(

() = b 1 +

LT
T

(1.1a)
)

(1.1b)

() , k , b
(background dielectric constant) ,
( LT )
mex T (k) = T + h
k 2 /2Mex
k

ck

)2

= (, k)
(

(, k) = b

LT
1+
T (k)

(1.2a)
)

(1.2b)

1.1(a) 1.1(a)
EL
2 EL


EL ET
()

ET

(
) k ' 0

ET

[2]
1.1(a)

(FE)
[3, 4, 5]

2
[6] [6]

EBX = EBX (0) +

h
2k2
2 MBX

b
EBX (0) = 2ET EBX

(1.3a)
(1.3b)

MBX , k ET EBX

k = 0 1.1(b)
tr

 1.1: (a):
(b): (c): MT , ML (d):
() () (e): M
() ()

lg mol

CuCl [7] (Mysyrowicz et al. 1968)

1 1.1(c)
1.1(d) (MT )
(ML ) 1.1(d) 1.1(e) MT ML

(
) [ 1.1(d)]
Gale Mysyrowicz [8, 9] CuCl
2
(M ) ( 2 )
[6]
2
1

2
1

NaCl CuCl [10]

[11]

CdS1x Sex CuCl1x Brx

[12, 13, 14]

1.2

1.1

PbI2

Pb1x Cdx I2
PbI2

1.3
1.3.1

PbI2 CdI2

PbI2 CdI2 (CdI2 ) [15] 1.2 PbI2

PbI2 Pb2+ CdI2 Cd2+ c

I-Pb-I(I-Cd-I)
[15] (I-I) (Pb-I)
PbI2 , CdI2 c

polytype PbI2 20
polytype [15, 16] 2H Type

(2HPbI2 ) 2HPbI2 D3d

(3 ) 2HPbI2 PbI2 CdI2
1 [15] Pb2+
Cd2+ Pb1x Cdx I2

1.3.2

PbI2 CdI2
PbI2 Pb2+ 6s,

6p cationic [17]E c, E k c
E c
E k c 4 E c

PbI2 (E c) 2 .50 eV (2H

PbI2 ) [18, 19] PbI2
Wannier 1.3 1.4
[5, 19] 1s
[5, 18] (2 K )

PbI2 LT ELT

 1.2: PbI2

1.3: PbI2

1.4: PbI2 [(a)] Pb1x Cdx I2 [(b)]

(
)

 1.1: PbI2

D3d

a = 4.56
A, c = 6.98
A

N = cm3

ET = 2.4979 eV

EL = 2.5059 eV

LT

ELT = 8.0 meV (EL ET )

Mex = 1.0me (me , k k c)

Gex = 63 meV

aex = 19
A

ET = 4.9912 eV

Gex = 4.6 meV

b = 9.6

Eg = 2.540 eV

 1s

CdI2 I 5p Cd2+ 5s
[20]3.47 eV
(
) [21]

PbI2 CdI2 Pb2+ Cd2+ PbI2

PbI2 :Cd (x = 0.01) 1.4(a), 1.4(b)
1.4(a) FE 1.4(b)
ET
Pb2+
[5]

PbI2

1.3.3

1.1
PbI2
(1.2) 1.1(a) PbI2
3.1
4 2.498 eV (FE)
[22] (BE)
[23]FE 12 meV

28 meV
[24]

PbI2

1.2 PbI2
[24]

 1.2: (Goto and Nishina [[24]] )

phonon energy(meV)

1.3.4

A1g

LO

12.0

13.9

PbI2
PbI2

[25]
(1.3) [6] 1.1 (b) PbI2
Mmol
2 (2Mex )

[26]
()

nM

nM =

kB T e
16 Gex a 3ex

(1.4)

Gex Te aex
kB PbI2 1 1017

[cm3 ] 1.9 nm 20 K
63 meV [19, 27]
0.7 1017 [cm3 ] ()

1.3.5

1.1 2

10

 2
2
CuCl 2 2 1013 [photons/cm2 sec] (
) [28] 4 1021 [photons/cm2 sec]

(Grun etal.) [29]

[6, 30]
1. : 2
1 1

2 1 2
102
2

2. : 2
2
PbI2 2
[25] PbI2 3 6.5 meV [25, 31]
1
PbI2 34 meV 1
Pb1x Cdx I2
PbI2
PbI2 2

11

PbI2

2.1
2.1.1

PbI2
1 2 3 Zone 3

1. :

2. : 1 (
6N) 1.23 (Aldrich Chemical 5N) (
) 1

3. zone : PbI2 Ar 30 mmHg 90 Zone

polytype 4H 1
2H bulk c
3 4 0.5mm3

2.1.2

Pb1x Cdx I2
Pb1x Cdx I2 PbI2 CdI2 1 x:x

400C
1

12

 polytype
polytype

2.2
2.2.1

YAG

(BMI 501 DNS) 10 Hz YAG

3 (355 nm)
Coumarin 481 1 102 [ mol/l ]
465 497 nm 6 nsec
0.3
A

2.2.2

64 cm (Jovin Yvon HR640)

2.4
A
optical multichannel analyzer ( oma:ATAGO)
(HTV R-928, HTV R-955)

strain free
E c, k k c

(Sony TEKTRONIX 2432A)

(Molectron J3-02)

13

2.3

2 K

10 K
(OSK CRYOMINI)
Au-Fe:Co
1 K
2.1

2.1:

14

 3 PbI2

3.1

3.1 PbI2

3.1: PbI2 2.511 eV

2 K%

2.511 eV 2 K ( 0.1 %)

15

PbI2 4 (FE,

BE, FE-2LO, FE-A1g ) 2.491 eV (MT

) BE [25, 32]
1 (ML ) MT ML
[33]

1. ilum iexc
2.
1 meV

3. MT ML LT
MT
2.486 eV ML [6]2.47 eV
(P) M
M

CuCl N2 P
[34, 35, 36, 37, 38] 3.1 MT BE
BE BE

3.2 ( 0.2%)
() (
) 3.1 2.511 eV
500 500
500 2.430 eV
(DA)
MT ML

16

 3.2: (0.2%) (100%)

(500)

17

 3.3 ( 0.4%) MT

3.3: PbI2
2.511eV 2 K

MT
ML
P MT ML
MT (
optical conversion) [6] 3.4
FE-2LO
FE-2LO 3

3
2.498 eV ()2.511 eV () 2.525 eV ()
2.498 eV 2.525 eV n = 1 n = 2

18

 3.4: PbI2
2 K3
2

19

 2.511 eV n = 1 n = 2
( 1.4 ) [19]

3
1.01022 [photons/cm2 sec]
3.5:2.5:1
2 1 (ilum i2exc ) 2
M FE

2 3.5

3.5: PbI2

2.525 eV [ (a) (f)]2.516 eV [ (b) (g)]

2.511 eV [ (c) (h)]2.506 eV [ (d) (i)] 2.498 eV [ (e) (j)]

20

 FE M
3.1 4
2.511 eV 2.525 eV
ET
2.516 eV 2 2.516eV
FE M
ET (2.5112.525 eV)
3.4 FE-2LO

2 ( 3.43.5) [5]
3.1: PbI2 (FE) (MT ML )

excitation energy (eV)

2.498
FWHM of FE (meV)
FWHM of M (meV)

7.9

21

2.511

2.516

2.525

3.2

8.0

3.3

10.2

13.2

9.7

3.2
3.2.1

1.1 (p.1)

(FE)

FE
FE-2LO

3.4 FE-2LO

3.2.2

3.4

3
3.5:2.5:1 1.01022 [photons/cm2 sec]
LIC
' 2 ' 1

22


LIC Knox
[39, 40] 3.6

3.6:

( n1 ) ( n2 ) ( N ) 3

dn1
= i (kR + kNR )n1
dt

(3.1a)

dn2
= kR n1 ex n2 n22 + m N
dt
dN
n22
=
m N
dt
2

(3.1b)
(3.1c)

i kR
kNR
m ex
( =
n2 )
kNR = 0
(3.1) :

n2 =

ex

2
ex
N =
2m

i
+ 1 1
i0

i
+ 1 1
i0

23

(3.2a)
)2

(3.2b)

 i0 :
2
i0 = ex
/ (2)

(3.3)

i  i0 [38]1

n=

ex i
2i0
(

N=

2
i
ex
2m 2i0

(3.4a)
)2

(3.4b)

(isg ibx ) (n2 , N )

isg n2 /, ibx N/

(3.5)

(3.4) isg ibx

3.5:2.5:1
3.2
[19, 42]
3.2: i0 hrthr iAV

excitation energy (eV)

2.498

2.511

2.525

[cm1 ][19, 22]

1.5 105

3.5 104

8.1 104

i0 [cm2 s1 ]

1.5 1022

7.0 1022

1.7 1022

[cm3 s1 ]

1.5 109

1.3 109

2.4 109

hrthr iAV [
A]

640

560

540

[41]

24

 2 1 3.4
LIC i0 ( 3.2)
()
i0 58 K 390 ps
[27, 42]

i0 3.2
(ithr )
hrthr iAV

hrthr iAV = (Ithr ex )1/3

(3.6)

[38] 3.2
(1.9 nm4.9 nm) (

[30])

3.2.3

3.1 FE M

2.516 eV FE, M
FE, M 2.511, 2.525 eV

2.516 eV 3.4

ET

25


(2.516 eV)
FE
2.525 eV2.511 eV
2.516 eV
3.7 PbI2 FE [5]
FE

3.7: PbI2 [(a)] Pb1x Cdx I2 [(b)]

( [[5]] )
(2.511, 2.525 eV)

M FE
M

1 ( 1.1(c) 1.1

26

 (p.1))

h = ET

b
EBX

h
2k2

4Mex

(3.7)

b
ET EBX

Mex

ibx (E) = E 1/2 exp

E
kB TM

(3.8)

b
E = ET EBX
h

(3.9)

(kB :TM :)
E = 0
b
EBX
2.4979 eV

4.2 meV

3 meV [25]
3.1 (p.15) M
20.4 K ( 2.511 eV )
(2 K)
CdS
TM = 17 20 K CuCl TM =24 K (4 K )
[6, 33]
3.8
() [43]
PbI2
(
63 meV [19])

27

 3.8:

3.3

PbI2

1. PbI2

2. 3.5:2.5:1

3.

4.

5.

28

 4 Pb1xCdxI2

4.1

()

[11, 44, 45]

E. Cohen
4.1 V (r) r

(mobility

edge) [ 4.1(a)4.1(b)]
[ 4.1(c), 4.1(d)]
[ 4.1(e),

4.1(f)]
PbI2 CdI2 Pb1x Cdx I2 PbI2

29

 4.1: (a)
(b) (c)

(d) (e) (f)

30

Pb2+ Cd2+ Pb2+

Pb2+ PbI2
4.2
[14] 4.2(a) x () (

4.2: (a): Pb1x Cdx I2

x Cd2+ (b):
()

) x
Cd2+ Pb2+
4.2(b) x
4.2(a) x = 0.03
(FE) x

31

 (LE)

4.2
4.2.1

Pb1x Cdx I2 (x = 0.03)

4.3 Pb1x Cdx I2 (x = 0.03)

2.540 eV 2 K

4.3: Pb1x Cdx I2 (x = 0.03)

2.540 eV 2 K %

( 0.3 %) 2 2.527 eV
FE 2.518 eV LE

2.514 eV (M) LE PbI2

M

32

 4.4 M

4.4: Pb1x Cdx I2 (x = 0.03) M

2.540 eV 2 K
%

PbI2 3.2
(p.22) [33]M

4.5

4.5 (a) 4.5(d) LE LE

[ 4.5(e) (f)] [4.5(f)]
LE
4.5(e) (f)

33

 4.5: Pb1x Cdx I2 (x = 0.03)

2 K

4.5(a) (d)

4.5(g) (j) [ 4.5(a) (d) ]

M
[ 4.5(k) (l)]
4.6
(

LE )
1 M

4.7 (M) (FE) LIC

3
2.540 eV () 2.524 eV () 2.519 eV ()
2.540 eV

34

 4.6: x = 0.03
1

35

 4.7: Pb1x Cdx I2 (x = 0.03)

3

2 2 K

36

2.524 eV2.519 eV
4:3:1
5 1021 [photons/cm2 sec]
= 1.6 2.0
2 PbI2
FE
2.540 eV = 0.98

4.2.2

Pb1x Cdx I2 (x = 0.05)

4.8 Pb1x Cdx I2 (x = 0.05)

2.561 eV

4.8: Pb1x Cdx I2 (x = 0.05)

2.561 eV 2 K %

2 K (:

37

 0.24 %) 2.538 eV LE

2.525 eV (M) 4.9

4.9: Pb1x Cdx I2 (x = 0.05)

2 K

[ (a) (f)] (a) (c)

LE
(d) (f)
[ (g) (k)] (g) (i)
M
[ (j), (k)] M
x = 0.03
M 11 meV

M0 4.10
38

 2.538 eV

4.10: Pb1x Cdx I2 (x = 0.05)

2.535 eV 2 K

12 % ( (a) ) M
(M0 ) M
M M
(PbI2 :
3.3[p. 18] ) M0
2
4.11 M
4.12
(M, M0 )
1

x = 0.03 M
39

 4.11: Pb1x Cdx I2 (x = 0.05) M

4.12: Pb1x Cdx I2 (x = 0.05)

1

40

 ( 22 meV) M0
4.13 (M M0
) 2.571 eV ()

4.13: Pb1x Cdx I2 (x = 0.05)

2
1.2
2 2 K

2.535 eV () 2.571 eV
2.535 eV
PbI2
=1.2 =2
x = 0.03 2.535 eV
LIC 5

41

 2.545 eV
2 2

x = 0.08, 0.2
x = 0.05 4.14
x=0.2
M0

4.14: Pb1x Cdx I2 (x = 0.20)

1

4.1: x = 0.05

3.0 1021 1.0 1023 [photons/cm2 sec]

excitation energy (eV)
2.571 2.550
slope

1.8

2.545

2.540

2.535

1.7

1.3

1.2

1.5

42

4.3
4.3.1

x = 0.03 FE

LE LIC

x = 0.03
M

1. M LE

2. LE FE

3. M
M
3
4.5 (x = 0.03 ) 4.10 4.11 (x = 0.05 )
M
M
1

4.3.2

4.11 x = 0.03 M

5 1021 [photons/cm2 sec]

[46]

43

 4:3:1 2

LIC PbI2 (3.2.2

(p. 22) ) 4.15 ( n1 )
( n2 ) ( N ) 3 4.7

4.15: (x = 0.03)

2 4.2
i0
ithr i0

x = 0.05
LIC
( 4.1 )
2

[46]

44

 4.2: x = 0.03 i0
ithr

excitation energy (eV)

2.540

2.524

2.522

2.519

i0 [cm2 s1 ] 8.4 1020

3.7 1021

6.7 1021

9.1 1021

ithr [cm2 s1 ] 4.8 1020

4.8 1021

2.4 1021

9.6 1021

.
3

4.3.3

4.6(x = 0.03) 4.12(x = 0.05) 4.14(x = 0.2 )

4.16 x = 0
PbI2 ML
3.8 3
63 meV
[14, 19] PbI2

1.
2.

6s 6p
()
3

x = 0.05

x = 0.03
[46]

45

 4.16: x = 0
PbI2

Cd

[10, 47]

4.3.4

x = 0.05 2
4.10 x = 0.05 2

M, M0

M (22 meV) M0
M0 2
4.17
1 (2.535 eV)
() 2 () 2

46

 4.17: (x = 0.05) M M0

M (22 meV)
M0
(11 meV) 4.10
M M0

M PbI2 MT
M, M0 PbI2 MT , ML
x = 0.05 LT 11 meV PbI2
(8.0 meV)
LT MT ML

4.10 M0 1.3.5
(p.10)2

47

M M0 M
( 4.17 energy transfer rate )

4.4

1. Pb1x Cdx I2 (x = 0.03, 0.05, 0.08, 0.2)

2. x = 0.05 2
M0

3. 1, 2
4.

48

 5
1. PbI2

2. PbI2

3. (x = 0.03, 0.05, 0.08, 0.2)

4. M

49

50


1. E. L. Ivchenko, in Excitons, edited by E. I. Rashba and M. Sturge (North Holland,
Amsterdam, 1982), pp. 141176.
2. Y. Toyozawa, Progr. Theor. Phys. Suppl. 12, 111 (1959).
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Technology Group III (Springer Verlag, Berlin, 1973), Vol. 7, p. 613.
51

16. R. G. Wyko, in Crystal Structures (International, 1964), Vol. 2, p. 66.

17. I. C. Schl
uter and M. Schl
uter, Phys. Rev. B 9, 959 (1974).
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