Wavelength (nm) Time (ps) 0 20 40 60 80 100 120 140 Time (ns)
1
• • Thicker ZnSe mid-shell Single exciton Negative trion - + - + - + - - + - k Auger 0.19 ns -1 0.05 ns -1 76% e-e repulsion delocalization - + - • • • • 0 10 20 30 0 100 200 300 400 500 PL intensity (counts/50 ms) Time (s) 0 50 100 150 0.1 1 PL intensity (norm.) Time (ns) τ X =36 ns τ X- =2.2 ns C/MS-1/S 10% 100% 0 50 100 150 0.1 1 PL intensity (norm.) Time (ns) τ X =33 ns τ X- =9.3 ns 0 10 20 30 40 0 100 200 300 400 PL intensity (counts/50 ms) Time (s) 36% 100% C/MS-3/S 0 50 100 150 0.1 1 PL intensity (norm.) Time (ns) τ X =35 ns τ X- =3.5 ns 0 10 20 30 40 50 0 100 200 300 400 PL intensity (counts/50 ms) Time (s) 17% 100% C/MS-2/S QY X- 700 650 600 550 500 450 Wavelength (nm) OD (norm.) PL intensity (norm.) C/MS-1/S C/MS-2/S C/MS-3/S 580 600 620 640 660 680 0.0 0.5 1.0 Wavelength (nm) ∆ XX 64 meV 0.0 0.5 1.0 2 mW 1000 mW difference ∆ XX 80 meV C/MS-1/S 0.0 0.5 1.0 PL intensity (norm.) ∆ XX 76 meV C/MS-2/S C/MS-3/S probe 450 500 550 600 650 700 0.1 1 10 Wavelength (nm) Time (ps) 450 500 550 600 650 700 0.1 1 10 Wavelength (nm) Time (ps) 450 500 550 600 650 700 0.1 1 10 Wavelength (nm) Time (ps) C/MS-2/S C/MS-3/S C/MS-1/S C/MS-2/S C/MS-3/S C/MS-1/S pump probe + - Hot electron 0 5 10 15 20 -20 -15 -10 -5 0 DmOD Time (ps) 0 5 10 15 20 -15 -10 -5 0 DmOD Time (ps) 0 5 10 15 20 -8 -6 -4 -2 0 DmOD Time (ps) -4 -2 0 DmOD -6 -4 -2 0 DmOD -2 0 DmOD 340±23 fs 1.6±0.3 ps 680±14 fs 2.6±0.1 ps 770±20 fs 3.3±0.2ps 340 fs 680 fs 770 fs 470 nm 615 nm 470 nm 615 nm 470 nm 615 nm 550 600 650 700 0 100 200 300 400 PL intensity (a.u.) Wavelength (nm) [(ET 3 BH) - ] 550 600 650 700 0 200 400 600 PL intensity (a.u.) Wavelength (nm) 550 600 650 700 0 200 400 600 PL intensity (a.u.) Wavelength (nm) [(ET 3 BH) - ] [(ET 3 BH) - ] C/MS-1/S C/MS-2/S C/MS-3/S 0 4.6 mM 7.6 mM 10.9 mM 14.1 mM 0 4.6 mM 7.6 mM 10.9 mM 14.1 mM 0 4.6 mM 7.6 mM 10.9 mM 14.1 mM 500 600 700 0.00 0.02 0.04 Absorbance Wavelength (nm) [(ET 3 BH) - ] 0 4.6 mM 7.6 mM 10.9 mM 14.1 mM 500 600 700 0.00 0.02 0.04 Absorbance Wavelength (nm) [(ET 3 BH) - ] 0 4.6 mM 7.6 mM 10.9 mM 14.1 mM 500 600 700 0.00 0.02 0.04 Absorbance Wavelength (nm) [(ET 3 BH) - ] 0 4.6 mM 7.6 mM 10.9 mM 14.1 mM 0 20 40 60 80 100 120 140 0.01 0.1 1 PL intensity (norm.) Time (ns) 4.1 ns [(ET 3 BH) - ] 0 4.6 mM 7.6 mM 10.9 mM 14.1 mM C/MS-1/S 0 20 40 60 80 100 120 140 0.01 0.1 1 PL intensity (norm.) Time (ns) 10.9 ns [(ET 3 BH) - ] 0 4.6 mM 7.6 mM 10.9 mM 14.1 mM C/MS-3/S 0 20 40 60 80 100 120 140 0.01 0.1 1 PL intensity (norm.) Time (ns) 6.9 ns [(ET 3 BH) - ] 0 4.6 mM 7.6 mM 10.9 mM 14.1 mM C/MS-2/S + OBJ Pinhole Single photon detector ps-pulsed laser PL - + − = ,− ,− + ,− − = 1/( ,− + ,− ) QY X- QY X- k Auger,X- k Auger,X- C/MS-1/S 0.24 0.15±0.1 0.19 0.29±0.13 C/MS-2/S 0.32 0.28±0.1 0.10 0.16±0.11 C/MS-3/S 0.50 0.35±0.1 0.05 0.10±0.06 • • • - + - Excitonic interaction e - e repulsion More realistic case < 2k r C/MS-1/S C/MS-2/S C/MS-3/S 0.0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 QY X- Photochemical e-doping Single dot C/MS-1/S C/MS-2/S C/MS-3/S 0.0 0.1 0.2 0.3 0.4 k Auger,X- (ns -1 ) Photochemical e-doping Single dot b • • • •
Transcript of Wavelength (nm) Time (ps) 0 20 40 60 80 100 120 140 Time (ns)
•
•
Thicker Zn
Se mid
-shell
Single exciton Negative trion
-
+
-
+
-
+
-
-
+
-kAuger
0.19 ns-1
0.05 ns-1
76%
InP/ZnSe/ZnS QD
e-e repulsion
delocalization
Thicker Zn
Se mid
-shell
Single exciton Negative trion
-
+
-
+
-
+
-
-
+
-kAuger
0.19 ns-1
0.05 ns-1
76%
InP/ZnSe/ZnS QD
e-e repulsion
delocalization
•
•
•
•
0 20 40 60 80 100 120 140
0.01
0.1
1
PL
inte
nsi
ty (
no
rm.)
Time (ns)
0 20 40 60 80 100 120 140
0.01
0.1
1
PL
inte
nsi
ty (
no
rm.)
Time (ns)
0 20 40 60 80 100 120 140
0.01
0.1
1
PL
inte
nsi
ty (
no
rm.)
Time (ns)
4.1 ns 6.9 ns 10.9 ns
C/MS-1/S C/MS-2/S C/MS-3/S0.0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
QY X
-
Photochemical e-doping
Single dot
0 10 20 300
100
200
300
400
500
PL
inte
nsi
ty (
cou
nts
/50
ms)
Time (s)
0 50 100 150
0.1
1
PL
inte
nsi
ty (
no
rm.)
Time (ns)
τX =36 ns
τX-
=2.2 ns
C/MS-1/S
10%
100%
0 50 100 150
0.1
1
PL
inte
nsi
ty (
no
rm.)
Time (ns)
τX =33 ns
τX-
=9.3 ns
0 10 20 30 400
100
200
300
400
PL
inte
nsi
ty (
cou
nts
/50
ms)
Time (s)
36%
100%
C/MS-3/S
0 50 100 150
0.1
1
PL
inte
nsi
ty (
no
rm.)
Time (ns)
τX =35 ns
τX-
=3.5 ns
0 10 20 30 40 500
100
200
300
400
PL
inte
nsi
ty (
cou
nts
/50
ms)
Time (s)
17%
100%
C/MS-2/S
[(ET3BH)-]04.6 mM7.6 mM10.9 mM14.1 mM
[(ET3BH)-]04.6 mM7.6 mM10.9 mM14.1 mM
[(ET3BH)-]04.6 mM7.6 mM10.9 mM14.1 mM
C/MS-1/S C/MS-2/S C/MS-3/S0.0
0.1
0.2
0.3
0.4
k Au
ger,
X- (
ns-1
)
Photochemical e-doping
Single dot
C/MS-1/S C/MS-3/SC/MS-2/S
QYX-
Energy (eV)1.81.92.12.32.52.8
700650600550500450Wavelength (nm)
OD
(n
orm
.)
PL in
tensity (n
orm
.)
C/MS-1/S
C/MS-2/S
C/MS-3/S
580 600 620 640 660 6800.0
0.5
1.0
Wavelength (nm)
∆XX
64 meV
0.0
0.5
1.0 2 mW
1000 mW
difference
Model Gauss
Equationy=y0 + (A/(w*sqrt(pi/2)))*exp(-2
*((x-xc)/w)^2)
Plot Normalized1
y0 -0.14459 ± 0.15287
xc 628.30435 ± 0.17302
w 31.25564 ± 3.15344
A 44.70058 ± 10.23112
Reduced Chi-Sqr 3.09705E-4
R-Square (COD) 0.99692
Adj. R-Square 0.99507
∆XX
80 meV
C/MS-1/S
0.0
0.5
1.0
PL
inte
nsi
ty (
no
rm.)
∆XX
76 meV
C/MS-2/S
C/MS-3/S
Energy (eV)1.81.92.12.32.52.8
700650600550500450Wavelength (nm)
OD
(n
orm
.)
PL in
tensity (n
orm
.)
C/MS-1/S
C/MS-2/S
C/MS-3/S
580 600 620 640 660 6800.0
0.5
1.0
Wavelength (nm)
∆XX
64 meV
0.0
0.5
1.0 2 mW
1000 mW
difference
Model Gauss
Equationy=y0 + (A/(w*sqrt(pi/2)))*exp(-2
*((x-xc)/w)^2)
Plot Normalized1
y0 -0.14459 ± 0.15287
xc 628.30435 ± 0.17302
w 31.25564 ± 3.15344
A 44.70058 ± 10.23112
Reduced Chi-Sqr 3.09705E-4
R-Square (COD) 0.99692
Adj. R-Square 0.99507
∆XX
80 meV
C/MS-1/S
0.0
0.5
1.0
PL
inte
nsi
ty (
no
rm.)
∆XX
76 meV
C/MS-2/S
C/MS-3/S
0 5 10 15 20-20
-15
-10
-5
0
Dm
OD
Time (ps)0 5 10 15 20
-15
-10
-5
0
Dm
OD
Time (ps)0 5 10 15 20
-8
-6
-4
-2
0
Dm
OD
Time (ps)
-4
-2
0
Dm
OD
-6
-4
-2
0
Dm
OD
-2
0
Dm
OD340±23 fs
1.6±0.3 ps
680±14 fs
2.6±0.1 ps
770±20 fs
3.3±0.2ps
pump probe
+
340 fs 680 fs 770 fs
probe
470 nm
615 nm
470 nm
615 nm
470 nm
615 nm
450 500 550 600 650 7000.1
1
10
Wavelength (nm)
Tim
e (p
s)
450 500 550 600 650 7000.1
1
10
Wavelength (nm)
Tim
e (p
s)
450 500 550 600 650 7000.1
1
10
Wavelength (nm)
Tim
e (p
s)
0.0
DOD
-Hot electron
C/MS-2/S C/MS-3/SC/MS-1/S
C/MS-2/S C/MS-3/SC/MS-1/S
0 5 10 15 20-20
-15
-10
-5
0
Dm
OD
Time (ps)0 5 10 15 20
-15
-10
-5
0
Dm
OD
Time (ps)0 5 10 15 20
-8
-6
-4
-2
0
Dm
OD
Time (ps)
-4
-2
0
Dm
OD
-6
-4
-2
0
Dm
OD
-2
0
Dm
OD340±23 fs
1.6±0.3 ps
680±14 fs
2.6±0.1 ps
770±20 fs
3.3±0.2ps
pump probe
+
340 fs 680 fs 770 fs
probe
470 nm
615 nm
470 nm
615 nm
470 nm
615 nm
450 500 550 600 650 7000.1
1
10
Wavelength (nm)
Tim
e (p
s)
450 500 550 600 650 7000.1
1
10
Wavelength (nm)
Tim
e (p
s)
450 500 550 600 650 7000.1
1
10
Wavelength (nm)
Tim
e (p
s)
0.0
DOD
-Hot electron
C/MS-2/S C/MS-3/SC/MS-1/S
C/MS-2/S C/MS-3/SC/MS-1/S
0 5 10 15 20-20
-15
-10
-5
0
Dm
OD
Time (ps)0 5 10 15 20
-15
-10
-5
0
Dm
OD
Time (ps)0 5 10 15 20
-8
-6
-4
-2
0
Dm
OD
Time (ps)
-4
-2
0
Dm
OD
-6
-4
-2
0
Dm
OD
-2
0
Dm
OD340±23 fs
1.6±0.3 ps
680±14 fs
2.6±0.1 ps
770±20 fs
3.3±0.2ps
pump probe
+
340 fs 680 fs 770 fs
probe
470 nm
615 nm
470 nm
615 nm
470 nm
615 nm
450 500 550 600 650 7000.1
1
10
Wavelength (nm)Ti
me
(ps)
450 500 550 600 650 7000.1
1
10
Wavelength (nm)
Tim
e (p
s)
450 500 550 600 650 7000.1
1
10
Wavelength (nm)
Tim
e (p
s)
0.0
DOD
-Hot electron
C/MS-2/S C/MS-3/SC/MS-1/S
C/MS-2/S C/MS-3/SC/MS-1/S
550 600 650 7000
100
200
300
400
PL
inte
nsi
ty (
a.u
.)
Wavelength (nm)
[(ET3BH)-]
550 600 650 7000
200
400
600
PL
inte
nsi
ty (
a.u
.)
Wavelength (nm)550 600 650 700
0
200
400
600
PL
inte
nsi
ty (
a.u
.)
Wavelength (nm)
[(ET3BH)-] [(ET3BH)-]
C/MS-1/S C/MS-2/S C/MS-3/S
04.6 mM7.6 mM10.9 mM14.1 mM
04.6 mM7.6 mM10.9 mM14.1 mM
04.6 mM7.6 mM10.9 mM14.1 mM
500 600 7000.00
0.02
0.04
Ab
sorb
ance
Wavelength (nm)
[(ET3BH)-]04.6 mM7.6 mM10.9 mM14.1 mM
500 600 7000.00
0.02
0.04
Ab
sorb
ance
Wavelength (nm)
[(ET3BH)-]04.6 mM7.6 mM10.9 mM14.1 mM
500 600 7000.00
0.02
0.04
Ab
sorb
ance
Wavelength (nm)
[(ET3BH)-]04.6 mM7.6 mM10.9 mM14.1 mM
0 20 40 60 80 100 120 140
0.01
0.1
1
PL
inte
nsi
ty (
no
rm.)
Time (ns)
4.1 ns
[(ET3BH)-]04.6 mM7.6 mM10.9 mM14.1 mM
C/MS-1/S
0 20 40 60 80 100 120 140
0.01
0.1
1
PL
inte
nsi
ty (
no
rm.)
Time (ns)
10.9 ns
[(ET3BH)-]04.6 mM7.6 mM10.9 mM14.1 mM
C/MS-3/S
0 20 40 60 80 100 120 140
0.01
0.1
1
PL
inte
nsi
ty (
no
rm.)
Time (ns)
6.9 ns
[(ET3BH)-]04.6 mM7.6 mM10.9 mM14.1 mM
C/MS-2/S
Energy (eV)
1.81.92.12.32.52.8
700650600550500450
Wavelength (nm)
OD
(n
orm
.)
PL in
tensity (n
orm
.)
C/MS-1/S
C/MS-2/S
C/MS-3/S
C/MS-1/S C/MS-2/S C/MS-3/SIn
P
ZnSe
ZnS
ZnSe
ZnS
ZnSe
ZnS
1.65 1.82.9
3.50.2
0.20.2
Dimension (nm)
C/MS-1/S
C/MS-2/S
C/MS-3/S
-5-4-3-2-10
0.03 0.3 0.7 1.1 2.3
0 200 400 600 800 1000
-5-4-3-2-10
0.03 0.3 0.7 1.1 2.3
<NX>
∆O
D (
inte
grat
ed)
Time (ps)
-8
-6
-4
-2
0
0.03 0.3 0.7 1.1 2.3
<NX>
<NX>
49±0.6 ps
38±0.4 ps
54±0.8 ps
+OBJ
Pinhole
Single photon detector
ps-pulsed laser
PL
-
+
𝑄𝑌𝑋− =𝑘𝑟,𝑋−
𝑘𝑟,𝑋− + 𝑘𝐴𝑢𝑔𝑒𝑟,𝑋−𝜏𝑋− = 1/(𝑘𝑟,𝑋− + 𝑘𝐴𝑢𝑔𝑒𝑟,𝑋−)
QYX- QYX- kAuger,X- kAuger,X-
C/MS-1/S 0.24 0.15±0.1 0.19 0.29±0.13
C/MS-2/S 0.32 0.28±0.1 0.10 0.16±0.11
C/MS-3/S 0.50 0.35±0.1 0.05 0.10±0.06
•
•
•
C/MS-1/S C/MS-2/S C/MS-3/S0.0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
QY X
-
Photochemical e-doping
Single dot
C/MS-1/SC/MS-2/SC/MS-3/S0.0
0.1
0.2
0.3
0.4
k Au
ger,
X- (
ns-1
)
Photochemical e-doping
Single dot
a b
--
+
-
+
-Excitonic
interaction
e-e repulsion
Ideal case (statistical scaling)
=2
More realistic case(with Coulomb interactions)
<2
2kr < 2kr
c
C/MS-1/S C/MS-2/S C/MS-3/S0.0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
QY X
-
Photochemical e-doping
Single dot
C/MS-1/SC/MS-2/SC/MS-3/S0.0
0.1
0.2
0.3
0.4
k Au
ger,
X- (
ns-1
)
Photochemical e-doping
Single dot
a b
--
+
-
+
-Excitonic
interaction
e-e repulsion
Ideal case (statistical scaling)
=2
More realistic case(with Coulomb interactions)
<2
2kr < 2kr
c
•
•
•
•
