Wavelength (nm) Time (ps) 0 20 40 60 80 100 120 140 Time (ns)

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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