Quantum Dot based Photonic Devices

Muhammad Usman

Tyndall National Institute, Lee Maltings, Cork Ireland

Network for Computational Nanotechnology (NCN), Purdue University, West
Lafayette IN, USA

Email: usman@alumni.purdue.edu
Web: http://web.ics.purdue.edu/~usman
 Ireland

Muhammad Usman
 Tyndall National Institute
Based in Cork, at Lee Maltings
Hosts about 450 full time
researchers and support staff,
including about 125 PhD students
from 38 nationalities

Dublin

Cork (UCC, Cork IT, Tyndall)

Muhammad Usman Borrowed from Prof. Eoins presentation
 Cork

Based in Cork, home of Henry Ford

Dublin

Cork (UCC, Cork IT, Tyndall)

Muhammad Usman Borrowed from Prof. Eoins presentation
 Outline

What are self-assembled semiconductor quantum dots?

Quantum dot based photonic devices Fundamental requirements
Strain engineered quantum dots
InGaAs strain reducing capping layer
Bilayers
Multi-layers
Quantum dot modeling challenges NEMO 3-D Simulator
Overview of my research work
Summary

Muhammad Usman
 What are Quantum Dots?
Man-made nano-scale structures in which electrons are confined in all 3 dimensions
Bulk Quantum Well Quantum Wire Quantum Dot

Atom Small Dye Molecule Fluorescent Protein Bacterium Animal Cell

D(E) D(E) D(E) D(E)

Electronic
1Ao
structure:
1nm 10nm 100nm 1um 10um 100um
E E E E
Electron energy is quantized -> artificial atoms (coupled QD->molecule)
Contains a countable number of electrons
Quantum Dot

Photon Photon Tunneling/Transport

Absorption Emission Occupancy of states

Detectors/ Lasers/ Logic / Memory

Input Output
Quantum dots are artificial atoms that can be custom designed for a variety of
Muhammad Usman
applications
 QD Example Implementations
Fabrication

I. Stranski - L.
Krastonov, 1938 Colloidal,
CdSe, ZnSe
Self-assembled ,
InGaAs on GaAs.

Pyramidal or
dome
shaped http://www.research.ibm.com/journal/rd/451
R.Leon,JPL(1998)
Electrostatic
Gates,
GaAs, Si, Ge
Create electron
puddles
Fluorescence induced by exposure
to ultraviolet light in vials containing
various sized cadmium selenide
Source: http://www.spectrum.ieee.org/WEBONLY/wonews/aug04/0804ndot.html (CdSe) quantum dots.
Source: http://en.wikipedia.org/wiki/Fluorescent

Muhammad Usman
 How do we get QDs? Stranski-Krastanov Growth
Self-Assembly Process InAs deposition on GaAs substrate
InAs (0.60583 nm) First Layer (wetting layer) ~ 1ML

GaAs (0.56532 nm)

Capping Layer
Quantum Dot
GaAs
Wetting Layer

InAs

InAs
QDs grown by self-assembly process have:

o Rough/AsymmetricGaAs
Interface
GaAs
o Strain
Substrate
Muhammad Usman o Stress-induced Polarization
 Quantum Dots Photonic Devices
Self Assembled Quantum Dots

Laser Photo-detector/Amplifier IB-Solar Cells

S. J. Xu Prof. Okada
Dept. of Physics , University of Hong Kong

Fujitsu
Temperature Independent QD laser
2004

While quantum Information Science is rapidly progressing, and QD based optical

Muhammad Usman devices are already available in the market !
 QDs based photonics Basic Requirements?

Requirement 1: Optical Emissions at 1.3,1.5m for optical fibers

Requirement 2: Optical Emissions should be polarization insensitive

Do QDs obtained from Stranski-Krastonov self-assembly process fulfill these

requirements?

NO

Muhammad Usman
 How Strain changes the Energy Band Edges?

[001]
xx+yy+zz GaAs

xx+yy-2zz
InAs QD

GaAs

Muhammad Usman
 QDs based photonics Basic Requirements

Requirement 1: Optical Emissions at 1.3-1.5m for optical fibers

1.1-1.2
m Single In(Ga)As QD

+InxGaAs
+Sb +Bi +N QW

1.3 Multi-layer
m InAs QD Bilayer InAs QD Stacks
InAsSb inside QD Stack
InxGaAs
QW
InGaNAs
InAs QD
Large InAs
1.5 Stack
GaBiAs QD Stack
m Inside
(Columnar
InxGaAs
QD)
QW

Band gap Engineering Strain Engineering

Muhammad Usman
 Poor Polarization Response
Requirement 2: Optical Emissions should be polarization insensitive

E3-H1 CB
E3 Large compressive biaxial strain
E2
splits HH and LH bands i.e.
E2-H1
highest few valence band states
E1
are HH
E1-H1
HH VB HH states does not couple to TM
H1
H2 mode (along 001 growth direction)
H3
LH due to their xy symmetry, TE mode
is dominant
First few VB states are
HH states due to biaxial strain Polarization response is measured
A typical Experimental Setup in terms of degree of polarization
TE TM
DOP =
Growth TE + TM
TE >> TM DOP ~ 1.0
Desired value of DOP is 0

Muhammad Usman
 I-Single InAs QDs, with InGaAs SRCL

M. Usman et al., IEEE Transactions on Nanotechnology, Vol. 8, No. 3, (2009)

Experiment:
Y. Aarakawa, Tokyo University Japan

Muhammad Usman
 Strain Band Edge
Deformations

Hydrostatic strain relaxation Band gap reduction Red shift of spectra

Biaxial strain reinforcement LH bands move opposite of HH bands
HH states
Muhammad dominate for large In concentrations! => Strong binding
Usman Ref: IEEE Trans. on Nanotechnology, vol. 8, No. 3, May 2009, pp.330-344
 QD Aspect Ratio Changes
SRCL introduces large in-plane strain
vertical strain is relaxed
Base decreases
Height increases

Aspect Ratio of QD Increase !

H red shift of emission spectra

B blue shift of emission spectra
E
H = 0.5 AR 3 RED SHIFT OF EMISSION SPECTRA
E
B
Ref: Phys. Rev. B 74, 245331 (2006)

Muhammad Usman AR + Strain Relaxation = Red Shift

Ref: IEEE Trans. on Nanotechnology, vol. 8, No. 3, May 2009, pp.330-344
 What is the reason for nonlinearity in experiment and theory?

NEMO 3-D (red line) matches

Electron energy levels Hole energy levels experiments non-linear behavior
change linearly change nonlinearly (black lines) ?

Nonlinearity Comes from Holes !

Ec = -5.08H
EHH = H 0.9 B
Biaxial Strain causes Nonlinearity !

Muhammad Usman Ref: IEEE Trans. on Nanotechnology, vol. 8, No. 3, May 2009, pp.330-344
 II-Bilayer QDs, with and without SRCL
M. Usman et al., Journal of Applied Physics 109, 104510 (2011)
M. Usman, Journal of Applied Physics 110, 094512, (2011)

Experiment: R. Murray, Imperial College London

Muhammad Usman
 1300nm+ Quantum Dot Devices
o Upper QD is optically active
o ~77nm red shift for QD Stack
o ~122nm red shift for QD Stack with SRCL
o Stacks of QDs provide red shifts of emission
spectra

Muhammad Usman
 How theory can help in understanding experiments?

Experimental Measurement: Top view of upper QD in bilayer QD stack

TE[110]
------------ = 1 + 0.1
TE[-110]

Hole Energy Level H1 is oriented along [110] direction

Hole energy levels are closely packed H1-H3 ~ 12.5meV < 1/2kT ~ 12.9meV

NEMO 3-D Calculations:

TE[110]
------------- ~11.4 1.52 1.07
TE[-110]

Multiple valence band energy levels

should be considered for RT ground
Muhammad Usman state optical emissions!
 Bilayers slightly improved polarization response

For bilayers, polarization

response was improved,
but we were not quite
there yet

Muhammad Usman
 III- Multi-Layer QD Stacks,
3, 6, and 9 QD Layers
M. Usman et al., Physical Review B 84, 115321 (2011)

Experiment:
T. Kita, Kobe University Japan

Muhammad Usman
 TM mode increases due to HH/LH intermixing

9
Muhammad Usman
 In-plane polarization anisotropy still plays a role

For 9 QD layers, TE110 < TM001

Muhammad Usman
 Hole wave functions are asymmetric

9 How can we design QDs for TE??? < TM001

E-fields
Geometry anisotropy, QD elongation along 110
Use of novel capping layers
Muhammad Usman
 Quantum Dot Modeling Challenges

NEMO 3-D Atomistic Simulator

Muhammad Usman
 What is required in a theoretical model for QDs?
Quantum Dots grown by self-assembly process have atomistic granularity!

Interface roughness and assymetry GaAs

Arbitrary alloy configuration
Long range strain InAs

Non-parabolic dispersion InGaAs

Piezoelectricity

IEEE Trans. on Nanotechnology (2009)

nanoHUB.org
Biaxial Strain

GaAs buffer
Strain Yes
Piezo No 60nm
InAs Dome QD
Strain Yes
Piezo Yes

What
In proc.we need:
of the IEEE (1) Atomistic calculation of strain, piezoelectricity, and Inelectronic
NEMS (2008) structure
proc. of the IEEE Nano (2008)

(2) Large simulation domain ~ millions of atoms!

Muhammad Usman
 NEMO 3-D A fully atomistic simulation tool
Input Deck Methodology1:

o Experimental geometry in input deck

Geometry
Construction
o Strain is calculated using Valence
Force Field (VFF) Method2,3
Atomistic
Relaxation o Linear and Quadratic Piezoelectric
potentials by solving Poissons
Piezoelectric Strain equation over polarization charge
Potential density4
Hamiltonian Electrical / o Empirical tight binding parameters --
Construction Magnetic field
sp3d5s* band model with spin orbital
coupling5
Capabilities:
Eigen Solver

o Arbitrary shape/size of devices

Optical Single Particle o Modeling of all III-V and IV materials and devices
Transition
Strengths
Energies o Interface roughness, atomistic representation of alloy
o External Electrical/Magnetic fields
Excitons o Zincblende/Wurtzite crystals
[1] IEEE Trans. Electron Devices,54, 9. (2007)
[4] Phys. Rev. B 76, 205324 (2007)
Muhammad Usman [2] Phys. Rev. 145, no. 2, pp.737 (1966)
[5] Phys. Rev. B 66, 125207 (2002)
[3] Appl. Phys. Lett. 85, 4193 (2004)
 Modeling of Growth Dynamics
InAs/GaAs QDs obtained by the self-ordering Stranski-Krastanov process are
significantly influenced by In-Ga intermixing and In-segregation effects during the
capping and post-growth annealing processes.

A complex QD composition
profile, which is strongly related
to the growth conditions.
A pure InAs or uniform InGaAs
type composition profile does
not explain experiment!
Systematic set of simulations
leads us to innovative two-
layered composition profile, in
accordance with experimental
findings.
Polarization response and
optical gap accurately
described.

M. UsmanMuhammad
et al., in press,
UsmanNanotechnology, (2012)
 Bilayer QD Molecule
Electrical Field Tuning of Excitons for QIP
Objective
o Coupling of bilayer QD electronic structure
under [001] electrical field
o Understand experimental optical strengths
identification of electronic states
Approach
o Electronic structure calculation
Experimental device geometry
[001] Electrical field from 15 to 23kV/cm
Strain, Linear and Quadratic piezoelectricity
o Optical transition strengths
Impact:
o First hole energy level H1 always in upper QD
o First two electron energy levels E1, E2 are in
the lower QD in the range of applied field
E1-H1, E2-H1 are dark excitons
o E3 and E4 exhibit inter-dot tunneling
E3-H1 and E4-H1 anti-cross at 18.4kV/cm
o Calculated anti-crossing quantitatively match
experimental measurement
M. UsmanMuhammad
et al., Nanotechnology,
Usman 22, 315709 (2011)
 Novel Materials for photonics and photovoltaics

First sp3s* tight binding parameter

set is reported for GaBi

Valence force field model is set up

to study Bismuth based random
alloys such as GaBiAs, GaBiP,
GaBiNAs, InGaBiAs etc

Bi-related defect state interact with GaAs

valence band via band-anticrossing interaction

Eg-so crossover indicates strong potential for

suppression of Auger recombination losses

14-band kp model is derived and investigation

of optical device performance underway
M. Usman et al.,Usman
Muhammad Phys. Rev. B 84, 245202 (2011)
 Education & Outreach

To promote Research, Collaboration, Education, User-friendly open source

Computation
Network for Computational Nanotechnology funded by National Science Foundation
Free access to all the simulation tools, learning modules, and teaching materials
Leader: Purdue, Other partners: Stanford, UIUC, UC Berkeley, Northwestern
Over 200,000 annual users, 354,607 simulations, 230 simulation tools, 64 video
courses and many more
Recently nanohub-university is established
Muhammad Usman
 Summary
We have developed a multi-scale atomistic simulator (NEMO 3-D) capable of
performing multi-million atom strain and electronic structure calculations with
Accurate description of material and device properties
Realistic sizes of simulation domains, scalable to 100 million atoms
Flexibility to a wide range of III-V and IV materials and devices

Applications:
Photonic devices based on quantum dots
Modeling of growth dynamics, may lead to an era of nano-TCAD
Quantum information science by charge or spin control in quantum dot
molecules
Novel materials and heterostructures for efficient photovoltaics
Muhammad Usman
 Acknowledgements
Prof. Gerhard Klimeck (Purdue, USA) and Prof. Eoin P. OReilly (UCC, Ireland)

Prof. Shaikh Ahmed (Southern Illinois University, IL, USA)

Prof. Timothy Boykin ( University of Alabama in Huntsville, AL, USA)

Prof. R. Murray (Imperial College London, UK)

Dr. Edmund Clark (Sheffield University, UK)

Prof. A. Passaseo (National Nanotechnology Labs, Lecce, Italy)

Prof. Takashi Kita (Kobe University Japan)

Prof. Stephen Sweeney (University of Surrey, UK)

Many thank to Prof. Christopher Levey for arrangement of this talk!

Muhammad Usman