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Photovoltaic
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Photovoltaic Devices
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Jan Valenta is professor of quantum optics and optoelectronics at the Department
Janof Valenta
Chemical
Jan Valenta isPhysics
professor andofOptics,
is professor Charles
of quantum
quantum optics University,
optics and Prague.
and optoelectronics His research
optoelectronics isthe
at theatDepartment oriented
Department
toward Jan
of Valentaproperties
optical
Chemical isPhysics
professor and of of quantum
semiconductor
Optics, Charles optics and optoelectronics
nanostructures,
University, Prague. especially
His at thesilicon.
research Department
is Heoriented
of Chemical Physics and Optics, Charles University, Prague. His research is oriented
of Chemical
is developing Physics
special and Optics,
spectroscopy Charles and
set-ups University,
methods Prague.
to measure Hisespecially
research
photo-issilicon.oriented
and
towardtoward opticaloptical properties properties of semiconductor
of semiconductor nanostructures,
nanostructures, especially silicon. He He
toward
electroluminescence
is developing optical special properties
spectra of semiconductor
(down
spectroscopy to set-ups nanostructures,
single nano-objects),
and methods especially
optical
to measure gain, silicon.
and He
is developing special spectroscopy set-ups and methods to measure photo-photo- and and

Light Energy Harvesting with

iselectroluminescence
absolute developing
quantum special yields. His spectroscopy
other interests set-ups include andthe methods
history of to science,
measure photo-
scientific and
electroluminescence spectra (down to single nano-objects), optical gain, and and
spectra (down to single nano-objects), optical gain,

Valenta
Light Energy Harvesting with
electroluminescence
photography, and spectra
science-for-art (down
applications. to single
He is nano-objects),
co-author (with I. optical
Pelant) ofgain,
the and

Light Energy Harvesting with

absolute absolute
quantum quantum yields.yields.
His other His otherinterests interests
include include
the history the history of science, of science,
scientific scientific

Light Energy Harvesting with

Valenta
absolute
textbook quantum
Luminescence yields.
Spectroscopy His other interests include
of Semiconductors the
(Oxford, history
2012). (with of science, scientific

Valenta
photography, and science-for-art applications. He is co-author (with I. Pelant) of the the
photography, and science-for-art applications. He is co-author I. Pelant) of

Valenta| |Mirabella
Group IV Nanostructures
photography,
textbook and science-for-art
Luminescence Spectroscopy applications.
of Semiconductors He is co-author(Oxford, (with I. Pelant) of the
textbook Luminescence Spectroscopy of Semiconductors (Oxford, 2012).2012).
textbook Luminescence
received Spectroscopy of Semiconductors (Oxford, 2012). from the
Group IV Nanostructures
Nanostructures
Salvo Mirabella his laurea (1999) and PhD (2003) in physics
University ofMirabella
Salvo Salvo
andSalvo
Catania, Italy,
Mirabella received
Mirabella
Microsystems,
received
received
National
and ishis
his laurea
now
his laurea
Council
researcher at and
laurea
(1999)(1999)
(1999)
of Research
the Institute
and PhD (2003)
and(CNR
PhD (2003)
PhD IMM),
for Microelectronics
in physics
(2003)
in physics
infor
Italy.
from the
physics
His research
from the
from the Group IV IV
Group Nanostructures
| Mirabella
University Universityof of
Catania, Catania,
Italy, andItaly, is and
now is now
researcher researcher
at the at the
Institute Institute
for Microelectronics
Microelectronics
activityand isMicrosystems,
University mainlyof Catania,experimental,
Italy, andfocusing
National is now researcher
Council ofonResearch
groupat IV theadvanced
Institute materials
for His for
Microelectronics
and Microsystems, National Council of Research (CNR (CNR IMM), in IMM),
Italy. Italy.
His research research
| Mirabella

applications
and in photovoltaics
Microsystems, National (lightCouncil absorption of Research mechanisms (CNRIVIMM), Si- Italy.
or Ge-basedHis research
activity activity
is mainlyis mainly experimental,
experimental, focusing focusing on on
group group
IV advanced advanced materials materials
for for
nanostructures, sunlight-energy conversion, and transparent conductive electrodes)
Mirabella
activity
applications is mainly experimental,
in photovoltaics (lightfocusing absorption on group mechanisms IV advanced materials
inorSi-Ge-basedor Ge-based for
applications
andapplications in
microelectronics photovoltaics (light
(point-defect engineering absorption mechanisms
and dopant in Si-
diffusionin inSi-crystalline
nanostructures, in sunlight-energy
photovoltaics (light
conversion, absorption mechanisms
and transparent conductive or electrodes)
Ge-based
nanostructures,
or amorphous sunlight-energy
semiconductors andconversion, beamand
ionconversion, transparent
modification conductive
of materials). electrodes)
nanostructures,
and microelectronics sunlight-energy
(point-defect engineering and transparent
and dopant conductive
diffusion inelectrodes)
crystalline
and microelectronics (point-defect engineering and dopant diffusion in crystalline
and microelectronics
or amorphous (point-defect
semiconductors and engineering
ion beam and dopant
modification diffusion in crystalline
of materials).
or amorphous semiconductors and ion beam modification of materials).
or amorphous semiconductors and ion beam modification of materials).
V411
V411
ISBN 978-981-4463-63-8
V411
V411 V411 V411 V411
ISBN 978-981-4463-63-8
ISBN 978-981-4463-63-8
V411
ISBN 978-981-4463-63-8
Nanotechnology and
Photovoltaic Devices
Pan Stanford Series on Renewable Energy — Volume 2

Nanotechnology and
Photovoltaic Devices
Light Energy Harvesting with
Group IV Nanostructures

editors
Preben Maegaard
Anna Krenz edited by
Wolfgang Palz
Jan Valenta and Salvo Mirabella

The Rise of Modern Wind Energy

Wind Power
for the World
CRC Press
Taylor & Francis Group
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© 2015 by Taylor & Francis Group, LLC
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March 12, 2015 16:6 PSP Book - 9in x 6in 00-Valenta–prelims

Contents

Preface xiii

1 Introduction to Photovoltaics and Potential Applications of

Group IV Nanostructures 1
Jan Valenta and Salvo Mirabella
1.1 Energy from the Sun 2
1.2 The Basic Principles of Photovoltaic Solar Cells 5
1.2.1 Energy Balance 5
1.2.2 Energy Conversion: Efficiency and Limits 7
1.3 Advanced Concepts for Photovoltaics 10
1.3.1 The Multijunction Approach 13
1.3.2 Up- and Down-Conversion 13
1.3.2.1 Wavelength conversion 13
1.3.2.2 Intermediate-band SCs 15
1.3.2.3 Carrier multiplication 15
1.3.3 Hot-Carrier Extraction 16
1.4 Group IV Nanostructures 16
1.4.1 Prospects of Nanomaterials in Photovoltaics 18
1.4.2 Light Management in Solar Cells 19
1.5 Conclusions 21

2 The Dielectric Function and Spectrophotometry: From Bulk

to Nanostructures 27
Caterina Summonte
2.1 Introduction 27
2.2 The Dielectric Function: Why do we Need an
Approximation? 29
2.2.1 Electromagnetic Mixing Formulas 29
2.3 The Dielectric Function at the Nanoscale 31
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vi Contents

2.3.1 Silicon Nanoparticles 32

2.3.2 Germanium Nanoparticles 34
2.3.3 Nanowires 35
2.3.4 Graphene 36
2.4 Measurements and Elaboration 36
2.4.1 Volume Fractions of Composite Materials 36
2.4.2 R&T Spectroscopy Experimental Setup 38
2.4.3 Elaboration of R&T Spectra 39
2.4.3.1 Determination of absorption 39
2.4.3.2 Determination of the optical gap 41
2.4.3.3 Qualitative evaluation of R&T spectra 43
2.4.3.4 Single layer on a transparent substrate 45
2.4.3.5 Spectral forms for the DF 47
2.4.4 The Generalized Transfer Matrix Approach 47
2.5 R&T Spectroscopy Applied to Nanoparticles 48
2.5.1 Single-Layer Approach 48
2.5.1.1 Management of the unknown
parameters 48
2.5.1.2 Determination of the dielectric
function of nc-Si 49
2.5.1.3 Volume fractions and Si crystallized
fractions 49
2.5.1.4 Detection of a low-density surface
layer 50
2.5.1.5 Phase separation in silicon-rich oxides 51
2.5.2 Single Layers and Multilayers 52
2.6 Conclusions 53

3 Ab initio Calculations of the Electronic and Optical

Properties of Silicon Quantum Dots Embedded in Different
Matrices 65
Roberto Guerra and Stefano Ossicini
3.1 Introduction 65
3.2 Structures 68
3.2.1 Embedded Silicon Quantum Dots 69
3.2.2 Freestanding Quantum Dots 71
3.3 Results 72
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Contents vii

3.3.1 Amorphization Effects 73

3.3.2 Size and Passivation 75
3.3.3 Embedding Insulating Materials 77
3.3.4 Optical Absorption 77
3.3.5 Applicability of Effective Medium
Approximation 78
3.3.6 Strain 81
3.3.7 Local-Field Effects 83
3.3.8 Ensembles of Quantum Dots 86
3.3.9 Beyond DFT 87
3.4 Conclusions 90

4 Silicon Nanoclusters Embedded in Dielectric Matrices:

Nucleation, Growth, Crystallization, and Defects 99
Daniel Hiller
4.1 Introduction 99
4.2 Silicon Quantum Dot Formation 102
4.2.1 Preparation Methods 102
4.2.2 Phase Separation for Matrix-Embedded Si
QDs 104
4.3 Silicon Quantum Dot Crystallization 108
4.4 Silicon Nanocrystal Size Control and Shape 111
4.4.1 The Superlattice Approach 113
4.5 Silicon Nanocrystals: The Role of Point Defects 116
4.5.1 Identification and Quantification of Defects 116
4.5.2 Classification of Point Defects 117
4.5.2.1 Defects in the Si/SiO2 system 118
4.5.2.2 Defects in the Si/Si3 N4 system 120
4.5.2.3 Defects in the Si/SiC system 121
4.5.3 Influence of Interface Defects on PL 122
4.5.3.1 Interaction of defects with PL in
SiO2 -embedded Si NCs 122
4.5.3.2 Interaction of defects with PL in
Si3 N4 -embedded Si NCs 128
4.5.4 Influence of Interface Defects on Electrical
Transport 129
4.6 Conclusions 130
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viii Contents

5 Excited-State Relaxation in Group IV Nanocrystals

Investigated Using Optical Methods 145
František Trojánek, Petr Malý, and Ivan Pelant
5.1 Introduction 145
5.2 Experimental Methods 147
5.2.1 Pump and Probe Technique 147
5.2.2 Up-Conversion Technique 150
5.2.3 Transient Grating Technique 152
5.2.4 Time-Resolved Terahertz Spectroscopy 153
5.3 Femtosecond Phenomena 154
5.4 Picosecond and Nanosecond Phenomena 165

6 Carrier Multiplication in Isolated and Interacting Silicon

Nanocrystals 177
Ivan Marri, Marco Govoni, and S. Ossicini
6.1 Introduction 177
6.2 Carrier Multiplication and Auger Recombination in
Low-Dimensional Nanosystems 181
6.3 Theory 183
6.4 One-Site CM: Absolute and Relative Energy Scale 186
6.5 Two-Site CM: Wavefunction-Sharing Regime 191
6.6 Conclusions 199

7 The Introduction of Majority Carriers into Group IV

Nanocrystals 203
Dirk König
7.1 Introduction 203
7.2 Theory of Conventional Nanocrystal Doping 205
7.2.1 Thermodynamics: Stable vs. Active Dopant
Configurations 206
7.2.2 Electronic Properties: Quantum Structure vs.
Point Defect 214
7.2.3 Phosphorous as an Example: Hybrid Density
Functional Theory Calculations 218
7.3 Survey on Experimental Results of Conventional Si
Nanovolume Doping 226
7.3.1 Si Nanovolumes in Next-Generation
Ultra-Large-Scale Integration 226
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Contents ix

7.3.2 Free-Standing Nanocrystals 227

7.3.3 Embedded Nanocrystals Formed by
Segregation Anneal 231
7.4 Alternatives to Conventional Doping 240
7.4.1 Modulation Doping 240
7.4.2 Exploiting Interface Energetics: Nanoscopic
Field Effect 244
7.5 Conclusion and Outlook 244

8 Electrical Transport in Si-Based Nanostructured

Superlattices 255
Blas Garrido, Sergi Hernández, Yonder Berencén,
Julian López-Vidrier, Joan Manel Ramı́rez, Oriol Blázquez,
and Bernat Mundet
8.1 Introduction and Scope 255
8.2 Superlattices and Minibands 256
8.3 Amorphous and Nanocrystal Superlattices 262
8.4 Transport in Nanocrystal Superlattices 267
8.4.1 Semiclassical Miniband and Band Transport 269
8.4.2 Transport with Field-Assisted Carrier
Exchange between Localized and Extended
States 272
8.4.3 Conduction through Localized States (Hopping
by Tunneling) 274
8.4.4 Injection and Space Charge–Limited Currents 278
8.4.5 Horizontal Transport 280
8.5 Vertical Transport in SRO/SiO2 Superlattices 283
8.6 Transport in SRON/SiO2 and SRC/SiC Superlattices 289
8.6.1 Horizontal Transport in SRC/SiC Superlattices 289
8.6.2 Vertical Transport in SRON/SiO2 Superlattices 293
8.7 Conclusions 299
Appendix A Band Structure of Nanocrystal
Superlattices 300
Appendix B Semiclassical Conduction in the
Extended States of a Superlattice 306
Appendix C Generalized Trap-Assisted Tunneling
Model 310
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x Contents

9 Ge Nanostructures for Harvesting and Detection of Light 317

Antonio Terrasi, Salvatore Cosentino, Isodiana Crupi,
and Salvo Mirabella
9.1 Introduction 317
9.2 Light Absorption, Confinement Effects, and
Experimental Methods 320
9.3 Synthesis of Ge Nanostructures 324
9.4 Light Absorption in Germanium QWs 329
9.5 Confining Effects in Germanium QDs 334
9.5.1 Matrix Effects: SiO2 vs. Si3 N4 334
9.5.2 QD–QD Interaction Effects 337
9.6 Light Detection with Germanium Nanostructures 342
9.7 Conclusions 348

10 Application of Surface-Engineered Silicon Nanocrystals

with Quantum Confinement and Nanocarbon Materials in
Solar Cells 355
Vladimir Svrcek and Davide Mariotti
10.1 Introduction 356
10.2 Si NC Surface Engineering in Liquids 358
10.3 Surface Engineering of Doped Si NCs 362
10.4 Tuning Optoelectronic Properties of Si NCs by
Carbon Terminations 364
10.5 Functionalization of Surface-Engineered Si NCs
with Carbon Nanotubes 366
10.6 Solar Cells Based on Si NCs and Nanocarbon
Materials 369
10.7 Conclusions and Outlooks 373

11 Prototype PV Cells with Si Nanoclusters 381

Stefan Janz, Philipp Löper, and Manuel Schnabel
11.1 Introduction 381
11.2 Motivation 382
11.3 Material Selection 384
11.4 Current Collection 389
11.5 Doping 391
11.6 Device Concepts for Si NC Test Structures 393
11.7 Device Results 398
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Contents xi

11.8 Tandem Solar Cell Development 410

11.8.1 Current Matching 412
11.9 Future Trends 413
11.9.1 Thermal Budget–Compatible Processing 413
11.9.2 Increased Conductivity of the Si NC
Material 413
11.9.3 Reduction of Electronic Defects 414
11.10 Conclusion 415

Index 425