Subject Index

Page numbers in italics refer to index entries in gures or tables.

absorption coecient 55absorption length 55, 56, 57accumulation layer 274activation barrier 411activation energy 2078adiabatic process 2778adsorption energy 279, 283AgBiW2O8 301, 3201algae 391, 398, 400allometric scaling law 433alumina 58, 69aluminium gallium nitride 195, 196,

197growth method 198materials improvement 21415point defects 2069system 2009

aluminium nitrideband gap alignments 1957properties 1945, 2003

AM1.5G spectrum 366, 367amorphous silicon (a-Si) 923, 95, 163annealing process 136, 137anomalous small angle X-ray

scattering (ASAXS) 182anti-phase disorder 249, 250aqueous CO2 reduction 3468arrays see microwire arrays;

photovoltaic (PV) arrays; spotarray electrodes

aryl halides 345, 346atomic force microscopy (AFM) 202,

237, 238

atomic layer deposition (ALD) 67, 69azimuthal symmetry 434, 435

B800/B850 rings 3945, 397BAC model 226, 227, 254back DSSC conguration 97background current 136, 143bacteria 391, 394, 397, 398bacteriochlorophylls (BChl) 3945,

397, 398band alignments

group III-nitrides 1957group III-Vsemiconductors 2279

band bending 46, 235, 360InP 248in nanostructures 24and overpotential 29and plasmonicnanoparticles 275

band edge energies 7, 8, 423metal oxides 3001, 302photoelectrode/PV 934

band gaps 56, 360design 26970direct and indirect 55, 61, 225,

226, 269doping eects 149, 170GaP tandem systems 254group III-nitrides 194, 1957group III-V systems 2256InGaN 215, 216, 217metal nitrides 119, 121

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metal oxides 267, 270metal oxynitrides 112, 114, 270PCEs 3701, 376S2 water splitting scheme 84singlet ssion molecule 375solar photoelectrolysis 89tandem cell concept 86vs PCE 366, 367, 368, 369in water splitting 110, 111, 364

band structures see energy bandstructures

barium tantalum oxynitride(BaTaO2N) 111, 124

Bell Laboratories 1bi-layer steps 202bias voltage 29, 30, 360, 3612bilin 398binary group III-nitrides 194, 195

aluminium gallium nitridesystem 2009

band alignments 196valence band position 197

binary group III-V, band alignments227

binary oxides, manganese 1658,1708

binodal critical points 203biomass 16, 267birnessite 162, 163, 164, 1656, 168,

170bismuth vanadate 678, 136, 138,

142, 438Bi-V-W oxide system 678doping and defect control 189doping eects 149, 150linear sweep voltammograms148, 149

tungsten-doped 146, 147black silicon 70Bode plot 41BornOppenheimer approximation

(BOA) 277bottom-up synthesis 70, 256bowing parameters 195, 196, 197bromine-methanol etch 237, 238Brnsted acids 344

Brownian walk 428, 429brute force strategies 856bulk lm electrodes 1489

hot carriers in 36971buried p-n junctions 248, 37986buserite 163, 166Butler Volmer equation 26, 42

cadmium sulde 20, 39calcination 66, 115, 125calcium complexes

Ca2Mn3O8 170CaFe2O4 101CaMn4Ox cluster 157, 162,1645

CaTaO2N 117Calvin cycle 335, 336capacitance measurements 150capture cross section 28, 32carbon dioxide emissions 13, 16, 333carbon dioxide xation 335, 336carbon dioxide hydrogenation

33742, 3523carbon dioxide reduction 155

electro- andphotocatalytic 28998

electrochemical 34254energetics 299301, 302energy and potential scheme

423using heterogeneouscatalysis 298, 33640

using homogeneouscatalysis 298, 3402

molecular catalysts 3016photoelectrochemical 1216,3512

Pt-C-TiO2 nanocomposites30613

using semiconductornanoparticles 3205

thermodynamics 299transition metal complexesfor 31319

carbon energy cycle 334carbon feedstock 333

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carbon monoxide 304, 305, 31317,321

electrochemical CO2 reduction344, 345, 3479

homogeneous catalysis of CO23412

from RWGS reaction 3367carbon monoxide dehydrogenase 348carbon nitride 115carboxylation, electrochemical 3456carotenoids 394, 4001carrier multiplication 9, 3789catalysis/catalysts

molecular 3016oxidation and reduction15661, 162

at structured semiconductors634

water splitting by structuredmaterials 714

see also electrocatalysis/electrocatalysts;heterogeneous catalysis;homogeneous catalysis;photocatalysis/photocatalysts

cell body 141, 143Central Limit Theorem 428cerium catalysts 336charge transfer 2779

and recombination 304charge transfer insulator 439, 440chemical catalysis 343chemical energy storage 1556chemical vapor deposition (CVD) 65,

434see also metal-organic chemicalvapor deposition (MOCVD)

chemicurrent 277a-chloroethylbenzene 346chlorophylls 390, 391, 398, 4001

bacteriochlorophylls 3945,397, 398

chromium oxide 71, 1201chromophores 382

generalized Forster theory 391in LH2 complex 397400

molecular 3748, 390in multi-subunit proteins 3946weakly-coupled 3914

coal production 1315cobalt catalysts

CO2 reduction 2934, 352Fischer-Tropsch 340

cobalt-molybdenum alloys 73cobalt oxide 65, 67, 68, 734, 142

as electrocatalyst 146, 147oxygen evolving catalyst 162,

163cobalt(II) solution 379colloidal particles 71combinatorial techniques 10, 445complex plane plot 41computational approaches 74, 270,

444, 445COMSOL multiphysics 62concentration overpotential 623conduction band edge 4, 93conduction band energy 55, 91conductivity, AlGaN alloys 2069contour plot, D4 devices 89convective transport 61copper

bonding to water 41415IR spectra 411water dissociation 411XAS spectra 409, 410, 411

copper catalysts 3367, 3389copper electrodes 34850copper oxide 69, 101, 102

band edge energies 301in CO2 reduction 3215

cost of hydrogen production 1112,104

Coulomb interaction 3912Coulomb repulsion 439coupled Forster excitation energy

transfer 4247coupling parameter 393, 396crack propagation 436, 437crystal momentum diagram 55crystalline semiconductors 549

see also nanocrystals

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current densitymanganese oxides 1745, 178photoanode/DSSC 100photocurrent 5960, 88photoelectrode/PV 94, 95ruthenium selenide 186saturation current 5960

current versus voltagedependence 365

current-voltage curves (j-U)InP 240photoanode/DSSC 100photocatalyst 143, 144photoelectrode/PV 94tandem photoelectrodes 368

cut-o wavelengths (l1 and l2)8990

cyclams 316, 317, 344, 348cyclic polarization 240cyclic voltammetry 170, 171, 175,

176, 177, 178, 185Pt-C-TiO2 3078, 309, 310

d-band model 414d-band splitting 438, 439, 440d0-oxynitrides 113, 114

water reduction activity 11417water splitting using 1248

D4 devicesarchitectures 91, 92photoanode/photocathodesystems 1002

strategy 8790d10 metal nitrides 11718dactylogram 435Debye length 23deleterious currents 59density functional theory (DFT) 10,

160, 269, 2712, 276, 277models 745

depletion layer 274, 363desorption 410, 41112deuterium oxide 409, 412Dexter electron exchange 392, 425dierential electrochemical mass

spectroscopy (DEMS) 171, 172, 173

diuse reectance spectra (DRS) 112,114, 119, 122

diusionof light 427superdiusion 428, 430

diusion length 567minority carrier 22, 23, 30

diusion-limited aggregationmodel 4356

diusive transport 61direct band gap 55, 61, 225, 226,

269dislocation densities 195, 2012, 210dissociation 410, 41112

partially dissociated waterlayer 40711

donor-acceptor system 3912, 394,396, 424, 425, 4267

doping eects 14950band gaps 149, 170and defect control 189electronhole separation 277

driving potential 280drop-casting 148dye-sensitized solar cell (DSSC) 61,

69, 91photoanode/DSSC 96100

electrocatalysis/electrocatalysts1458

characterization 1869CO2 reduction 28998, 3016criteria in development 190heterogeneous 34651homogeneous 3436oxygen evolving 16178

electrochemical carboxylation 3456electrochemical cells 133

NEXAFS measurements 184scheme and picture 181surface preparation 179see also photoelectrochemicalcells (PECs)

electrochemical CO2 reduction34254

electrochemical conversion 27984

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electrochemical quartz crystalmicrogravimetry (EQCM) 322, 325

electrochemical transport 613electrode potential

and adsorption energy 279nanocomposites 311perturbation 25, 40

electrodesbulk lm 1489, 36971fuel cell electrodenanocomposites 30613

gas diusion 155normal hydrogen electrode 299,

300, 361rotating disk 185, 186standard calomel electrode 361standard hydrogenelectrode 279

structural aspects 4338surface functionalization17886

see also metal electrodes; n-typeelectrodes; p-type electrodes;photoelectrodes; spot arrayelectrodes

electrolyte redox couple 360electron anities 360

group III-nitrides 203InP 248

electron energy levelssemiconductor-electrolytejunction 274

singlet ssion molecules 376electron energy scheme 84, 86, 92electron ux 99, 100electronhole pair multiplication

(EHPM) 372electronhole pairs

PCEs 36971separation 2727

electron hopping 440, 441electron scavengers 11electron transfer 2778

microwave reectivitymeasurements 427

multiple proton-coupled 299

in plants 390rate constant 268and recombination 304

electron tunneling 440, 441electronegativity equilibration 243ellipsometry 442energy band structures

InP 2479metal oxides/oxynitrides 111, 112tantalum compounds 113titania and hematite 442transition metal oxides 4389,

440energy level diagrams

CO2 reduction 423metal nitrides 120photochemical diode 361photoelectrolysis cell 263semiconductor-electrolytejunction 360

tandem photoelectrolysiscell 381

energy lossD4 devices 88, 89, 90processes 845

energy saved eciency method 5energy transfer

coupled Forster excitation4247

in nature 3904, 397epitaxial alloy fabrication 1979epitaxial III-V systems 22531equilibrium potentials, CO2

reduction 342, 343escape cone 422ethylene glycol 137ethylene production 34850excitation energy transfer 4247extended X-ray absorption ne

structure (EXAFS) 169, 170, 175,176, 177, 180, 189

external bias voltage 29, 360, 3612

feedback 137femtosecond-resolved 2-photon

photoemission (fs-2PPE) 233, 2556

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Fermi level pinning 21, 27, 32, 33, 38,275, 364

Fermi levels 2930, 3614Fermis golden rule 269, 393ber optic 133, 138, 139, 1401, 142,

143eld eect transistor (FET) 195lm relaxation 205, 206Fischer-Tropsch catalysts 340Fischer-Tropsch process 320, 349at band potential 201, 274, 360,

362, 364uorine-doped tin oxide (FTO) 125,

133, 136, 137, 142, 148formaldehyde 303, 345formate 303, 305, 31317, 320, 341

electrochemical CO2reduction 344, 345, 351

formate dehydrogenase 348formate-mechanism 337, 338, 339formic acid 303, 320, 3401, 345, 347Forster radius 393, 4245Forster Resonance Energy Transfer

(FRET) 3914fossil fuels 266, 333Fourier transform infrared

spectroscopy (FTIR) 233, 445fractals 4337fractional energy yield 158, 159free energy diagram 349free OH-groups 411Frenkel excitons 395front DSSC conguration 96, 97, 98fuel cell electrode nanocomposites

30613

gallium arsenide 38, 55, 56, 70electrochemical CO2 reduction352

MOCVD 230photoelectrode/PV system 93

gallium indium arsenide 226gallium indium phosphide 93, 101, 226gallium nitride 11822

band gap alignments 1957properties 1945, 2003

gallium phosphide 71, 225band alignments 227GaPN/GaPNAs 230, 254hetero-interfaces 24958MOCVD 2324photoanode/photocathodesystems 1001

preparation 2501Si tandem system 2534water interface 2513water splitting 229

gallium-rich surface 251, 252galvanostatic electrolysis 311Gartner equation 22, 23, 31, 32, 33gas bubbles 61, 1034gas chromatography

CO2 reduction 321Pt-C-TiO2 312

gas collection 103, 104gas diusion electrodes 155gas phase water 412gas separation 75, 103Gaussian function 428, 429generalized Forster theory 391, 3947geometric scan rate 141germanium, amorphous silicon

(a-Si) 95germanium nitride 11718germanium oxide 121, 122Gibbs free energy 283glass frit/membrane 7, 103, 104GLLB-SC 269, 270glyceraldehyde 3-phosphates 335gold nanoparticles 66, 70Gratzel cell 374, 382group III-nitrides 1937

AlGaN system 2009fabrication 1979InGaN system 20914materials improvement/integration 21415

group III-V semiconductors 2245,2589

band alignments 2279heteroepitaxy 2301micro-and nanostructured 2548

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group III-V semiconductors(continued)

preparation 2314solar energy conversion 22531water splitting 22930

growth temperature 211, 212, 214

H-down water layer 40711H-up water layer 40711Haber Bosch process 16haloacids, photoelectrolysis 34Hamilton operator 439, 440, 441hausmannite 164, 170Helmholtz capacitance 21, 27Helmholtz layer 21, 25, 27, 32, 39Helmholtz layer potential drop 360,

364hematite see iron oxideHER see hydrogen evolution reaction

(HER)heteroepitaxy 2301heterogeneous catalysis

CO2 reduction 298, 33640electrocatalysis 34651modeling 745

heterojunctions, III-Vsemiconductors 228, 229

heterostructuresGaP 24958InGaN 20910InP 23549

high aspect ratio structures 6971high frequency resistance 40high resolution electron energy loss

spectroscopy (HREELS) 238hits in screening 133, 144, 148hole scavengers 11homogeneous catalysis

CO2 reduction 298, 3402electrocatalysis 3436

hot carriers 36971hot electrons/hot holes 273hot excitons 3714Hubbard band 439, 440hybrids, reduction using 31719hydride formation 305, 306, 314, 341

hydride vapor phase epitaxy 198hydrocarbon production 334,

33940, 34850hydrochloric acid, cycling in 240,

244, 245, 246hydrodynamic voltammetry 309, 310hydrogen bonding 413hydrogen bromide 3, 382, 383hydrogen evolution reaction (HER)

64, 71catalysts used in 723copper oxide studies 322electrocatalysis 1467InP used in 23649and redox potentials 301

hydrogen productionfrom CO2 reduction 305cost of 1112, 104fractional energy yield 158, 159InGaN-PECs 21617microwave reectancemeasurements 44

multiphoton systems 834by photosystems I/II 159solar photoelectrolysis 38

hydrogen storage 155hydrogenases 159hydrogenation, CO2 33742, 3524

ice 409, 411, 412impact ionization 371in-line synchrotron radiation

XPS 17980in operando studies 17886in situ surface conditioning 23742,

249in situ X-ray absorption

spectroscopy 1806in-system surface analysis 239,

2437incident photon to current conversion

eciency (IPCE) 23, 32oxynitrides 124, 126photoanode/DSSC 98, 99, 100

increment distance 141increment time 141

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indirect band gap 55, 61, 225, 226,269

indium aluminium nitride 195, 196,197, 215

indium antimony 227, 228indium gallium arsenide 236, 237indium gallium arsenide

phosphide 236, 237indium gallium nitride 195, 196, 197,

199growth method 198hydrogen generation 21617InN and Indium-richepilayers 21014

materials improvement 215ternary alloys andheterostructures 20910

indium nitride 199band gap alignments 1957in InGaN epilayers 21014InN-GaN-AlN 196properties 1945

indium oxide 239, 243, 245, 246indium oxide phosphate 180indium phosphates 239, 2434, 246indium phosphide 70, 225

absorbers 23549band alignments 228MOCVD 2324photon recycling 431, 432water splitting 230

indium phosphites 2434, 246indium-rich surfaces 235, 236inductively coupled plasma optical

emission spectroscopy(ICP-OES) 118

inelastic photoelectron scatteringlength 242, 245, 255

infrared (IR) spectra 411FTIR 233, 445

inkjet printing 133, 137intensity-modulated photocurrent

spectroscopy (IMPS) 3640, 45, 46inversion layer 274iodate/iodide shuttle redox 1234iridium 123, 124

iridium oxide 66, 68, 69, 74, 125, 126,127, 146, 147

iron catalysts 340iron oxide 20, 656

broccoli-type structure 438with cobalt oxide 74doping and defect control 189doping eects 149electronhole separation 276energy band structure 442IMPS plot 37, 38, 39LMAS and PMAS 47, 48PEIS response 43, 44photoanode/DSSC 96, 98, 99,

100photoanode/photocathodesystems 101

photoelectrode/PV devices 95plasmon-assisted photonabsorption 271

transient photocurrentresponse 34

iron porphyrin 31617irradiation diameter 140isopropanol 312, 313isotope eect 412

Joint Center for ArticialPhotosynthesis (JCAP) 10, 17,446

ket (rate constant for electron transfer)268

kineticsat metal electrodes 256minority carrier reactions 268

Korean Center for ArticialPhotosynthesis (KCAP) 17

krec (rate constant for recombination)31, 35, 369, 41, 44

ktr (rate constant for hole transfer)31, 33, 35, 369, 41, 44

Lambertian limit 56Landau damping 272LandauZener model 278

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lanthanum titanium oxynitride 125,127

lattice constants 205group III-nitrides 194III-V systems 226, 228

lattice parameters 195Levich plots 309, 311Le`vy ights 428, 429Le`vy glass 427, 430Le`vy processes 42733Le`vy random walk 428, 429Lewis acids 344, 351light absorption, crystalline

semiconductors 549light-harvesting 1 complex (LH1)

394, 397light-harvesting 2 complex (LH2)

393, 3945, 397quantum coherence397400

light-harvesting systems 38991,4012

light intensity, and photocurrentvalues 323, 324

light-modulated absorptionspectroscopy (LMAS) 478

light-modulated microwavereectivity (LMMR) 456

light scattering 428, 429, 430, 432linear sweep voltammogram 144,

148, 149local-density approximation (LDA)

method 197localized surface plasmon resonances

(LSPR) 271localized surface plasmons (LSPs)

423, 424lone-pair interactions 41516low energy electron diraction/

microscopy (LEED/LEEM) 233,238

low frequency capacitance (CLF) 40,41, 42, 44

low frequency resistance (RLF) 40, 41,42, 44

low-pressure MOCVD 198, 211

magnesium as dopant 2089manganese

Mn3Ca 160, 161Mn4Ca 157, 158, 160

manganese oxides 4, 67electrochemistry and structure-function analysis 16878

a-Mn2O3 164, 165, 167, 168,169, 172, 1735, 177, 178

Mn3O4 164, 165, 167, 168, 170,1735

Mn(O,OH)x 167, 168, 172,1734, 175

oxygen evolving catalysts 1635preparation and phaseformation 1658

Marcus theory 276, 278marokite 164Maxwell Boltzmann equation 23mesoporous photoelectrodes 235metal electrodes

in aqueous media 3467kinetics at 256in non-aqueous media 350, 351photoelectrolysis cell 363

metal nitridesd10 conguration 11718GaN-ZnO and ZnGeN2-ZnO 11822

see also individual metal nitridesmetal-organic chemical vapor

deposition (MOCVD) 202, 204GaP 249, 252III-V semiconductors 230, 231,2324

InP absorbers 235low-pressure 198, 211superatmospheric 199, 21112,213, 214

metal oxides 10, 659band edge energies 3001, 302band gaps 267, 270band structures 111, 112electronic properties 43842inkjet printing 133tandem 934

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in water splitting 11011see also individual metal oxides

metal oxynitridesband gaps 112, 114, 270band structures 111, 112early-transition metals 11214two-step water splitting 1234water reduction activity 11417water splitting using 1248

metal phthalocyanines 302metal surface-water

interactions 40616metathesis, s-bond 341methane production 3378, 34850methanol 113, 114, 115methanol-mediated synthesis 33940methanol production 15, 3389

from CO2 reduction 302, 303,312, 313, 31819

electrochemical CO2reduction 350

homogeneous catalysis of CO23412

methanol-to-gasoline (MTG)process 340

microstructuredphotoelectrodes 2548

microwave reectivitymeasurements 427

microwire arrays 578, 60, 62, 70catalysis at 63

migration 61minority carrier diusion length

(Lp) 22, 23, 30minority carrier lifetime 30minority carriers

collection 223kinetics 268overpotential 2930photon recycling 4312

molar fraction 203, 204, 205, 206molar free energy of mixing 203, 204molecular beam epitaxy (MBE) 198,

211, 212molecular catalysts 3016molecular chromophores 3748, 390

molecular orbital energy diagram301, 302

molybdenum alloys 73molybdenum oxide 72molybdenum sulde 70, 72, 75Mott-Hubbard gap 439, 440MottSchottky equation/analysis 21,

148, 149, 150, 362Mulliken electronegativity 243multi-absorber systems

brute force strategies 856D4 architectures 91, 92D4 strategy 8790III-V systems 2257InP 23549tandem cell concept 867see also tandem photoelectrodes

multi-subunit proteincomplexes 3947

multiphoton systems 834multiple exciton generation (MEG)

365, 369, 3724, 375, 376, 379, 380multiple proton-coupled electron

transfer 299multiple quantum wells 212, 213

n-type electrodes 91, 92electronic energy levels 274, 363overpotential 29photoelectrochemistry 267, 268systems 1002water photoelectrolysis 56water splitting systems 125, 187

Naon lms 170, 171, 178, 306nanocomposites, Pt-C-TiO2 30613nanocrystals

buried p-n junctions using 3846hot excitons in 3714TiO2 374, 376, 377, 382

nanoemitters 60, 74nanoparticles 24

CO2 reduction using 3205gold 66, 70plasmonic 66, 271, 275silver 271, 423, 424tantalum nitride 11415

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nanorods 24, 3846nanostructured photoelectrodes

235, 2548nanowires 6970, 2567near edge X-ray absorption ne

structure (NEXAFS) 175, 180, 184Nernst equation 26nickel catalysts 337, 343, 345, 346, 352

NiMoZn 163nickel cyclams 344, 348nickel-molybdenum alloys 73nitrogen xation 16non-adiabatic process 277, 278non-aqueous CO2 reduction 3501non-methanol-mediated synthesis 340non-photochemical quenching (NPQ)

4001normal hydrogen electrode (NHE)

299, 300, 361normalized photocurrent (EQW)

voltage plot 33nuclear magnetic resonance (NMR)

spectroscopy 303numerical aperture (NA) 140

O-ring 141, 143one-electron reduction of CO2 304one sun intensity 3657online electrochemical mass

spectrometry (OLEMS) 350open-circuit photovoltage 5961operating potential/voltage 94, 366optical in situ control 2314optical prole image 135, 136overpotential (Z) 256, 84

and band bending 29CO2 reduction 299concentration 623D4 devices 88electrochemical wateroxidation 160, 2824

losses 8, 9minority carrierreactions 2930

and PCEs 368, 369vs maximum PCE values 373

oxalate 3501oxidation catalysts

characterization 1869in nature 15661, 162see also oxygen evolvingcatalysts

oxygen as impurity 208oxygen evolution reaction (OER) 64,

678, 71, 189catalysts used in 734complexity of 445electrocatalysis 1467iron oxide electrodes 47manganese oxide catalysts1645, 1668

overpotential 2823oxygen evolving catalysts 16178

electrochemistry and structure-function analysis 16878

preparation and phaseformation 1658

structural features 1635oxygen evolving complex 1567, 158oxygen reduction reaction (ORR)

163, 164, 182, 185, 189overpotential 2823

oxynitrides see metal oxynitrides

p-band 440p-i-n core shell-shell devices 256, 257,

258p-n junctions, buried 248, 37986P-rich surfaces 234, 235, 236, 252, 253p-type electrodes 91, 92

InP 23549systems 1002water photoelectrolysis 56water splitting systems 125, 187see also metal electrodes

P680 159, 445palladium complexes

CO2 reduction 293Pt-Pd-C-TiO2 307, 308, 309, 313

palladium porphyrins 343panchromatic dyes 96, 98para-terphenyls 296, 313

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partial pressures 210, 211, 212partially dissociated water

layer 40711particle polarizability 423Pauli repulsion 415PBESol 269, 270PCE see power conversion eciency

(PCE)PECs see photoelectrochemical cells

(PECs)Pendellosung fringes 206, 207perovskite 270, 438pH

band edge energies 300in CO2 reduction 342, 343copper oxideelectrodeposition 322

and electrochemicalbehaviour 175

and photocatalysis 121phenazine 296, 313photo-Dember eect 274photoactive oxide semiconductors

1889photoadaptation 4001photoanodes see n-type electrodesphotocatalysis/photocatalysts

CO2 reduction 28998, 31325and pH 121rapid screening 13250

photocathodes see p-type electrodesphotochemical diode 361, 362photochemical systems 298photocorrosion 364, 380, 381, 445photocurrent density (J) 5960, 88photocurrent ow 325photocurrent onset 32, 33, 34photocurrent values, and light

intensity 323, 324photodegradation 364photoelastic modulator 231photoelectric emission microscopy

(PEEM) 436photoelectrochemical cells (PECs)

buried p-n junction 384eciency 9

eciency equation 5eciency losses 8energy level diagrams 263in-system surface analysis 239InGaN-based 21617MEG or SF 380solar water-splitting 36579STH conversion eciency1112

tandem see tandemphotoelectrodes

water splitting 359, 364see also electrochemical cells

photoelectrochemical CO2reduction 1216, 3512

photoelectrochemical etching 435photoelectrochemical impedance

spectroscopy (PEIS) 402, 43, 44photoelectrochemical (PEC)

analysis 113, 114photoelectrochemistry

history 13, 267, 35960n-type electrodes 267, 268see also solar photoelectrolysis;water photoelectrolysis; watersplitting

photoelectrode/PV systems 93100photoelectrodes

conventional semiconductor 20microstructured 2548nanostructured 235, 2548nanostructured andmesoporous 235

see also semiconductorphotoelectrodes; tandemphotoelectrodes

photoelectron spectroscopy (PES)303, 412

GaP 2523photoemission-into-electrolyte

spectrum 421, 422photogenerated carriers,

collection 549photogenerated current 365, 367photoluminescence spectra 427, 431,

432, 442

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photon capture 26872photon dispersion 420photon energy 2689

gas phase water and ice 412III-V compounds 255, 258InP 242, 245, 246for multiple excitongeneration 373, 375

photon recycling 4312photon scattering cross-section 423photoprotection 4001photoreactions, in SECM 142photoresponse 138photosensitizers 3512photostationary state 11photosynthesis 87, 1234, 155, 334

eciency of 390oxygenic 160Z-scheme 361, 362

photosynthetic unit, purplebacteria 397

photosystems I/II 1567, 158, 159,160, 361, 4445

in higher plants 390photovoltaic (PV) arrays

brute force strategies 856CO2 reduction 1415III-V materials 225photoelectrode/PVsystems 93100

see also PV/PV tandem cellsphyllomanganates 163, 1656,

16870, 171piezoelectric dispenser 135piezoelectric polarization 201, 210pigment 680* 157, 159pixel resolution 140, 141pL-drops 135plasma-assisted molecular beam

epitaxy (PA-MBE) 198, 211, 212plasmon-assisted photon

absorption 2712plasmon hybridization model 272plasmonic nanoparticles 66, 271,

275plastoquinone 160

platinum 68, 69, 72, 113, 114bonding to water 414, 415as electrocatalyst 146, 147and oxynitrides 123Pt-C-TiO2 30613XAS and IR spectra 411XES studies 41314XPS spectra 408, 409

pn-junction 91, 92point defects 2069polar orientation 2001polarons 2756, 278poly(dimethylsiloxane) 58Polymer Electrolyte Membrane

(PEM) electrolyzer 155polymethylmethacrylate 426porphyrins 313, 31617, 343, 352potential-modulated absorption

spectroscopy (PMAS) 478potential-modulated reectance

spectroscopy (PMRS) 47Pourbaix diagram 280, 281, 342,

343power conversion eciency (PCE)

366, 367, 368using hot carriers 36971using hot excitons innanocrystals 3714

and singlet ssion 3748, 380tandem cells 379

precursor solutions 1367, 148probability distribution function 428,

429proteins

energy transfer 3901LH2 complex 393, 3945,397400

multi-subunit complexes3947

proton electrolyte membrane (PEM)fuel cell 306

proton-permeable membrane 53, 54,61

purple bacteria 391, 394, 397PV arrays see photovoltaic (PV)

arrays

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PV/PV tandem cells 87, 913, 187oxygen evolving catalysts 161,

163theoretical eciency 226, 227

pyridine 3023, 310, 31819, 3215pyridinium 302, 303, 307, 308, 309,

311electrochemical CO2reduction 345

quantum coherence 397400quantum conned Stark eect 213quantum connement 372quantum dots (QDs) 372, 376, 382

buried p-n junctions using3846

quantum lms 372quantum rods/wires 372, 3846quantum walk 399quantum wells 229, 2556, 258

1-D 372multiple 212, 213

quantum yield (QY) 366, 369, 371,373, 375

photoemission 421, 422

radiative limit 370Raman spectra 167random hop model 391random walk 399, 4278, 429rapid screening 1323

on arrays 1347doping eects and theory14950

with electrocatalysts 1458follow-up studies 1489with SECM 13745

rate constants 2534from transient photocurrents346

RC network 40RC time constant 368, 41reaction orders 2534reactor pressure 211, 212, 214recombination, and charge

transfer 304

recombination current 365, 367Redeld theory 3956redox catalysis 343redox mechanism 337redox potentials 3612, 364

CO2 3001, 302oxygen and hydrogen 196

reduction catalystscharacterization 1869in nature 15661, 162see also oxygen reductionreaction (ORR)

reductive elimination 341reection anisotropy spectroscopy

(RAS) 2312, 234, 235, 236GaP 24951, 252

regular solution model 203relaxation process 273relaxation time constant 36, 37remote-plasma-enhanced CVD 199resistivities 165resonant cavity light emitting

diode 195resonant photoemission 442resonant tunneling diodes 236reverse water-gas shift reaction

(RWGS) 3367, 3389RF-sputtering CVD 199rhenium complexes

CO2 reduction 292multinuclear 315, 316photocatalytic reduction 297,31316

polypyridyl (Re(bpy)) 3034,314

rhodamine 6Gin 426rhodium 71rhodium electrodeposition 238, 240,

241, 2434, 245, 246, 248rhodium oxide 1201rotating disk electrode (RDE) 185,

186rubisco 335, 336ruthenium

water dissociation 41112XPS spectra 408, 409, 410

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ruthenium complexesCO2 reduction 2912electrochemical CO2reduction 345

formic acid production 341photocatalytic reduction 2956,313, 31516

ruthenium oxide (RuO2) 117, 118,123, 124, 172, 173, 185

ruthenium polypyridylcomplexes 3056, 351

[Ru(bpy)3]2+ 301, 351

[Ru(phen)3]2+ 301, 302,

31819ruthenium selenide 180, 182, 184,

185, 186ruthenium sulde 182, 183, 1856rutile see titanium dioxide

S-Q thermodynamic calculations374, 376

S-shape plot 38, 39S-transitions 160, 161, 162Sabatier reaction 337sacricial reagents 11, 113, 114,

142Sanderson electronegativity 243sapphire 199, 201, 202saturation current density 5960scanning electrochemical microscopy

(SECM) 678, 133data analysis 1445electrocatalysts 147guidelines 1414method 13741spot array electrodes 1346

scanning electron microscopy (SEM),manganese oxides 167, 169

scanning photoelectrochemicalmicroscopy (SPECM) 138

scanning tunneling microscopy(STM) 233, 235

screen printing 170seawater, photoelectrolysis 4self-repair 445self-trapping process 275, 276

semiconductor-electrolyte junctioncollection of minority carriers223

electronic energy levels 274energy level diagram 360ideal 363open-circuit voltage 5960potential and chargedistribution 201

semiconductor liquid junctions 91semiconductor nanoparticles 3205semiconductor photoelectrodes 20

crystalline 549minority carrier reactions 268water splitting on 110see also structuredsemiconductors

separately illuminated electrodes 8Shockley-Queisser limit 2545Shockley-Queisser model 365, 370Shockley-Read-Hall

recombination 230signal resolution 140silica

electronhole separation 276formation 436, 437

silicon as substrate 199, 2068GaP 24951, 2534III-V semiconductors 230

silicon carbide 199silicon electrodes 44, 45, 46

absorption length 56amorphous silicon 923, 95,

163band edge energies 423fractals 434, 435, 436indirect band gap 55triple junction 163, 188, 189

silicon germanium, band gaps 270silicon microspheres 3824silicon microwire arrays 578, 60,

62, 70silicon nanowires 6970silicon nitride antireective

coating 58silver back reector 58

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silver complexes,AgBiW2O8 301, 3201silver lms 4212, 423, 4267silver nanoparticles 271, 423, 424silver nitrate 113, 114silver porphyrins 343single-absorber, two-photon

approach 835single photoelectrodes, water

photoelectrolysis 5, 8, 187singlet ssion (SF) 365, 382

and PCE 3748, 380sodium sulfate/sodium sulde

solution 145sodium tantalum oxide 111sol-gel processes 133, 166, 170solar cells, one sun intensity 3657solar concentration 3789solar energy

harvesting of 267, 389storage 155

solar energy conversion eciency 2, 70equation 5III-V systems 2257losses 8see also solar-to-hydrogen(STH) conversion eciency

solar ux 99solar hub 3solar photoelectrolysis

band gaps 89commercial viability 1112hydrogen 38

solar-to-electricity powerconversion 867

solar-to-hydrogen (STH) conversioneciency 1112, 84

D4 devices 87, 89, 90III-V semiconductors 225in nature 159oxygen evolving catalysts 163photoanode/DSSC 96, 98photoelectrode/PV devices94, 95

PV/PV devices 91, 93see also solar energy conversioneciency

solar water-splitting PECs 36579solid solutions 11822solvothermal method 66space charge capacitance 21, 27space charge eects 24space charge region 21, 22, 30, 363spectral density function 393, 396spontaneous polarization 200, 201spot array electrodes 1347

in SECM 138, 139, 140, 141,145

spot current 136spot diameter 140SQ1 dye 96squaraine dyes 96, 98, 99staircase function 3734standard calomel electrode (SCE) 361standard hydrogen electrode (SHE)

279steady state photocurrent 35steam methane reforming 3, 104strain 436stress 436strontium niobium oxynitride 1278structured semiconductors

advantages 6476catalysis at 634electrochemical transport 613high aspect ratio 6971open-circuit photovoltage5961

water splitting catalysis 714superatmospheric MOCVD 199,

21112, 213, 214superdiusion 428, 430support electrode 136, 137surface conditioning, in situ 23742,

249surface coordination number 409surface functionalization

electrodes 17886InP 23649

surface passivation 256surface plasmon dispersion 420surface plasmon polaritons 4267surface plasmon resonance 4223

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surface plasmons 41924surface reaction 27984surface roughness 4212surface-to-volume ratio 433synchrotron radiation photoelectron

spectroscopy (SRPES) 242, 2437syngas 3201, 337, 338

Tafel relation 88tandem photoelectrodes

buried p-n junctions 37982concept 867GaP/Si 2534motivation for using 835PCEs and Egs 379photoanode/DSSC 96100photoanode/photocathodesystems 1002

photoelectrode/PVsystems 93100

practical device design 1024silicon thin lm 188with singlet ifssionmolecules 378

water photoelectrolysis 5, 6,7, 8

water splitting 125, 3679water splitting membrane 156see also multi-absorber systems;PV/PV tandem cells

tandem solar absorbers 53, 54tantalum chloride 125, 126tantalum nitride 113, 114, 123, 124

nanoparticles 11415water splitting 125, 127

tantalum oxide 113, 114, 116tantalum oxynitride 113, 114

nanoparticles 115surface defects reduction 116two-step water splitting 123, 124water splitting 125, 126

Teon block 133ternary group III-nitrides 195

aluminium gallium nitridesystem 2009

band alignments 196

InGaN alloys 20914valence band position 197

ternary group III-V, bandalignments 227

tert-butylphosphine (TBP) 232, 233,250

Texas Instruments 3, 3824thermal dissociation 410, 41112thermodynamic calculations 36579thylakoid membrane 155, 156, 157,

159tip-collection/substrate-generation

(TC/SG) 141, 142, 147tip scan rate 140titanium dioxide 12, 20, 69, 74

advantages and drawbacks 267doping eects 149eciency 216electronhole separation 2756energy band structure 442light scattering 430nanocrystalline 374, 376, 377,

382overpotential 283photoanode/photocathodesystems 100, 101, 102

photoelectrode/PV devices 93,95

plasmon-assisted photonabsorption 272

Pt-C-TiO2 30613two-step water splitting 123,

124top-down synthesis 6970, 256transient absorption (TA)

spectroscopy 372transient photocurrents, rate

constants from 346transition density cube (TDC)

method 392transition metal complexes

CO2 reduction 31319oxynitrides 11214see also individual transition

metalstransition metal oxides 43842

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transmission electron microscopy(TEM)

manganese oxides 167, 169, 173oxynitrides 115Pt-C-TiO2 307, 308

triethylamine 317triethylgallium 204, 232, 233, 250trilevel conguration 97, 98, 99trimethylaluminium 204trimethylindium 232, 233triose phosphates 335tungsten oxide 667, 68, 74, 90

doping eects 149overpotential 283photoanode/DSSC 96, 98, 100photoanode/photocathodesystems 101

photoelectrode/PV devices 95two-step water splitting 123,

124two-dimensional electronic

spectroscopy (2DES) 398, 399two-electron reduction of CO2 302,

304two-step water splitting 12342-photon photoemission 835, 233,

2556, 258tyrosine 1578, 162

ultrahigh vacuum (UHV)chamber 180, 232, 233, 234

water adsorption in 2512ultramicroelectrode 137UV light in water splitting 111UV photoelectron spectroscopy

(UPS) 113, 238, 241, 242, 247

valence band edge 4, 93valence band energy 55, 91valence band onset 247valence band position/osets 196, 197valence-force eld (VFF) model 203vapor-liquid-solid (VLS) silicon

microwires 578, 70vertical cavity surface emitting

laser 195

visible light in water splitting 11011voltage see bias voltage; current versus

voltage dependence; current-voltage curves (j-U); open-circuitphotovoltage; operating potential/voltage

volume plasmon dispersion 420

wateradsorption 2513, 407electronic structure and bondingmechanism 41216

metal surface interactions40616

water-gas shift (WGS) reaction3367

water oxidationbismuth vanadate 678Mn lms 176overpotential 2824potentials 4reaction mechanism 2812S transitions 160, 161, 162

water photoelectrolysisCO2 reduction 15rst reports 361hydrogen production 37new materials 811various congurations 8see also water splitting

water reductiond0-oxynitrides 11417potentials 4

water splittingapproaches underdevelopment 1879

band gaps in 84, 110, 111, 364by colloidal particles 71group III-V semiconductors22930, 258

history of 359light driven 4446by metal nitrides see metalnitrides

by metal oxynitrides see metaloxynitrides

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water splitting (continued)model device 53, 54process of 3612reaction 109solar PECs 36579structured semiconductors usedin 6476

surface reaction 27984systems 125, 224by tandem photoelectrodes seetandem photoelectrodes

Texas Instruments systemfor 3824

two-step 1234in visible light 11011

water splitting membrane 156weak coupling limit 394, 395weakly-coupled chromophores

3914work function 360, 422, 423wurtzite 194, 195, 200, 210

X-ray absorption near edgespectroscopy (XANES) 171, 176,180, 182, 185, 189

X-ray absorption spectroscopy (XAS)407, 408, 409, 41011, 415

catalyst characterization 187in situ 1806

see also extended X-rayabsorption ne structure(EXAFS); near edge X-rayabsorption ne structure(NEXAFS)

X-ray diraction (XRD) 150, 167,182, 183, 214

X-ray emission spectroscopy (XES)41314

X-ray photoelectron spectroscopy(XPS) 1723, 174, 175, 4078,409, 410

III-V semiconductors 233, 234,238, 2412, 243, 247

in-line synchrotron radiation17980

xenon lamp 143

Z-scheme 1234, 224, 361, 362and singlet ssionmolecules 377, 378

zinc blende 194, 249zinc germanium nitride 11822zinc oxide 20, 69, 74

Cu/ZnO system 339metal nitride solidsolutions 11822

zirconium oxide 116, 123ZnxCd1xSySe1y array 134, 137

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