Building Next Generation Solar Cells with Nanotechnology and I MP respectively. The Fill Factor (FF)...
Transcript of Building Next Generation Solar Cells with Nanotechnology and I MP respectively. The Fill Factor (FF)...
Building Next Generation Solar Cells with Nanotechnology
Prashant V. Kamat
http://www.nd.edu/~kamatlabOR Kamatlab.com
Department of Chemistry & Biochemistry and Radiation LaboratoryDepartment of Chemical & Bimolecular EngineeringUniversity of Notre Dame, Notre Dame, IN 46530
2018 Energy Outlookhttps://www.eia.gov/pressroom/presentations/Capuano_02052018.pdf
http://www.bloomberg.com/news/articles/2016-06-13/we-ve-almost-reached-peak-fossil-fuels-for-electricity
….. a Solar Wave
Progress in Photovoltaics: Research and Applications 2017, 25, 3-13.
Photovoltaic Advances
Can we address clean energy
challenge with Nanotechnolgy?Perovskite[22.7%]QDSC[13.4%]
How Nanotechnology came into play?
The Birth of Renewable Energy
1970’s
Oil crisis (OPEC oil embargo) of 1973 brings attention to Renewable Energy
Artificial Photosynthesis was coined to mimic photosynthesis-Photoinduced Electron Transfer Reactions
Semiconductor Photoelectrochemistry became a popular research topic
Photocatalytic properties of semiconductor particle systems were explored
Fujishima HondaBardGerischer Henglein
Energy (eV)2.0 2.5 3.0 3.5 4.0
Lu
min
esce
nce A
bso
rba
nce
10K 45Å
27Å
22Å
19Å
16Å
13Å
12Å
Colloidal Quantum Dots
CdSe
Murray, C.; Norris, D.; Bawendi, M., Synthesis and characterization of nearly monodisperse CdE (E=S, Se, Te) semiconductor. J. Amer. Chem. Soc. 1993,115, 8706-8715
Courtesy: M. Kuno
A Major Turning Point
Synthesis of QDs by Hot-Injection Method
"The technology works by harnessing nanocrystals that range in size from 2 to 10 nanometers. Each dot emits a different color depending on its size. By adding a film of quantum dots in front of the LCD backlight, picture color reproduction rate and overall brightness are significantly improved."
http://www.cnet.com/news/lg-leaps-quantum-dot-rivals-with-new-tv/
<$500
• The I-III-VI chalcopyrite structure is derived from the fact that the group II element in the II-VI zinc blende structure is substituted by group I and III elements.
Omata, T. et al. Size dependent optical band gap of ternary I-III-VI(2) semiconductor nanocrystals. J. Appl. Phys. 2009, 105, Art no 073106.
Ternary semiconductor nanocrystals
AgInSe2
CuGaSe2
CuInSe2
CuInS2
CuGaS2
AgGaS2
AgGaSe2
• Optical band gap of the QDs covers a wide wavelength range from near-infrared to ultraviolet.
• Bulk CuInS2 has a direct bandgap of 1.53 eV with size tunable absorption and emission (Bohr radius ~4.1 nm).
Nanostructured Hybrid Assemblies for Harvesting Light Energy
Quantum Dot Solar Cells
Tunable band edge Offers the possibility to harvest light energy over a wide range of visible-ir light with selectivity
Hot carrier injection from higher excited state (minimizing energy loss during thermalization of excited state)
Multiple carrier generation solar cells.Utilization of high energy photon to multiple electron-hole pairs
Polymer-SemiconductorHybrid Cell
Semiconductor Hetero-junction Solar Cell
Quantum Dot Senistized Solar Cell
PEDOT/PSS
P3HT/SC Nanocrystals
• Tuning properties of Nanomaterials
• Surface modification• Assembly on
Electrodes • Photon Capture (Light Absorption)
• Excited State Dynamics• Charge Separation
• ETL & HTL to capture charges
• Surface modification• Efficiency
Synthesis & Characterization
Photochemistry & Photophysics
Photovoltaic Performance
Deposition of QD Films
TiO2 CdSe
SILAR
ElectrophoreticdepositionChemical
bath
Drop cast/spin coat
Molecular linker
Cd2+
precursorSe2- or S2-
precursorOTE/TiO2/CdSe
or (CdS)OTE/TiO2
ea
bd
c
Experimental Approach
Synthesis of QDs by Hot-Injection Method
1-8 Cycles CdSe SILAR
15
Liquid Junction
Solid State
Optically Transparent Electrode
Substrate (Metal Oxide)
Sensitizer
Electrolyte / Hole Conductor
Counter Electrode
Anatomy of a Quantum Dot Solar Cell
350 400 450 500 550 600 650 7000
10
20
30
40
50 (A) 3.7 nm 3.0 nm 2.6 nm 2.3 nm
Wavelength (nm)
IPC
E (%
)
Quantum Dot Solar Cells
hν
e
OR
CdSeTiO2
VB
CB
ee
e
hh h
O
e
h
R
E
IPCE or Ext. Quantum Eff.= (1240/λ) x (Isc/Iinc) x 100
• Size selective deposition of CdSe QDs to TiO2 films
• Ability to tune the photoresponse of
QDSC
• Higher efficiency with smaller size QDs
1. Illuminate Solar Cell• 100 mW/cm2, Air Mass 1.5G solar
irradiation
2. Measure current at different voltage output
3. Simulates possible “real world” operating conditions
4. Gives us Power Conversion Efficiency
Current-Voltage Measuremnts (I-V curves)
Recombination and VOC
Pote
ntia
l
+
-
FTOTiO2
CdSe
S2-/Sn2-
EFermiCu2S/RGO
Desired ElectronTransfer
Recombination
Step by Step:1. Excitation2. Electron Transfer3. Recombination4. Build up e- in CB until
Rexcitation = Rrecombination
5. If recombination rate is increased, VOC is decreased
VOCVOC 1
2
345
Introduction 2-Electrode 3-Electrode Other Conclusions
In the Dark (at Equilibrium)FT
O
Cu2 S/
RGO
i
- +
Eappl
Pote
ntia
l
+
-
FTOTiO2
CdSeS2-/Sn
2- Cu2S/RGOEFermi
-+
Hodes, G., Gratzel, M. et. al, J. Phys. Chem. B, 2000, 104, 2053-2059
S2-/Sn2-
TiO2/CdSe
Let There Be Light!
Pote
ntia
l
+
-
FTOTiO2
CdSeS2-/Sn
2-
ΔV = Efermi - Ecounter
Eappl = - Voc i = 0Eappl > -Voc i < JscEappl= 0 V i = Jsc
Cu2S/RGO
EFermi ΔV
Hodes, G., Gratzel, M. et. al, J. Phys. Chem. B, 2000, 104, 2053-2059
FTO
Cu2 S/
RGO
i
- +
Eappl
-+
S2-/Sn2-
TiO2/CdSe
Short Circuit Current (ISC)The short circuit current ISC corresponds to the short circuit condition when the impedance is low and is calculated when the voltage equals 0.
I (at V=0) = ISC
ISC occurs at the beginning of the forward-bias sweep and is the maximum current value in the power quadrant. For an ideal cell, this maximum current value is the total current produced in the solar cell by photon excitation.
ISC = IMAX = Iℓ for forward-bias power quadrant
Open Circuit Voltage (VOC)The open circuit voltage (VOC) occurs when there is no current passing through the cell.
V (at I=0) = VOC
VOC is also the maximum voltage difference across the cell for a forward-bias sweep in the power quadrant.
VOC= VMAX for forward-bias power quadrant
Solar Cell characteristics
Maximum Power (PMAX), Current at PMAX (IMP), Voltage at PMAX (VMP)The power produced by the cell in Watts can be easily calculated along the I-V sweep by the equation P=IV. At the ISC and VOC points, the power will be zero and the maximum value for power will occur between the two. The voltage and current at this maximum power point are denoted as VMP and IMP respectively.
The Fill Factor (FF) is essentially a measure of quality of the solar cell.
FF = = PMAX
PT
IMP ×VMP
ISC ×VOC
Overall Power Conversion Efficiency (η)Efficiency is the ratio of the electrical power output Pout, compared to the solar power input, Pin, into the PV cell. Pout can be taken to bePMAX since the solar cell can be operated up to its maximum power output to get the maximum efficiency.
Pin is taken as the product of the irradiance of the incident light, measured in mW/cm2 (or one sun =100 mW/cm2), with the surface area of the solar cell [cm2]. The maximum efficiency (ηMAX) found from a light test is not only an indication of the performance of the device under test, but, like all of the I-V parameters, can also be affected by ambient conditions such as temperature and the intensity and spectrum of the incident light.
0 0.2 0.4 0.6 0.8 1.00
5
10
15
20
25
Steady-state current @ 0.85 V (averaged over 30 s) Average of forward & reverse scans
Forward: Jsc = 22.4 mA/cm2 VOC = 1.01 Vff = 0.66η = 15.0%
Voltage (V)
Curre
nt D
ensi
ty ( m
A cm
-2)
Reverse: Jsc = 22.4 mA/cm2
VOC = 1.04 Vff = 0.73η = 17.0%
Area = 0.13 cm2
i
V
hν
Semiconductor bandgap determines maximum achievable efficiency
I-V Curve of PV Cell and Associated Electrical Diagram
where I0 is the saturation current of the diode, q is the elementary charge 1.6x10-19 Coulombs, k is a constant of value 1.38x10-23J/K, T is the cell temperature in Kelvin, and V is the measured cell voltage that is either produced (power quadrant) or applied (voltage bias).
The solar cell performance is further evaluated in terms of
1. External Quantum Efficiency (EQE) isthe ratio of the number of charge carrierscollected by the solar cell to the number ofphotons of a given energy shining on thesolar cell from outside (incident photons).
2.Internal Quantum Efficiency (IQE) isthe ratio of the number of charge carrierscollected by the solar cell to the number ofphotons of a given energy that shine onthe solar cell from outside and areabsorbed by the cell.
Spectral responsivity is how much current comes out of the device per incoming photon of a given energy and wavelength and expressed as : amperes per watt (A/W); Both the quantum efficiency and the responsivity are functions of the photon energy or excitation wavelength (indicated by the subscript λ).
ηEQE
Probing Photoinduced Electron Transfer Process
VB
CB
Ox
Redhν
et ht
VB
–
+
+
–CB
TiO2
CdSe
hν
e
OR
Photoelectrochemistry
pump probe
detector
Spectroscopy
GERISCHER H, LUBKE MA PARTICLE-SIZE EFFECT IN THE SENSITIZATION OF TIO2 ELECTRODES BY A CdS DEPOSITJOURNAL OF ELECTROANALYTICAL CHEMISTRY 204 (1-2): 225-227 1986
450 500 550 600 650
-0.08
-0.04
0.00B
CdSe-MPA∆A
Wavelength, nm
1 ps 35 ps 400 ps 1500 ps
Charge Separation in TiO2/CdSe (3 nm)
CdSe
VB
CB e
h
pump
probe
detector
450 500 550 600 650
-0.08
-0.04
0.00C
CdSe-MPA-TiO2
∆A
Wavelength, nm
1 ps 35 ps 400 ps 1500 ps
TiO2
k= 1.95x1011 s-1
CB
VB
Time, ps
ket= 107 s-1 ket= 1.2x1010 s-1
CdSe2.4 nm
CdSe7.5 nm
TiO2
ee
Size Dependent Electron transfer between CdSe and TiO2
The energy gap between donor and acceptor influences kinetics of electron injection.
2007; 129, 4136
Dependence of Electron Transfer Rate with CdSe Particle Size and Oxide Substrates
I. Robel; M. Kuno; P. V. Kamat, J. Am. Chem. Soc. 2007, 129, 4136-4137. K. Tvrdy; P. A. Frantsuzov; P. V Kamat, Proc. Natl. Acd. Sci. USA 2011, 108, 29-34.
• Electron transfer in QDSCs has been widely studied many research groups
• Not the limiting factor in solar cell performance in most cases
Follows Many-State Marcus Theory
Evolution of Thin Film Solar Cells
3623−3630
DOI: 10.1021/acs.jpclett.5b02524
Lead Halide “Perovskites”
• Prototypical compound is CH3NH3PbI3• Hybrid organic-inorganic materials• Adopt a perovskite (ABX3) crystal
structure• Possible substitution of A sites with Cs,
MA & FA
CH3NH3+
Pb2+
I-
M. Saliba et al., Science 10.1126/science.aah5557 (2016)
Late 1990s - Early 2000s: The Mitzi Era
David Mitzi - IBM: T. J. Watson Research Center
1. (C4H9NH3)2(CH3NH3)n-1SnnI3n+1
2. [NH2C(I)=NH2]2(CH3NH3)mSnmI3m+2
3. (C4H9NH3)2MI4 (M = Ge, Sn, Pb)
4. (C4H9NH3)2EuI4
5. (NH2CH=NH2)SnI3
1. D. B. Mitzi, C. A. Feild, W. T. A. Harrison, and A. M. Guloy, Nature, 1994, 369, 467–469.2. D. B. Mitzi, S. Wang, C. a Feild, C. a Chess, and a M. Guloy, Science, 1995, 267, 1473–6.3. D. B. Mitzi, Chem. Mater., 1996, 8, 791–800.4. D. B. Mitzi and K. Liang, Chem. Mater., 1997, 9, 2990–2995.5. D. B. Mitzi and K. Liang, J. Solid State Chem., 1997, 134, 376–381.6. D. B. Mitzi, K. Chondroudis, and C. R. Kagan, IBM J. Res. Dev., 2001, 45, 29–45
4
Explored Applications inOLED and Transistors
2012: Emergence of Perovskite Solar Cell
1. A. Kojima, K. Teshima, Y. Shirai, and T. Miyasaka, 214th ECS Meeting 2008.2. H.-S. Kim, et al. Sci. Rep., 2012, 2, 591.3. M. M. Lee, J. Teuscher, T. Miyasaka, T. N. Murakami, and H. J. Snaith, Science, 2012, 338, 643–647.
• Initial attempt in 2008 with polypyrrole1
• Spiro-OMeTAD as HTM: A Landmark Development
Received May 31, 2012Received July 5, 2012
9.7% 10.9%
Published August 2012 Published October 2012
Nature 2013, 499, 316-319
Organic-Metal Halide Perovskite
1. Mix PbI2 and methyl ammonium iodide in chlorobenzene and stir for 2 hours at 70 °C –yellow colored solution
2. Spin coat the solution onto electrode surface kept on a hot plate (70-80 C)
3. The film turns black as it crystallizes into pervoskite structure
4. Make metal contact
Single Step Two Step
1. Spin PbI2
2. Dry
3. Dip in CH3NH3I
4. Anneal
36
Design of Perovskite Solar CellsDevice Components1. Optically Transparent Electrode2. Electron Transport Material3. Perovskite Absorber4. Hole Transport Material (HTM)5. Gold Counter Electrode
1
2 3
4 5
ETL
CH3NH3PbI3 Solar Cell with 16% Efficiency
37
1 μm
0 0.2 0.4 0.6 0.8 1.00
5
10
15
20
25
Steady-state current @ 0.85 V (averaged over 30 s) Average of forward & reverse scans
Forward: Jsc = 22.4 mA/cm2 VOC = 1.01 Vff = 0.66η = 15.0%
Voltage (V)
C
urre
nt D
ensi
ty (m
A c
m-2)
Reverse: Jsc = 22.4 mA/cm2
VOC = 1.04 Vff = 0.73η = 17.0%
Area = 0.13 cm2
300 400 500 600 700 8000
102030405060708090
100
Wavelength (nm)
EQE
(%)
0
5
10
15
20
Inte
grat
ed C
urre
nt D
ensi
ty (m
A c
m-2)
2-step deposition of MAPbI3 onto mp-TiO2 (~200 nm thick)
Best Solar Cell Certified Efficiencies
The PSCs fabricated with LBSO and methylammonium lead iodide (MAPbI3) show a steady-state power conversion efficiency of 21.2%, versus 19.7% for a mp-TiO2 device.
6500+ Papers in 6y with>220,000 Citations
~1000 Highly Cited Papers>165000 Citations
2017, 2, 922−923
Source: Clarivate Analytics(Web of Science )
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Most Read/Most Cited Articles in Leading Journals are on Perovskites(JACS, ACS Nano, Nano Lett, ACE Energy Lett, Chem Mater………
Intriguing Optical Properties of Lead Halide Perovskites(Manser, Christians, Kamat Chem. Rev. 2016 10.1021/acs.chemrev.6b00136)
• Low exciton binding energy –complete charge separation at room temperature
• Nonthermalized carrier recombination • Excitation intensity dependent quantum efficiency of
emission• Two-photon amplified spontaneous emission• Lasing properties• Tuning of bandgap through halide composition ratio
J. Phys. Chem. Lett.,2015, 6, 5027–5033
J. Phys. Chem. Lett.,2014 5 1300–
ACSPhotonics, 2016DOI: 10.1021/acsphotonics.6b00209
Lasing Spontaneous emission Line Broadening
• Excitons are rapidly dissociated at room temperature, and that, under typical photovoltaic operating conditions, the recombination dynamics of CH3NH3PbI3are primarily governed by the interactions of free electrons and holes.
• Ultrafast evolution of the PL peak is attributed to emission from non-thermalized free carriers. (PL does not arise from excitonic states
EXCITED STATE DYNAMICS
Chen, et al. J. Phys. Chem. Lett. 2015, 6, 153–158.
Wu, X.; et al J. Am. Chem. Soc. 2015, 137, 2089–2096
• Primary emission band arising from charge carrier recombination becomes narrower and increases in intensity with decreasing temperature. At very low temperature (< 100K) a longer wavelength emission (800-950 nm) arising from the trap sites become dominant
Excited State Dynamics
43
1. b ~ 1.5 until 10 W/cm2 – trapping regime (single carrier)2. b ~ 1 above 10 W/cm2 for thin film3. Single crystal shows transitions at 1 order of magnitude lower intensity (lower
defect density)
Draguta, S.; Thakur, S.; Morozov, Y. V.; Wang, Y.; Manser, J. S.; Kamat, P. V.; Kuno, M. J. Phys. Chem. Lett. 2016, 7, 715–721.
Nt = 6.3 x 1017 cm-3Iem ∝ Iexcb
Nanocrystals of Cesium Lead Halide Perovskites (CsPbX3, X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color GamutProtesescu et al. Nano Lett 2015, 15 (6), pp 3692–3696
Reaction of Organometal Trihalide Perovskite Colloidal Nanocrystals for Full-Range Band Gap TuningDong Myung Jang et alNano Lett., 2015, 15, 5191
Mixed Halide Lead Perovskites
Transforming Hybrid Organic Inorganic Perovskites by Rapid HalideExchangeNorman Pellet, Joël Teuscher, Joachim Maier, and Michael GrätzelChem. Mater., 2015, 27, 2181–2188
Ion migration in a solid material is characterized by the activation energy (EA), and the migration rate (rm) is influenced by the EA as
where kBT represents thermal activationenergy. The EA is sensitive to the material’s crystal structure, ionic radius, ion-jumping distance, and the charge of ions.
Nat. Mater. 2014, 13, 897−903
Nat. Mater. 2015, 14, 193−198Acc. Chem. Res. 2016, 49, 286−293
Ion Migration and Hysteresis in Perovskite Solar Cells
Computational models suggest that I−
ions (EA ~ 0.33 -0.58 eV) are more readily mobile than MA+ and Pb2+ ions
schematics of ion migration in perovskite during positive and negative poling
Ion Migration in Organometal Trihalide Perovskites
Migration path of I− ions along the I−−I− edge of the PbI6
4− octahedron in the MAPbI3 crystal calculated from density functionaltheory (DFT) method.
FTIR images of the distribution of MA+
Optical images of the lateral MAPbI3 perovskite solar cell with a mobile PbI2
thread
Nat. Commun. 2015, 6, 7497.
Adv. Energy Mater. 2015, 5, 1500615
Adv. Energy Mater. 2016, 6, 1501803.
Acc. Chem. Res. 2016, 49, 286−293
CsPbX3 Perovskite Quantum Dots
• Highly luminescent QDs• CsPbX3 perovskites are seen as a
more stable alternative to MAPbX3 species.
• Ease of synthesis and control of surface chemistry
• Features a cubic perovskite structure and broad spectral control through size and composition.
Kulbak, M. et al. J. Phys. Chem. Lett. 2016, 7 (1), 167–172.
Guria et al., ACS Energy Lett. 2017, 2, 1014−1021.Eperon, G. E. et al. J. Mater. Chem. A 2015, 3 (39), 19688–19695.
47
Experimental Approach
QD Synthesis
Spectroscopy
Assembly
PbBr2, OctadeceneOleic acid, Olylamine
Cesium Oleate
120 °C
DOI: 10.1021/jacs.6b04661
2016,138, 8603–8611
Transformation of Sintered CsPbBr3 Nanocrystals to Cubic CsPbI3 and Gradient CsPbBrxI3-x Through Halide Exchange
CsPbBr3 Film
DOI: 10.1021/jacs.6b04661
2016,138, 8603–8611
Tracking the Halide Exchange
(a) 0, (b) 1, (c) 3, (d) 7, (e) 15, and (f) 40 min
Compositional Depth Profile through EDX
• Using Energy Dispersive X-ray Spectroscopy an elemental composition depth profile was obtained.
• At film surface, Br-:I- ratio was ~1:1, but I- dropped to zero at film depths of 150 nm.
• Process likely governed by diffusion of halide in and out of the film.
52
The Thickness Dependence
The PCE of the solar cells increases with CsPbBr3 thickness until 250 nm140 nm 340 nm
The AX treatment strategy provides a general method for tuning the electronic properties of the CsPbI3 QD films.
FAI coating yields a doubling of the already-high mobility of CsPbI3QD films and results in a certified record PCE of 13.43% - above the best reported PCE for dye-sensitized solar cells, organic PVs, and CZTSSe PV technologies
Sci. Adv. 2017;3: eaao4204 27 October 2017
Moving Forward
Hybrid Metal Halide Perovskites
• Mixed halide (I/Br) systems –to further understand the role of charge transfer complex, halide ion mobility and establish the mechanism of phase segregation
• Surface treatment to modulate surface defects
• Multijunction Tandem Solar Cells(All Perovskite and Si-Perovskite double and triple junction can deliver 36-38% efficiency)
To minimize optical losses, it is necessary to develop routes to deposit the multilayers without destroying the underlying materials and with continuous charge extraction layers of minimal thickness (on the order of 5 nm) 2017, 2, 2506−2513
• Semiconductor quantum dotswith size and shape dependenttunability of bandgap offer newways to design energyconversion systems
• High Photoconversion Efficiencyof lead halide perovskites isattractive for developing thinfilm photovoltaics
• Challenges exist towardscommercialization ofsemiconductor nanostructurebased photovoltaic systems
Summary
Intriguing Optoelectronic Properties of Metal Halide PerovskitesChem. Rev. 2016, 116, 12956–13008
Making and Breaking of Lead Halide Perovskites Acc. Chem. Res. 2016, 49, 330–338
Multifaceted Excited State of CH3NH3PbI3. Charge Separation, Recombination, and Trapping (Perspective). J. Phys. Chem. Lett. 2015, 6, 2086-2095
Shift Happens.How Halide Ion Defects Influence Photoinduced Segregation in Mixed Halide Perovskites ACS Energy Lett. 2017, 2, 1507-1514
What will the future hold?
Over the last twenty five years, the per-
kWh price of photovoltaics has
dropped from about $500 to ~ $0.50;
think of what the next twenty five years will bring.
It is Sun-Believable
Researchers who make it possible in our groupGraduate students
Jacob Hoffman (Chemistry)Danilo JaraQuinteros (Chemistry)Seog Joon Yoon (Chemistry)Steven Kobosko(Chem. Eng.) Victoria Bridewell (Chemistry)Rebecca Scheidt (Chemistry)Olivia Cracchiolo (Chemistry)Jeffrey Dubois (Chemistry)
Summer 2012
CollaboratorsHartland, Kuno, McGinn, Vinodgopal, George Thomas, Osman Bakr, K. O’Shea, G. Hodes, C. Janaky, E. Selli
Post-Docs/Visiting ScientistsSubila Balakrishnan, Gary Zaitas, M.Shanthil, Roxana Nicolaescu; Julie Peller, Geeta Balakrshna
Undergraduate studentsRebecca Radomsky, SavennahButler, Elisabeth Kerns
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