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Metal Halide Perovskites: a New Family of Semiconductors for Photovoltaics and Optoelectronics Henry J. Snaith Department of Physics Clarendon Laboratory Parks Road Oxford OX1 3PU Photovoltaics and henry.snaith@physics.ox.ac.uk e-mail:

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Department of Physics Clarendon Laboratory Parks Road Oxford OX1 3PU e-mail: james.ball@physics.ox.ac.uk Photovoltaics and Optoelectronic Devices Group

Metal Halide Perovskites: a New Family of Semiconductors for Photovoltaics and Optoelectronics

Henry J. Snaith henry.snaith@physics.ox.ac.uk

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Perovskites

Perovskite is a calcium titanium oxide, with the chemical formula CaTiO3. The mineral was discovered in the Ural Mountains of Russia by Gustav Rose in 1839 and is named after Russian mineralogist Count Lev Alekseevich Perovski (1792–1856).” All materials with the same crystal structure as CaTiO3, namely ABX3, are termed perovskites.

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1892: 1st paper on lead halide perovskites

Structure deduced 1959: Kongelige Danske Videnskabernes Selskab, Matematisk-Fysike Meddelelser (1959) 32, p1-p17 Author: Moller, C.K. Title: The structure of cesium plumbo iodide Cs Pb I3

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First Solar Cells

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Perovskite solar cells

Meso-Al2O3 η =10.9% Meso-TiO2 η =7.6% Planar Junction η =1.8%

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Efficient Planar Heterojunction Solar Cells

  • M. Liu et al. Nature 2013
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Publications on perovskites

High T

c Superconductors

Perovskite solar cells

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Publications Vs Efficiency

Perovskite Solar Cells

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Crystallisation of Perovskite Thin Films

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PbX2+ 3 CH3NH3I CH3NH3PbI3+ 2 CH3NH3X (X= Cl, I, Ac)

  • W. Zhang et al. 2014 Nature Communications

Crystallisation of perovskite thin films

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XRD The more volatile the MAX component, the faster crystallisation occurs

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“Anti-solvent” quenching crystallisation

(a) (c)

Routes developed by Seok et al. and Spiccia et al.

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Anti-solvent + Excess organic

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Excess organic + excess PbI2

3MAI:PbCl2 2% PbI2 5% PbI2 40% PbI2 100% PbI2 3MAI:(PbCl(2-2x)PbI(2x))

  • N. Saki et al. Small 2017 (in-press)
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Excess organic + excess PbI2

3MAI:PbCl2 2% PbI2 5% PbI2 30% PbI2 100% PbI2

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Control over “nucleation” and growth

Formulation 1 Formulation 2 Formulation 3 Formulation 1 Formulation 2 Formulation 3 Formulation 1 Jsc Formulation 1 SPO Formulation 2 Jsc Formulation 2 SPO Formulation 3 Jsc Formulation 3 SPO

19.1% Efficiency

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What are the cation options?

Goldshmidt Tolerance factor

  • G. Eperon et al. 2014
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Adding a small amount of Cs to FAPb(I1-xBrx)3

Ability to crystallise throughout the entire I-Br compositional range

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Influence of Colloids In solution

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Influence of Addition of Acid (HI and HBr)

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Increased crystallinity and crystal orientation

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Microstrain and Charge Carrier Mobility

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Crystallinity Matters

  • D. McMeekin et al. 2017 Submitted
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A new route for single crystal Growth

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Breaking up of colloids

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Breaking up of colloids

Nature Communications 2016 ( Accepted )

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What we think about the mechanism

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Solvent Mixtures

H2O/MA EtOH/MA ACN ACN/MA

  • Solvent needs

to be polar and aprotic.

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  • N. Noel et al. EES 2016 In-press
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Devices from ACN/MA solvent mix

annealed unannealed inverted

  • N. Noel et al. EES 2016 In-press
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Enhanced Stability Perovskite Solar Cells

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Thermal stability good

400 500 600 700 800 1.0 1.5 2.0 2.5 3.0 3.5

MAPb(I0.6Br0.4)3

Absorption (a.u.) Wavelength (nm)

t = 0h t = 1h t = 2h t = 3h t = 4h t = 6h

B

400 500 600 700 800 1 2 3 4 5

C

FA0.83Cs0.17Pb(I0.6Br0.4)3

Absorption (a.u.) Wavelength (nm)

t = 0h t = 1h t = 2h t = 3h t = 4h t = 6h

  • D. McMeekin et al. Science 2016
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1.6eV gap

Champion Devices

PCBM n-type PCBCB n-type

C60 derivative

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Inverted Cell Architecture

ITO Substrates NiO FA(MA)CsPb(I0.9Br0.1)3 PCBM ZnO nanocrystal Ag/Au

JSC (mA cm-2) VOC(V) FF PCE (%) FB-SC 23.27 1.04 0.78 18.9 SC-FB 23.30 1.03 0.76 18.1 JSC (mA cm-2) VOC(V) FF PCE (%) FB-SC 23.05 1.08 0.79 19.7 SC-FB 23.15 1.07 0.78 19.2

FA0.79MA0.16Cs0.05Pb(I0.9 Br0.1)3 SPO: 19.3%

FA0.85Cs0.15Pb(I0.9Br0.1)3 SPO: 18.2%

  • S. Bai et al. (In preparation) 2017
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Non-encapsulated solar cells

The devices are aged under full spectrum simulated AM1.5, 76 mWcm-2 average irradiance at VOC in air without a UV filter, 53 ̊C. The Suntest XLS+ aging box irradiates pulsed light.

Burn-in

t80 = 694 h t80 = 1050 h t80 = 20.7 h

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Sealed vs unsealed

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But…

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And cheaper…

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Best Way to Raise Efficiency

Epitaxially Grown Single Crystal III-V Tandem

46% efficient >$40,000/m2

Perovskite on Conventional Silicon Tandem

Up to 33% efficient <$100/m2

Image: US Naval Research Lab

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Perovskite on Si

  • Eg. See papers by

Baliff et al and McGehee et al,

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Simple 4-T configuration

Ai

  • (p)a-Si:H (~10nm)

(n)c-Si (~200µm) ITO (80 nm) (n+)a-Si:H (~30nm) Al (i)a-Si:H (<10nm) (i)a-Si:H (<10nm) + Glass FTO SnO2/PCBM Perovskite Spiro-OMeTAD ITO Buffer layer

Demonstrates Feasibility for > 25% efficiency

  • D. McMeekin et al. Science 2016 DOI 10.1126/science.aad5845
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Perovskite-on-Si Tandem EQE and 1-R

10 20 30 40 50 60 70 80 90 100 300 400 500 600 700 800 900 1000 1100 1200 EQE and 1-R (%) Wavelength (nm) EQE Sum IR HIT2 - Perovskite EQE - 18.57mA IR HIT2 - Silicon EQE - 18.26mA IR HIT 2 - 1-R

In collaboration with m. McGehee et al. in Stanford University

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23.6%-Efficient Monolithic Perovskite/Silicon Tandem Solar Cells with Improved Stability

Kevin A. Bush†1, Axel F. Palmstrom†1, Zhengshan J. Yu†2, Mathieu Boccard2, Rongrong Cheacharoen1, Jonathan P. Mailoa3, David P. McMeekin4, Robert L. Z. Hoye3, Colin D. Bailie1, Tomas Leijtens1, Ian Marius Peters3, Maxmillian C. Minichetti1, Nicholas Rolston1, Rohit Prasanna1, Sarah Sofia3, Duncan Harwood5, Wen Ma6, Farhad Moghadam6, Henry J. Snaith4, Tonio Buonassisi3, Zachary C. Holman*2, Stacey F. Bent1, and Michael D. McGehee*1

1 Stanford University, Stanford, 94305, USA. 2 Arizona State University, Tempe, 85281, USA. 3 Massachusetts Institute of Technology, Cambridge, 02139,

USA.

4 University of Oxford, Oxford, UK. 5 D2 Solar LLC, San Jose, 95131, USA. 6 SunPreme, Sunnyvale, 94085, USA.

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Can we go to “All-Perovskite” tandem

We need a low band gap perovskite cell

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1.2eV planar devices?

…not so promising morphology. Tin-based materials seem to crystallise very rapidly, during spin-coating

1:1 MAI:SnI2 in DMF? Noel et al, EES 2014

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Precursor-phase Antisolvent Immersion for high quality films

  • 1. After spin-coating
  • 2. After immersion

in anisole bath

  • 4. After annealing.

50um 10um 2um

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FAPb1-xSnxI3: Photoluminescence

700 750 800 850 900 950 1000 1050 0.0 0.2 0.4 0.6 0.8 1.0

PL counts (norm) Wavelength (nm) Sn percentage 0% 12.5% 25% 37.5% 50% 62.5% 75% 87.5% 100%

0% 12.5% 25% 37.5% 50% 62.5% 75% 87.5% 100% 1.20 1.25 1.30 1.35 1.40 1.45 1.50 1.55

Eg from absorption(Tauc) (eV) PL peak (BP measured - new samples) (eV) Bandgap (eV) Sn %

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Cs addition enables a very high VOC for a 1.2 eV band gap material

  • G. Eperon et al. Science 2016
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All perovskite tandems

  • G. Eperon et al. Science 2016
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Sn-Pb devices show unprecedented stability

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Is it worth “going tandem” without the low gap perovskites?

Calculated EQE and JVs assuming KRICT record cell parameters

A 22.1% APbX3 single junction becomes a 25.9% APbX3/APbX3 tandem Target: cell with a band gap of 2.06eV and Voc of 1.59V On Silicon, a 30.1% hybrid-tandem becomes a 33.6% “triple junction” (+ 0.7V Voc due to Si rear, and FF boost to 0.85)

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Beyond Group XIV elements:

  • G. Volonakis et al. JPCL 2016

ALSO See: Slavney, A. H et al. JACS 2016 McClure, E. T. et al. Chem. Matter. 2016

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Calculated Band-gaps and effective mass

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Single Crystal Data

  • G. Volonakis et al. JPCL 2016
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Device and mini-module development

Present Target:

  • Develop stable and efficient materials stack
  • Develop processing methodology to deliver

Efficient perovskite/Silicon tandem cells at high yield

  • Partner with existing Si-PV industry to

manufacture

Commercialisation

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Test and reliability laboratory Requirements:

  • Climatic testing to IEC61646
  • 85̊C/85% RH >1000hrs
  • +85 to -40̊C cycling >200 cycles
  • “Full Spectrum” Light soaking to AM1.5G

3000hrs (not IEC)

  • High UV exposure
  • Etc etc etc
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IEC Stability testing

  • 85 ̊C for 1000’s of hrs
  • 85 ̊C 85% RH for 1000’s hrs
  • High levels of UV light exposure
  • Thermal Cycling from -40 to

+85 ̊C

  • Full sun light exposure at 60 to

85C

Important note: IEC = 1000hrs

25 years = 218,850 hrs

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20 40 60 80 100 120 200 400 600 800 1000 1200

Normalised perovskite Colour Intensity (%) Stressing Time (hours)

Control (140) Control (115) A B C

Proper Encapsulation of Cells

Interlayer assembly only

Encapsulation selection using 1000hr 85oC/85% baseline

Perovskite layer degradation by moisture ingress after early lamination failure

350hrs 0 hrs

Moisture ingress accelerates degradation

Cover Glass Interlayer Perovskite Film Module Glass

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Stability: IEC61646 Results

Thermal Cycling: Pass Full sun light soaking: Pass Damp heat: Pass

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Next Steps: Development Through to Manufacturing

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Oxford PV acquires thin-film development line for perovskite scale-up

It has acquired the production site previously operated by Bosch Solar CISTech GmbH. The site, located in Brandenburg an der Havel, Germany, will be equipped to provide modern, pilot-scale capacity to scale-up Oxford PV’s perovskite technology to industry-standard wafer size and to perfect the manufacturing processes necessary for commercial deployment.

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S-Q from R.Milo,WIS

qVhν – qVoperation(=MP) [eV]

Evolution of Operational loss in perovskite cells

1.0 1.2 1.4 1.6 1.8 2.0 0.2 0.4 0.6 0.8 1.0 1.2

CdTe a-Si

22.1% 20.1% 17.9% 14.1% 10.9%

GaAs

Absorption Edge (eV)

SQ- Limit Loss

GaInP c-Si

9.7%

Nayak et al. Adv. Mater., 5-2011,3-2014; updated 09-2016

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Why are metal halide perovskites such good solar cell materials???

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Sharp and strong absorption edge

Urbach energy as low as 13 meV Steepness of absorption edge depicts quality of semiconductor Steeper = lower disorder = higher voltage

Technology Urbach Energy (meV)

GaAs 7 c-Si 11 Perovskite 15 CIGS 25 Organics 25-50

Christoph Baliff and co workers JPCL 2014 5 (6), pp 1035–1039

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Electroluminescence vs Absorption onset.

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PLQE and lasing!!

500 1000 1500 2000 30 40 50 60 70 PLQE (%) Excitation power (mW/cm²)

Very High Photo Luminescent quantum yield  Negligible non- radiative decay

740 760 780 800 820 0.0 0.5 1.0 1.5 2.0 Counts (x10

6)

Fluence (J/cm

2)

100 4 (scaled x25) PL Spectrum

Wavelength (nm)

Even room temperature lasing of as cast films within a cavity

Felix Deschler et al. JPCL 2014

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Acknowledgements

Funding EPSRC, ERC & FP7, Oxford John Fell Fund, Oxford Martin School, Royal Society.

Research group

Collaborators: Oxford: Laura Herz, Michael Johnston, Robin Nicholas, Moritz Reide Cambridge: Richard Friend and co-workers Stanford: M. McGehee et al. GT: Seth Marder et al. Bordeaux: Guillaume Wantz et al.

Group