1. Summary
This repository contains the key raw data discussed in the manuscript:

L. D. Whalley, J. M. Skelton, J. M. Frost, and A. Walsh, “Phonon anharmonicity, lifetimes and thermal transport in CH3NH3PbI3 from many-body perturbation theory”, Physical Review B 94, 220301(R) (2016), DOI: 10.1103/PhysRevB.94.220301

	A preprint is available on arXiv under arXiv:1609.00825.

2. Overview
The files in this repository provide the main raw and processed data necessary to reproduce the calculations and analysis presented in the paper. Any data not available in this repository may be requested from the authors.
The data includes a set of input files for the Vienna Ab initio Simulation Package (VASP) electronic-structure code,[1] together with input and output files for the Phonopy and Phono3py packages[2, 3] used to set up and post-process the lattice-dynamics calculations. Users are referred to the comprehensive documentation on these codes available online for further information:

•	VASP: https://www.vasp.at/ (accessed 17/02/2017)
•	Phonopy: http://atztogo.github.io/phonopy/ (accessed 17/02/2017)
•	Phono3py: http://atztogo.github.io/phono3py/ (accessed 17/02/2017)

We note that we have not included the projector augmented-wave (PAW) pseudopotentials[4, 5] with the VASP input files, as these were taken from the pseudopotential databases distributed under licence as part of the code. The elemental pseudopotentials used for the calculations are summarised in the following table:

Element	Pseudopotential	
Ga	PAW_PBE Ga_d 06Jul2010	
As	PAW_PBE As 22Sep2009	
Cd	PAW_PBE Cd 06Sep2000	
Te	PAW_PBE Te 08Apr2002	
H	PAW_PBE H 15Jun2001	
C	PAW_PBE C 08Apr2002	
N	PAW_PBE N 08Apr2002	
Pb	PAW_PBE Pb_d 06Sep2000	
I	PAW_PBE I 08Apr2002	

3. Available Data
The data is collected into five GZip-compressed TAR archives, one containing sample input files and four containing data from the calculations on GaAs, CdTe and the orthorhombic and cubic phases of (CH3NH3)PbI3 (MAPbI3; o-MAPbI3/c-MAPbI3). The archives can be unpacked using the tar utility on macOS and Linux, or the free PeaZip software on Windows (http://www.peazip.org/, accessed 17/02/2017).
The contents of the archives are outlined in the following subsections. We note that within some archives a small number of files have been duplicated across subfolders containing groups of input and output files, in order to keep the groups self-contained.

3.1 Sample input files
This archive contains a minimal set of input files for the VASP calculations and Phonopy post processing performed for the four materials.
VASP INCAR and KPOINTS files for the structural relaxations and/or the single-point calculations to evaluate the second and third-order force-constant matrices are provided. The POTCAR file may be reconstructed from the pseudopotential databases distributed with the code (see table on Page 1). We note that the two MAPbI3 structures were taken from our earlier work[6] and were not re-relaxed for the calculations in this study, so input files for the geometry relaxation on these two systems are not included.
The Phonopy configuration files provide example settings for computing the phonon density of states (DoS) curves and band dispersions of the four systems from the calculated second-order force constants.

3.2 Raw data from the calculations on GaAs, CdTe, o-MAPbI3 and c-MAPbI3
Each archive contains the optimised structure (in the VASP POSCAR format; “POSCAR.vasp”) along with input and output from the Phonopy and Phono3py calculations described in the paper, which is stored under the “Phonopy” and “Phono3py” subdirectories, respectively.
For further information about the content and format of these files, readers are referred to the documentation of the respective codes (see Section 2). For the Phono3py calculation, the calculated lattice thermal conductivity tensors as a function of temperature have been extracted from the HDF5 files and written to a CSV-format file for convenience (“kappa-m*.csv”).
For c-MAPbI3, two Phono3py calculations were performed with different supercell expansions used to evaluate the third-order force-constant matrices - these are stored in the subfolders “Phono3py-111” and “Phono3py-222”.
Also for c-MAPbI3, a series of calculations were performed to test convergence of the interaction range of the third-order force constants (see the ESI associated with the paper for details); the data from these calculations has been omitted from this deposit for brevity, but may be obtained from the authors on request.

4. Additional Resources
	This work made use of two custom-written codes, ModeMap and TISH, for performing a more detailed analysis of the phonon instabilities (“soft modes”) in c-MAPbI3. Both codes use the Phonopy calculations included in this repository as input. Both codes are open-source and available online from:

•	ModeMap: https://github.com/JMSkelton/ModeMap (accessed 17/02/2017)
•	TISH: https://github.com/jarvist/Julia-SoftModeTISH-DeformationPotential (accessed 17/02/2017)

Users are referred to the paper and/or the documentation of these codes for further information.

5. References
[1] G. Kresse and J. Hafner, “Ab initio molecular dynamics for liquid metals”, Physical Review B 47, 558(R) (1993)
[2] A. Togo and I. Tanaka, “First principles phonon calculations in materials science”, Scripta Materialia 108, 1 (2015)
[3] A. Togo, L. Chaput and I. Tanaka, “Distributions of phonon lifetimes in Brillouin zones”, Physical Review B 91, 094306 (2015)
[4] P. E. Blochl, “Projector augmented-wave method”, Physical Review B 50, 17953 (1994)
[5] G. Kresse and D. Joubert, “From ultrasoft pseudopotentials to the projector augmented-wave method”, Physical Review B 59, 1758 (1999)
[6] F. Brivio, J. M. Frost, J. M. Skelton, A. J. Jackson, O. J. Weber, M. T. Weller, A. R. Goni, A. M. A. Leguy, P. R. F. Barnes, and A. Walsh, “Lattice dynamics and vibrational spectra of the orthorhombic, tetragonal, and cubic phases of methylammonium lead iodide”, Physical Review B 92, 144308 (2015).