From 02f68a2565b75c0e2d80b68888f91d872c096bf6 Mon Sep 17 00:00:00 2001 From: esoteric-ephemera Date: Fri, 3 May 2024 14:10:57 -0700 Subject: [PATCH 1/3] add initial recommendation decision draft in template style --- .DS_Store | Bin 0 -> 6148 bytes decisions/0016-mp-parameter-updates.md | 151 +++++++++++++++++++++++++ 2 files changed, 151 insertions(+) create mode 100644 .DS_Store create mode 100644 decisions/0016-mp-parameter-updates.md diff --git a/.DS_Store b/.DS_Store new file mode 100644 index 0000000000000000000000000000000000000000..15c851258764d5f137a311c43f72973c2f0788d1 GIT binary patch literal 6148 zcmeHKOG?B*5UtJx%pk}tT?P*z%mt(!;#y%=?j(tfLShd@_t|(8@8Ai%hZk_;&V}Hs z?qWG5Mcs=L+a%TFs?9a*k+-<#eY+1oz7Vqq0!Kp9X5 z{w@Q2$U>6+fI2Dz%78MkVSvwv6v}7?+kpP)z~EZ|U<|Vt%(<7~oK(;XwgKURn2-t# zsYY516VhQ%CC&=A0Yf?&X+DgsY@|ames$bG_2Fb}Kpm9?u!xR + +# Updating the MP parameter sets + +## Context and Problem Statement + +The last systematic audits of parameters used in the Materials Project workflows occurred in 2011 for PBE, and in 2020-2021 for r$^2$SCAN. Over those years, various parameters in those workflows have been updated as need arose. + +This work aims to systematically update a few critical parameters used in the workflows that need updating: `ISMEAR`, `LREAL`, `LMAXMIX`, `KSPACING`, and `POTCARs`. + +[Link to relevant issue with early discussion.](https://github.com/materialsproject/foundation/issues/25). + +This document is a summary of a longer document which includes, for each parameter recommendation, a background and motivation section which explains physically what a parameter controls. These sections can safely be skipped if one is already familiar with the parameter. The method and discussion sections present all required descriptions of how tests were conceived, executed, and interpreted. + +At present, this [longer document](https://drive.google.com/file/d/1fUUx0wrrtMRcSss5yv3NiQuC7J5IiEKL/view?usp=sharing) is a living document. After a community discussion and foundation vote, it will be frozen with a specific set of recommended parameter changes. + + + +## Decision Drivers + +* MP is a global leader in data reliability; periodically updating our computational parameters ensures consistent data quality. + +## Considered Options + +### Current data-driven recommendation + +For INCAR settings: + +- `ALGO` = "NORMAL", as this is robust enough and "ALL" can be quite slow. + +- For relaxations in any solid, `ISMEAR`= 0 (Gaussian smearing) with + smearing width (SIGMA) 0.05 eV + +- For statics in any solid, `ISMEAR`= -5 (unchanged from prior works) + +- LMAXMIX = 6 in all solids and for plain DFT without Hubbard $U$ + +- LREAL = False always + +- Bringing the PBE workflow parameters (ENCUT, EDIFF, EDIFFG, etc.) in + line with the r$^2$SCAN workflow + +For KPOINTS updates: Use $\Gamma$-centered meshes with the following +formula for KSPACING, based on bandgap $$\begin{aligned} + \mathrm{KSPACING} &= \frac{1}{2} \left\{ \Delta k_\text{min} + \Delta k_\text{max} + (\Delta k_\text{max} - \Delta k_\text{min})\frac{\delta}{[1 + \delta^c]^{1/c}} \right\}, \\ + \delta &= a(E_g - b), \\ + \Delta k_\text{min} &= 0.2, \\ + \Delta k_\text{max} &= 0.45, \\ + a &= 0.9,\\ + b &= 2.35,\\ + c &= 8. \\ +\end{aligned}$$ + +For POTCAR updates: + +- The current actinide series of POTCARs used by MP is inconsistent + with all-electron data and must be updated. + +- Some issues are also noted for Ba and Xe + +- Recommendations for new POTCARs are given in Ref. 1, + which results in GW-derived pseudopotentials being recommended for + Ba and Xe. We have also benchmarked these for higher accuracy, and + present them in Table [1](#tab:potcar_changes){reference-type="ref" + reference="tab:potcar_changes"} + +::: {#tab:potcar_changes} + Element MP r$^2$SCAN POTCAR New POTCAR New POTCAR ENMAX (eV) + --------- --------------------- ------------ ----------------------- + Ba Ba_sv Ba_sv_GW 267.02 + Dy Dy_3 Dy_h 405.886 + Er Er_3 Er_h 429.583 + Ho Ho_3 Ho_h 415.91 + Nd Nd_3 Nd_h 402.016 + Pm Pm_3 Pm_h 404.406 + Pr Pr_3 Pr_h 400.742 + Sm Sm_3 Sm_h 405.382 + Tb Tb_3 Tb_h 405.043 + Tm Tm_3 Tm_h 419.812 + Xe Xe Xe_GW 179.547 + Yb Yb_3 Yb_h 409.285 + + : Summary of recommended POTCAR changes. The POTCARs used in the + r$^2$SCAN are listed in the second column for each element in the + first column (from the left). The recommended POTCARs from Ref. + 1 are listed in the third column, and their minimum + required plane-wave cutoff energies are listed in the rightmost column + (ENMAX). +::: + +For Hubbard $U$ updates: + +- PBE+$U$ is demonstrably worse for describing formation enthalpies + +- An attempt to determine optimal $U$'s for PBE (and later r$^2$SCAN) + using experimental formation enthalpies for the whole $d$-block was + unsuccessful + +- Fitting redox enthalpies may represent one path to expanding the + $U$'s used by MP + +We do not present data for PBE$+U$, as this may go into a separate +publication (this can be shared privately). + + 1 E. Bosoni et al. , Nature Rev. Phys. 6 , 45 (2024). DOI: [10.1038/s42254-023-00655-3](https://doi.org/10.1038/s42254-023-00655-3) + + +### Alternatives + +A few other alternatives are listed in the longer document. + +## Decision Outcome + +N/A right now. + + + +## Implementation Plan + +The updated parameters currently in [this fork of atomate2](https://github.com/esoteric-ephemera/atomate2/tree/updated_mp), but will be migrated to a pymatgen PR pending a change in atomate2 to move input sets there. (Hence the `~`) + +- [~] `pymatgen`: ... +- [~] `atomate2`: ... +- [N/A] `emmet`: ... +- [N/A] `crystal-toolkit`: ... +- [N/A] `jobflow`: ... +- [N/A] `maggma`: ... + + +## More Information + +See the longer document for extensive validation of these recommendations by a large set of VASP calculations. + +This work was prepared with valuable suggestions and contributions by +(alphabetical): Matthew Horton, Patrick Huck, Anubhav Jain, Ryan +Kingsbury, Matthew Kuner, Jason Munro, Kristin Persson, Janosh +Riebesell, Andrew Rosen, and Ruoxi Yang. \ No newline at end of file From 4cb32522343058ea693d381f694e1716c8d75b23 Mon Sep 17 00:00:00 2001 From: esoteric-ephemera Date: Fri, 3 May 2024 14:11:50 -0700 Subject: [PATCH 2/3] add gitignore, remove DS_Store mac hidden file --- .DS_Store | Bin 6148 -> 0 bytes .gitignore | 1 + 2 files changed, 1 insertion(+) delete mode 100644 .DS_Store create mode 100644 .gitignore diff --git a/.DS_Store b/.DS_Store deleted file mode 100644 index 15c851258764d5f137a311c43f72973c2f0788d1..0000000000000000000000000000000000000000 GIT binary patch literal 0 HcmV?d00001 literal 6148 zcmeHKOG?B*5UtJx%pk}tT?P*z%mt(!;#y%=?j(tfLShd@_t|(8@8Ai%hZk_;&V}Hs z?qWG5Mcs=L+a%TFs?9a*k+-<#eY+1oz7Vqq0!Kp9X5 z{w@Q2$U>6+fI2Dz%78MkVSvwv6v}7?+kpP)z~EZ|U<|Vt%(<7~oK(;XwgKURn2-t# zsYY516VhQ%CC&=A0Yf?&X+DgsY@|ames$bG_2Fb}Kpm9?u!xR Date: Wed, 8 May 2024 11:22:51 -0700 Subject: [PATCH 3/3] update potcar results --- ...pdates.md => 00xx-mp-parameter-updates.md} | 49 +++++++++---------- 1 file changed, 22 insertions(+), 27 deletions(-) rename decisions/{0016-mp-parameter-updates.md => 00xx-mp-parameter-updates.md} (76%) diff --git a/decisions/0016-mp-parameter-updates.md b/decisions/00xx-mp-parameter-updates.md similarity index 76% rename from decisions/0016-mp-parameter-updates.md rename to decisions/00xx-mp-parameter-updates.md index be9c9f0..52e7d80 100644 --- a/decisions/0016-mp-parameter-updates.md +++ b/decisions/00xx-mp-parameter-updates.md @@ -70,37 +70,32 @@ For POTCAR updates: - The current actinide series of POTCARs used by MP is inconsistent with all-electron data and must be updated. -- Some issues are also noted for Ba and Xe +- "Optimal" POTCARs are determined by minimizing the error in + equation-of-state-fitted equilibrium volumes, bulk moduli, and the + pressure derivative of the bulk modulus. Reference values are taken + from all-electron data [@bosoni2024] -- Recommendations for new POTCARs are given in Ref. 1, +- By this criteria, 58 POTCARs in total would be updated + +- Alternately, updating only those 12 elements which show $\geq 3$% + MAPE in equilibrium volumes yields very comparable accuracy to the + fully optimized set. This is the "minimal update" set + +- Recommendations for new POTCARs are given in Ref. [@bosoni2024], which results in GW-derived pseudopotentials being recommended for - Ba and Xe. We have also benchmarked these for higher accuracy, and - present them in Table [1](#tab:potcar_changes){reference-type="ref" + Ba and Xe, among other elements We have also benchmarked these for + higher accuracy, and present them in Table + [\[tab:potcar_changes\]](#tab:potcar_changes){reference-type="ref" reference="tab:potcar_changes"} -::: {#tab:potcar_changes} - Element MP r$^2$SCAN POTCAR New POTCAR New POTCAR ENMAX (eV) - --------- --------------------- ------------ ----------------------- - Ba Ba_sv Ba_sv_GW 267.02 - Dy Dy_3 Dy_h 405.886 - Er Er_3 Er_h 429.583 - Ho Ho_3 Ho_h 415.91 - Nd Nd_3 Nd_h 402.016 - Pm Pm_3 Pm_h 404.406 - Pr Pr_3 Pr_h 400.742 - Sm Sm_3 Sm_h 405.382 - Tb Tb_3 Tb_h 405.043 - Tm Tm_3 Tm_h 419.812 - Xe Xe Xe_GW 179.547 - Yb Yb_3 Yb_h 409.285 - - : Summary of recommended POTCAR changes. The POTCARs used in the - r$^2$SCAN are listed in the second column for each element in the - first column (from the left). The recommended POTCARs from Ref. - 1 are listed in the third column, and their minimum - required plane-wave cutoff energies are listed in the rightmost column - (ENMAX). -::: +- From Table + [\[tab:potcar_changes\]](#tab:potcar_changes){reference-type="ref" + reference="tab:potcar_changes"}: going from MP's current POTCAR set + to the minimal update set reduces the volume MAPE from 2.2% to 0.7%; + going to the optimal set reduces this further to 0.5%. Similarly, + for the bulk modulus, going from MP's set to the minimal update set + reduces the bulk modulus MAPE from 10.7% to 4.0%, and then to 3.9% + for the optimal set. For Hubbard $U$ updates: