Computational Modelling — Metallic Metal-Organic Frameworks Predicted by the Combination of Machine Learning Methods and Ab Initio Calculations

Measurement evidence

Computational Modelling

Metallic Metal-Organic Frameworks Predicted by the Combination of Machine Learning Methods and Ab Initio Calculations · He Y., Cubuk E.D., Allendorf M.D. et al. · Journal of Physical Chemistry Letters · 2018 · 4562-4569

13 measurement groups · 137 results

Reported values remain attached to the sample, method, conditions, extraction quality and source location that produced them.

DFT+HSE electronic band-structure calculation

DFT model of CdC4 (Cd2C8 model) · Model

Hybrid-functional check of the Cd2C8 CdC4 model beyond DFT+PBE to assess whether semilocal self-interaction caused fictitious metallisation.

Geometry
periodic crystal model
Context
pristine computational framework model
Measurement source
4 · Results and discussion · Figure S6
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
HSE band-structure figure supportband structure computed at high-symmetry points——Caption
Qualitative
13 · Ab Initio Calculations · Figure S6
DFT+HSE metallicity checkMarked as a best value within this paperCd2C8 remains metallic——Text
Qualitative
4 · Results and discussion · Figure S6

VASP DFT with GGA-PBE functional and PAW pseudopotentials

DFT model of CdC4 (Cd2C8 model) · Model

Kinetic energy cutoff 450 eV; Monkhorst-Pack grid 8x8x8; structures relaxed in volume and atomic positions until forces were below 0.01 eV/angstrom before self-consistent density and band-structure calculations.

Geometry
periodic crystal model
Context
pristine computational framework model
Measurement source
9-10 · Ab Initio Calculations · Table SIV
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
large band dispersion / bandwidthup to a few hundred meV, particularly for Cd2C8 and Mn4Re12Te16C12N12——Text
Approximate
5 · Results and discussion · Figure 4
DFT-optimised crystal structure typeface centered cubic——SI Table
Qualitative
10 · Ab Initio Calculations · Table SIV
calculated DOS near Fermi levelDOS around the Fermi level calculated——Caption
Qualitative
12 · Ab Initio Calculations · Figure S5
Monkhorst-Pack k-point grid8x8x8——Text
Exact Reported
9-10 · Ab Initio Calculations · Methods paragraph
DFT-optimised lattice parameter a8.9364——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter b8.9364——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter c8.9364——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT+PBE metallicity statusMarked as a best value within this paperDFT-confirmed metallic——Table
Qualitative
4 · Results and discussion · Table 2
classifier metallic votesLR=metallic; SVC=not reported metallic; NN=not reported metallic; RF=metallic——Table
Qualitative
4 · Results and discussion · Table 2
estimated Mott constant C0.0838——Table
Exact Reported
4 · Results and discussion · Table 2
DFT+PBE band gapMarked as a best value within this paper0——Table
Exact Reported
4 · Results and discussion · Table 2

VASP DFT with GGA-PBE functional and PAW pseudopotentials

DFT model of CdC4 (Cd8C32 model) · Model

Kinetic energy cutoff 450 eV; Monkhorst-Pack grid 4x4x2; structures relaxed in volume and atomic positions until forces were below 0.01 eV/angstrom before self-consistent density and band-structure calculations.

Geometry
periodic crystal model
Context
pristine computational framework model
Measurement source
9-10 · Ab Initio Calculations · Table SIV
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
DFT-optimised crystal structure typesimple monoclinic——SI Table
Qualitative
10 · Ab Initio Calculations · Table SIV
Monkhorst-Pack k-point grid4x4x2——Text
Exact Reported
9-10 · Ab Initio Calculations · Methods paragraph
DFT-optimised lattice parameter a9.003——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter b12.046——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter c18.87——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT+PBE metallicity statusnot DFT-confirmed metallic——Table
Qualitative
4 · Results and discussion · Table 2
classifier metallic votesLR=metallic; SVC=not reported metallic; NN=not reported metallic; RF=metallic——Table
Qualitative
4 · Results and discussion · Table 2
DFT+PBE band gap2.19——Table
Exact Reported
4 · Results and discussion · Table 2

VASP DFT with GGA-PBE functional and PAW pseudopotentials

DFT model of Hg[SCN]4Co[NCS]4 · Model

Kinetic energy cutoff 450 eV; Monkhorst-Pack grid 8x4x4; structures relaxed in volume and atomic positions until forces were below 0.01 eV/angstrom before self-consistent density and band-structure calculations.

Geometry
periodic crystal model
Context
pristine computational framework model
Measurement source
9-10 · Ab Initio Calculations · Table SIV
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
DFT-optimised crystal structure typesimple orthorhombic——SI Table
Qualitative
10 · Ab Initio Calculations · Table SIV
calculated DOS near Fermi levelDOS around the Fermi level calculated——Caption
Qualitative
12 · Ab Initio Calculations · Figure S5
Monkhorst-Pack k-point grid8x4x4——Text
Exact Reported
9-10 · Ab Initio Calculations · Methods paragraph
DFT-optimised lattice parameter a7.6237——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter b14.2872——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter c15.4499——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT+PBE metallicity statusMarked as a best value within this paperDFT-confirmed metallic——Table
Qualitative
4 · Results and discussion · Table 2
classifier metallic votesLR=not reported metallic; SVC=metallic; NN=metallic; RF=metallic——Table
Qualitative
4 · Results and discussion · Table 2
estimated Mott constant C0.089——Table
Exact Reported
4 · Results and discussion · Table 2
DFT+PBE band gapMarked as a best value within this paper0——Table
Exact Reported
4 · Results and discussion · Table 2

VASP DFT with GGA-PBE functional and PAW pseudopotentials

DFT model of KNd[Re4Te4(CN)12] · Model

Kinetic energy cutoff 450 eV; Monkhorst-Pack grid 4x4x2; structures relaxed in volume and atomic positions until forces were below 0.01 eV/angstrom before self-consistent density and band-structure calculations.

Geometry
periodic crystal model
Context
pristine computational framework model
Measurement source
9-10 · Ab Initio Calculations · Table SIV
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
DFT-optimised crystal structure typebase centered orthorhombic——SI Table
Qualitative
10 · Ab Initio Calculations · Table SIV
Monkhorst-Pack k-point grid4x4x2——Text
Exact Reported
9-10 · Ab Initio Calculations · Methods paragraph
DFT-optimised lattice parameter a12.2367——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter b12.2367——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter c18.9469——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT+PBE metallicity statusnot DFT-confirmed metallic——Table
Qualitative
4 · Results and discussion · Table 2
classifier metallic votesLR=metallic; SVC=not reported metallic; NN=metallic; RF=not reported metallic——Table
Qualitative
4 · Results and discussion · Table 2
DFT+PBE band gap1.49——Table
Exact Reported
4 · Results and discussion · Table 2

VASP DFT with GGA-PBE functional and PAW pseudopotentials

DFT model of Mn[Re3Te4(CN)3] · Model

Kinetic energy cutoff 450 eV; Monkhorst-Pack grid 6x6x4; structures relaxed in volume and atomic positions until forces were below 0.01 eV/angstrom before self-consistent density and band-structure calculations.

Geometry
periodic crystal model
Context
pristine computational framework model
Measurement source
9-10 · Ab Initio Calculations · Table SIV
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
DFT-optimised crystal structure typesimple monoclinic——SI Table
Qualitative
10 · Ab Initio Calculations · Table SIV
calculated DOS near Fermi levelDOS around the Fermi level calculated——Caption
Qualitative
12 · Ab Initio Calculations · Figure S5
Monkhorst-Pack k-point grid6x6x4——Text
Exact Reported
9-10 · Ab Initio Calculations · Methods paragraph
DFT-optimised lattice parameter a9.6777——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter b10.8246——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter c16.0906——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT+PBE metallicity statusMarked as a best value within this paperDFT-confirmed metallic——Table
Qualitative
4 · Results and discussion · Table 2
classifier metallic votesLR=metallic; SVC=not reported metallic; NN=metallic; RF=not reported metallic——Table
Qualitative
4 · Results and discussion · Table 2
estimated Mott constant C0.1152——Table
Exact Reported
4 · Results and discussion · Table 2
DFT+PBE band gapMarked as a best value within this paper0——Table
Exact Reported
4 · Results and discussion · Table 2

VASP DFT with GGA-PBE functional and PAW pseudopotentials

DFT model of Mn2[Re6S8(CN)6]4 · Model

Kinetic energy cutoff 450 eV; Monkhorst-Pack grid 4x4x4; structures relaxed in volume and atomic positions until forces were below 0.01 eV/angstrom before self-consistent density and band-structure calculations.

Geometry
periodic crystal model
Context
pristine computational framework model
Measurement source
9-10 · Ab Initio Calculations · Table SIV
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
DFT-optimised crystal structure typesimple cubic——SI Table
Qualitative
10 · Ab Initio Calculations · Table SIV
calculated DOS near Fermi levelDOS around the Fermi level calculated——Caption
Qualitative
12 · Ab Initio Calculations · Figure S5
Monkhorst-Pack k-point grid4x4x4——Text
Exact Reported
9-10 · Ab Initio Calculations · Methods paragraph
DFT-optimised lattice parameter a16.3842——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter b16.3842——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter c16.3842——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT+PBE metallicity statusMarked as a best value within this paperDFT-confirmed metallic——Table
Qualitative
4 · Results and discussion · Table 2
classifier metallic votesLR=metallic; SVC=not reported metallic; NN=metallic; RF=not reported metallic——Table
Qualitative
4 · Results and discussion · Table 2
estimated Mott constant C0.1025——Table
Exact Reported
4 · Results and discussion · Table 2
DFT+PBE band gapMarked as a best value within this paper0——Table
Exact Reported
4 · Results and discussion · Table 2

VASP DFT with GGA-PBE functional and PAW pseudopotentials

DFT model of Mn2[Re6Se8(CN)6]4 · Model

Kinetic energy cutoff 450 eV; Monkhorst-Pack grid 4x4x4; structures relaxed in volume and atomic positions until forces were below 0.01 eV/angstrom before self-consistent density and band-structure calculations.

Geometry
periodic crystal model
Context
pristine computational framework model
Measurement source
9-10 · Ab Initio Calculations · Table SIV
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
DFT-optimised crystal structure typesimple orthorhombic——SI Table
Qualitative
10 · Ab Initio Calculations · Table SIV
calculated DOS near Fermi levelDOS around the Fermi level calculated——Caption
Qualitative
12 · Ab Initio Calculations · Figure S5
Monkhorst-Pack k-point grid4x4x4——Text
Exact Reported
9-10 · Ab Initio Calculations · Methods paragraph
DFT-optimised lattice parameter a16.3862——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter b16.0077——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter c15.9653——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT+PBE metallicity statusMarked as a best value within this paperDFT-confirmed metallic——Table
Qualitative
4 · Results and discussion · Table 2
classifier metallic votesLR=metallic; SVC=not reported metallic; NN=metallic; RF=not reported metallic——Table
Qualitative
4 · Results and discussion · Table 2
estimated Mott constant C0.1042——Table
Exact Reported
4 · Results and discussion · Table 2
DFT+PBE band gapMarked as a best value within this paper0——Table
Exact Reported
4 · Results and discussion · Table 2

VASP DFT with GGA-PBE functional and PAW pseudopotentials

DFT model of Mn2[Re6Te8(CN)6]4 · Model

Kinetic energy cutoff 450 eV; Monkhorst-Pack grid 4x4x4; structures relaxed in volume and atomic positions until forces were below 0.01 eV/angstrom before self-consistent density and band-structure calculations.

Geometry
periodic crystal model
Context
pristine computational framework model
Measurement source
9-10 · Ab Initio Calculations · Table SIV
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
DFT-optimised crystal structure typesimple orthorhombic——SI Table
Qualitative
10 · Ab Initio Calculations · Table SIV
calculated DOS near Fermi levelDOS around the Fermi level calculated——Caption
Qualitative
12 · Ab Initio Calculations · Figure S5
Monkhorst-Pack k-point grid4x4x4——Text
Exact Reported
9-10 · Ab Initio Calculations · Methods paragraph
DFT-optimised lattice parameter a16.7127——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter b16.1979——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter c15.8171——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT+PBE metallicity statusMarked as a best value within this paperDFT-confirmed metallic——Table
Qualitative
4 · Results and discussion · Table 2
classifier metallic votesLR=metallic; SVC=not reported metallic; NN=metallic; RF=not reported metallic——Table
Qualitative
4 · Results and discussion · Table 2
estimated Mott constant C0.1034——Table
Exact Reported
4 · Results and discussion · Table 2
DFT+PBE band gapMarked as a best value within this paper0——Table
Exact Reported
4 · Results and discussion · Table 2

VASP DFT with GGA-PBE functional and PAW pseudopotentials

DFT model of Na13Fe4Sb2W18(C4O43)2 · Model

Kinetic energy cutoff 450 eV; Monkhorst-Pack grid 4x4x4; structures relaxed in volume and atomic positions until forces were below 0.01 eV/angstrom before self-consistent density and band-structure calculations.

Geometry
periodic crystal model
Context
pristine computational framework model
Measurement source
9-10 · Ab Initio Calculations · Table SIV
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
DFT-optimised crystal structure typetriclinic——SI Table
Qualitative
10 · Ab Initio Calculations · Table SIV
Monkhorst-Pack k-point grid4x4x4——Text
Exact Reported
9-10 · Ab Initio Calculations · Methods paragraph
DFT-optimised lattice parameter a12.9005——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter b14.399——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT-optimised lattice parameter c19.9229——SI Table
Exact Reported
10 · Ab Initio Calculations · Table SIV
DFT+PBE metallicity statusnot DFT-confirmed metallic——Table
Qualitative
4 · Results and discussion · Table 2
classifier metallic votesLR=metallic; SVC=not reported metallic; NN=metallic; RF=not reported metallic——Table
Qualitative
4 · Results and discussion · Table 2
DFT+PBE band gap0.52——Table
Exact Reported
4 · Results and discussion · Table 2

t-SNE/MDS reduction of 45-dimensional feature spaces

Paper-level ML/DFT screening workflow · Model

Inorganic and MOF feature spaces reduced to two dimensions to assess transfer-learning overlap. SI Figure S3 evaluates overlap ratio versus number of inorganic materials.

Context
computational model screening
Measurement source
3 · Feature-space analysis · Figure 3
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
MOF/inorganic feature-space overlaplarge regions of overlap——Caption
Qualitative
3 · Feature-space analysis · Figure 3
feature selection outcomeall 45 generated material descriptors were used——Text
Exact Reported
4 · Feature Selection · Figure S2

Classifier performance evaluation on inorganic training/test sets

Paper-level ML/DFT screening workflow · Model

52,300 inorganic data split 70% training and 30% test; 5-fold cross-validation for model optimisation; metrics reported as accuracy, precision, recall and classifier-specific candidate counts.

Context
computational model screening
Measurement source
3 · Model evaluation · Table 1
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
testing DC accuracy50%——Table
Exact Reported
3 · Model evaluation · Table 1
testing DC precision50%——Table
Exact Reported
3 · Model evaluation · Table 1
testing DC recall50%——Table
Exact Reported
3 · Model evaluation · Table 1
testing LR accuracy88%——Table
Exact Reported
3 · Model evaluation · Table 1
testing LR precision85%——Table
Exact Reported
3 · Model evaluation · Table 1
testing LR recall92%——Table
Exact Reported
3 · Model evaluation · Table 1
testing NN accuracy94%——Table
Exact Reported
3 · Model evaluation · Table 1
testing NN precision92%——Table
Exact Reported
3 · Model evaluation · Table 1
testing NN recall96%——Table
Exact Reported
3 · Model evaluation · Table 1
testing RF accuracy97%——Table
Exact Reported
3 · Model evaluation · Table 1
testing RF precision96%——Table
Exact Reported
3 · Model evaluation · Table 1
testing RF recall97%——Table
Exact Reported
3 · Model evaluation · Table 1
testing SVC_rbf accuracy95%——Table
Exact Reported
3 · Model evaluation · Table 1
testing SVC_rbf precision94%——Table
Exact Reported
3 · Model evaluation · Table 1
testing SVC_rbf recall96%——Table
Exact Reported
3 · Model evaluation · Table 1
training DC accuracy50%——Table
Exact Reported
3 · Model evaluation · Table 1
training DC precision50%——Table
Exact Reported
3 · Model evaluation · Table 1
training DC recall50%——Table
Exact Reported
3 · Model evaluation · Table 1
training LR accuracy87%——Table
Exact Reported
3 · Model evaluation · Table 1
training LR precision84%——Table
Exact Reported
3 · Model evaluation · Table 1
training LR recall92%——Table
Exact Reported
3 · Model evaluation · Table 1
training NN accuracy95%——Table
Exact Reported
3 · Model evaluation · Table 1
training NN precision94%——Table
Exact Reported
3 · Model evaluation · Table 1
training NN recall97%——Table
Exact Reported
3 · Model evaluation · Table 1
training RF accuracy98%——Table
Exact Reported
3 · Model evaluation · Table 1
training RF precision98%——Table
Exact Reported
3 · Model evaluation · Table 1
training RF recall99%——Table
Exact Reported
3 · Model evaluation · Table 1
training SVC_rbf accuracy97%——Table
Exact Reported
3 · Model evaluation · Table 1
training SVC_rbf precision96%——Table
Exact Reported
3 · Model evaluation · Table 1
training SVC_rbf recall98%——Table
Exact Reported
3 · Model evaluation · Table 1
LR dft confirmed5——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII
LR ml predicted13——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII
LR mv predicted8——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII
NN dft confirmed5——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII
NN ml predicted26——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII
NN mv predicted7——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII
RF dft confirmed2——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII
RF ml predicted3——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII
RF mv predicted3——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII
SVC_rbf dft confirmed1——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII
SVC_rbf ml predicted40——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII
SVC_rbf mv predicted1——SI Table
Exact Reported
7 · Machine Learning Methods · Table SIII

Transfer learning with logistic regression, SVC with rbf kernel, neural network, random forest, and statistical multivoting

Paper-level ML/DFT screening workflow · Model

Models trained on about 52,300 OQMD inorganic compounds using 45 material descriptors; 2932 CoRE-MOF structures screened; candidates predicted metallic by multivoting were validated with DFT.

Context
computational model screening
Measurement source
2 · Methods/results narrative · Figure 1
PropertyReported valueNormalised valueUncertaintyOrigin and qualitySource
dft confirmed metallic countsix intrinsic metallic MOFs——Text
Exact Reported
2-6 · Methods/results narrative · Table 2
generated descriptor count45 material descriptors——Text
Exact Reported
2-6 · Methods/results narrative · Table 2
multivoting accuracy67%——Text
Rounded Reported
2-6 · Methods/results narrative · Table 2
multivoting candidate countnine predicted metallic MOFs——Text
Exact Reported
2-6 · Methods/results narrative · Table 2
oqmd training pool countabout 52,300 inorganic compounds——Text
Approximate
2-6 · Methods/results narrative · Table 2
screened mofs count2932 MOF structures screened——Text
Exact Reported
2-6 · Methods/results narrative · Table 2