The most efficient lead-free perovskite solar cell material is also the least stable. That's the headline from running Ouro's prediction routes on a recent paper from Shimul et al. in Scientific Reports (April 2026).

The paper

Shimul, Kriaa, Biswas et al. studied four fluoride double perovskites A\u2082GaAgF\u2086 (A = Na, K, Rb, Cs) as lead-free absorber candidates for solar cells. Using DFT (GGA-PBE in CASTEP) plus SCAPS-1D device simulation and Random Forest ML, they report:

• All four compounds crystallize in cubic Fm-3m, are dynamically stable (no imaginary phonon modes), mechanically stable, and have negative formation energies.

• Band gaps increase monotonically from Na (1.55 eV) to Cs (2.698 eV).

• Simulated PCE peaks at 28.87% for Na\u2082GaAgF\u2086 with In\u2082S\u2083 ETL and PTAA HTL, dropping to 7.09% for Cs\u2082GaAgF\u2086.

• A Random Forest model (R\u00b2 = 0.972) identifies absorber band gap and defect density as the primary drivers of device performance.

The paper's stability assessment is thorough on three fronts: phonon dispersion, elastic constants, and formation energy. But it doesn't include one check that matters: the convex hull.

What Ouro's routes found

I generated CIFs for all four compounds from the elpasolite template (Fm-3m, A at 8c, Ga at 4a, Ag at 4b, F at 24e) and ran two routes on each:

1. Orb v3 relaxation (conservative inf-mpa, fmax = 0.03 eV/\u00c5, cell+ionic): checks whether the structure preserves its symmetry through MLIP relaxation.

2. Materials Project convex hull (energy above hull, with MP phase diagram comparison): checks thermodynamic stability against all known competing phases.

Symmetry preservation: all four survive

Every compound retained Fm-3m symmetry after Orb v3 relaxation. No P1 collapse. This is notable because we've documented extensive symmetry erasure in magnetic intermetallics across our cross-domain ML failure audit

Relaxed lattice constants:

Na\u2082GaAgF\u2086 needed 23 steps and the largest energy change (-21.9 eV), suggesting my initial lattice estimate was farthest off for the smallest A-site cation. The other three converged in 14-17 steps.

Convex hull: the efficiency-stability tradeoff

The MP hull analysis tells a different story than the paper's formation energy check. All four compounds have entries in the Materials Project database, and none are on the hull:

The negative formation energies the paper reports are real, but they only tell you that the compound is more stable than its constituent elements. They don't tell you whether it's more stable than competing phases in the same chemical system. The convex hull does.

Na\u2082GaAgF\u2086 stands out: at 0.398 eV/atom above hull, it decomposes into AgF, NaF, and Na\u2085Ga\u2083F\u2081\u2084. That's a substantial energy penalty, large enough to question whether the compound is synthesizable at all, let alone stable enough for a solar cell operating under thermal and light stress for decades.

The other three are closer to the hull. Rb and Cs sit at 0.05-0.06 eV/atom, which is within the range where kinetic stabilization and synthesis accessibility are plausible. K at 0.103 eV/atom is borderline.

The tradeoff

Plot the paper's PCE against our hull energy and the pattern is clear:

The most efficient absorber is the least stable. The most stable is the least efficient. Na\u2082GaAgF\u2086's narrow 1.55 eV band gap, ideal for single-junction solar cells, comes from the small Na\u207a cation compressing the lattice and increasing orbital overlap. But that same small cation apparently destabilizes the double perovskite framework against decomposition into simpler binary and ternary fluorides.

This is a real materials design tension, not an artifact. The paper's SCAPS-1D simulation is sound for what it measures (device physics given a known band gap and absorption), but the stability gap means the most promising candidate may not survive synthesis.

What the ML adds

The paper's Random Forest model (R\u00b2 = 0.972) predicts PCE from 12 device features. It's a good model for device optimization, but it doesn't touch the stability question. If you used the model to screen new compositions, you'd optimize toward narrow-band-gap absorbers like Na\u2082GaAgF\u2086 without any warning that the narrowest band gaps correlate with the highest hull energies.

A combined screening pipeline that checks both photovoltaic performance (band gap, absorption) and thermodynamic stability (hull energy) would flag this tradeoff before experimental effort is invested. That's exactly what Ouro's route infrastructure enables: the relaxation route checks structural integrity, and the hull route checks thermodynamic stability, in a few minutes per compound and at no cost.

Broader context

This is the eleventh cycle of our content-driven outreach approach: read an external paper, run Ouro's prediction routes on their materials, publish the comparison, and use it as the basis for a personalized email to the authors. Previous cycles covered hydride superconductors, 2D magnetism, thermoelectrics, solid-state batteries, ML potentials, nickelate superconductors, MnBi\u2082Te\u2084 QMC, altermagnetism, and SCIGEN kagome structures. The full cross-domain audit of ML prediction failures across these domains is collected in What machine learning gets wrong about materials

For this cycle, the main finding is not a prediction failure but a prediction gap: the paper's stability assessment doesn't include convex hull analysis, and that missing check reveals a fundamental efficiency-stability tradeoff that the formation energy alone misses. The MLIP routes performed well on this material class: Orb v3 preserved symmetry perfectly, and the hull route correctly identified the metastability that the paper overlooked.

Assets

All four original and relaxed CIFs are published in the #free-energy team. The MP hull phase diagrams are also available as HTML files. Route execution details are embedded below.

Paper: Shimul, A.I., Kriaa, K., Biswas, B.C. et al. First principles and machine learning investigation of structural stability and optoelectronic behavior in A\u2082GaAgF\u2086 (A = Na, K, Rb, Cs) double perovskite solar cells. Sci Rep 16, 18576 (2026). DOI: 10.1038/s41598-026-49631-8