Compound characterization data — Buxi et al., 2026

Krishnendu Buxi, Achintya Lakshan, Koustuv Ray, Partha Pratim Jana. “Vacancy ordering mediated symmetry breaking in a twinned lacunar CsCl-related phase: Cr₁₋δNi₂Ga₄ (δ ≈ 0.2).” ChemRxiv (2026). https://doi.org/10.26434/chemrxiv.15007989/v1

Values presented only in scanning electron micrographs, elemental maps, diffraction patterns, reciprocal-lattice reconstructions, or other plots or images were not transcribed. Computed and simulated data were not retained

Cr₁₋δNi₂Ga₄, δ = 0.2, quenched at 673 K without isothermal annealing (Q0)
EDS, atom %	Cr₁₃.₇₍₂₎Ni₂₈.₉₍₅₎Ga₅₇.₃₍₅₎
Single-crystal X-ray diffraction, 293 K, Mo Kα	Cr₀.₈₄₆Ni₂Ga₄; Cr₁₂.₃₅₇Ni₂₉.₂₁₄Ga₅₈.₄₂₈ atom %; cubic; Fm3̅m (225); Z = 2; a = 5.7748(5) Å; V = 192.58(3) Å³; ρcalcd = 7.5922 g cm⁻³; μ = 39.176 mm⁻¹; F(000) = 401; θ = 6.11–38.87°; 1680 reflections measured; 58 unique reflections; Rint = 0.0768; 53 observed reflections, I > 3σ(I); R(F² > 3σ(F²)) = 0.0332; R(F), all data = 0.0378; wR(F²), all data = 0.1202; GOF = 2.77; Δρmin/ρmax = −2.00/2.28 e Å⁻³
Single-crystal X-ray diffraction, refined atomic coordinates and parameters	Ga1: 8c, x/a = 1/4, y/b = x, z/c = x, SOF = 1, Ueq = 0.0117(5) Å²; Ni1: 4b, x/a = 1/2, y/b = x, z/c = x, SOF = 1, Ueq = 0.0075(5) Å²; Cr1: 4a, x/a = 0, y/b = x, z/c = x, SOF = 0.42(4), Ueq = 0.0038(15) Å²
PXRD, Le Bail refinement	P1: Cr₁₋δNi₂Ga₄, δ = 0.2 (Fm3̅m); P2: Ni₂Ga₃ (P3̅m1); P3: CrGa₄ (Im3̅m); GOF = 1.89; Rp = 0.0379; wRp = 0.056

Cr₁₋δNi₂Ga₄, δ = 0.2, annealed at 673 K for 53 h and quenched (Q1)
PXRD, Le Bail refinement	P1: Cr₁₋δNi₂Ga₄, δ = 0.2 (I4₁/amd); P2: Ni₂Ga₃ (P3̅m1); P3: CrGa₄ (Im3̅m); P4: Cr₃Ga₄ (C2/m); GOF = 1.71; Rp = 0.0312; wRp = 0.0430

Cr₁₋δNi₂Ga₄, δ = 0.2, annealed at 673 K for 106 h and quenched (Q2)
Single-crystal X-ray diffraction, reciprocal-space analysis	Superstructure reflections began to emerge after annealing at 673 K for 106 h and progressively intensified with longer annealing; the transformation proceeded from cubic Fm3̅m to a tetragonal phase with three orthogonal domains
PXRD, Le Bail refinement	P1: Cr₁₋δNi₂Ga₄, δ = 0.2 (I4₁/amd); P2: Ni₂Ga₃ (P3̅m1); P3: CrGa₄ (Im3̅m); P4: Cr₃Ga₄ (C2/m); GOF = 1.74; Rp = 0.0355; wRp = 0.0503

Cr₁₋δNi₂Ga₄, δ = 0.2, annealed at 673 K for 160 h and quenched (Q3)
PXRD, Le Bail refinement	P1: Cr₁₋δNi₂Ga₄, δ = 0.2 (I4₁/amd); P2: Ni₂Ga₃ (P3̅m1); P3: CrGa₄ (Im3̅m); P4: Cr₃Ga₄ (C2/m); GOF = 1.63; Rp = 0.0334; wRp = 0.0448

Cr₁₋δNi₂Ga₄, δ = 0.2, annealed at 673 K for 213 h and quenched (Q4)
PXRD, Le Bail refinement	P1: Cr₁₋δNi₂Ga₄, δ = 0.2 (I4₁/amd); P2: Ni₂Ga₃ (P3̅m1); P3: CrGa₄ (Im3̅m); P4: Cr₃Ga₄ (C2/m); GOF = 1.62; Rp = 0.0265; wRp = 0.0366

Cr₁₋δNi₂Ga₄, δ = 0.2, annealed at 673 K for 213 h and slowly cooled (Q5)
EDS, atom %	Cr₁₃.₈₍₃₎Ni₂₈.₆₍₅₎Ga₅₇.₆₍₅₎
Single-crystal X-ray diffraction, 293 K, Mo Kα	Cr₀.₈₃₁Ni₂Ga₄; Cr₁₂.₁₆₅Ni₂₉.₂₇₈Ga₅₈.₅₅₆ atom %; tetragonal; I4₁/amd (141); Z = 4; a = 5.7792(1) Å; c = 11.5427(3) Å; V = 385.52(1) Å³; ρcalcd = 7.5717 g cm⁻³; μ = 39.1 mm⁻¹; F(000) = 800; θ = 3.94–32.76°; 255 reflections measured; 212 unique reflections; Rint = 0.0173; 187 observed reflections, I > 3σ(I); R(F² > 3σ(F²)) = 0.0210; R(F), all data = 0.0224; wR(F²), all data = 0.0517; GOF = 1.89; Δρmin/ρmax = −0.95/0.92 e Å⁻³; twin fractions: 0.299(18), 0.276(9), 0.426(16)
Single-crystal X-ray diffraction, refined atomic coordinates and parameters	Ga1: 16f, x/a = 0.2715(2), y/b = 1/4, z/c = 1/8, SOF = 1, Ueq = 0.00846(14) Å²; Ni1: 8e, x/a = 0, y/b = 0, z/c = 0.24169(10), SOF = 1, Ueq = 0.0074(2) Å²; Cr1: 4a, x/a = 0, y/b = x, z/c = x, SOF = 0.837(10), Ueq = 0.0045(3) Å²
PXRD, Le Bail refinement	P1: Cr₁₋δNi₂Ga₄, δ = 0.2 (I4₁/amd); P2: Ni₂Ga₃ (P3̅m1); P3: CrGa₄ (Im3̅m); P4: Cr₃Ga₄ (C2/m); GOF = 1.52; Rp = 0.0259; wRp = 0.0365