The collection

Every essay — page 8

Page 8 of 36, continuing through the fields in the same order.

Orbitals Where the atoms go Bonding models What symmetry decides Beyond the octet What a spectrum settles When the molecule does not stop What the shape is for What is taught wrongly Series Named objects Orbitals Refutations Search

Beyond the octet

Hypervalency without d orbitals, delocalisation, aromaticity, and the structures the first-year rules quietly cannot describe.

One steps, the other slides — and the step is at the far end. The repulsion energy and the orphan count along the path from a tetrahedron to a square plane. The energy rises smoothly and monotonically, lowest at the tetrahedron and highest at the plane. The count is zero everywhere — including at 89.99° — and becomes one only at 90° exactly. The step is not near the energy's minimum; it is at its maximum, and it is at a single point.

A count that changes at one point

Where does the orphan count step along a distortion, relative to where the energy's minimum sits? A rule that depends on an exact symmetry may have no answer for a real molecule. On the path from a tetrahedron to a square plane the count is the same at every angle up to 89.99° and changes only at 90° exactly — which is the energy's maximum, not its minimum, and a single geometry out of a continuum.

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How many descriptions, against how much they differ. Every cage-and-filling pair, by the number of distinct descriptions its localisation finds and by how far apart they are in the functional. If the count measured ambiguity the points would rise from left to right. The case with the most descriptions — 44 of them — has a spread of two parts in a hundred thousand, and sits at the bottom right.

Counting was right except where it mattered

A cage whose localisation gives dozens of descriptions that are all the same answer raises a worry: if degeneracy is common across the family, counting descriptions is the wrong measure of ambiguity. Across forty-eight cage-and-filling pairs it is the right measure on eleven of the thirteen that have anything to count — and it fails on the one leaned on hardest.

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The energy runs the whole way; the count exists at the two ends. The Coulomb repulsion of six ligands along the Bailar twist, from the trigonal prism at 0° to the octahedron at 60°, with the geometries that have an orphan count marked underneath. The energy is smooth and monotone, lowest at the octahedron. The count is defined at the two ends and at the handful of angles the symmetry finder rounds into them, and nowhere else — not because the geometry is unsymmetrical, but because its group is not tabulated.

The group nobody wrote a table for

The orphan count is predicted to be constant along the Bailar twist, because the twist keeps D3 the whole way. The premise is exactly right — at every angle strictly between the prism and the octahedron the symmetry finder assembles six operations that hold to four parts in 10¹⁶. The conclusion cannot be tested here, because a count is a reduction, and the calculation's nineteen character tables did not include D3.

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The same number, in three different groups, all the way along. The orphan count along the Bailar twist once the D3 character table is written. It is 2 at every one of the 15 geometries the symmetry finder answers for, across D3h at the prism, D3 through the whole interior and Oh at the octahedron. The lower row shows what the same sweep gave before the table existed: two ends and nothing between. This constancy was predicted from the premise that the twist keeps D3 throughout, and the premise was right.

The count the table was hiding

The interior of the Bailar twist looks uncountable — exactly D3 at every angle, and D3 is a point group whose character table is rarely written out. Writing it takes nine lines and settles the prediction made for the path: the orphan count is two at every geometry on the path that can be answered, in three different groups, out of three different decompositions.

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Both criteria leave a gap, and Boys leaves a chasm. Every non-zero relative spread under each criterion, on one logarithmic axis, with the largest empty stretch shaded. Pipek–Mezey's runs a factor of 206; Boys's runs 2.8e+7 — seven decades, from numerical zero to a real spread with nothing between. So the bimodality belongs to the cages rather than to the functional, and under the second criterion the threshold matters even less.

A second criterion left a gap too

The localisation spreads are bimodal — an empty factor of two hundred around the degeneracy threshold — and the gap might belong to the criterion rather than to the cages. Boys localisation leaves a gap of seven decades on the same forty-eight pairs, so it belongs to the cages. But the two criteria disagree about six of them, in both directions, and the family's most ambiguous cage under one is exactly degenerate under the other.

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Six pairs off the diagonal, and every one of them on an axis. Each cage-and-filling pair's Pipek–Mezey spread against its Boys spread, both logarithmic, with the two thresholds drawn. Agreements sit in the two opposite corners: spreads that are zero in both, or large in both. The six disagreements do not sit between them — they sit on the axes, with one coordinate at the floor. A criterion-dependent cage is not one the two criteria half-agree about; it is one where the difference between its descriptions is invisible to one of them entirely.

The cage is on both sides

Two localisation criteria classify six cage-and-filling pairs differently, and a symmetry explanation for the six is the natural first guess. The icosahedron's graph has a hundred and twenty automorphisms, the most in the family, and supplies three of the six disagreements and nine of the agreements. What the six do have in common is sharper than a symmetry: in every one, one criterion's spread is not small but zero.

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Two centres, one path, and the leftover changes sides. The count of leftover orbitals along the Bailar twist, for a main-group centre and for a transition metal. At four valence orbitals against six ligand combinations, two combinations are left with no partner and the count is a count of orphans; at nine against six, every combination finds one and three metal orbitals are left instead. Both are constant along the whole path, in three different point groups, out of decompositions that share no species — which is the replacement rule holding in a case where the arithmetic runs the other way.

The leftover changes sides

A main-group centre brings four valence orbitals against six ligand combinations, so two are orphaned. A transition metal brings nine, so the arithmetic inverts and three metal orbitals are left instead — three at every geometry of the Bailar twist, out of decompositions that share no species. Run past the whole arrangement census, exactly one arrangement orphans anything at a metal, and it needs an f orbital to fix.

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Eighteen paths, two hundred and seventy geometries, one gap. Every one-parameter path between two arrangements of the same ligand count, each sampled at 15 geometries, with each geometry coloured by whether its group is named and tabulated, refused by the finder's tolerance, or a finite group with no table. The one gap is a group of order 10 at the pentagonal-pyramidal end of two paths — C5v, which no table here reaches. The path with a linear end is excluded, since a continuous group is declined deliberately rather than missing.

The gap found on purpose

A twist between two coordination arrangements passes through a point group with no character table among the twenty in use, and that was found by accident. Running every path between the arrangements — eighteen of them, two hundred and seventy geometries — finds exactly one more gap, at a group of order ten. It also finds something the search was not looking for: a group without a table had been reported as an infinite group.

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Forty-eight rows, thirty-three calculations. Every cage-and-filling pair the family survey covers, one cell per pair, with cells that hand the localisation the same set of orbitals joined. A localisation here selects its occupied orbitals by asking which have any occupation at all, and Hund's rule puts one electron into each member of a degenerate shell before pairing any of them — so adding two electrons to a half-filled shell pairs a spin and changes nothing the search can see. Fifteen of the forty-eight rows repeat an input already in the table.

Six disagreements and three calculations

Two localisation criteria classified six of the family's forty-eight cage-and-filling pairs differently, and three of the six were consecutive fillings of one icosahedron with spreads identical to three figures. They are not three coincidences and not one degeneracy being filled: they are one calculation, because the survey's forty-eight rows are thirty-three distinct questions.

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The boundary falls inside a shell, and the shell has no inside. The 12-vertex cage at 10 electrons: its Hückel levels, with each degenerate shell drawn as its members and the occupied ones filled. The occupied set takes 2 of the 5 members of one shell — and the members of a degenerate shell are not distinguishable. Whichever combinations the eigenvalue routine happened to return are the ones that get occupied, so the density being localised is a choice made by a diagonaliser rather than a property of the cage.

The basis a diagonaliser happened to return

Six of the cage family's thirty-three inputs have their occupied set cut through the middle of a degenerate shell, and the members of a degenerate shell are interchangeable. Re-orienting the shell changes nothing about the cage, the filling or the criterion — and it moves the best localisation functional by up to twenty-one per cent, moves the count of descriptions from ten to fourteen, and flips the degeneracy label on three of the six.

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Angular rings leave the heteroatom's own ring alone and scale the rest. Each ring's response as a fraction of the straight chain's, with the heteroatom on ring 0 and the first one, two, four or ten interior rings angularly fused, on a logarithmic axis. The heteroatom's ring stays within one and a half per cent in every case. The rings beyond the angular fusions fall, to under half by the third ring once two are angular, and to between an eighth and a third along the fully angular chain, alternating from ring to ring.

An angular ring rescales what lies beyond it

A heteroatom's influence along a chain of fused rings decays with a length near 0.7 rings, and one bend was found to change almost nothing. Counted properly, that bend was two angular rings, and counting angular rings one at a time shows what they do: the heteroatom's own ring never moves by more than one and a half per cent, the rings beyond angular fusions fall to between an eighth and a half of their response — or rise by up to two fifths — and the decay length changes by a tenth.

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Folding the ring off its plane never gives the orbital back. For rings of four to eight ligands round a centre with no lone pair, the orphan count minus the formula n + L − 4, at polar angles from 60° to 120°. The upper dot in each row is the bare ring and the lower the same ring with a ligand on the axis. The bare ring is one over the formula at every angle, including 90°, where the ring is flat and its group is D₄ₕ, D₅ₕ or D₆ₕ; there is no table here for D₇ₕ or D₈ₕ. The capped ring agrees with the formula at every angle, 90° included, where the ring is exactly flat and the apex alone keeps its group C₄ᵥ to C₈ᵥ.

Folding the ring does not give the orbital back

Three arrangements break the orphan count n + L − 4, all flat, and the reason given was flatness: the p orbital perpendicular to the ring has no ligand combination of its species. Fold the ring into an umbrella at any angle and that orbital becomes totally symmetric — and the count stays wrong by exactly one, for rings of four to eight. The ring offers one symmetric combination to a centre with two symmetric orbitals. Writing C₅ᵥ to see it also counts the pentagonal pyramid at last, and the formula holds there.

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