Concept

Closed form — where it appears

An expression giving a quantity outright rather than by iteration or quadrature. It is kept here so that a numerical answer has something independent to be checked against, which is what stops a plausible wrong number from surviving.

Named by 89 essays across 9 fields — each of them below, with the objects they name alongside it.

Overlap does not always fall as the atoms are pulled apart. The overlap integral of two pairs of orbitals against the separation between their centres, with the turning point and the sign change of each found by bisection on the integral itself. A pair with a radial node in it does not fall monotonically and does not keep one sign.

Closer is not more overlap

Two 1s orbitals overlap more the closer they are, and every curve drawn from that pair says the same thing. Put a radial node into one of them and the rule fails: a 1s with a 2s overlaps by 0.016 at contact, by 0.282 near four bohr, and less again beyond — and two 2p orbitals head-on change sign at 5.06 bohr and are more strongly coupled at eight bohr than at four.

bonding · Overlap
H₂O with 1→D: what each mode is made of. H₂O with 1→D. Each row is one distinct frequency and each column one internal coordinate; the bar is the share of the motion in that coordinate. A mode whose largest share reaches nine tenths is a motion of one bond or one angle and is named for it. 3 of 3 here are.

When a mode becomes a bond stretch

Water's two stretching modes are each exactly half in one O–H bond and half in the other, which is why neither of them belongs to a bond. Change one hydrogen to deuterium and the same force field at the same geometry gives two modes that are 99.5 and 99.7 per cent in a single bond each. Nothing about the bonding changed; a mass did.

spectra · Normal mode
A moment that is not an integer's worth of anything. The effective magnetic moment against temperature for an iron(II) complex whose two spin states lie close together, with the moments belonging to whole numbers of unpaired electrons drawn across. The curve spends its time between them and settles on neither.

A moment between two integers

A magnetic moment is celebrated as one of the few chemical measurements that returns an integer: count the unpaired electrons, feed the count into a formula, and nine first-row ions come out right. That works when one state lies far below the others. Sit a complex at its own crossover and the same measurement returns 0.30 at 80 K and 3.61 at 400 K — a quantity that counts nothing and is a temperature in disguise.

applied · Magnetism
Five sixths of the bonds, nine tenths of the binding. What a site in the outer layer of an open block keeps, measured three ways: the fraction of its bonds, the fraction the second-moment rule predicts of its binding, and the fraction the calculation gives. The last two agree and the first does not.

A surface is not a count of broken bonds

Cut a crystal and every atom in the new face has lost one of its six neighbours. The standard estimate follows immediately: a surface costs one sixth of the cohesive energy per atom exposed. Computed, it costs a little over half that — the atom keeps 91.2 per cent of its binding while keeping only 83.3 per cent of its bonds, because the bonds that survive get stronger when their competitors are removed.

wrong · Cohesion
ammonia's rotational levels, sorted by K. The rigid rotational levels of ammonia up to J = 4, each drawn at its computed energy and grouped by J. Within a group the levels are pushed apart by the second rotational constant, so it is plainly there in the level pattern.

The constant a spectrum cannot see

A symmetric top has two rotational constants and its microwave spectrum reports one of them. Not badly, not with difficulty: ammonia's A of 6.3406 wavenumbers appears in none of its lines at any J and any K, because the term it belongs to cancels exactly out of every transition. The molecule turns about that axis, the energy is real, and the measurement is blind to it.

spectra · Rotation
One band width, three shapes. three densities of states, each computed from a wrapped structure of 4,096 levels and drawn against the band scaled to run from −1 to +1. A chain piles its states into the two edges; a cubic structure piles them into the middle and thins to nothing at the edges.

Where the states pile up

Two bands of the same width can be entirely different objects. Scale a chain, a square net and a cubic structure to one width and what is left varies by a factor of four — a chain puts more than half its levels in the outer thirds of its band and a cubic structure puts more than half in the middle third — and that difference alone decides how strongly each of them binds.

solids · Bands in a solid
water, drawn with its nuclei the size they are. The molecule with a disc round each nucleus whose radius is the computed root-mean-square displacement of that nucleus in the vibrational ground state. The hydrogens' discs are a substantial fraction of the bond length, and this is at no temperature at all.

The atoms are not at the points

Every structure in this collection is a set of points, and every bond angle it argues about is a property of that set. Computed from the fitted force fields it already has, water's hydrogens are 0.094 Å from where they are drawn and its bond angle has a spread of 8.9 degrees — larger than the difference between 104.5 and the tetrahedral value that half the essays here are about. This is at no temperature at all.

shape · Approximation
The same difference, at five repulsions. The charge transferred to the more electronegative of two atoms against the difference in their orbital energies, at five strengths of the repulsion between the two electrons. Only the topmost curve is the two-level result; every other one moves far less charge at the same difference.

A difference does not make a transfer

Every electronegativity scale reports one thing: how far apart two atoms are in their appetite for electrons. Put that difference into a model with repulsion in it and the charge it actually moves is not determined at all — the same difference of one moves 0.447 of an electron with no repulsion and 0.0019 with a strong one, a factor of two hundred and forty-two, and nothing on any scale distinguishes the two cases.

bonding · Electronegativity
The Compton profile, exact and fitted. The momentum density integrated over the two perpendicular directions, for the exact 1s and for three fitted bases. The exact curve is 8/3π(1 + q²)³ in closed form; the fitted ones are sums of Gaussians and are cusped differently at the origin, which is the position-space cusp showing up as a shape in momentum.

The measurement a basis was not fitted to

Six Gaussians reproduce hydrogen's energy to eleven parts in a hundred thousand and its Compton profile to three parts in a thousand — twenty-five times worse, on a quantity an X-ray scattering experiment measures directly. The gap between the two errors widens as the basis is improved, because the energy is the one property a variational fit is best at.

orbitals · Basis
A field splits the n = 2 shell into whole numbers. The eigenvalues of z inside the shell, which are the shifts a uniform field produces to first order. There are three distinct ones and each is a whole number times (3/2)n, so the splitting is proportional to the field itself rather than to its square — which is what no other atom does.

The symmetry that is not a rotation

Hydrogen's n = 2 shell holds four states at one energy and its rotation group accounts for at most three. The operator that accounts for the fourth is built here out of computed integrals: three matrices whose commutators close into the rotations, whose product with the angular momentum vanishes, and whose Casimir comes out at exactly n² − 1.

symmetry · Representation
A σ contour at 90 per cent, and the two atomic ones. The section through both nuclei of the surface enclosing 90 per cent of the bonding orbital's density at 2 bohr, with circles marking where two atomic contours of the same stated fraction would be. The two pictures are different shapes and enclose different amounts, and the atomic pair encloses 91.70 per cent of the molecular orbital's density. Contours drawn: 1s at 90% of its density, |ψ| = 3.94e-2.

A bond is not two atoms overlapping

The surface enclosing ninety per cent of a σ orbital's density is one closed surface with both nuclei inside it, at a level of 0.0359. The two atomic surfaces usually drawn instead sit at 0.0394, are a different shape, and enclose 91.70 per cent of the same orbital — and whether the molecular one is one object or two is decided by the fraction the caption claims, anywhere between 2.1 and 5.2 ångström.

orbitals · Contour
The error, against the repulsion it is an error about. The energy a mean field misses, for two electron counts on 4 sites, against the strength of the repulsion. Each is a straight line at large repulsion and the dashed line through it is not a fit: its slope is the count of coincidences a uniform density forces, computed from the electron number and the site number alone.

A mean field cannot get out of the way

The energy a mean field misses grows without limit as the repulsion rises — 27.82 at U = 32 for four electrons on four sites, against an exact energy of −0.2946, so the error is ninety-four times the answer. The rate it grows at is not an energy at all: it is n²/4N, a count of the coincidences a spread-out density cannot avoid.

beyond · Correlation
Flat rings: the angles, the torsions and what is measured. For each ring from three to eight, held flat: its interior angle, how far that is from tetrahedral, the angle strain that follows, the torsional strain of having every bond eclipsed, and the measured strain energy. The five-ring is the row the essay is about — its angles are almost ideal and it is strained.

The strain that is not in the angles

Cyclopentane's flat bond angles are 108°, a degree and a half from tetrahedral, and its angle strain computed from a standard bending constant is 0.4 kJ mol⁻¹. Its measured strain is twenty-six. The missing sixty kilojoules are torsional — one ethane barrier for every bond in the ring, which no account built on bond angles mentions.

shape · Strain
water: every level up to J = 4, from a matrix. The rotational levels of water at κ = -0.4322, each J diagonalised in the symmetric-top basis. A symmetric top would show one level per K with everything above K = 0 doubly degenerate; here every degeneracy is split, and the size of each splitting is what the third constant is measured from.

The top that reports all three

A symmetric top hides one of its two rotational constants in every line of its spectrum. Break the symmetry and the hiding stops: for water, twenty-three of the twenty-five levels up to J = 4 move when A is changed, and the two that do not are the ground state and the one at B + C. There is no formula for any of them.

spectra · Rotation
One impurity is a level; many are a band. The impurity levels of a ring of 160 with sites of depth -3, drawn as a bar from the lowest to the highest, against the fraction of sites that are impurities. At the lowest concentration every level is at the same energy and the bar has no height at all. By 30 per cent the levels span 2.44 and have closed to within 0.25 of the host band, which is shaded.

One defect is a level, many are a band

A single deepened site in a chain pulls one state out of the band to −√(h² + 4), exactly, and holds it on 1.42 sites. Put in more and the levels spread: at one site in ten they span 1.45 in the same units and have closed to within 0.69 of the host band, and above one site in eight the count of levels stops matching the count of defects, because two defects on neighbouring sites push one of their pair back into the band.

solids · Defect
The same sample, fitted over four temperature ranges. A pair coupled at -50 cm⁻¹, its susceptibility computed exactly, fitted to a Curie–Weiss law over four ranges. The moment and the Weiss temperature the fit reports both depend on which range was used, and the quality of the fit does not warn about it.

The moment a fit invents

One coupled pair of spins, its susceptibility computed exactly, fitted to a Curie–Weiss law over four temperature ranges. The moments reported are 2.471, 2.535, 2.566 and 3.590 Bohr magnetons, and the Weiss temperatures −51, −78, −78 and −292 K — from one sample, measured perfectly, with three of the four fits agreeing with their own data to better than a part in three hundred.

applied · Magnetism
One of these is guaranteed to improve, and it is not the one anybody measures. The relative error in the energy and in four properties of the fitted function, against the number of Gaussians. The energy falls at every step, because that is what the variational principle promises. The mean radius is exact for the single-function basis and 332 thousand times worse for the two-function one, and the density at the nucleus is still 6.2 per cent wrong where the energy is wrong by 0.011 per cent.

The property that gets worse

One Gaussian fitted to hydrogen gets the mean radius exactly right — 1.500000, against an exact 1.5. Two Gaussians get it wrong by 1.4 per cent, which is three hundred and thirty-two thousand times further out, while the energy improves fivefold. The variational principle bounds one number and says nothing whatever about any other, and the sequence of errors in everything else need not even be monotone.

orbitals · Basis
Three bands of one spectrum, and the bond length behind each. Nitrogen's three photoelectron bands, drawn as the vibrational intensity distributions computed from the measured bond lengths and vibrational constants of the three states of the ion. Each band's lines add to one. The middle band is spread over five lines because the electron removed came out of a strongly bonding orbital and the bond lengthened by 77.22 thousandths of an ångström; the outer two keep 92 and 88 per cent of their strength in a single line.

The width of a band is a bond length

Nitrogen's three photoelectron bands are one sharp line, a progression of five, and a line with a shoulder. Computed from the measured bond lengths of the three states of the ion, the intensities come out at 0.917, 0.263 and 0.880 in the first line of each — because removing a weakly bonding electron lengthens the bond by 18.7 thousandths of an ångström, a strongly bonding one by 77.2, and an antibonding one shortens it by 23.7.

spectra · Photoelectron
The part of the bond that is outside the picture. The share of the overlap integral between two 1s orbitals that lies outside both of their 90 per cent contours, against how far apart the atoms are. At a bond length it is 8.3 per cent; by 7 bohr it is 53.4. The two drawn surfaces stop touching at 5.32 bohr, where the overlap is still 0.08 — so the picture separates well before the interaction does.

The tenth that is not drawn

A ninety per cent contour of a hydrogen 1s orbital is a sphere of radius 2.661 bohr, and two of them stop touching at 5.322 bohr — where the overlap between the two orbitals is still 0.0768 and rising in importance. At a three-ångström contact, 36.9 per cent of the overlap integral lies outside both drawn surfaces, and holding nine tenths of it inside the picture would take a contour enclosing 97.28 per cent.

orbitals · Contour
Two kinds of answer to a flux, and only one of them is a curve. The π binding of three rings against the magnetic flux through them, in units of beta and of the flux quantum, measured from each ring's own value at zero flux. Beta is negative, so a binding that FALLS is an energy that rises: benzene's does, which is what a diamagnetic ring current is. Cyclobutadiene's rises in both directions from a corner — its energy has no second derivative at zero field at all, and the two one-sided slopes differ by 12.57.

Two rules that share no arithmetic

Hückel's rule is a statement about a gap. Put a magnetic flux through the same rings instead and ask which of them push the field out, and the answer is the same set — eighty cases, no exceptions — although the second calculation counts nothing and has no shells in it. And the rings the rule excludes turn out to have no magnetic susceptibility at all: their energy has a corner at zero field.

symmetry · Aromaticity
A band becomes a bell curve, and the dimension is the sample size. The normalised fourth moment of a wrapped hypercubic structure's density of states against its dimension, with the closed form 3 − 3/2d drawn through it. They agree to eight decimal places at every dimension from one to 6, and the reason is a limit theorem: a hypercubic spectrum is the sum of d independent one-dimensional ones, so its cumulants fall as powers of d exactly as a sum of independent samples does. The Gaussian value of three is approached and never reached.

A band becomes a bell curve

The normalised fourth moment of a hypercubic structure's density of states is 3 − 3/2d exactly, from one dimension to six, to eight decimal places — because the spectrum is a sum of d independent one-dimensional ones and the central limit theorem is what it is obeying. Reach further in one dimension instead and the shape overshoots a Gaussian rather than approaching it: a chain touching its third neighbour has a cubic structure's coordination and a fourth moment of 3.389 against 2.500.

solids · Bands in a solid
The bonding follows the overlap over, and turns where it turns. The stabilisation of three pairs of orbitals against how far apart they are, each scaled to its own largest, with the coupling taken from the computed overlap. Two orbitals with no radial node are stabilised less at every separation further out; the two with one turn over — and the maximum of the bonding is at exactly the separation of maximum overlap, to five decimal places, because a coupling proportional to the overlap makes the stabilisation a strictly increasing function of it.

The same overlap, a different bond

A 1s and a 2s change their overlap by two thirds between two and seven bohr, and change what they are bonded by by 0.154 per cent. The overlap turns over and the bonding turns over with it, at exactly the same separation to five decimal places — the arithmetic refused the expectation that the secular denominators would move it — and what separates one pair from another is not where the maximum is but how little of it there is.

wrong · Overlap
Every sign, lost. Formaldehyde in its own principal axes. Open circles are the atoms where they are; filled ones are where Kraitchman's equations put them, from the change in the three moments when each atom in turn is made heavier. The two agree to 7.6e-8 ångström — the equations are an identity for a rigid structure — but they return the square of each coordinate, so the two hydrogens at b = ±0.9348 both come back at +0.9348 and land on the same point.

The coordinate an isotope reports

Kraitchman's equations return an atom's position from the change in the moments when that atom alone is made heavier, and for a rigid structure they are an identity — formaldehyde's four atoms come back to a part in ten million. What they return is the square of each coordinate, so both hydrogens at b = ±0.9348 come back at +0.9348; every out-of-plane coordinate comes back imaginary at a moment error of one part in a hundred thousand; and the famous error cancellation, measured at a factor of thirteen, still leaves the answer two and a half times worse than a direct fit.

spectra · Rotation
How anisotropic a structure has to be. The fourth moment of a layered band, divided by the square of its second so that the width drops out, against the coupling between layers. The curve is the closed form that follows from adding cumulants — 3 − 3(2 + λ⁴)/(2(2 + λ²)²) — with nothing fitted; the points are eigenvalues. At λ = 1 it is the three-dimensional value 2.5 and at λ = 0 the two-dimensional 2.25, and it is halfway between them at λ = 0.47 — so the question of when a band is effectively two-dimensional has a number rather than an opinion.

Two bands, and the shape of each

A band's shape has a closed form when the structure it belongs to factorises. Put a second band beside it and the form survives exactly while the two do not talk, and fails as the square of the coupling once they do. Make one direction weaker instead and the form survives everywhere — 3 − 3(2 + λ⁴)/(2(2 + λ²)²), agreeing with eigenvalues to nine decimal places — so how anisotropic a structure has to be before its band is two-dimensional is a number: λ = 0.46518.

solids · Bands in a solid
Two errors, opposite signs, four orders of magnitude apart. A finite basis makes H₂⁺'s binding too large by letting each atom borrow the other's functions, and too small by describing the molecule incompletely. Both are computed here against the exact binding of 0.102634 hartree. The second is thousands of times the first at every basis size, and it is the first that counterpoise removes — so the corrected number is further from the true one than the uncorrected at every row of this table.

The basis the other atom lent

Two atoms in a molecule are described in each other's functions and the separated atoms are not, so the molecule is treated better than the pieces and the binding comes out too large. That is the basis set superposition error, it is removed by a standard correction, and for H₂⁺ in four Gaussians a centre it is six tenths of a microhartree against an incompleteness error of twelve millihartree — a factor of eighteen thousand the other way.

orbitals · Basis
Carbon is not one number. The charge equalisation puts on carbon in the four fluoromethanes, and on hydrogen in the three that have one. Carbon's runs from 0.07 to 0.31, and hydrogen's changes sign between methane and fluoromethane, so the same C–H bond is polarised one way in one molecule and the other way in the next. A table with one number for carbon is printing the value an iteration starts from.

The value that only exists in the bond

A difference in electronegativity moves charge, and moving charge closes the difference — until every atom in the molecule has the same chemical potential. Solving that gives one number per molecule and a charge per atom, and carbon's runs from +0.0692 in methane to +0.3074 in tetrafluoromethane. Hydrogen's changes sign between the first and the second, so the same C–H bond is polarised one way in one compound and the other way in the next.

bonding · Electronegativity
The ceiling rises and the measurements fall, so they cross. The largest acceleration the rotamer account can produce, against the ring being closed, with the measured gem-dimethyl accelerations on the same axis. Closing a bigger ring means freezing more rotations, so the ceiling rises steeply; the measurements go the other way. The five-membered ring's 250-fold acceleration is above its own ceiling of 36.5 and the six-membered ring's tenfold one is far below its 121 — so the account is refused at one size and sufficient at the next.

A ceiling that rises where the measurements fall

The rotamer account of the gem-dimethyl effect has a largest possible acceleration, which looks like a limitation. It is a prediction: the ceiling is a closed form in the number of rotations a closure freezes, it rises steeply with ring size, and the measurements fall — so the account is refuted for the five-membered ring and more than sufficient for the six.

shape · Strain
A correction computed at 3 bohr and used everywhere. Three binding curves for H₂⁺ in 2 Gaussians a centre: uncorrected, properly counterpoise corrected at every separation, and corrected once at 3 bohr with that value subtracted throughout. The frozen curve is the uncorrected one shifted down by a constant, so its minimum sits at 2.2270 bohr — exactly where the uncorrected minimum is, and 4.2 millibohr from where the full correction puts it. The depth moves and the structure does not.

A correction computed at one length

The counterpoise correction is expensive, so it is evaluated once at a reference geometry and subtracted across a whole potential surface. A constant does not move a minimum — so a frozen correction returns the uncorrected bond length exactly, at every reference geometry and in every basis, and everything the correction does to a structure is the part that has just been thrown away.

orbitals · Basis
Four unweighted rules against the answer the hardnesses give. Twelve molecules, each drawn with the exact equalised electronegativity as a filled mark and the four unweighted means of the free atoms' values as open ones. The geometric mean — Sanderson's rule — is the closest on average, at 0.0706 eV against the arithmetic mean's 0.1666, and it is the closest on only 4 of the twelve. Every rule below the arithmetic mean is constrained to sit below it, and 2 of the exact answers do not.

A mean that is low rather than right

Sanderson's rule takes the geometric mean of the atoms' electronegativities, and it works better than the plain average. Computed against the exact equalised answer for twelve molecules it is better by erring downwards — and two of the twelve have exact answers above the plain average, where no geometric mean can go at any parameter.

wrong · Electronegativity
The current does not divide equally between equal rings. The current each ring of an acene carries under a uniform field, ring by ring, for four acenes. Naphthalene's two rings are equal by symmetry; anthracene's middle ring carries 1.180 times what its outer ones do, and tetracene's inner rings 1.222 times. Every ring has the same area and the same six carbons, and the response is a matrix rather than a set of parallel loops.

The current does not divide

A fused ring system's response was computed from the areas of its rings, and the obvious next question was whether the current divides between them the way it divides between two resistors. Giving each ring its own flux and taking the second derivatives says no: the response is a matrix, its off-diagonal entries are nearly half its diagonal ones, and anthracene's middle ring carries 1.18 times what its outer rings do.

symmetry · Aromaticity
How nearly a broken symmetry survives. A screened potential splits the n = 2 shell and destroys the degeneracy the linear Stark effect depends on. The field needed to overcome the splitting and restore the linear behaviour runs from 4.3e+4 volts a centimetre at a quantum defect of 0.00040 to 2.9e+7 at a defect of 0.208. The dipole between the states is 3.000 throughout, so the field is exactly the splitting divided by twice it.

How nearly a broken symmetry survives

The hydrogen shell's extra symmetry is what makes its Stark effect linear, and a real atom does not have it. Screening splits the shell, and the field needed to overcome the splitting and restore the linear behaviour is a curve — from forty thousand volts a centimetre at a quantum defect of 0.0004 to thirty million at a defect of 0.21.

symmetry · Representation
The hybrids do not point at the atoms. For each cycloalkane, the angle between its two ring hybrids — fixed by orthogonality once the measured H–C–H angle has said how much s character the hydrogens take — against the angle between its carbons. Cyclopropane's differ by 45.5°, so each hybrid points 22.75° outside the bond it makes; cyclohexane's agree to 0.035°, which is the control.

The hybrids that point outside the bonds

Coulson's relation says two equivalent hybrids sharing an s orbital are orthogonal only between ninety and a hundred and eighty degrees. Cyclopropane's carbons make sixty, so its ring hybrids cannot point at the atoms they bond to — and the same relation says by how much they miss: 22.75 degrees each, falling to 0.03 in cyclohexane.

bonding · Hybrids
A ninety per cent surface with a neighbour beside it. The contour enclosing 90 per cent of a one-electron ion's density at an effective charge of 1.6, drawn with no field as a circle and in a field of 0.05 atomic units as the closed curve. The surface moves out by 47.3 millibohr on the side the field pulls the density towards and in by the same amount on the far side — 2.84 per cent of its own radius. What the sphere encloses does not change to first order; only where the surface is does.

The surface a neighbour moves

An ion in a crystal sits in the field of the ion next to it, and that field moves its contour. The displacement has a closed form, it is checked against the polarisability it implies, and it turns out to be almost perfectly anti-correlated with the discrepancy it was proposed to explain — the pairs that need the most correction get the least.

orbitals · Contour
The shared bond's response falls and reverses, at every coupling. How far the relaxation moves the most interior cross bond of an acene, against the number of rings, at three couplings. Every series falls monotonically and every one changes sign — at λ = 0.2 between 3 and 4 rings, at λ = 0.4 between 3 and 4 rings, at λ = 0.6 between 4 and 5 rings. Where it crosses is a property of the coupling; that it crosses is not. The natural reading — that the effect grows with the number of rings feeding a bond — is refused by every one of these curves.

An anomaly that is not the first of a series

Naphthalene's shared bond behaves differently when the geometry is allowed to answer back, and the obvious reading is that two rings feeding one bond is what does it. Run it up the acenes and the effect falls at every step and changes sign: +0.02036 for two rings, +0.00678 for three, −0.00029 for four, −0.00603 for five. Two rings feeding a bond is not the beginning of anything.

bonding · Delocalisation
How far the rotor count would have to be wrong. The ceiling against the number of rotations a closure freezes, with the two measured accelerations drawn across it. The five-membered closure freezes three and its ceiling is 36.46; the ceiling does not reach the measured 250 until 5 rotors, so the count would have to be wrong by 2 on a ring that has three rotations to freeze. The six-membered closure freezes four at a ceiling of 120.88, and stays above its measured 10 down to 2 — so the refusal is airtight and the sufficiency is comfortable.

An estimate that can be wrong by two

The ceiling on the gem-dimethyl effect is exponential in the number of rotations a closure freezes, and that number was taken as n − 2 without counting — which left the refutation at five rings probable rather than airtight. It is airtight. The ceiling does not reach the measured 250 until five rotors, on a ring that has three, and no hindering of the tether can raise it.

shape · Strain
The two halves change places. What fraction of the counterpoise correction belongs to the lighter of two unlike atoms, against their separation. At a bonding distance it is 1.26 per cent — essentially the whole correction is the heavier atom's — and by 9.0 bohr it is 67. The two change places at 6.29 bohr. A symmetric pair's share is exactly a half everywhere, which is what makes one frozen number a complete description there and nowhere else.

A correction that is two functions

A symmetric pair's counterpoise correction splits exactly in half, at every separation, to the last digit — which is why one frozen number describes it. Give the two atoms different charges and the split runs from 0.03 per cent to 67, changing places at 6.29 bohr: the correction a single number was standing in for is two functions of different shapes.

orbitals · Basis
The same hole, priced three ways. The correlation hole of a ring of 6 at a repulsion of 8, weighted by three interactions. With an on-site interaction the answer is 100 per cent at separation zero — as an identity, since the interaction is zero everywhere else. With one that reaches a neighbour, the enhancement at separation one costs rather than pays, and gives back 44.0 per cent of the on-site saving; with a Coulomb tail, 46.9. Everything beyond one neighbour is worth under a twentieth of the on-site term.

Half of it is given back at one bond

The correlation hole of a ring removes 1.2653 pairs from zero separation and puts 1.1126 of them one site away. With an on-site repulsion that second number costs nothing, because the interaction is zero there — but with anything that reaches a neighbour it costs 44 per cent of what the hole saved, and with a Coulomb tail 46.9.

beyond · Correlation
The two rows of a table, and the curve between them. The rotamer ceiling of a closure freezing 4 rotations, against how hard each of a stated number of them is to turn. The top curve is the free-rotor row and the right-hand end of the bottom curve is the absent-rotor row; everything else is what a real hindered tether does. The measured acceleration of 10-fold is drawn across it. It falls below that line when 3 of the 4 are hindered by 4.09 kJ/mol, or when 4 of the 4 are hindered by 2.70 kJ/mol.

The curve between two rows

A rotation a ring closure has to freeze was treated as free or as absent, and the two answers sat in adjacent rows of a table. A real hindered rotor is neither. The factor one rotor contributes runs from 3.316 to one along a curve nobody had drawn, and where it matters is between one and eight kilojoules a mole — which is a torsional barrier rather than a conformational preference.

shape · Strain
The slope goes to a half, and a window fit stops short of it. The local slope of the alternation against the reduced temperature, between each neighbouring pair of points, on a ring of 40 at K = 1.6. It rises monotonically from 0.4115 to 0.5053 as the transition is approached, crossing a half at about a part in a thousand of the reduced temperature. The fitted 0.44 is the average of the left-hand end of this curve; the exponent is one half, which is what a free energy analytic in one order parameter is obliged to give.

The exponent was the window's

A fit over the last decade before a distortion vanishes gives an exponent of 0.44, and running it on larger rings should say whether the number belongs to the transition or to a forty-site ring. It belongs to neither. The local slope runs to 0.5020 as the transition is approached, and 0.44 is what a fit over that particular decade returns — on every ring size and every stiffness, because the whole curve is one curve.

wrong · Metal
Two curves that cross, and two that do not. Every pair of parameters that reproduces one measured number, for three numbers, with the true system marked at Δ = 12 and t⊥ = 0.06. The lower band's shape is a function of the ratio of the two, so its curve is a straight line through the origin; the excess gap is a function of the coupling squared over the separation, so its curve bends. The two cross at one point. The upper band's shape draws a line almost on top of the first, because it is a function of the same ratio — a second measurement lying along the first fixes nothing the first had not already fixed.

Two ways of being second order

A band's shape and a band's gap are both second order in the coupling that mixes two bands, which sounds like a reason to measure only one of them. They are second order in different ways — one goes as the square of the ratio and the other as the square over the separation — and that single difference of one power is what turns a curve of possible answers into a point.

solids · Bands in a solid
A state in the gap is a particle in a box the alloy happened to make. The participation ratio of the 40 levels nearest the gap centre, over 5 chains of 400 sites, against the length of the run of like sites each one sits on. The line is 2(L+1)/3, the participation ratio of the ground state of an isolated chain of L sites, with nothing fitted. 38 of 40 lie on it to within 3.1 per cent. The ones above it are states shared between two runs close enough to talk, which is a defect band beginning.

A particle in a box the alloy made

A random alloy's gap is set by the longest run of like sites. What sits at the edge of that gap turns out to be the simplest state in quantum mechanics: a particle in a box of L sites, occupying 2(L+1)/3 of them, to within three per cent and with nothing fitted — except for the two states in forty that found a second run to share.

solids · Defect
A length that keeps growing, and one that stops. The fitted decay length of the ring-current response, against the number of rings. The bare acene's runs 1.397, 1.669, 1.896, 2.104, 2.302 — up by a factor of 1.65 and still climbing — while its own gap falls from 0.590 to 0.1102. With a gap held open the same measurement gives 0.678, 0.642, 0.636, 0.636, 0.639, which has stopped moving by the third molecule. There is a magnetic reach, and an acene is too nearly gapless to have one.

A reach that has no length

A ring current's response to a neighbouring ring falls with distance, which invites asking for the length. Every acene computed gives a longer one — 1.397, 1.669, 1.896, 2.104, 2.302 rings — because the gap that would set the length is closing at the same time. Give the same molecule a gap that stays open and the number settles at 0.636 by the third one and does not move.

symmetry · Aromaticity
A functional with no interior maximum. The Boys functional against the mixing angle for a carbonyl, evaluated directly at a hundred and eighty-one angles. It is a quadratic in cos²θ − ½ with no linear term, so it is symmetric about forty-five degrees and its maximum is at the middle or at the ends and nowhere else. Here the coefficient is positive, so the best is at 0° — the canonical σ and π. There is no angle to search for, however unsymmetrical the molecule is.

The angle that does not have to be searched for

A carbonyl's two bent components have no symmetry making them equivalent, so the mixing that best localises them looks like something to search for and their s characters look like two different numbers. Neither happens. The localisation functional is a quadratic with no linear term, so its maximum is at forty-five degrees or at the ends — bent bonds or canonical ones, decided by one inequality, with nothing in between.

bonding · Hybrids
The four things a susceptibility curve measures, in order. The four directions in the parameter space, best fixed first, each written as the product of powers it is. The Jacobian is logarithmic, so a direction is a set of exponents and a combination is a product — which is why the answer can be printed. The best-determined is g · J^-0.33, fixed to 0.08 per cent by a curve measured to one per cent; the worst is tip · rho^-0.40, fixed to 40. Neither is one parameter's own axis.

The product a curve measures

A susceptibility curve's fourth parameter is undetermined, and the question is which combination the free direction actually is. It is a product of powers, because the Jacobian is logarithmic — and at the usual window it is the temperature-independent term divided by the 0.40 power of the monomer fraction, fixed to forty per cent, while the product one place up is fixed to 6.7. A paper could print that instead of four numbers.

applied · Magnetism
A fourth data point, and 3 negative electronegativities. Each element's electronegativity from three points on its energy curve, the cubic coefficient a fourth point adds, and what the fourth point leaves. The cubic coefficient is one sixth of a second difference of the ionisation series, so it is largest where that series has a kink — and the alkali metals, whose second electron comes out of a closed shell, are pushed to Li -7.91, Na -3.42, K -1.49 eV. The last column is where the two roots of the fixed-point equation collide, beyond which the atom has no solution at all.

Where a closed form stops being one

What happens when the quadratic energy is not enough? A cubic makes the equalisation condition a quadratic with two roots, and something has to choose between them. The choice is easy and the finding is somewhere else — a cubic fitted through the dication gives lithium an electronegativity of −7.907 eV, a capacity of 0.073 of an electron, and a molecule of two alkali metals no solution at all.

wrong · Electronegativity
Two lengths off the same chains, and only one of them has an exponent. The length an end's influence reaches into a chain of 320, against the gap the bulk has opened, over ten elastic constants and a factor of twenty in the gap. Fitted over the first twelve bonds — as a short-window fit does — the exponent is -0.476. Taken from the local decay rate extrapolated to a bond infinitely far from the end, it is -1.029, and every neighbouring pair of points gives between -1.06 and -0.91. The argument says −1. The two lines are the same ten profiles read two ways.

A decay that keeps slowing down

A healing length fitted over the first twelve bonds of each relaxed chain goes as the gap to the power −0.60, against an argument that says −1. A fitted exponent can belong to its window, and this one does — but not because the window is too short for the chain. The profile is not an exponential at all, so there is no single length for an exponent to be of.

solids · Peierls distortion
One expression, four molecules, a factor of eleven. The computed zero-point correction to each molecule's moment of inertia against the expression A²·Σ(1/ν)/I, which has no fitted quantity in it. The dashed line is the mean dimensionless coefficient, 0.6343; the four points lie within 18 per cent of it, on corrections that span a factor of 11.4. The expression is evaluated from a moment of inertia and a list of wavenumbers, which is what a spectroscopist has before doing anything.

An expression for what was a warning

The zero-point correction to a moment of inertia comes out at 1.88 per cent where a few tenths had been assumed, and heavy molecules are safer. Written out, the correction is a mean curvature times the sum of reciprocal wavenumbers over the moment — one line, evaluated from things a spectroscopist has before starting. One coefficient serves four molecules whose corrections span a factor of eleven.

spectra · Rotation
The two sides of a verdict, with error bars. The computed ceiling for the six-membered closure — 10.9945 — with the band a gauche energy of 3.8 ± 0.4 kJ/mol puts on it, against the measured tenfold rate ratio with an assumed 20 per cent uncertainty. The two bands overlap over most of their length, and the nine per cent margin the verdict was decided by sits inside both of them.

A verdict inside its own error bar

The tightest comparison in the rotamer argument is a computed 10.99 against a measured 10 — a nine per cent margin, offered as a verdict. The computed side is built on one quoted energy known to ±0.4 kJ/mol, and that alone puts a band of twenty-three per cent on it. The verdict turns on four tenths of one standard deviation of a number nobody had put an error bar on.

shape · Strain
One half is a curve and the other is not. The two halves of a counterpoise correction for an unequal pair, against separation, on a logarithmic axis. The heavier centre's falls smoothly over two decades; the lighter centre's scatters over more than one decade between neighbouring points. It is not a rough function — it is a difference of two energies of order a hartree whose difference is a millionth, and the solver does not have seven figures to spare.

The half that cannot be computed

How many points does each half of a counterpoise correction need to interpolate? The natural expectation is two different numbers. The answer is that the question is not yet askable: the lighter centre's half is a difference of two energies agreeing to six figures, its second differences are seven per cent of its own value, and no interpolation of it means anything. The third thing worth checking — the symmetric-pair check — works perfectly.

orbitals · Basis
The count is a curve, and the curve flattens. How many distinct localised descriptions of a twelve-vertex cage had been found after each batch, out of 4,000 random starts. The last new one appears at start 124; the remaining 3,876 add nothing. The dashed curve is what the basin sizes measured here predict — the chance of having hit each description at least once — and it is a closed form rather than a fit to the points.

Where the count stops being an effort

A cage's localised descriptions were counted by a search that stopped when it stopped finding new ones, which makes the count a property of the stopping rule. Run to four thousand starts the count is fourteen and the last new description appears at start 124 — after which three thousand eight hundred and seventy-six starts add nothing. The four rarest are found six times in a thousand, which is what says nothing rarer is hiding.

beyond · Multicentre
The capacity, against whether the anion exists. Each atom at its electron affinity and the capacity the cubic model gives it — the largest amount of electron the model says it can accept. A negative affinity is an anion that is not bound, which is the statement that the true capacity at the integer is zero. The three atoms with negative affinities are beryllium, magnesium and nitrogen, and they have the largest capacities in the set: two of them infinite and the third 31.5. The three smallest capacities all belong to atoms whose anions are bound.

A capacity that is largest where there is none

A cubic through four charge states implies a largest amount of electron an atom can accept, and it is natural to ask whether the idea survives its own model. It does not. The three atoms whose anions are not bound — beryllium, magnesium and nitrogen — have the largest capacities in the set, two of them infinite; the three smallest capacities all belong to atoms whose anions are bound. And among the fourteen where the test cannot bite, the ordering is sensible.

wrong · Electronegativity
The trimer's correction, and the sum of its pairs. The counterpoise correction of a three-fragment system computed directly — each fragment's energy alone less its energy in the whole trimer's basis — against the sum of the three pairwise corrections, on a logarithmic axis. The sum is the larger everywhere the difference is above the solver's noise: 30.4 per cent at 1.6 bohr and nothing by six.

The assembly that counts one share twice

A counterpoise correction is divided unequally between its two centres, and the first place that matters is a three-fragment system, where the pairwise corrections are added up and the assembly must double-count one share and undercount another. It does: the heavy centre is over-corrected by seventeen per cent and the light ones under-corrected by two and a half, and the two do not cancel.

orbitals · Basis
Where the coupling overtakes the spacing. Two quantities that both depend on the chain length, for runs of 6. The coupling is the splitting of the closest pair of runs, which rises as the chain grows because a longer chain brings some pair closer together. The spacing is the mean separation of the gap levels in energy, which falls as the chain grows because there are more of them. They cross at 8,675 sites, and a set of levels coupled more strongly than they are spaced is a band.

The length at which levels become a band

Two runs of low sites share a state when they are close enough, and the splitting falls exponentially over two sites. A longer chain brings some pair closer while spreading its levels thinner, so the two quantities run against each other and cross — at about a thousand sites for runs of four and eighty thousand for runs of eight. Chains of four hundred sites are far below that, which is why every gap state on them is a box.

solids · Defect
Two events, not one — and both below the n = 2 shell's. The field at which each coupled pair's shift stops being quadratic and starts being linear, for the n = 3 shell and for the n = 2 shell. The n = 3 shell has two, a factor of 3.66 apart, and both are far below n = 2's single one — so the linear effect returns is two events in a shell with a d, and it happens at a field thirty times weaker than in a shell without one.

Two events where there was one

A broken symmetry returns at a field where the coupling matches the gap it has to overcome, and in a shell with two levels that field is a single number. The next shell up has three, two gaps and two dipoles — so there are two crossovers, a factor of 3.66 apart, both of them below the single one of the shell below, and the exponent takes more than a decade of field to travel between them.

symmetry · Representation
The contrast, out to a repulsion of sixteen thousand. The ratio of the weakest fundamental to the strongest satellite, against the on-site repulsion, for eight systems with two electrons each. Both axes logarithmic. The dashed line at two is the factor the intensity test needs. Every curve flattens above it and none of them crosses, at any repulsion — including a repulsion sixteen thousand times the hopping.

A contrast with a closed form

Below half filling the satellite test flattens instead of failing, and the value it flattens at could be above or below the factor of two the test needs. It is — on all eight systems, by between 1.25 and 3.7 times. And on a ring the limit is (1 + 2cos(π/n))², to six figures, on every ring tried.

spectra · Photoelectron
6 rings fused two ways. Two catacondensed chains of 6 hexagons: the linear one, where every fusion continues the line, and the angular one, where the fusions alternate. They have the same formula and the same number of bonds and they are not the same graph. Ring centres are numbered; in the linear molecule two rings k steps apart have centres 1.7321k units apart and in the angular one they do not, which is the whole reason this pair can be asked the question.

Neither of the two separations

A linear acene cannot pose the question, because the number of fusions between two rings and the distance between their centres are the same variable there. Bending the molecule pulls them apart — and the response follows neither. Two pairs of rings the same distance apart differ by two thirds, and the larger one is at the greater distance.

symmetry · Aromaticity
The measurement is not a horizontal line. The rotamer ceiling against temperature, with the measured tenfold drawn four ways: flat, and as a rate ratio whose two activation energies differ by 3, 5.31 and 8 kJ/mol. Flat, it is crossed at 312.1 K, which is the flat-rotor answer. At 5.31 kJ/mol the two curves are parallel and never meet. At 8 they meet on the other side, and it is cooling rather than heating that refutes the account.

One number decides which way it breaks

The six-membered verdict gives way at 312.1 K, and that is a statement about the ceiling rather than a prediction about the ratio — because a real rate ratio has a temperature dependence the model has no term for. Putting that term in moves the crossing, and at 5.308 kJ/mol it removes it entirely.

shape · Strain
Two bands, square below, triangular above. The 128 levels of a structure carrying two orbitals on every one of its 64 sites, where the lower orbitals hop on a square net and the upper ones on a triangular net, separated by 12 and coupled at 0.06. The two bands have different widths and different shapes before anything mixes, which is the situation a single net cannot construct. Every level here is also reproduced by a two-by-two problem, one per mode, to 3e-13.

The constant that belonged to one net

Divide one second-order departure by another and the coupling cancels, leaving one constant times the gap — which reads as arithmetic. It was arithmetic about a square net. On a triangular one — the same graph for both bands, nothing else changed — the quotient drifts by a hundred and twenty-eight per cent.

solids · Bands in a solid
The sixteen-electron gap, from a plane to a tetrahedron. The gap above eight d electrons as four ligands are folded out of a square plane towards a tetrahedron, at three π strengths. It is 2eσ exactly at the plane whatever the π strength is, and exactly zero at the tetrahedron whatever it is — the upper three levels there are the degenerate t₂ set. In between the three curves separate, and the separation is what the π channel is doing.

The gap that only a tetrahedron closes

The sixteen-electron gap is 2eσ exactly, and a square-planar π set cannot touch it because d(z²) has no partner there. Fold the ligands out of the plane and the gap survives almost intact for fifteen degrees, closes to nothing only at the tetrahedron — and loses its exactness at the very first degree.

applied · Electron count
Four ways of predicting the same six separations. How far each model's predicted separation is from the measured one, pair by pair. The best additive model misses by 0.0098 ångström on average, the tabulated radii by 0.0237, radii read off the ions' own densities by 0.1828, and the balance of a Madelung attraction against a computed repulsion by 0.2421.

The residue that is two numbers

Is a shortfall between a sum of radii and a measured separation a property of the pairs, or of the compromise a universal table makes? The eight separations are two complete two-by-two blocks, so what no assignment of radii can reproduce is not a residual at all — it is an alternating sum, computed by subtraction, and it comes to three hundredths of an ångström and six.

orbitals · Contour
Three basin populations from one search. The share of 4000 random starts landing on each localised description, in rank order, on a logarithmic axis, for three cages and fillings. a twelve-vertex cage at twelve electrons gives 14 descriptions and two groups with a gap; a nine-vertex cage at eight electrons gives 63 descriptions and a smooth tail; a twelve-vertex cage at twenty electrons gives 15 descriptions and one basin and dust. Only the first is the twelve-vertex shape, and the rule it suggests is a rule about that shape.

Three shapes from one search

A cage's fourteen localised descriptions fell into two groups with a factor of five between them and nothing in the gap, which made counting the big basins look like a stopping rule. Two more cases from the same family give a smooth tail over sixty-three descriptions and a single basin holding ninety-eight per cent. One search, one family, three shapes.

beyond · Multicentre
The repulsion against the count, and they do not sort together. Every arrangement of the census by how many ligand σ combinations are left without a central partner and by how far its ligand repulsion sits above the best arrangement of that many points. The three that break the formula are marked. They are not the expensive ones: they sit at 4.2, 6.3, 9.8 per cent while the arrangements the formula gets right run to 26.5.

Expensive is not the same as unadopted

A counting formula right for twenty-three arrangements and wrong for three invites a reading: the failures are the arrangements nothing adopts, so the formula is reliable because chemistry stays away from where it breaks. Put the repulsion energy on the same axis and the reading fails — the most expensive arrangement in the census is one the formula gets right.

beyond · Hypervalency
The alternation a spring buys, three ways. The alternation against the elastic constant, on a logarithmic axis. The middle line solves (2/π)(K − E)/(1 − δ²) = K for the complete elliptic integrals; the lower one is the exponential form every account of a Peierls distortion quotes, which is its own asymptote and is 6.5 per cent low at K = 1.2; the upper one is a ring of 40, which leaves the infinite chain as the spring stiffens because a smaller alternation is a longer coherence length.

The amplitude the collapse left behind

Five Peierls curves became one curve when each was divided by the alternation its ring settles at cold, so that amplitude is the whole of what distinguished them — and it was five golden-section searches over diagonalisations with no formula anywhere. It has one, exactly, as a sum of square roots; and writing it down says that one of the five rings was never measuring a long chain.

wrong · Metal
The coefficient each principal axis needs. The dimensionless coefficient the molecule-averaged expression requires, evaluated on each principal axis separately rather than on the mean of the three. Across the twelve axes the positive ones span a factor of 2.33, against the 1.36 the molecule-averaged version spans — and one of them is negative, which no positive constant can be.

The axis that goes the other way

One dimensionless coefficient turned a zero-point correction into an expression a spectroscopist could evaluate, and the three principal axes were averaged over to get it. Split by axis it gets worse, not better — the coefficients span 2.3 where the molecule-averaged ones span 1.36 — and water's smallest moment does not grow at all. It shrinks.

spectra · Rotation
One heteroatom, and how far the relaxation carries it. The change every ring's bonds undergo when one carbon of the end ring is given a site energy, on a chain of 12 fused hexagons with its gap held open. The upper curve measures each molecule's couplings from its own mean bond order, which is what this collection's relaxation has always done; it stops falling at 4.48e-5 and stays there. The lower curve measures both from the same mean and keeps falling to 7.89e-9. Nothing about the molecule differs between them.

The floor was in the bookkeeping

A heteroatom in one ring of a fused chain is a perturbation with a place, and the relaxation carries it along the molecule. Measured directly, the response stops falling after five rings and sits at four hundredths of a millionth for ever. That floor is not the molecule. It is the relaxation measuring each system's couplings from its own mean, and removing it recovers nine orders of magnitude.

bonding · Delocalisation
Every crossover a shell has. The field at which each coupled pair's linear behaviour returns — the gap between the two levels divided by twice the dipole joining them — on a logarithmic axis. The n = 3 shell has 3 distinct fields rather than four, because its m = ±1 half is a two-level ladder with one coupled pair. All three are below the n = 2 shell's single one.

Three events, and a ratio of two dipoles

The m = 0 half of a shell has two crossovers because it has three levels and two coupled pairs. The other half has two levels and one, so the whole shell has three distinct fields rather than four — and two of the three share a gap exactly, which makes the ratio between them a ratio of two dipoles, 2/√3.

symmetry · Representation
The coupling at the closest pair, and at the typical one. For runs of four to eight low sites at half concentration: the splitting between two runs one site apart, which is the largest coupling any chain can produce, and the splitting at the separation two runs typically have. Both on a logarithmic axis spanning 173 decades. A band width taken from the second is not a small number; it is not a number.

A band that is a hundred and seventy decades of nothing

The chain length at which a defect's levels become a band can be located by asking when the coupling between the closest pair exceeds the level spacing. A band also has a width, and a width is set by the typical coupling rather than the closest one. For runs of eight at half concentration those two numbers differ by a hundred and seventy-three orders of magnitude.

solids · Defect
What a rotation group buys over a single angle. The Boys functional at the canonical orbitals, at the best mixing of the two bonds with the lone pair left alone, and at the maximum over the whole three-dimensional rotation group. The first step is 11.70 per cent and the second, which no two-orbital treatment can reach, is a further 2.50.

An interior maximum a third orbital allows

Two orbitals related by a mirror plane give a Boys functional with no linear term, so it has no interior maximum and no angle is ever searched for. Add the oxygen lone pair and the search over a three-dimensional rotation group finds one — eight and a half degrees of lone pair mixed into two bent bonds, worth a further two and a half per cent that no pair of orbitals could reach.

bonding · Hybrids
What a fifth ligand does to the gap above eight electrons. The gap between the fourth and fifth d levels as one axial σ donor is brought in, and as two are. It closes exactly linearly — 2eσ less one eσ for each unit of axial σ strength — and a full octahedron has none of it left. The rule of sixteen has a gap to be about only while the axial positions are empty, and how much of it survives is a number rather than a yes or no.

The ligand the rule was waiting for

A sixteen-electron complex is called reactive because it can add a ligand, and the gap that makes it sixteen points straight at where the ligand arrives. Bringing one in closes the gap exactly linearly — and leaves its exactness completely untouched, which is the opposite of what bending the same complex does.

applied · Electron count
A pair with no overlap, and a third orbital swept past it. The three levels of a trio in which the two outer orbitals have exactly no overlap with each other, as the third orbital's energy is swept. The middle line is at -13.6 at every point — the antisymmetric combination of the two, which has no partner of its own symmetry and cannot mix with anything. The other two move, so the pair is split by an orbital it has no direct contact through.

A bond order between atoms that do not interact

A diatomic held where its overlap changes sign has no interaction between its two orbitals at all — which is what the sign change of its overlap means. Put a third orbital beside it and the pair is still split, one line sits exactly at the free-atom energy at every third-orbital energy, and the bond order between the two runs to −0.9999. Three measures of the same bond disagree completely.

wrong · Overlap
Seven nets, and the one column that sorts them. Every wrapped net here, with its dimension, coordination, third moment and band shape, beside the exponent the coupled-band measurement returns for it. The 4 nets whose third moment vanishes all give an exponent within 0.03 of −2 and a quotient constant to a fiftieth of a per cent; the 3 that do not all give one near −1 and no constant at all. Dimension does not sort them and neither does coordination — each takes values in both groups.

Seven points that looked like a switch

A constant belongs to a square net and not to a triangular one, which points at the coupling graph. Seven wrapped nets say which property of it: the third moment, and neither the dimension nor the coordination. They also say it is a switch — and made continuous, it is a crossover that every one of the seven sits twenty-five times past.

solids · Bands in a solid
The residue is four times below the model's own error. The quantity whose sign is wanted, beside the accuracy of the numbers it is a difference of. The measured residues are 0.031 and 0.056 ångström; the model gets a single separation right to 0.242 on average. A fourfold alternating difference of quantities known that badly cannot resolve something that small, and that arithmetic was available before any of this was computed.

The residue is below its own noise

Two interaction terms, both negative, leave the sign a coin toss — and a larger block would settle it. There is a larger block: a model that needs no measured separations supplies twenty-one. It cannot settle anything, because a fourfold alternating difference of distances known to a quarter of an ångström cannot resolve three hundredths of one.

orbitals · Contour
One geometry, four electron counts, four answers. The bond order between two orbitals with exactly no overlap and no resonance integral, as the third orbital's energy is swept, at every count the trio can hold. With none it is identically zero. With two it is positive and rises past one. With four it is negative and reaches -0.954. With six it is a horizontal line — the third orbital's energy stops mattering entirely.

A filled shell is not an empty statement

A bond order of −0.954 between two orbitals with no overlap and no resonance integral invites the prediction that at six electrons — every level occupied, the sum over a complete set — it would be exactly zero. It is exactly one seventh, and the reason is that a complete set in a non-orthogonal basis sums to the inverse of the overlap matrix, which has entries where the overlap has none.

wrong · Overlap
Nine combinations, and the column that sorts them is not the bands'. Two bands and a coupling, varied separately. The composite graph's third moment splits into triangles that lie inside a band and triangles that use two coupling bonds, and only the second sorts the table: every row with no gap-crossing triangle gives an exponent near −2 and a nearly constant quotient, whatever its bands are made of. Triangular bands carrying an intra-band moment of 7.296 behave exactly like square ones when the coupling is a matching.

The triangles that were never in the bands

A switch in how a gap scales is usually attributed to a band's third moment, and the attribution cannot be tested while the coupling runs along one of the bands. Separated, the bands turn out to decide nothing. Two triangular bands coupled along a matching — which cannot close a triangle across the gap — behave exactly like square ones.

solids · Bands in a solid
The count, for five run lengths. The fraction of runs whose nearest neighbour of the same length is coupled more strongly than a threshold, against how many decades below the closest possible coupling that threshold sits. Every curve is a straight line over this range, because the fraction is small and the geometric tail is linear in the separation there. The slope is what the next figure is about: it is the whole content of the distribution, and it is a product of two numbers.

A count rather than an average

Two couplings quoted from one distribution sit a hundred and seventy decades apart. Neither is a summary of it. The quantity that decides how much of a spectrum near a box level is resonant pairs is a count of pairs above a threshold — and it has a closed form, which is a density times a reach times the logarithm of ten.

solids · Defect
The criterion is the reciprocal of the p amplitude. The two lone pairs' mixing criterion — twice the dipole between them over the separation of their centroids — against the p fraction of the outward hybrid. The curve is 1/√(p fraction), written down rather than fitted; the marks are the numerical integrals. They agree to 15 parts in a million at every hybrid, and the criterion never falls to one, so the mixed description wins at every s character there is.

The five figures were an identity

Two lone pairs satisfy the two-orbital mixing criterion by a margin of 1.732128, against √3 = 1.732051 — agreement to five figures on a number assembled from three integrals over a numerical grid. It is exact. The criterion is the reciprocal of the p amplitude of the outward hybrid, and everything else in the molecule cancels out of it.

bonding · Hybrids
What happens to the level that was exact. The three levels of the trio as one of the two outer orbitals is raised. At zero detuning the middle one sits at -13.6 exactly — it is the antisymmetric combination, and nothing of its symmetry exists for it to mix with. The moment the two are made inequivalent that statement is gone: the level leaves linearly, and the other two barely move by comparison.

A symmetry holds or it does not

One level of a three-orbital trio sits at the free-atom energy exactly, at every third-orbital energy, because the antisymmetric combination of the pair has nothing of its own symmetry to mix with. Detuning one of the two by a twentieth of an electron volt moves it by half of that — first order, immediately, with no protected regime at all.

wrong · Overlap
The bracket has no upper end. Every price is multiplied by √2 over √(1 + r² − 2ρr), where ρ is the correlation between the two measurements' errors and r is the ratio of their sizes. For equal precision the factor is 1/√(1 − ρ), which is one at independence and unbounded at perfect correlation. The other extreme the question asked for is not a number.

The other end of the bracket is not a number

Every claim can be priced by the measurement error it would take to overturn it, assuming the two errors independent, and the correlated extreme ought to turn each price into a bracket. At perfect correlation between equally precise measurements the difference is exact and the price is infinite — and every price is multiplied by the same factor, so the ordering of prices cannot change.

bonding · Models
The input the question named is the worst of the six. For each candidate input, the largest capacity ratio between two atoms that are neighbours in that input. A quantity the capacity were a function of would have a small bar. The dashed line is the floor — neighbours in the capacity itself still differ by ×5.0, because fourteen atoms spread over a factor of four hundred cannot do better. The second ionisation energy is ×193, which is 39 times that floor.

The worst of the six was the one we asked about

The capacity's correlation with the second ionisation energy explains 2.9 per cent, and the natural next step is the same pair test against every other candidate input. Every input fails it — but the second ionisation energy fails it by a factor of twenty-four more than the best, and the test itself had to be repaired first, because the version the question implied reports the capacity failing to be a function of itself.

wrong · Electronegativity
Adding one measurement, and six of fifteen change verdict. Each atom's chemical capacity from a cubic fitted through four electron counts and from a quartic fitted through five, on a logarithmic axis, with an unbounded capacity drawn at the right-hand margin. Five atoms go from a finite capacity to an unbounded one and one goes the other way — and the five are exactly the five largest the cubic reported. The seven that stay finite keep their order and change their values.

Six of fifteen change verdict

The chemical capacity is finite or infinite according to the sign of a coefficient that is one sixth of a second difference of three measurements, and the pair test asked how much of its reported ordering is the quantity and how much is the fit's resolution. Adding a fifth point changes the verdict on six of fifteen atoms — and the five it unbounds are the five it had largest.

wrong · Electronegativity
A fixed offset against a rising threshold. The offset at which a shell's coupled minimum disappears, against the principal quantum number, with the offset every shell's own d level actually has. The threshold is 2(n² − 4)/(5(n² − 1)) — zero at the second shell, a quarter at the third, and rising to two fifths. The shell's own offset is one fifth whatever the shell, because it comes from the reciprocal of l plus a half and carries no n at all. So the comparison is a constant against a curve, and it changes answer exactly once.

The quarter, generalised

A shell's one coupled minimum exists because its d level sits within a quarter of the s–p gap, and the quarter was found by bisecting a numerical search on one shell. It is exactly 2(n² − 4)/(5(n² − 1)) for every shell — zero at the second, a quarter at the third, two fifths in the limit — while the offset it is compared against is one fifth whatever the shell.

symmetry · Representation
The ranking is fragile and the headline is not. The correlation required to disturb two different things. Reordering the easiest neighbouring pair needs ρ = 0.154, which is weak enough to expect. Displacing the collection's most fragile claim outright needs ρ = 0.954, which is near-perfect correlation. So a per-predictor structure scrambles the middle of the ordering and leaves the top of it alone.

The ranking moved and the headline did not

One correlation applied across a collection multiplies every price by the same number, so it slides the fragility ordering rigidly and cannot scramble it. Give each predictor its own correlation and the ordering does move — but not at the top. The two most fragile claims come from the same predictor, share a factor, and are locked in order at every correlation whatever; the easiest swap anywhere below them needs only ρ = 0.15.

bonding · Models
The resonant share is not a straight line; it bends over and saturates. The share of runs of six in a resonant pair against the logarithm of the chain length, from a thousand sites to 10⁵⁰, at five concentrations of low sites. Dashed lines carry the slope from 10³ to 10¹² straight on. At x = 0.5 the share is 16.1 per cent at 10¹² and 57.7 per cent at 10⁵⁰, where the straight line would be at 78.6. At x = 0.75, the concentration with the most runs of six, it passes 76 per cent by 10³⁰.

The share that was read as a line

The share of defect runs sitting in a resonant pair was read as a straight line in the logarithm of the chain length, rising by a density times a reach per decade and never saturating. The exact rise is that amount times the share of runs not yet resonant. At the concentration first studied the difference is small over nine decades and large beyond them; swept to the concentration with the most runs, the rise falls to a third, and half of all runs are resonant ten orders of magnitude later than the straight line says.

solids · Defect
Two sweeps, and one of them covers 28 per cent less ground than the other. What each of the two sweeps reaches, measured in the one variable the rotamer ceiling has: g/RT. The temperature sweep lies entirely inside the gauche sweep, so it explored no arrangement the other does not. Their widths are 0.581 and 0.807, their union is 0.807, and treating them as independent would have credited them with 1.387.

Two sweeps and one lever

The rotamer ceiling depends on the gauche energy and on the temperature only through their ratio, so a sweep of either traces the same curve. Measured in that one variable, the temperature sweep lies entirely inside the gauche sweep — it covered no ground the other does not, and the whole reported spread in one energy is worth a temperature swing from 196 to 353 kelvin.

shape · Strain
The same count in both pictures, and no rule between them. Every hydrogenic orbital with a radial node, drawn twice: its position nodes on the left axis and its momentum nodes on the right, at the same nuclear charge. The counts are identical and exact — n − l − 1 in each — because the two radial functions are polynomials of the same degree. The positions are unrelated: a node three quarters of the way out in one picture is not three quarters of the way out, or anywhere in particular, in the other.

The nodes in the other variable

An orbital has n − l − 1 radial nodes, and it has exactly that many in momentum too — the two radial functions are polynomials of the same degree. Nothing pairs one node with another: they are zeros of two different classical families. What is exact is the product over all of them, which is a ratio of factorials and does not depend on the nuclear charge at all.

orbitals · Orbital
A bond is a cosine in momentum space. The two factors a two-centre bonding orbital's momentum density is made of. One is the atomic momentum density, unchanged by the bond and falling as the eighth power of the momentum. The other is cos²(q·R/2), the interference between the two centres, whose period is fixed by the bond length and by nothing else. Everything that distinguishes a bond from two atoms in this picture is that cosine — and it has zeros where the atomic factor has none.

Oblate in the picture nobody draws

Every drawing of a σ bond shows a density stretched along the bond, and the position-space calculation agrees: the second moment along the axis is twice the one across it. In momentum the same orbital is flattened in the same direction, because the interference between the two centres cuts the distribution off at π over the bond length — and that cut-off is a zero a measurement could find.

orbitals · Orbital
The covariant operator is BenDaniel–Duke plus this. The difference between the Laplace–Beltrami operator — the one a one-dimensional manifold with metric μ(x) distinguishes, carried across to the flat measure by the unitary map ψ ↦ μ^(¼)ψ — and the BenDaniel–Duke ordering, divided by the function it was applied to, at forty-one positions inside the molecule's own range. The curve drawn through the marks is the two-function fit every ordering is a combination of, and it passes through them to a part in ten million.

The ordering a manifold picks

A position-dependent mass leaves the kinetic energy with no unique quantum form, and an earlier sweep of the five orderings in use found half a per cent between them. A one-dimensional reduction is a one-dimensional manifold, a manifold has a distinguished Laplacian, and carrying it to the flat measure lands on exactly one of those five — not the one with no extra potential, and not the one anybody reaches for.

shape · Inversion
An antibonding occupation fills the zero and moves the minimum. The profile along the bond near π/R, per electron, on a logarithmic scale, for five antibonding occupations of the same two orbitals. With nothing in the antibonding orbital the profile is exactly zero at π/R = 1.573. Two hundredths of an electron leave a minimum at 1.608, which reads the separation as 1.954 bohr instead of 1.997. At 0.104 the minimum becomes a flat shoulder, and the Heitler–London bond, at 0.236, has none.

The zero belongs to one determinant

A bonding orbital's momentum profile along the bond is exactly zero at π/R, and that zero reads a bond length with nothing fitted. It is a property of putting every electron into that one orbital. Any antibonding occupation fills it in linearly and drags the minimum outward, a tenth of an electron erases it, and the valence-bond wavefunction built from the same two functions never has one at any separation.

orbitals · Orbital
The zero at π/R follows parity, not bonding. The bonding and antibonding combinations of three atomic functions on nitrogen, each along the bond and each normalised to its own largest value, against momentum in units of π/R. For 2s the bonding combination is zero at π/R and the antibonding one is not. For 2p along the bond it is the other way round: the σ bond carries a sine, is zero at the origin and near its largest at π/R, and the antibonding combination carries the cosine. For 2p across the bond the π bond carries the cosine again. The factor is a cosine exactly when the orbital's inversion parity matches the atomic function's.

The zero is a parity, not a bond

A hydrogen-like σ bond has a momentum profile along its axis that vanishes at π/R, and it is natural to read that zero as a bond's signature. Built from 2p functions pointing along the axis, the σ bond carries a sine instead and sits at 83 per cent of its peak there. Which factor an orbital carries is decided by whether its inversion parity matches its atom's, and bonding has nothing to do with it.

orbitals · Orbital

Named alongside it

The objects these essays reach for when they reach for this one.

Model limitConventionApproximationReference stateDegeneracyTight-binding modelsLeast-squaresEigenvalueUnderdeterminationConvergenceOne-electron modelsOverlap integral

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