Concept

Ionisation energy — where it appears

The energy needed to remove an electron from a molecule entirely. It is what a photoelectron spectrum measures, and it differs from an orbital energy by the relaxation of the ion and by the correlation neither calculation has.

Named by 28 essays across 4 fields — each of them below, with the objects they name alongside it.

methane — Td. The molecule with the point group found from its coordinates rather than looked up: every candidate operation was applied and kept when it permuted the atoms among themselves.

Hybridisation does not explain

Methane's photoelectron spectrum has two bands, not one. Four equivalent sp³ bonding orbitals cannot produce that, and the resolution is that hybridisation was never a claim about what a measurement would find.

wrong · Hybrids
4s and 3d from K to Zn. The mean radius of the 4s and 3d orbitals across the elements K to Zn, at the nuclear charge each shell actually feels. The screening is Slater's, which is fitted; the radius that follows from it is the closed form for a hydrogen-like orbital, which is not.

The aufbau order is not a property of the atom

Iron's 3d orbital is more than four times smaller than its 4s and, by every one-electron estimate available, far lower in energy. The 4s fills first anyway, and it empties first too — which is not a paradox but a sign that the filling order was never a list of orbital energies.

wrong · Approximation
methane: 2 valence bands. The measured valence photoelectron bands of methane, each labelled with the symmetry species of the orbital it comes from, and beside them the species the valence basis spans — the central atom's s and p functions and one s on each ligand, reduced in the molecule's own group. A band carrying a species the reduction does not produce would stop this figure being drawn.

What a photoelectron spectrum measures

The bands of a photoelectron spectrum are routinely read off as orbital energies. They are ionisation energies, which is a different quantity — and the identification rests on two errors of about an electronvolt each that happen to have opposite signs.

wrong · Photoelectron
water: 4 valence bands. The measured valence photoelectron bands of water, each labelled with the symmetry species of the orbital it comes from, and beside them the species the valence basis spans — the central atom's s and p functions and one s on each ligand, reduced in the molecule's own group. A band carrying a species the reduction does not produce would stop this figure being drawn.

Water's lone pairs are not a pair

Every course draws two equivalent lone pairs on water, pointing away from the hydrogens like a pair of ears. Its photoelectron spectrum shows the two bands they would produce at 12.6 and 14.7 electronvolts, two point one apart, in different symmetry species.

bonding · Photoelectron
The gap against size: uniform against δ = 0.15. The HOMO–LUMO gap of a half-filled chain plotted against the number of sites, on log axes, for a uniform chain and for one whose bonds alternate. The uniform sequence falls without limit; the alternating one settles at four times the alternation.

A band gap is not a bond energy

Silicon's gap is 1.1 electronvolts and its Si–Si bond is 2.3. Both are quoted in the same units, both describe the same material, and neither is convertible into the other — one is the cost of promoting an electron and the other is the cost of taking two atoms apart.

wrong · Bands in a solid
ammonia: 3 valence bands. The measured valence photoelectron bands of ammonia, each labelled with the symmetry species of the orbital it comes from, and beside them the species the valence basis spans — the central atom's s and p functions and one s on each ligand, reduced in the molecule's own group. A band carrying a species the reduction does not produce would stop this figure being drawn.

Fewer bands than electrons

Methane has eight valence electrons and two photoelectron bands. Ammonia has eight and three; water has eight and four. The count is not of electrons, not of bonds and not of orbitals — it is of the symmetry species the occupied orbitals fall into, and it falls as the symmetry rises.

spectra · Photoelectron
Three answers to one question. The energy to remove an electron from a half-filled four-site system, computed three ways against the repulsion: exactly, by solving a self-consistent field twice — once for the molecule and once for the ion — and by reading the highest occupied orbital energy straight off the molecule, which is Koopmans' theorem. All three agree exactly at zero repulsion. The theorem always sits above the two-calculation answer, because letting the ion relax can only lower it; the exact answer sits above both, because the molecule is more correlated than its ion. The two errors have opposite signs and do not cancel: the residue grows to 6.03.

Koopmans' theorem is exact for nothing

Reading an ionisation energy off an orbital energy neglects two things that pull in opposite directions, and the cancellation between them is quoted as the reason it works. Compute all three energies in a model where the exact answer is available and the cancellation is real, partial, and gone by the time the repulsion is twice the hopping.

wrong · Photoelectron
Two derivatives of the same energy, and only one is tabulated. The 18 elements of the electronegativity tables, placed by their chemical potential — half the sum of the ionisation energy and the electron affinity, which is the Mulliken electronegativity — against their hardness, half the difference of the same two numbers. Hardness runs from 1.92 to 7.3 electronvolts, a factor of 3.8, and does not follow the horizontal axis. Ringed points are the three elements whose anion is not bound, so whose affinity is not a measurement.

The quantity no scale prints

Every electronegativity table is half of a calculation. The other half is the hardness — half the difference of the same two measurements the Mulliken scale is half the sum of — and it varies by a factor of 3.8 across eighteen elements. Put both halves in and B–F, with an electronegativity difference of 6.12 electronvolts, moves less charge than lithium iodide, whose difference is 3.75.

bonding · Electronegativity
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
Three lines, then a hundred. The exact removal spectrum of a 6-site Hubbard ring at half filling: every final state of the ion, at the energy it costs to reach and with the intensity the matrix element gives it. With no repulsion there are 3 lines and they are the occupied orbital energies. At U = 8 there are 100, on a molecule with 6 orbitals — so the spectrum cannot be read as a list of orbital energies, because there are more bands in it than there are orbitals to name.

More bands than there are orbitals

A photoelectron spectrum is read as a list of orbital energies, one band per occupied orbital. Computed exactly for a six-orbital ring, it has three bands with no repulsion and a hundred with eight — and by then fifty-three per cent of the intensity is in lines that no orbital corresponds to. The total intensity is three at every repulsion, exactly, because that is a sum rule and not a fit.

spectra · Photoelectron
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 test that works until it does not. How many times stronger the weakest fundamental is than the strongest satellite, against the repulsion, on a half-filled ring of six. It starts at 23.8 and falls to 1.15 — a spectrum whose tallest satellite is as tall as its shortest band. The marked repulsion is where the other test fails as well: satellites start appearing inside the range the fundamentals span, so neither height nor position sorts the spectrum.

A hundred lines and no way to sort them

A spectrum with a hundred lines has six fundamentals in it somewhere. Sorting by height works until the tallest satellite is as tall as the shortest band, and sorting by position works until satellites start arriving between the bands — and on a ring of six both stop working at the same repulsion.

spectra · Photoelectron
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
Two molecules, one eigenvalue, and 1.27 eV between them. Six alternant hydrocarbons placed by the Hückel eigenvalue of their highest occupied level — computed by diagonalising each molecule's own adjacency matrix — against the measured first π ionisation energy. Ethene and benzene share an eigenvalue of exactly 1 and their measurements differ by 1.27 eV; butadiene and naphthalene share 0.618 and differ by 0.94. A model that reads only the eigenvalue is a function of it, so it must give each pair one answer, and the two vertical pairs are the whole of its error.

A parameter that never finds a value

Show a two-parameter model six measurements instead of two and it stops being underdetermined and starts being wrong. Adding the third parameter improves the fit by one part in eighty, moves the resonance integral by a factor of four, and never finds a best value at all — because nine tenths of the error is a term the model does not have.

bonding · Models
The boundary belongs to the gap, not to the repulsion. The repulsion at which a satellite stops being tellable from a fundamental by intensity, against the system's own one-electron gap. Four systems: ring of 6, gap 2.000, boundary 8; chain of 4, gap 1.236, boundary 4; chain of 6, gap 0.890, boundary 2; ring of 4, gap 0.000, boundary 0.25. The three with a gap order exactly with it, and the ring of four — whose half-filled ground state is degenerate and whose gap is zero — has no boundary at all: its contrast is one at every repulsion, so its satellites are never distinguishable and there is nothing for a boundary to separate.

The boundary belongs to the gap

A satellite stops being tellable from a fundamental somewhere, and it can be located on one ring at one filling. Four systems put it at repulsions of 2, 4 and 8 — ordering exactly with each one's own one-electron gap and not with its band width — and the fourth, whose gap is zero, has no boundary at all: its satellites are indistinguishable at every repulsion including none.

spectra · Photoelectron
What each of these predictors cannot see. Four predictors built elsewhere in this collection, each audited by its ties: the share of the variation in what was measured that the predictor demonstrably cannot account for, because two systems it assigns the same number to were measured to differ by that much. the spin-only moment leaves 23 per cent; the VSEPR angle leaves 92 per cent; the highest occupied Hückel eigenvalue leaves 41 per cent. The control has no ties at all and the instrument returns nothing for it, which is what it must do. No fitting anywhere: a tie is a claim a model of that form cannot escape.

Two systems a model cannot tell apart

Two molecules that share a Hückel eigenvalue but were measured to differ bound a whole family of models at 0.456 eV. That is a reusable instrument, and chemistry has plenty of predictors of exactly the same shape. Turned on themselves: VSEPR cannot account for 92 per cent of the variation in the four angles it predicts, and no fitting is involved anywhere.

bonding · Models
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 instruments, and they do not agree. Each of this collection's four predictors under both tests. The exact-tie instrument reports the share of the variation a predictor demonstrably cannot account for, and it ranks VSEPR worst and has nothing at all to say about the ring-strain control. The near-tie instrument reports how much steeper any model must be somewhere than the set is overall, and it ranks the control worst and cannot speak about VSEPR, whose predictor is a label rather than a number. Neither instrument is the general one, and a predictor that passes one has not been audited.

The pair that is not a tie

An exact tie bounds every model of a form with no fitting, and it is available only for predictors that read integers. A near tie bounds the model's derivative instead, and a pair the predictor orders the wrong way round refuses monotonicity outright. Run on four standard predictors, the new instrument ranks them in a different order from the old one — and its worst case is the control the old one could not see.

bonding · Models
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
What the gap alone would predict, and what was fitted. Each halide's π scale as a multiple of fluoride's: the value fitted to the spectrochemical series, against what the energy denominator alone gives with the metal orbital at the vacuum level — which is the weakest the denominator effect can be. It over-predicts at every ligand, and moving the metal level down makes it worse.

The gap that would have to be smaller

An angular overlap parameter is an overlap squared over an energy denominator, and the usual fit folds the denominator away. Put the measured ionisation energies back in and the denominator alone over-predicts the trend down the halide group at every metal level a donor permits — the smallest it can give is 1.67 against a fitted 1.43. So the overlap has to shrink down the group, which is the opposite of the usual expectation.

applied · Ligand field
How much stronger a fundamental is than a satellite, against the repulsion. The weakest fundamental divided by the strongest satellite, for a six-site ring and chain at every filling from a third to a half, against the on-site repulsion. Below the line at two the two kinds of line cannot be told apart by their height. The half-filled systems cross it and the third-filled ones do not — not at any repulsion up to sixty-four times the hopping, where the third-filled ring is still at 8.3.

A satellite that never loses its place

The repulsion at which a satellite stops being tellable from a fundamental orders exactly with the one-electron gap across four systems. Changing the gap by the filling instead is the sharper test, and the ordering does not survive it: a six-site chain has a larger gap at half filling and a smaller boundary. Below half filling there is no boundary at all, at any repulsion up to sixty-four times the hopping.

wrong · Photoelectron
The acceptors' π* levels, as measured. For each π acceptor: the energy at which a slow electron is temporarily captured, which is the π level above the vacuum, and the π scale this collection's series carries for it. Carbon monoxide's and dinitrogen's resonances are measured on the molecule itself; cyanide's cannot be, because an electron cannot be attached to an anion, so hydrogen cyanide's stands in for it — the same π with a proton where the metal would be.

A denominator that fails both ways

The energy gap an e_π folds away over-predicts the halide trend at every metal level a donor allows, and the acceptors look out of reach because a π* is not an atomic level. It is measurable — a slow electron is captured by it — and on that side the same denominator under-predicts. No metal level fixes either, and the two want it moved in opposite directions.

applied · Ligand field
The contrast at three fillings, and the floor two of them reach. The intensity contrast on a ring of 6 against the on-site repulsion, at three fillings. At two electrons it settles on a number well above the factor of two the test needs. At half filling it falls through two and lands on exactly one from U = 64 upward — and every point where it reads exactly one is a point where the cut between fundamental and satellite falls between two lines of identical weight. Those are drawn hollow.

A ratio of exactly one is a tie

Does the intensity contrast fall below two at half filling? It does — it falls to exactly one. But one is the floor of a ratio between two ranked quantities, and it is reached here because the cut between fundamental and satellite lands between two lines of identical weight. The guard installed to catch that case tests the wrong degeneracy, and the guard installed to license the extrapolation cannot tell an exact answer from a divergent one.

spectra · Photoelectron
The capacity against the quantity it was supposed to be. The chemical capacity of 14 atoms against their second ionisation energy, with the capacity on a logarithmic axis because it spans nearly three orders of magnitude. The suspected relation is not there: N and K are 2.02 electronvolts apart in the second ionisation energy and differ by a factor of 193 in capacity, which no function of one variable can produce.

A correlation is not an account

A quantity called the chemical capacity is ordered against the thing it was supposed to predict and correlates instead with the second ionisation energy, which invites asking how much of it that accounts for — on the reasoning that a quantity which is ninety per cent of one input has a simpler name than the one it carries. It is three per cent of it. Nitrogen and potassium sit two electronvolts apart in the second ionisation energy and differ two hundredfold in capacity.

wrong · Electronegativity
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
Two interactions, and they push the metal in opposite directions. Each ligand's filled π and empty π against a metal d level, on one energy scale with the vacuum at zero. The π lies below the metal and pushes it up, which is the only interaction the model's derivation has; the π lies above and pushes it down, which is the one it lacks. Both level positions are measured — an ionisation energy and an attachment energy — and the metal's is the single quantity nothing here measures, drawn at -8.0 electronvolts and swept elsewhere.

The channel that points at the metal

Two ligands in the spectrochemical series carry a fitted π parameter no quotient of squared overlaps can produce, because it is negative. Giving the derivation the second interaction it lacks makes both of them negative at every metal level — and the reason is not the energy denominators, which favour the donor channel in all three cases. It is where each orbital keeps its amplitude.

applied · Ligand field
Straight segments, and the curve fitted through their ends. Cl's energy against the charge it carries. The exact theory says the energy is straight between integers, with a kink at each one: the slope below the neutral atom is the electron affinity and the slope above it is the first ionisation energy, and the two are different numbers. Every quantity in this argument comes from the smooth curve fitted through those points instead — and the curve's second derivative, which is the hardness, is a property the segments do not have at all.

Four quantities go and one question stays

The exact theory says an atom's energy against electron count is straight segments between integers, and that model gets the alkali metals right for free — which is exactly where the fitted curves give lithium a negative electronegativity. What it costs is the hardness, the capacity, the electronegativity and equalisation, and what it leaves is a question whose answer is an integer.

wrong · Electronegativity

Named alongside it

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

Model limitConventionElectron affinityElectronegativityApproximationPhotoelectron spectroscopyPhotoelectron spectrumClosed formExact diagonalisationHubbard modelKoopmans theoremLeast-squares

All concepts