Concept

Expectation value — where it appears

The average a measurement would return in a given state, computed as an integral. Different powers of the same coordinate give different averages, which is why one potential produces several bond lengths.

Named by 28 essays across 9 fields — each of them below, with the objects they name alongside it.

The radial function of 1s. The radial part of the wavefunction, which changes sign at each node, and the radial distribution, which is the probability of finding the electron in a shell at that radius. The second vanishes at the nucleus and the first does not.

Where the electron is

The wavefunction is largest at the nucleus, the electron is most likely to be found a bohr out, and the ninety-per-cent contour is at 2.66. Three numbers, all correct, all answering different questions.

orbitals · Orbital
Four measures of size for 6 orbitals. The most probable radius, the mean radius, the root-mean-square radius and the radius of the sphere holding ninety per cent of the density, for 1s, 2s, 2pz, 3s, 3dz2, 4s. All four are computed from the same radial function, all four are correct, and they are not the same number.

How big is an orbital

Four measures of size, all computed from the same radial function, all correct, and spanning a factor of two and a half for a 1s orbital. The one that governs chemistry is a fifth, and it is not a measure of size at all.

orbitals · Contour
The exponent the molecule chooses, and what it buys. The 1s exponent that minimises the energy of a one-electron diatomic, against the separation of the nuclei, with the binding curves at that exponent and at the free atom's. Held at ζ = 1 the bond comes out at 2.49 bohr and binds 0.0648 hartree; with the exponent free it comes out at 2.00 bohr at ζ = 1.238 and binds 0.0865. The exact answer for this molecule is 2.00 bohr and 0.1026.

The atom does not bring its own orbital

Build a one-electron diatomic from two hydrogen 1s functions and it comes out 25 per cent too long and 37 per cent too weakly bound. Let the molecule choose how large those functions are and the bond length is right to three figures, at an exponent of 1.238 — the orbital contracts by a quarter when the bond forms.

orbitals · Orbital
What the angular momentum operator connects. The five real d functions, with a line between each pair the z component of orbital angular momentum connects and the size of the connection on it. Written in this basis the operator is i times an antisymmetric matrix, so its expectation in any real function is exactly zero — that is the quenching, and it holds before any field is applied. The three t₂g functions are connected among themselves, so as a SET they carry eigenvalues 1, 0, -1; the two eg functions are each connected only to something outside the pair, so as a set they carry nothing.

An orbital carries no angular momentum

The d orbitals every chemist draws carry exactly no orbital angular momentum, and the proof is one line about a matrix being antisymmetric. A set of three of them carries a whole unit, which is why the spin-only formula works for most ions and fails for cobalt by nearly a Bohr magneton.

applied · Magnetism
The energy is the last thing a wrong wavefunction gets wrong. Two errors against the error in the wavefunction, on log axes, for a chain of 2 at U = 4t. The energy's line has slope 2.00 and the double occupancy's has slope 1.01: the first is second order in the error and the second is first order. So the two lines diverge as the wavefunction improves, and the energy stops being evidence about anything else long before it stops improving.

A better energy is not a better answer

The variational principle makes the energy a one-way test: lower is closer. It also makes the energy the least sensitive thing a wavefunction gets wrong — second order in the error where every other property is first — so the two diverge without limit as a calculation improves.

wrong · Approximation
Where the electron is, and how fast it is going. The radial distribution in position on the left and in momentum on the right, for the same orbitals. The two run opposite ways: the 1s is the most compact in space and the widest in momentum, and every excited orbital that spreads out in one narrows in the other. Both are normalised, both are the same function, and neither is more fundamental than the other — the transform loses nothing and adds nothing.

The orbital in momentum space

Every orbital has a second picture as complete as the first and almost never drawn. Nothing is added by taking it — it is the same function in the other variable — but the uncertainty product falls out of it, and the functions quantum chemistry is built from turn out to be the only ones that attain the bound.

orbitals · Orbital
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
H³⁵Cl: the well, its states and their averages. The Morse potential built from H³⁵Cl's measured vibrational constants, with the lowest four states drawn at their computed energies and the average separation of each marked. Every average lies to the right of the minimum, because the well is not symmetric — and they move outward as the state rises.

The bond length that depends on the isotope

Hydrogen chloride and deuterium chloride have the same potential energy curve, and their measured equilibrium lengths agree to three hundredths of a milliångström. Their average bond lengths differ by 4.34 mÅ — a hundred times more — because a lighter atom explores more of a well that is not symmetric.

wrong · Approximation
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
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
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 bonds, or one a₁ and three t₂. The same four occupied orbitals written in two bases. On the left each orbital sits on one bond; on the right one is shared over all four hydrogens and three follow the Cartesian directions. The transformation between them is orthogonal, so the density is unchanged.

The answer a search is most likely to give

If a cage has ten equally good localised descriptions, why does the literature agree about its picture? The hoped-for answer was that one basin is very large. Counting four hundred and eighty starting points says it is not: two independent searches agree one time in ten, and the description they most often return is not the best one.

beyond · Multicentre
A ratio that measures a distortion, and squares it first. How far ammonia's depolarised bands come off three quarters against how far one of its bonds has been stretched. Undistorted the departure is 3.1e-8, which is the rounding in the stored coordinates rather than a physical effect; at 0.1 Å it is 0.04239, and the slope is 1.999 — the departure goes as the square of the distortion, so a ratio measured to three decimals fixes a length to one and a half.

A ratio that squares what it measures

A depolarised Raman band sits at exactly three quarters because symmetry says its mean polarisability derivative is zero. Distort the molecule and it comes off — by 4.5 × 10⁻⁴ for a hundredth of an ångström and 0.042 for a tenth, going as the square of the distortion, which makes a ratio measured to three decimals a length known to one and a half.

spectra · Spectrum
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
Where the electrons are, without subtracting anything. The opposite-spin pair distribution of a half-filled ring of 6 at six repulsions, by separation, each divided by what uncorrelated electrons of the same density would give. At no repulsion it is one everywhere; at a repulsion of 16 the chance of finding two electrons on one site is 0.0430 of that, and what is missing has turned up next door. Nothing here is a difference between two calculations.

Where the electrons are, without subtracting anything

A correlation energy is an exact energy less a mean-field one, so the answer depends on which mean field was picked — by a factor of 259. The pair distribution says the same thing with no subtraction in it, and two systems matched to the same correlation energy turn out to have electrons in visibly different places.

beyond · Correlation
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
How much of a curve each extra parameter has left to work with. The singular values of the design matrix for a susceptibility curve, for two, three and four parameters fitted to the same data, on a logarithmic scale. With four they run 12.411, 2.026, 0.149, 0.025 — a span of 500 — so one per cent data fix the first two to under 3 per cent and the last to 37. Each value is what is left of the measurement after the directions above it have taken their share, so a short bar is not a hard parameter but an absent one.

How many parameters a curve is worth

A susceptibility curve routinely carries four fitted parameters and the question of whether it can support them is never asked. It has an arithmetic answer: the four directions the fit sees span a factor of five hundred, so one per cent data fix the first two to under three per cent and the last to thirty-seven — and forty points reaching two kelvin are worth more than sixteen thousand starting at twenty.

applied · Magnetism
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
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
The two terms in a vibrationally averaged rotational constant. A rotational constant averages 1/r², not r², so the moment it reports carries +2⟨Δr⟩/rₑ from the anharmonicity and −3⟨Δr²⟩/rₑ² from the harmonic spread. The two have opposite signs in every molecule here, and the anharmonic one — which is exactly zero in any symmetric well and therefore absent from every harmonic force field — is larger by a factor of 1.94 to 2.58.

The term a harmonic field cannot produce

The usual zero-point correction to a moment of inertia comes from a harmonic force field, which contains the mean square displacement and nothing else. A rotational constant does not average that. It averages one over r squared, whose leading correction is the mean displacement — zero in any symmetric well — and which enters with the opposite sign and about twice the size.

spectra · Rotation
A Morse curve's αₑ falls 4 to 15 per cent short of the measurement. The vibration–rotation constant αₑ of each diatomic, averaged over the states of a Morse curve built from its measured ωₑ, ωₑxₑ and rₑ, as a fraction of the tabulated value. H³⁵Cl: 0.27747 against 0.3072 cm⁻¹, ×0.903; D³⁵Cl: 0.10240 against 0.1133 cm⁻¹, ×0.904; ¹²C¹⁶O: 0.01674 against 0.0175 cm⁻¹, ×0.957; H¹⁹F: 0.68164 against 0.798 cm⁻¹, ×0.854. Every one is short, and HCl and DCl — one potential with two masses on it — are short by the same fraction.

The cubic a Morse curve guesses

The two terms in a vibrationally averaged rotational constant were computed on Morse curves built from measured constants, and the vibration–rotation constant αₑ is the measurement that tests them. In all four molecules the Morse curve's αₑ is short, by four to fifteen per cent. The averaging is not the error — it matches the closed form to four parts in ten thousand. The curve's cubic is, and the measurement asks for more of exactly the term a harmonic field cannot produce.

spectra · Rotation
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
One size scale, computed for every atom at once. Each atom's valence shell at the effective charge Slater's rules give it, with the mean radius of a hydrogenic orbital of that shell and that charge, and its root-mean-square radius. Both are closed forms in the principal and angular quantum numbers and the charge, so both are on one scale for every atom by construction — which is the difficulty a tabulated radius has and this does not. Neither quantity is anywhere in the cubic, which knows three energies and no length.

A size the fit was not made from

Every input tested against the chemical capacity so far has been inside the cubic that produced it, so the search was constrained to fail. A size is not: a hydrogenic orbital at the effective charge Slater's rules give an atom's valence shell has an exact radius, on one scale for every atom, and the cubic knows three energies and no length at all. It fails the test by sixteen times the floor.

wrong · Electronegativity
The measured cubic and quartic overshoot what Morse fell short of. Each molecule's αₑ as a fraction of the measured value, from its Morse curve and from a quartic potential built with the cubic and quartic coefficients the measured αₑ and ωₑxₑ imply. Every Morse curve is short, by 4 to 15 per cent. Every quartic is over, by 1 to 5 per cent: the repair moves αₑ past the measurement rather than onto it.

Two coefficients are not a potential

A Morse curve built from measured constants gets the vibration–rotation constant αₑ short by four to fifteen per cent, and the measured αₑ and anharmonicity imply the cubic and quartic a real potential should have. Built with exactly those two coefficients and solved, the potential overshoots instead. The reason is that the Morse curve's own series, cut after its quartic, moves αₑ by a sixth to a half of the error being repaired — so a quartic cannot tell whether the shortfall was the cubic.

spectra · Rotation
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

Named alongside it

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

Model limitClosed formApproximationConventionProbability densityBond lengthWavefunctionLeast-squaresOne-electron modelsReference stateConvergenceDegeneracy

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