Astrophysics

The limit that belonged to a simpler atom

The theory of laser cooling predicted a floor, and the first careful measurement came in six times below it. Nothing was wrong with the measurement or the arithmetic. The floor belonged to an atom with one ground state, and real atoms have several — which lets the light build a hill in front of every atom, move it to the bottom before it can roll back, and repeat the trick until the atom is a few microkelvin from rest.

Assumes: The friction made of light · The light that pulls rather than pushes

In the summer of 1988 a group at the National Bureau of Standards in Maryland measured the temperature of a cloud of sodium atoms held in optical molasses, and did it carefully. They switched the beams off, let the atoms fall and spread, and timed their arrival at a probe beam below: a hot cloud spreads fast and arrives smeared, a cold one arrives in a sharp pulse. The answer was 43 microkelvin, give or take 20.

The theory of the friction made of light put a floor under that number at ħΓ/2kB, which for sodium is 240 microkelvin. A measurement six times below a theoretical minimum is not a small discrepancy to be absorbed into the error bars. Either the thermometer was wrong, or the minimum was not a minimum.

The thermometer was checked, repeatedly, by several groups with different methods, and it was right. What made the result impossible to dismiss was a second observation made at the same time: the atoms got colder as the lasers were tuned further from resonance and as their intensity was turned down. The Doppler theory predicts the opposite of both.

Two theories that disagree about which way to tune. The temperature caesium-133 should reach in beams of fixed intensity (saturation 5 on resonance) against the detuning below resonance, on logarithmic axes, by two mechanisms. The Doppler theory has its minimum near half a linewidth and then rises in proportion to the detuning, because the friction falls faster than the heating. The polarisation-gradient mechanism does the opposite: its temperature is the straight line in the light-shift well depth that the stochastic runs give, 39 recoil energies plus 0.33 of the depth, and at fixed intensity the depth falls as one over the detuning — so it gets colder the further the beams are tuned away. The heavy part of that curve is where the wells are at least a hundred recoil energies deep and the detuning at least three linewidths, the range the model is built for; it ends at 10.5 linewidths. At five linewidths the two predictions are 664 µK and 10.8 µK. A temperature that fell as the light was tuned away was the sign that the first theory was not describing the atoms.
Fig. 1 The temperature caesium should reach at fixed beam intensity against the detuning, by two mechanisms. The Doppler theory’s temperature rises as the beams are tuned away. The polarisation-gradient temperature — computed from the stochastic model later on this page — falls: 664 µK against 10.8 µK at five linewidths. The heavy stretch is the range in which that model applies.

The trend that gave it away

A floor that is lower than predicted could be a correction. A trend that runs backwards cannot be. The Doppler temperature has a minimum near half a linewidth, and on the far side of it the friction falls faster than the heating: tune further away and every atom is heard more faintly by both beams, and a faint velocity sensor cools badly. At a fixed intensity the predicted temperature rises almost in proportion to the detuning.

The measured temperatures fell. That is what a second mechanism looks like when it is hiding behind a first: a quantity that depends on the knobs differently, so that the knob settings which weaken the known mechanism strengthen the unknown one. Within a year two groups had worked out what it was, Jean Dalibard and Claude Cohen-Tannoudji in Paris and Steven Chu’s group at Stanford, and the answer was contained in an assumption so ordinary that nobody had thought of it as an assumption.

What the simple atom left out

The Doppler theory treats the atom as having one ground state and one excited state, with light of any polarisation driving the transition equally. No real alkali atom is like that. Sodium’s ground state has angular momentum, which means it has sublevels — orientations of an angular momentum that is not a rotation — and circularly polarised light of one handedness couples those sublevels to the excited state with different strengths.

The second ingredient is already on the page in the light that pulls rather than pushes. Light tuned below a resonance does not only scatter; it shifts the energy of the ground state downward by an amount proportional to the intensity, and a spatially varying shift is a potential the atom moves in. For a single ground state that potential is the gradient force of an optical trap. For a ground state with sublevels, each sublevel is shifted by a different amount, depending on how strongly it couples to the local light.

Now arrange the two beams of a molasses with their linear polarisations at right angles. Where they overlap they add into a standing pattern whose polarisation changes along the axis: circular of one handedness at one point, linear an eighth of a wavelength further on, circular of the other handedness a quarter of a wavelength from the start. The intensity is uniform; the handedness is not.

A hill that is always ahead of the atom. The light-shift potentials of the two ground sublevels of a spin-½ atom in two counter-propagating beams with crossed linear polarisations, over one and a half wavelengths, in units of the well depth. The polarisation of the light turns from σ+ to linear to σ− every quarter wavelength, and the two sublevels see sinusoidal potentials a quarter wavelength out of step. Optical pumping transfers the atom from one sublevel to the other fastest exactly where its own potential is highest — the fastest pumping and the hilltop coincide, which the figure checks — and that is the bottom of the other potential. The heavy line is an atom that starts with 3.3 well depths of kinetic energy: each time it reaches a hilltop it is pumped down by exactly one well depth, climbs the next hill, and is pumped down again, 3 times, until it no longer has the energy to reach a hilltop and is left oscillating in one well. The energy is carried off by the pumping photon, which leaves bluer than the light that drove it by the depth of the well.
Fig. 2 The light-shift potentials of the two ground sublevels of a spin-½ atom in beams with crossed linear polarisations, in units of the well depth, over one and a half wavelengths. The heavy line is an atom that starts with 3.3 well depths of kinetic energy: at each hilltop it is optically pumped down by exactly one well depth, onto the bottom of the other potential, until after three such steps it cannot reach a hilltop and is left in one well.

For the simplest atom that shows the effect, with a spin-½ ground state, the two sublevels see the two potentials drawn: sinusoids with a period of half a wavelength, one the other shifted by a quarter. Where the light is circular of one handedness the sublevel aligned with it is shifted most and sits at the bottom of its well; the other sublevel, which couples weakly there, sits at the top of its hill. A quarter of a wavelength later the roles are exchanged.

Climbing a hill that keeps moving

The last ingredient is optical pumping. An atom that scatters a photon of one circular polarisation tends to fall back into the sublevel aligned with that polarisation, so scattering redistributes atoms between the sublevels — and the rate at which it moves an atom out of a sublevel is highest exactly where that sublevel couples weakly to the local light. That is the top of its hill. The figure checks the coincidence rather than taking it on trust: the pumping rate out of the upper potential peaks at the same position as the potential itself, to within the resolution of the search.

So an atom moving along the axis climbs a hill, slowing as it goes, and near the top it is most likely to be pumped into the other sublevel — whose potential at that point is at the bottom of a well. The atom finds itself at the bottom of a new hill with the kinetic energy it had at the top of the old one, and starts climbing again. Each such transfer removes one well depth of energy.

Where the energy goes is the same bookkeeping the friction made of light found for the Doppler case, with a different shift. The pumping photon is emitted from a level that sits one well depth lower than the level it was absorbed from, so it leaves bluer than the laser light by exactly that energy. The atom is being cooled by photons that climb out of the light-shift potential it was forced to climb into.

Dalibard and Cohen-Tannoudji named it after the king condemned to roll a boulder up a hill for ever and see it roll back. The naming is apt with one inversion that matters: Sisyphus lost his boulder at the top, and the atom loses its hill.

The staircase, drawn by chance. One atom in a lattice 200 recoil energies deep, started with 6 well depths of kinetic energy and followed through the stochastic model: its position and velocity integrated in whichever sublevel potential it is in, photons scattered at the rates the local polarisation sets, and each scattering allowed to move it to the other sublevel with the pumping probability. Its total energy is drawn against time in units of the mean interval between scatterings, with the pumping events marked. The energy does not fall smoothly; it falls in steps at pumping events, and the steps are down far more often than up because pumping happens preferentially at hilltops. Late in the run the energy hovers around −0.62 well depths and the atom is below the hilltops at −0.5 for 67% of the time — trapped in a well, still being kicked, and occasionally kicked out of it. 68 pumping events occurred in about 600 scatterings.
Fig. 3 One atom in a lattice 200 recoil energies deep, started with six well depths of kinetic energy and followed through the stochastic model — position and velocity integrated in whichever potential it is in, photons scattered at the rates the local polarisation sets, pumping allowed with the pumping probability. The energy falls in steps at the marked pumping events. Late in the run it sits below the hilltops two thirds of the time: trapped, kicked, and occasionally kicked out.

The drawn staircase of the landscape figure is the idealised mechanism. The stochastic run is what it looks like when pumping is a matter of probability rather than of position, and it has three features the idealisation hides. Some pumping events happen away from the hilltops and take energy out of the well depth rather than removing it, which the jagged steps upward show. Every scattering, pumping or not, kicks the atom by a photon’s momentum, so the energy never settles on a single value. And the atom that ends up in a well is not stuck there: a large enough kick lifts it over a hilltop, and the climbing begins again.

A friction set by a delay

The mechanism has a structure worth pulling out, because it is not special to atoms. The atom’s internal state follows the polarisation of the light it is in, but it follows with a lag — a pumping time. An atom standing still has its sublevel populations in equilibrium with the local light and feels no net force. An atom moving through the pattern carries populations appropriate to where it was, and so it is always in the wrong sublevel for where it is: more often on the uphill side than the downhill one. The force that results opposes the motion, and it is largest when the atom crosses a quarter wavelength in about one pumping time.

That is a relaxation loss. A response that lags a periodic drive absorbs energy from it at a rate that peaks when the drive period matches the relaxation time, which is the liquid that remembers absorbing energy most strongly when it is sheared at the inverse of its relaxation time, and it is the reason a dielectric heats most at the frequency its dipoles can just follow. The atom is the lagging medium, the pattern of polarisation it moves through is the drive, and the friction is the absorption.

One consequence of that picture is decisive for what follows. The friction coefficient for slow atoms comes out independent of the intensity: brighter light makes the hills higher, which strengthens the force, and pumps faster, which shortens the lag, and the two effects cancel. The heating, on the other hand, follows the scattering, which grows with intensity. So the equilibrium temperature — heating over friction — grows in proportion to the light.

A floor that falls with the light

A floor that falls with the light, until the light stops holding. The temperature the stochastic model settles at, against the depth of the light-shift lattice, both in recoil energies, for caesium-133 with the beams 3 linewidths below resonance. Each point is 120 atoms followed through about 600 scatterings each, seeded. From a hundred recoil energies up the temperature is a straight line in the depth — 39 plus 0.33 of the depth, drawn dashed — because the friction does not depend on how bright the light is and the heating does; the intercept is the recoil heating of the scattered photons, which does not go away. Below that the line fails: a well a few tens of recoil energies deep no longer holds an atom as hot as the cooling leaves it, and the temperature climbs. 25 deep: 170 (16.8 µK); 50 deep: 83 (8.25 µK); 100 deep: 70 (6.96 µK); 200 deep: 98 (9.72 µK); 400 deep: 187 (18.6 µK); 800 deep: 300 (29.8 µK). The coldest run is 6.96 µK, against a Doppler limit of 125 µK for the same atom, drawn across the top.
Fig. 4 The temperature the stochastic model settles at against the depth of the light-shift lattice, both in recoil energies, for caesium three linewidths below resonance: 120 atoms per point, seeded. From a hundred recoil energies up the temperature is a straight line in the depth, 39 plus 0.33 of the depth. Below that the line fails and the temperature climbs. The coldest run is 6.96 µK; the Doppler limit is drawn across the top at 125 µK.

The runs bear the argument out and add two corrections to it. The temperature is a straight line in the well depth from a hundred recoil energies to eight hundred, with a slope of a third — roughly a third of a well depth of thermal energy, which is the statement that cooling stops mattering once the atom can no longer reach a hilltop. It is a straight line and not a proportion: it has an intercept of about forty recoil energies, which is the heating from the photons’ own recoils, a heating that does not vanish when the light is turned down.

And below a hundred recoil energies the line fails outright. At fifty the atoms are warmer than at a hundred, and at twenty-five warmer again. A well that shallow does not hold an atom with the energy the cooling leaves it, the atom stops being localised on a hill, and the lag argument that produced the friction no longer applies. Measured sub-Doppler temperatures show the same shape — linear in intensity over detuning, with an offset, and a sharp rise when the light is made too weak — and in three dimensions caesium molasses reach a few microkelvin.

That explains the 1988 measurement completely. The temperature depends on the well depth, which is proportional to intensity over detuning, so dimmer beams and larger detunings make colder atoms. The Doppler mechanism is still there, and at a few microkelvin it is irrelevant: its own floor is a hundred times higher.

Two floors, set by different things

A mechanism that lowers the temperature in proportion to the light cannot do so for ever, even in principle, and the reason is not in any of the potentials. Every cooling scheme that works by scattering photons delivers the last kick with a photon, and that kick has a size.

Two floors, set by different things. For each atom, the Doppler limit ħΓ/2kB and the recoil temperature ħ²k²/mkB — the temperature at which a single photon's kick is the whole width of the velocity distribution — on a logarithmic scale. The first is set by the linewidth and contains no mass; the second is set by the mass and the wavelength and contains no linewidth. sodium-23: Doppler 235 µK, recoil 2.40 µK; rubidium-87: Doppler 146 µK, recoil 362 nK; caesium-133: Doppler 125 µK, recoil 198 nK; strontium-88 (461 nm): Doppler 732 µK, recoil 1.03 µK; strontium-88 (689 nm): Doppler 180 nK, recoil 458 nK. For every broad line the Doppler floor is hundreds of times higher, and a cooling mechanism that does not depend on the linewidth can go a long way below it before one photon becomes too coarse a tool. Strontium's 689 nm line is the exception: its linewidth is so narrow that the Doppler floor is below the recoil one, and there the photon itself is the limit.
Fig. 5 For five cooling transitions, the Doppler limit ħΓ/2kB and the recoil temperature ħ²k²/mkB, at which one photon’s kick is the whole width of the velocity distribution. For caesium they are 125 µK and 198 nK; for sodium 235 µK and 2.40 µK. Strontium’s narrow 689 nm line is the exception: its Doppler limit of 180 nK is below its recoil temperature of 458 nK.

The two floors contain different things, and the figure is the clearest way to see it. The Doppler limit contains the linewidth, which is a lifetime, and nothing about the atom’s mass; the recoil temperature contains the mass and the wavelength and nothing about the linewidth. For every broad line the first sits hundreds of times above the second, which is the room polarisation-gradient cooling works in — and the minimum of the stochastic runs, 70 recoil energies for caesium, sits a factor of thirty-five above the recoil floor, which is about where real molasses stop.

Strontium’s intercombination line is the case that exposes the logic. Its linewidth is so narrow that the Doppler limit falls below the recoil, and cooling on that line reaches the recoil floor by the ordinary Doppler mechanism with no sublevel tricks at all. The limit a scheme runs into is whichever of its floors is higher, and a scheme is only as good as its worst assumption.

Past the last photon

The recoil floor is a statement about photons that are absorbed and re-emitted at random, and like the Doppler floor it was treated as fundamental until it was not.

The first escape was to arrange for the coldest atoms to stop scattering. An atom in a suitable superposition of sublevels can be in a state that the light cannot excite at all — a dark state — and if the dark state is also a state of zero velocity, atoms that random-walk into it stay there while the others keep being kicked. Aspect, Cohen-Tannoudji and collaborators demonstrated it with helium in 1988, reaching half the recoil temperature, and the scheme’s name, velocity-selective coherent population trapping, is a precise description of what it does. The atoms are not cooled below the recoil so much as collected there.

The second escape removed the light. A cloud of atoms in a magnetic trap, precooled by the methods on these pages, is let lose its most energetic members over the rim of the trap; the rest re-thermalise by collisions at a lower temperature, and the rim is lowered again. Evaporation needs no photons and has no recoil floor, and in 1995 it took a cloud of rubidium to 170 nanokelvin, where the atoms’ de Broglie wavelengths overlapped and a Bose–Einstein condensate formed — the regime in which everything has a wavelength stops being a remark about small numbers.

It is worth noticing the shape of the whole sequence, because it recurs. A limit is derived; it holds for the model it was derived for; a measurement beats it by exploiting something the model left out; a new limit appears for the new mechanism. The staircase that never reaches the floor is the same pattern in magnetic cooling, where each technique hands over to one with a lower floor. What does not change is that each floor is real for the mechanism it belongs to.

Where the model stops

The atom is the simplest one that shows the effect. A spin-½ ground state and a spin-3/2 excited state give two sublevels and two potentials. Sodium, rubidium and caesium have many more, with a hyperfine structure that makes the potentials more complicated and the numerical factors different; the mechanism — potentials that depend on polarisation, pumping that lags them — is the same, and so is the scaling with intensity over detuning.

The polarisation arrangement is one of two. Beams with opposite circular polarisations also cool below the Doppler limit, by a different mechanism in which the atom’s orientation rather than its sublevel populations lags a polarisation that rotates along the axis. The scaling is similar and the picture of a hill is not.

The atom is treated as a classical particle with a quantum internal state. That is the semiclassical approximation, and it is good while the atom’s wavepacket is much smaller than a well. At a few tens of recoil energies of depth it is not, the atom is spread over several wells, and a full quantum treatment — which gives the atom a band structure in the periodic potential, like an electron in a crystal — replaces the stochastic particle. The failure of the straight line at low depth is partly the physics and partly the model announcing its own edge.

There is no magnetic field. Sub-Doppler cooling depends on degenerate sublevels, and a field of a fraction of a gauss splits them by more than the light shift. The laboratories that first saw 43 microkelvin had to null the Earth’s field to see it at all, and a molasses in an uncancelled field quietly returns to the Doppler limit.

What the pictures cannot show

The landscape figure draws two potentials and an atom on one of them at a time, and hides that between pumping events the atom is in a definite sublevel only in the stochastic model’s bookkeeping. The quantum state is generally a superposition of the two, and the pumping that the model treats as a jump is a rate at which coherence is destroyed.

Nor does any figure show what the atoms look like when they are cold enough. A few tens of recoil energies of depth, with atoms at a third of it, is a gas whose members spend most of their time sitting in individual wells half a wavelength apart — an array of atoms held in place by nothing but the interference pattern of two laser beams. That array is an optical lattice, and it became a laboratory in its own right: a crystal whose spacing, depth and dimensionality are set by optics, in which atoms play the part electrons play in a solid and meet the gaps a repeat opens in their own motion. The picture of a moving hill is the moment a crystal of light first appeared, and none of these drawings has the resolution to show it.

Still open: how cold light can make a gas that it keeps touching

The recoil floor was escaped by arranging for the coldest atoms to stop interacting with the light, and by removing the light entirely. Neither is cooling by light in the sense of this page, and the question they leave is whether there is a scheme that goes on scattering photons and still reaches below the kick of a single one.

The candidates are all schemes in which the scattering is made to depend steeply on velocity near zero — so that an atom which has been kicked out of the coldest state is kicked back far more readily than one inside it is kicked out. Raman cooling with carefully shaped pulses and cooling on transitions whose linewidth is narrower than the recoil both do this, and both reach temperatures below the recoil in some directions. Whether a steady, scattering, three-dimensional scheme can do it is an argument about how narrow a velocity filter can be made while photons keep arriving, and it is not settled by any figure here.

The habit worth carrying away is the one the 1988 measurement enforced twice. When an experiment beats a limit, look first at the trend rather than the value. A value below a floor can be an error; a dependence on the knobs that runs backwards cannot be, and it points directly at the assumption that has to go.

Part 6 of 6

This essay is one argument about Radiation pressure. The others:

The objects named here

The third axis, after the field and the reading path: the things themselves, and every essay that touches each one.

Doppler limitLaser coolingLight shiftOptical latticeOptical molassesOptical pumpingPolarisationRadiation pressureRecoil limitSisyphus cooling