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Rydberg to plasma evolution in a dense gas of very excited atoms

This article has been downloaded from IOPscience. Please scroll down to see the full text article. 1982 J. Phys. B: At. Mol. Phys. 15 L49 (http://iopscience.iop.org/0022-3700/15/2/004) View the table of contents for this issue, or go to the journal homepage for more

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J. Phys. B: At. Mol. Phys. 15 (1982) L49-L55. Printed in Great Britain

LETTER TO THE EDITOR

Rydberg to plasma evolution in a dense gas of very excited atoms?

G Vitrant, J M Raimond, M Gross and S Haroche
Laboratoire de Physique de IEcole Normale SupCrieure, 24 rue Lhomond, 75005 Paris, France Received 5 October 1981

Abstract. A Rydberg atom gas quickly evolves into a plasma above a threshold density. The process is attributed to Rydberg-Rydberg and Rydberg-electron collisions occurring faster than themedium expansion. Observations are found in good agreement with a simple rate equation model. This effect is different from a Mott transition. Conditions for the occurrence of this latter effect in a Rydberg atom gas are briefly discussed.

The development of far infrared and millimetre wave amplifiers and detectors using Rydberg atoms as their active medium naturally leads to the study of the behaviour of a dense sample of very excited atoms. In those systems, the Rydberg atoms are bound to interact very strongly with each other via van der Waals forces (Raimond er a1 1981) and also to break at a very fast rate due to various ionising mechanisms. Worden et a1 (1978) have., for example, observed that strontium Rydberg states undergo strong ionisation dominated by electron-Rydberg collisions at densities in the 10 cmV3 range. In the course of our maser and superradiance experiments, we have observed a related phenomenon in a Cs high-density Rydberg gas (atoms with principal quantum number n = 30-45). The ion-electron production presents a marked threshold behaviour with a sharp onset for a well defined atom density depending on the principal quantum number U. The main characteristics of this effect are accounted for by a simple model based on rate equations describing an avalanche due to Rydberg-electron collisions. This effect puts an upper limit to the density of achievable Rydberg atom samples at room temperature, the smallest average interatomic distance to Rydberg atom size ratio, x , being of the order of 15. Obviously, this sets an absolute upper limit to the inversion densities achievable in Rydberg masers or detectors (the actual limit is in fact smaller). More importantly, the avalanche mechanism reported here seems also to preclude the observation of interesting phase transition phenomena expected for x 3-5 (Mott transition in a densely packed Rydberg gas). In this letter, we describe our experiment and give a simple interpretation. We also discuss the possibility of eliminating this avalanche effect in an experiment allowing us to observe the more fundamental Mott transition. Our experimental apparatus is similar to the one described in previous publications (Fabre et a1 1978). The Rydberg atoms are prepared at the intersection of a caesium atomic beam with two collinear pulsed dye laser beams tuned on resonance with the 6 s + 6P3/2 and 6P312 + nD or 6P3/2 + nS transitions. The sample has a length 1 1 cm

i Work partly supported by DRET Contract No 80/187.

0022-3700/82/020049 + 07$02.00

@ 1982 The Institute of Physics

L49

L50

Letter to the Editor

and a diameter WO 150 50 pm defined by the laser beams focus. In this 2 x lo-'' m3 volume, one can prepare, in the 10 ns laser duration, as many as 108-109 Rydberg atoms. The initial Rydberg density ( N 1012-1013 cmP3) decreases as the volume expands at thermal velocity, and is reduced by a factor of ten after about 1 ps. The Rydberg medium is analysed by the selective field ionisation technique (Fabre et a1 1978). A delay to after the laser pulses, a ramp of electric field rising in about 1 ps is applied to the atoms. It reaches the thresholds for ionisation of successive levels at different times. The resulting electrons are detected by a gain calibrated electron multiplier: one thus gets a time-resolved spectrum of the Rydberg states populated in the gas. Figure 1 gives typical time-resolved signals for increasing Rydberg densities with to 1~ s On figure 1(a) observes a narrow peak corresponding to the level initially . one prepared by the lasers. Figure l(6) shows broader structures characteristic of energy transfers towards states less and more excited than the initial one (which ionise in stronger and weaker fields, respectively, i.e. at later and earlier times). We attribute these transfers to van der Waals interactions between Rydberg atoms (Raimond et a1 1981). Above a well defined density, one observes suddenly, in addition to these transfers, a sharp peak occurring near zero electric field and corresponding to free electrons. Near the threshold density (figure l(c)),this peak is rather small and strongly fluctuates from pulse to pulse, due to the intensity jitter of the laser. For slightly larger densities, the signal from the free electrons becomes huge at the expense of the initial level signal (figure l(d)). In figure 2 the points represent the ratio 7 of the free-electron to the total Rydberg atom signal, as a function of the initially prepared Rydberg density No,for the case of the 41d level. The threshold effect clearly appears as a turn-on of the

- *

Ito

f,,o

Time

to

-+,lo

Time

Figure 1 Time-resolved ionisation signals for various initial Rydberg densities. ( a ) . N = 10' ~ m - ~( , ) N = 2.5 X 10" ~ m - ~( c ) N = 2.65 x 10" cm-3 and ( d ) N = b , 4.5 x 10'' ~ m - ~ .

Letter to the Editor

L5 1

Figure 2. Ionised fraction q after a delay to = 1 ~ sfor n = 38.5 (41d level), as a function of , x ) the initial density (ranging from 4 x 107-5.7 lo1' ~ m - ~ 0. : experimental results; full mz (k = 0.25) (the curve: theoretical prediction from equation (7) with U = 1.02 X value u,/uR is 100).

ratio 7 above a given density NT. The value of NT depends on the principal quantum number of the level. The points in figure 3 show the measured threshold variation as a function of n on a logarithmic scale. NT decreases roughly as (n* is the effective quantum number, equal to n - 2.47 for D states, and to n -4.06 for S states). Finally, we have studied the influence of the delay to on this effect and observed that the

5 x10"
L

+ .VI
W

.=

10"

145 30d 32d 34s

15 34d 36s 36d 38s

155
38d 40s 40d
I I

16 42d
I I

1 6 5 Lg(n*i 44d
I

n
n

42s

44s

46s

Figure 3. Threshold density NT ( ~ m - ~ ) a function of n* on a logarithmic scale. 0 : as experimental results; full line: predictions of equation (7) (k = 0.23), exhibiting a n*-4 dependence.

L52

l e t t e r to the Editor

free-electron signal is not instantaneous and, near threshold, requires a few tens of nanoseconds to occur. These observations clearly indicate that, above a given density the Rydberg gas is unstable and evolves into a plasma, from which electrons are extracted by a very small electric field (we have checked that the free-electron signal can be collected in a field as small as 1 V cm-', near threshold, as opposed to the 300 V cm-' field necessary to break the initially prepared Rydberg atoms for y1 30). It is tempting to compare this Rydberg atom to plasma evolution with a metalinsulator phase transition of the Mott type (Mott 1974). Let us recall that these transitions occur in a disordered system (atomic vapour, excitons in a doped semiconductor, . . .), when the average interparticle distance (particles = atoms, excitons, , , .) is of the order of a few times the particle size (Mott criterion); the electrons then become delocalised, and the Mott criterion can be justified by electronic freeenergy considerations. Our Rydberg to plasma transition does indeed exhibit some features reminiscent of such a Mott phenomenon; in particular the threshold behaviour and the very strong dependence of the electron number on the initial density. The Mott criterion for such a Rydberg gas can be estimated by comparing the negative binding energy g1of a Rydberg atom with the negative polarisation energy g 2 of the Rydberg gas by a free electron and a free ion, produced in the sample by the ionisation of a Rydberg atom. When 1 2 is larger than lgll,which occurs for an interatomic distance to g1 atomic size ratio x of the order of 3, the delocalised plasma state becomes the stable one, and the Rydberg to plasma transition should occur. Several features of the observed effect, however, do not support this interpretation: the existence of a long delay time compared with the atomic characteristic times s), the order of magnitude of the threshold density, corresponding to x 15 instead of 3, the NT versus y1 variation which should be y1? in a Mott transition. In fact, the relatively long time scale of the ionisation process indicates that the slow motion of the nuclei plays an important part in the phenomenon, whereas it is irrelevant in a Mott process, whose description is simple only at low temperature. We are thus led to take into account the various Rydberg atom collision processes. The following mechanisms have to be considered:

Cs* + hv

+ Cs+ +e-

Cs* + Cs+ Cs++Cs + e-

Cs* + Cs+ Cs:

+ eCS"+ CS*+ Cs* + Cs' + eCs* + e- + Cs' + 2eCS"+ CS++ CS++ Cs' +e-

which respectively describe photoionisation, Rydberg-ground-state ionising collisions, associative ionisation (Worden et a1 1978), Rydberg-Rydberg ionising collisions (Olson 1976), Rydberg-electron and Rydberg-ion collisions (Percival and Richards 1975). Photoionisation has an exceedingly small cross section; furthermore it cannot occur during most of the avalanche evolution, since the laser excitation lasts only 10 ns. The second and third processes can also be neglected compared with the fourth one in a medium where the number of Rydberg atoms is of the order of the number of ground-state atoms (Rydberg-Rydberg cross sections are of the order of the geometric

Letter to the Editor

L53

cross sections, and the Rydberg-ground-state cross sections are at least an order of magnitude smaller for n 40). In a neutral medium, the last reaction is slower than the fifth, approximately in the ratio of the ion to electron speeds (the cross sections are of the same order of magnitude). Finally reactions (4) and ( 5 ) are the only processes one need take into account in a simple model. The cross sections of these two reactions are of similar orders of magnitude (Olson 1976, Percival and Richards 1975). Their rates are in the ratio of the electron to Rydberg densities times the Rydberg to electron velocities. We are thus led to describe the phenomenon in the following way: immediately after the laser excitation, Rydberg atoms start to collide at a rate inversely proportional to their geometric ionisation cross section. This process provides the first electrons in the system. These electrons escape from the sample with an energy of the order of lo-* eV, i.e. the electron binding energy in the Rydberg states, which turns out to be of the order of the thermal energy at the atomic beam temperature. After a few thousand electrons have escaped, the remaining much slower ions build up a space charge which traps the electrons produced subsequently. These electrons travel back and forth in the medium, with a velocity 100 to 1000 times larger than that of the ions. Reaction ( 5 ) then becomes more and more important and rapidly dominates the system evolution. In other words, the initial Rydberg-Rydberg collisions produce seed blectrons which induce an avalanche effect in the medium. The exponential increase of the electron density is limited only by the sample expansion. The threshold results from the competition between the avalanche and the expansion speeds. This interpretation links this effect to the one observed in strontium (Worden et a1 1978) and also to the strong ionisation observed in particular by McIlrath and Lucatorto (1977) in high-density alkali gases irradiated on their principal resonance line by powerful laser beams. We should note, however, the large difference of the orders of magnitude between this last effect and the Rydberg experiments. Whereas in McIlrath and Lucatorto (1977) the ~ m - the, Rydberg ionisation effects are observed for ~ densities are of the order of densities as small as 1 O I 2 cmP3, reflecting the large ionisation cross sections in the Rydberg gas. The above explanation can be supported by a quantitative calculation based on a R rate equation. Let us call No the total initial population, N the remaining Rydberg population at time t after the excitation, U the total ionisation cross section for a Rydberg atom by another very excited atom or by an electron (that we assume to be of the same order of magnitude), ue the mean electron velocity, ur the mean relative + Rydberg velocity; W the medium diameter at time t ( W = WO u,t) (the length 1 of the medium is approximately constant during the experiment time); 1/ Tot h e initial Rydberg-Rydberg collision rate:

1 OT , -=- N C U
To

lWi*
NR

The evolution of

is described by the following rate equation NRWO-NR)WO o e MOTo (F)

2

__ dNR dt

(7)

The first term in the right-hand side of this equation corresponds to RydbergW factor takes into account the expansion of the Rydberg collision effects. The (WO/ ) 2 medium. The second term corresponds to the Rydberg-electron collisions (the number

L54

Letter to the Editor

of electrons at time t is N o - N ~ ) whose collision rate is V J V R times larger than the , Rydberg-Rydberg one. This equation obviously describes an avalanche process in the Rydberg gas. All the parameters are known or measured, expect for (T which we assume to be r ( k a 0 n * 2 ) 2 , where k is a free parameter. Solving (7) and defining the threshold N r as the No value giving

at we can calculate NT(n).We can also calculate 7(No)time to == I ps, We choose for k the value giving the best fits with the experimental points of figure 2 and 3 : with k = 0.25 one finds the full curves in these figures, which are in fair agreemeilt with the observations. Using this k value, we have also calculated q ( t ) for increasing initial densities No, and for n* = 38.5. Results are plotted in figure 4. The onset of the avalanche phenomenon is clearly apparent for No= NT= 1.4 x 10'' cm- '~

0.0

Time

a .L

IO-'

Figure 4. Theoretical calculation o the ionised fraction q plotted against time for various f densities (curve A, 3 . 1 . ~ ~ m - ~ ; 1.4 X 10" ~ m - C, ; 2.5 X 10" ~ m - ~ ; 3.6 X lo1' B, ~ D, 10" ~ m - E, ; X 10" ~ 4.7 with U = 1.02 x m2 and r;,/vR = 100.

This model thus explains fairly well the main features of the observed phenomena. It assumes, however, a value of the Rydberg-Rydberg and Rydberg-electron cross section one order of magnitude smaller than the one given by Olson (1976) and Percival and Richards (1975). An explanation would be an overestimation of the Rydberg density (it is, in particular, difficult to determine the exact size of the medium, which could be wider than the light focus due to optical saturation). We should also point out that the Rydberg ionisation occurs in a medium where the atoms are already strongly perturbed by van der Waals coupling between neutrals (Raimond et a1 1981). It is thus possible that the two-body analysis developed here is too nai've. Let us conclude by a few remarks concerning the connection with various experiments involving large numbers of Rydberg atoms. It is clear that the density in the active medium of a maser or an amplifier should be kept lower than the avalanche threshold. In fact the van der Waals dephasing, which

Letter to the Editor

L55

already becomes important for x 30, perturbs the electric dipoles and inhibits the superradiance or maser effect well before the ionisation process described here occurs. The avalanche threshold is thus certainly higher than the maximum possible density for Rydberg masers or amplifiers. As for the Mott transition effect, this experiment indicates that its observation in a Rydberg system would be possible only if the effect of the atomic motion could be suppressed. Rather than reducing the atom temperature to a fraction of a kelvin which should be very difficult, it could be worth trying to perform the experiment in a time so short that the atoms cannot move over distances larger than their own diameter. This requires, in practice, picosecond excitation and detection times. Under these conditions, it should be possible to pack the atoms at much higher densities than in this experiment and to observe phenomena related to Mott transitions. Another recent subject of interest is the study of Rydberg-Rydberg ionising collisions themselves. Our experiment shows that in a dense sample they are quickly masked by the much faster electron-Rydberg processes. The only way to investigate them would be to use a true collision apparatus involving two intersecting low-density Rydberg atomic beams. References
Fabre C, Haroche S and Goy P 1978 Phys. Rev. A 18 229 McIlrath T J and Lucatorto T B 1977 Phys. Rev. Lett. 38 1390 Mott Sir N F 1974 Metal Insulator Transitions (London: Taylor and Francis) Olson R E 1976 Phys. Rev. Lett. 43 126 Percival I C and Richards D 1975 Advances in Atomic and Molecular Physics vol 11, ed D R Bates and B Bederson (New York: Academic) p 1 Raimond J M, Vitrant G and Haroche S 1981 J. Phys. B: At. Mol. Phys. 14 L655-60 Worden E F, Paisner J A and Conway J G 1978 Opt. Lett. 3 156