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# Cross Section Limits for the 208Pb(86Kr,n)293118 Reaction

## I Introduction

In 1999, the synthesis of element 118 (and its decay products) using the 208Pb(86Kr,n) reaction was reported . This claim was based on the apparent occurrence of three decay chains, each consisting of an implanted heavy atom and six subsequent alpha decays, correlated in time and position. A fourth event involving a number of “escape” alpha particles (depositing only part of their energy in the detector) was reported also . Based upon the above three chains, and a revised estimate of the beam dose in the 1999 experiments, a cross section of 7$`{}_{}{}^{+9}{}_{3}{}^{}`$pb was deduced for the synthesis of element 118 at a projectile energy (center of target, lab system) of 449 MeV. A new calibration of the magnetic rigidities (B$`\rho `$) of the Berkeley Gas-Filled Separator (BGS) indicates that the reported element 118 compound nucleus evaporation residues (EVRs) recoiling from the target would have had a B$`\rho `$ of 2.00-$`Tm`$ in the 130 Pa He gas of the separator. Attempts to reproduce this result by other groups  were unsuccessful.

Subsequently, the claim to synthesis of element 118 using the 208Pb(86Kr,n) reaction has been retracted . That retraction was based upon the absence of the reported  chains in a re-analysis of the binary data on the original 1999 data tapes. An investigation into this matter has concluded that there was scientific misconduct and data fabrication by one individual. GSI has also reported similar spurious data. Despite the retraction of this claim, the current work is important in establishing definitive upper limits on the production of element 118 in the 208Pb(86Kr,n) reaction.

Motivated in part by the erroneous report , there have been a number of papers  predicting the structure and decay properties of element 118 and its daughters. Should element 118 be synthesized, it will be interesting to compare these predictions with the observations. In a similar vein, there have been a number of papers  dealing with the synthesis of element 118 and the reported production cross section, which was unexpectedly large. Special mention should be made of the work of Smolańczuk  which prompted the experimental measurement . Smolańczuk originally estimated  a production cross section of 670 pb for the 208Pb(86Kr,n) reaction, an estimate that was later revised  to 5.9 pb. Other predictions  for the evaporation residue production cross section for the reaction of 449 MeV 86Kr with 208Pb range from 0.005 to 2 pb. These predicted cross sections are generally larger than expected from a simple logarithmic extrapolation of the trend of cross sections for reactions of the type 208Pb(X,n)  (fig. 1). Similar predictions of a non-exponential decrease in cold fusion cross sections for reactions leading to elements 116 and lighter elements have been made . The physical effect behind this trend was pointed out by Myers and Swiatecki as due to a sinking of the Coulomb barrier below the bombarding energy for symmetric target-projectile combinations, thus “unshielding” the saddle point. As pointed out by Siwek-Wilczynska and Wilczynski, the system in these cases must still evolve from the dinuclear composite system into the compound nucleus. Thus, even the establishment of upper limits for the 208Pb(86Kr,n) cross section may contribute to our understanding of the large scale collective motion in very heavy nuclei.

Besides the work reported herein, three recent attempts to reproduce the observations of  have been reported . We summarize these attempts in table 1 in terms of the beam energy used, the particle dose and the observed upper limit cross section. All upper limit cross sections are reported as “one event upper limits”, i.e., the cross section that would have been reported had one event been observed with the given particle dose, target thickness, separator efficiency, etc. In the case of the data in , a separator efficiency of 50%  was used to calculate the cross section. All excitation energies were calculated from .

## II 2001 Experimental Setup

The reaction 208Pb(86Kr,n) was studied at the 88-Inch Cyclotron of the Lawrence Berkeley National Laboratory, using the Berkeley Gas-filled Separator . The experimental apparatus was a modified, improved version of the apparatus used in , including improved detectors and data acquisition systems, continuous monitoring of the separator gas purity, and a better monitoring of the 86Kr beam intensity. A 86Kr19+ beam was accelerated to 457 MeV with an average current of $``$1.3 x 1012 ions/s. The beam went through the 40 $`\mu `$g/cm2 carbon entrance window of the separator before passing through the 208Pb target placed 0.5 cm downstream from the window. The targets were 470 $`\mu `$g/cm2 thick (sandwiched between 40 $`\mu `$g/cm2 C on the upstream side and 10 $`\mu `$g/cm2 C on the downstream side). Nine of the arc-shaped targets were mounted on a 35-cm wheel that was rotated at 300 rpm. The beam energy in the target was 453 - 445 MeV , encompassing the in-target energies used in . The beam intensity was monitored by two silicon p-i-n detectors (mounted at $`\pm `$ 27 degrees with respect to the incident beam) that detected elastically scattered beam particles from the target. Attenuating screens were installed in front of these detectors to reduce the number of particles reaching them (and any subsequent radiation damage to the detector). These detectors, the 208Pb targets and the separator entrance window were replaced periodically during the run which lasted three weeks.

The EVRs (E$``$131 MeV) were separated spatially in flight from beam particles and transfer reaction products by their differing magnetic rigidities in the gas-filled separator. The separator was filled with helium gas at a pressure of 130 Pa. The expected magnetic rigidities of 131-MeV 293118 EVRs were estimated using the data of Ghiorso et al. . These estimates were 2.00 $`Tm`$ from extrapolation of the data in their Fig. 3, and 2.10 $`Tm`$ from their semi-empirical formula for EVR charge. In the current experiments, two settings of the magnetic fields of the separator were used, 2.00 $`Tm`$ and 2.12 $`Tm`$. These settings differ by 6%, the width in magnetic rigidity of the focal plane detector. The efficiency of the separator for transport and implantation of Z=118 EVRs was estimated to be $``$79 % using a Monte Carlo simulation described below.

The detector setup at the focal plane of the separator consisted of a parallel plate avalanche counter (PPAC)  placed $``$29 cm upstream of a Si strip detector. The 10 cm x 10 cm PPAC registered time, energy loss, and x,y position of the particles passing through it. It has a thickness equivalent to $``$0.6 mg/cm2 of carbon. The time-of-flight of the EVRs between the PPAC and the Si-strip detector was also recorded. The PPAC was used to distinguish between events arising from beam-related particles being implanted into the Si-strip detector, and those arising from the decay of previously implanted atoms. During these experiments, the PPAC efficiency for detecting beam-related particles depositing between 8 and 14 MeV in the Si-strip detectror was 97.5-99.5%.

The 300 $`\mu `$m thick passivated ion implanted silicon strip detector had 32 vertical strips and an active area of 116 mm x 58 mm. The strips were position sensitive in the vertical (58 mm) direction. The sources used for position and energy calibrations are summarized in table 2. The energy resolution of the focal plane detector was measured during the 86Kr + 208Pb experiments using the 7.45 MeV 211Po background peak. The energy resolution was 42 keV (FWHM). The differences in measured positions for the 252No - 248Fm full energy $`\alpha \alpha `$ correlations in the 48Ca + 206Pb study had a Gaussian distribution with a FWHM of 0.52 mm ($`\sigma `$ = 0.22 mm). The measured position resolution for full energy alpha particles correlated to “escape” alpha particles (which deposited only 0.5 - 3.0 MeV in the detector) was $``$1.2 mm (FWHM). A second silicon strip “punch-through” detector was installed behind this detector to reject particles passing through the primary detector. A “top” and a “bottom” detector were installed upstream of the focal plane detector to detect escaping alpha particles and fission fragments. The focal plane detector combined with these “top” and “bottom” detectors had an estimated efficiency of 75 % for the detection of full energy 11 MeV $`\alpha `$-particles following implantation of a 293118 nucleus.

Any event with E $`>`$0.5 MeV in the focal plane Si-strip detector triggered the data acquisition. Data were recorded in list mode, and included the time of the trigger, the position and energy signals from the PPAC and the Si-strip detectors, and energy signals from the “top”, “bottom” and “punch-through” detectors. With the use of buffering ADCs and scalers, the minimum time between successive events was 15 $`\mu `$s.

The energies of the 293118 EVRs, after passing through the PPAC, were estimated to be $``$73 MeV by extrapolation of heavy ion stopping powers, calculated with SRIM2000 . The 293118 implantation pulse height in the Si-strip detector was estimated to be 24-48 MeV after applying the pulse-height defect determined for Rn EVRs from the 365-MeV 86Kr + 120Sn reaction.

With a beam current of 1.3 x 1012 86Kr ions striking the target, the average total counting rates (E $`>`$0.5 MeV) in the focal plane detector were $``$40/s and $``$10/s at B$`\rho `$ settings of 2.00 and 2.12 $`Tm`$, respectively. The average rate of “alpha particles” (8-14 MeV with no PPAC signal) was $``$0.2/s.

## III Results

At separator magnet settings corresponding to EVR magnetic rigidities of 2.00 and 2.12 $`Tm`$, the projectile doses were 1.1 x 1018 and 1.5 x 1018, respectively. No event chains similar to those reported in  or as predicted  for the decay of 293118 were observed. Two independent searches were performed for superheavy element decay sequences. In the first, a search routine in the GOOSY  environment was used to search for events similar to those reported in , i.e., a search was made for events in which two alpha particle decays were detected in the focal plane detector within 30 ms and with positions differing by $`<`$1.5 mm. The energies of the alpha particles had to be greater than 10 MeV and they had to be unrelated to beam events (no PPAC signal). No such $`\alpha \alpha `$ correlations were found.

A second, less restrictive search was made for EVRs ($`>`$20 MeV with a PPAC signal) followed by alpha decays (8-14 MeV in the focal plane Si-strip detector, no PPAC signal) correlated in position ($`\pm `$2mm, same strip) and time (within 10 sec). For this search, one detector strip on the low-B$`\rho `$ edge of the detector and three strips on the high-B$`\rho `$ edge of the detector were excluded because they detected relatively high rates of scattered beam particles with trajectories bypassing the PPAC. Two potential EVR-$`\alpha `$-$`\alpha `$ chains were identified. Based on the singles rates for alpha-like events and EVRs, the expected number of random EVR-$`\alpha `$-$`\alpha `$ chains is $``$4. Both of the observed EVR-$`\alpha `$-$`\alpha `$ chains had large differences in the vertical positions for the parent and daughter alpha particles, $`|`$$`\mathrm{\Delta }`$p$`|`$$``$ 0.78mm =3.5$`\sigma `$. Thus, we conclude that there are no valid EVR-$`\alpha `$-$`\alpha `$ correlations in the data set from this experiment.

One must also consider the possibility that SHEs decay by spontaneous fission (SF). Spontaneous fission events in which one fragment was detected in the focal plane detector (E $`>`$90 MeV, no PPAC signal) can be confused with scattered 86Kr beam particles not vetoed by the PPAC signal. Therefore, we excluded, from the analysis, three strips on the low-B$`\rho `$ edge of the detector and four strips on the high-B$`\rho `$ edge of the detector to discriminate against these scattered beam particles. We observed no single fission fragment signals during the run using these gating conditions, i.e., no EVR-SF events.

There were no correlation chains containing at least EVR-$`\alpha `$-$`\alpha `$ or EVR-SF with additional full-energy alpha particles (8-14 MeV with no PPAC signal) or escape alpha particles (with energy deposited in the focal plane detector $`>`$0.5 MeV and no PPAC signal).

The implantation depth in the Si-strip detector for the 293118 recoils (E $``$73 MeV after passing through the PPAC) was extrapolated from heavy ion ranges calculated with SRIM2000 , and is estimated to be 7 $`\mu `$m. From this depth, the efficiency for detecting full energy for isotropically emitted 8-14 MeV alpha particles is 55%. The expected decay sequence  following implantation of a 293118 EVR consists of 6 $`\alpha `$-particles emitted sequentially within the first 10 seconds after implantation. Using the 55% $`\alpha `$-particle efficiency, $`\epsilon ,`$ together with a binomial series for the probability P, of observing at least n members of an N-member chain,

$$P=\underset{a=n}{\overset{N}{}}\frac{N!}{a!(Na)!}\epsilon ^a(1\epsilon )^{Na}$$
(1)
the probability for detecting at least two full-energy $`\alpha `$-particles from a sequence of six is 93%. Such a binomial treatment can be used to calculate the efficiency for detection of other postulated decay chains. Assuming a 100% event chain detection efficency results in “one event” upper limit cross sections of 0.9 pb and 0.6 pb for B$`\rho `$ settings of 2.00 and 2.12 $`Tm`$, respectively. These cross section limits assume detection of one event, whereas none were observed, and a constant production cross section throughout the target thickness.

## IV Discussion

### A Cross Section Calculation

The standard cross section calculation assumes a constant cross section, $`\sigma _{const}`$, for all beam energies within the target. The number of events observed, nobs, is given by

$$n_{obs}=\varphi tN_t\sigma _{const}\epsilon $$
(2)
where $`\varphi `$t is the integrated beam current, Nt is the areal density of target atoms, and $`\epsilon `$ is the experimental efficiency. This formalism was used in \[4-6\] for the cross section limits quoted in those works and used above in Table I and related discussion. However, in the case of the 208Pb(86Kr,n)293118 reaction, the excitation function is expected to be narrow and the energy loss of the beam in traversing the target material is relatively large ($`\mathrm{\Delta }`$E $``$ 8 MeV) , so the assumption of a constant cross section for all beam energies within the target does not hold. For the purpose of an improved determination of cross section limits in this experiment, a Gaussian excitation function, $`\sigma `$(E), with a full-width at half-maximum (FWHM) of 5 MeV in the lab frame has been assumed:

$$\sigma (E)=\sigma _c\mathrm{exp}((Ec)^2/2s^2)$$
(3)
where $`\sigma _c`$ is the cross section at c, the centroid energy, E is the beam energy at the corresponding target depth, and s is the standard deviation of the Gaussian (s = 2.12 MeV for a 5-MeV FWHM). This results in the differential equation

$$n_{obs}=\varphi t\frac{N_t(E)}{E}\sigma (E)\epsilon (E)E$$
(4)
where the separator efficiency, $`\epsilon `$(E), depends on the beam energy (depth in target). Since the areal number density of target atoms and the dE/dx of the beam are nearly constant throughout the target, the areal number density of target atoms within a differential target thickness element, $`\frac{N_t(E)}{E}`$, is constant and equal to Nt/$`\mathrm{\Delta }`$E, where $`\mathrm{\Delta }`$E is 8.0 MeV for the 86Kr beam in the 208Pb targets. Integrating over the energy range in the target, and solving for $`\sigma _c`$ results in

$$\sigma _c=\frac{n_{obs}}{\left[\varphi t\frac{N_t}{\mathrm{\Delta }E}\underset{E_i}{\overset{E_f}{}}\epsilon (E)\mathrm{exp}\left[\frac{\left(Ec\right)^2}{2s^2}\right]𝑑E\right]}$$
(5)
where Ei and Ef are the beam energies at the upstream and downstream limits of the target. For our experiment, assuming the centroid of the excitation function corresponds to the center of the target and that the efficiency is constant throughout the target, $`\sigma _c`$/ $`\sigma _{const}`$ = 1.6, and thus the cross section limits presented below are larger than those calculated in the traditional way by this factor.

### B BGS Efficiency Simulation

The efficiency of the BGS is limited by the initial position, energy and angular distributions of recoils exiting the target, and by transmission of these recoils through the BGS under the influence of the magnetic fields, and energy loss, multiple scattering and charge exchange in the He fill gas. All of these effects, together with the effects of the estimated angular and energy distributions of the 86Kr beam entering the BGS were calculated with a Monte Carlo simulation. In this simulation, the initial 86Kr beam energies and directions were chosen from an assumed Gaussian energy distribution (with a centroid of 457 MeV - chosen to put c at the center of the target, and a 0.3% FWHM - a typical beam energy width from the 88-Inch Cyclotron) and Gaussian angular (FWHM=0.9o\- typical for the beamline leading to the BGS) distributions. The beam energy was corrected for energy loss in the carbon entrance window and target backings. Points were randomly chosen from the assumed Gaussian excitation function (c=449 MeV, s=2.12 MeV), and if they were within the energy range subtended by the target (thickness=0.47 mg/cm2, dE/dx=17 MeV/(mg/cm2)), the depth of interaction in the target was calculated, and a simulation of the trajectory of an EVR was initiated. The initial energy and angle of the EVR were corrected for the effect of isotropic evaporation of a single neutron. Energy loss and angular scattering in the remaining target material was calculated for each EVR using SRIM2000. After exiting the target, the trajectories through the BGS were simulated, including the effects of the magnetic fields, charge exchange in the gas, scattering in the gas, and energy loss in the gas. By comparing the number of EVRs reaching the focal plane detector in the simulation with the initial number of 86Kr beam particles, the effects of the fraction of the excitation function contained in the target and the BGS efficiency as a function of target depth were accounted for. The “average” separator transport efficiency for the EVRs produced in this reaction was calculated to be 79%.

### C Improved 293118 Cross Section Upper Limits

Since neither the centroid of the element 118 excitation function nor the magnetic rigidity of the Z = 118 EVRs are known, numerical simulations of the BGS efficiency were run using several different choices for the excitation function centroid energy and average EVR magnetic rigidity. These simulations gave a set of experimental sensitivities as a function of the assumed excitation function centroid, and of the assumed magnetic rigidity. The results from two bombardments, the first with 1.1 x 1018 86Kr ions at a BGS magnetic rigidity (B$`\rho `$ ) of 2.00 $`Tm`$ and the second with 1.5 x 1018 Kr ions and B$`\rho `$ = 2.12 $`Tm`$ were combined. The one-event cross section limits (assuming observation of one element 118 chain where zero events were observed) as a function of assumed $`\sigma _c`$ and B$`\rho `$ are presented in Fig. 2. The cross section limits reached were as low as 1.1 pb, and a limit of less than 4.5 pb was reached for compound nucleus excitation energies from 10.0-16.8 MeV (444.5 $`<`$Elab(MeV) $`<`$454.0), covering magnetic rigidities for the recoiling products from 1.94-2.18 $`Tm`$.

## V Summary

Several experiments have led to one-event cross section upper limits near 0.6 pb for the 449-MeV 208Pb(86Kr,n)293118 reaction (table 1). In fig. 1, we compare this 0.6 pb limit with various theoretical predictions  for the production of 293118 in the reaction of 449-MeV 86Kr with 208Pb. This limit is below some of the predicted values. Combination of sets of upper limit cross sections from Table 1 results in an upper limit cross section of $``$0.2 pb, placing more stringent limitations on the validity of some of the models. The most pessimistic estimate  of the evaporation residue cross section assumes the probability of forming a true compound nucleus, after capture of the projectile, decreases approximately four orders of magnitude in going from 70Zn + 208Pb to 86Kr + 208Pb. This decrease may counteract any fusion enhancement due to a lowering of the Coulomb barrier relative to the energy of the fused system in the latter reaction. Observation of the production of element 118 in the 208Pb(86Kr,n) reaction will require sensitivity to cross sections smaller than $``$ 0.2 pb.

## VI Acknowlegments

We gratefully acknowledge the operations staff of the 88-Inch Cyclotron and its ion source person D. Wutte for providing intense, steady beams of 86Kr. We thank L.W. Phair for his help in the re-analysis of the 1999 data. We thank Patrick Gamman and Helmut Folger for providing the carbon entrance windows, and the lead targets. Financial support was provided by the Office of High Energy and Nuclear Physics, Nuclear Physics Division of the U.S. Dept. of Energy, under contract DE-AC03-76SF00098 and grant DE-FG06-97ER41026, the Norwegian Research Council (project no. 138507/410) and The Swedish Foundation for International Cooperation in Research and Higher Education.


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# Summary of Results on Hard Probes

## 1 INTRODUCTION

With the new experiments at the RHIC accelerator at BNL, experimental heavy ion physics has truly reached the domain of hard probes. At RHIC energies hard scatterings as observed via jet structures are important in p+p collisions, and it was expected that hard scatterings should also be an important feature of heavy ion collisions at the collider. It has been predicted  that hard scattered partons should suffer energy loss from medium induced gluon radiation in a hot and dense system like the expected quark-gluon plasma phase of strongly interacting matter. This “jet-quenching”, which will lead to a suppression of hadron production at large transverse momenta, is therefore considered a signature of the partonic initial state. (For a review see .)

Two main avenues are being followed to get access to hard scattering processes:

* The study of high $`p_T`$ particle production via singles spectra and their comparison for different centralities and reaction systems (including p+p collisions).
* The study of azimuthal correlations reminiscent of jet topologies.

At the last Quark Matter conference  a suppression of high $`p_T`$ hadron production has already been reported , and the results have been published by the PHENIX and STAR experiments .

At this conference, new results from all four RHIC experiments have been reported. The BRAHMS  and PHOBOS  experiments have presented spectra of hadrons out to relatively high $`p_T`$, while PHENIX and STAR  have shown truly impressive results on hadrons out to very high $`p_T`$. I will try to summarize the highlights in the following.

## 2 SCALING OF PARTICLE PRODUCTION

The role of hard scattering even in understanding the global observables has been discussed in a number of papers , where it has been suggested that, in studying the centrality dependence of the charged particle pseudorapidity density $`dN_{ch}/d\eta `$, one might extract information on the relative contribution from hard scatterings. In particular, a parameterization as a function of the number of participants and the number of collisions has been proposed:

$$\frac{dN_{ch}}{d\eta }=AN_{part}+BN_{coll},$$
(1)
where the necessity of a term proportional to the number of collisions to explain the experimental data was taken as a hint for hard scattering production. In this context, the investigation of the scaling properties of particle production as presented by the PHOBOS experiment  is interesting. PHOBOS reported that the total charged multiplicity scales in good approximation with the number of participants and no additional term proportional to the number of collisions is necessary. The produced particles are however distributed differently in rapidity for varying centrality. This possibly implies that the observed stronger variation of $`dN_{ch}/d\eta `$ with centrality may be due to a measurement in a limited phase space region combined with a redistribution of particles in phase space. In light of these observations, the interpretation of the parameterization (1) as related to hard scattering appears to be premature.

## 3 PRODUCTION OF HIGH $`𝐏_𝐓`$ INCLUSIVE HADRONS

Momentum spectra of hadrons have been reported by all four RHIC experiments. Qualitatively, the suppression reported from the measurements at $`\sqrt{s_{NN}}=130\mathrm{GeV}`$ has also been found at $`\sqrt{s_{NN}}=200\mathrm{GeV}`$. Charged hadrons have been measured out to $`p_T=9\mathrm{GeV}/c`$ by PHENIX  and to $`p_T=11\mathrm{GeV}/c`$ by STAR . Identified hadrons at very high $`p_T`$, which do not suffer from uncertainties due to the unknown flavour composition, have only been presented by the PHENIX experiment , which has measured neutral pion spectra out to $`p_T=10\mathrm{GeV}/c`$.

To quantitatively judge the measured hadron yield in central Au+Au collisions one tries to compare it to the expectations from p+p collisions, which must be appropriately scaled to the larger systems. As hard scatterings have a very small cross section and are expected to be incoherent, it is reasonable to assume that the multiplicity should scale with the number of binary nucleon-nucleon collisions. In fact, the scaling of high $`p_T`$ hadron production in p+A collisions at somewhat lower energies has been shown to be stronger than with the number of collisions (“Cronin-effect”) . A qualitatively similar enhancement compared to p+p collisions was found in central Pb+Pb collisions at 17.3 $`A`$GeV for neutral pion production by the WA98 experiment . In the light of this known enhancement at lower energies, the suppression observed at RHIC is even more striking.

It has become customary to illustrate the suppression by using the so-called nuclear modification factor:

$$R_{AA}(p_T)\frac{d^2N^{A+A}/dp_Td\eta }{N_{coll}d^2N^{N+N}/dp_Td\eta }.$$
(2)
In addition to the measurement of the hadron spectrum in heavy ion collisions this requires the knowledge of

1. the number of binary collisions and
2. the spectrum in nucleon-nucleon collisions (or p+p collisions) at the same energy.

(1) is usually obtained by calculating the nuclear overlap in a Glauber-like approach. The systematic errors involved are among others related to uncertainties in the nucleon-nucleon cross section, the nuclear density profile and the trigger bias in the heavy ion measurement. While for peripheral collisions these do result in considerable uncertainties, the systematic error of the number of binary collisions $`N_{coll}`$ in central collisions is estimated to be at most $`10\%`$. As a nucleon-nucleon spectrum (2) up to now data from earlier experiments at different energies were extrapolated to the RHIC conditions. At $`\sqrt{s_{NN}}=200\mathrm{GeV}`$ charged hadron spectra from UA1  in $`\overline{\mathrm{p}}+\mathrm{p}`$-collisions are available up to $`p_T=6\mathrm{GeV}/c`$. The small momentum range and the possibly different systematic errors due to the measurement in a different experiment do however limit the usefulness of these data.

In this situation it is extremely important that PHENIX has measured the neutral pion spectra in p+p collisions at the same energy in the same apparatus . This reduces the systematic uncertainties of the comparison (i.e. in $`R_{AA}`$). Together with the fact that the neutral pions are the only identified hadrons at high $`p_T`$ this makes their measurement superior for the study of hadron suppression compared to the charged hadrons.

The left hand side of Fig. 1 shows neutral pion spectra from p+p collisions. They agree relatively well with estimates from pQCD calculations . For comparison a parameterization based on the UA1 data is also shown, which agrees with the neutral pions at low $`p_T`$ but starts to deviate for $`p_T>6\mathrm{GeV}/c`$. The right hand side of Fig. 1 shows pion spectra in minimum bias Au+Au collisions. In the PHENIX experiment charged pions can be identified by time-of-flight at low momenta. They compare nicely with the neutral pions, which extend out to much higher momenta. In addition, at very high $`p_T`$ there are first attempts to identify charged pions in the RICH – the (scaled) spectra show also nice agreement in shape with the neutral pions.

Fig. 2 (left) shows the nuclear modification factor (see equation 2) for the $`10\%`$ most central collisions of Au+Au at $`\sqrt{s_{NN}}=200\mathrm{GeV}`$ as presented by the PHENIX experiment. $`R_{AA}`$ is well below one for all of the covered $`p_T`$ range, decreasing from $`0.4`$ at $`p_T=12\mathrm{GeV}/c`$ to less than 0.2 for $`p_T>6\mathrm{GeV}/c`$. The values are consistent with the results published for $`\sqrt{s_{NN}}=130\mathrm{GeV}`$  for a much smaller $`p_T`$ range.

It is not surprising that $`R_{AA}<1`$ at low $`p_T`$, as one would rather expect a scaling with the number of participants for soft particle production. A scaling of the yield with the number of participants would however lead to a value of $`R_{AA}0.17`$ for this centrality selection. This limit is not reached for the lowest momenta covered ($`p_T1\mathrm{GeV}/c`$), which is most likely due to the broadening of the spectra in Au+Au compared to p+p, which will increase the yield at finite $`p_T`$ more strongly than the total multiplicity. At SPS energies it was observed  that $`R_{AA}`$ was increasing with $`p_T`$ reaching a value of 1 already at $`p_T2\mathrm{GeV}/c`$ – this increase is most likely due to a combined influence of increasing importance of hard scattering at higher $`p_T`$ with possible initial state multiple scattering and other momentum broadening effects like collective transverse flow. The new results at RHIC, however, show a continuous decrease of $`R_{AA}`$ for higher $`p_T`$. This result is not explained by theoretical calculations which are shown in Fig. 2 for comparison . Calculations without energy loss fail completely, the calculations with energy loss are closer in magnitude to the experimental results, but can so far not explain the $`p_T`$ dependence.

It has been argued by the PHOBOS collaboration  that the particle yield even at high $`p_T`$ is compatible with participant scaling for Au+Au collisions with $`N_{part}>65`$. This scaling is in general not seen in peripheral Au+Au data and for the transition from p+p to Au+Au, a closer look at data from all experiments also shows that even the approximate scaling is only valid in limited $`p_T`$ regions. So while the participant scaling of the total multiplicities may well have a fundamental origin, this is not at all clear for the same (approximate) scaling at a fixed $`p_T`$. Still it is interesting to note that $`R_{AA}`$ from neutral pions as shown in Fig. 2 is compatible with participant scaling for the highest $`p_T`$.

It has been discussed whether the emission of high $`p_T`$ hadrons is dominated by the surface of the reaction zone, and thus $`R_{AA}`$ would be determined by the surface-to-volume ratio. This in turn contains further uncertainties from the surface thickness assumed. To obtain a realistic numerical value of the scaling in this scenario one would have to take into account the transverse edge of the reaction zone and the varying density of the nuclear overlap. No precise value is available at present. Besides, it is noteworthy that even at relatively high $`p_T`$ hydrodynamic particle emission might contribute significantly to hadron spectra . For a locally thermalized system, which is the necessary condition for hydrodynamics, a scaling with the number of participants is very natural, so this might apply to the hydrodynamic fraction of the emitted hadrons. At the present moment, however, it is unclear, whether the observed scaling with the number of participants is purely a coincidence, or whether it can be related to a physical mechanism. In any case, even if this scaling holds, it does require a suppression mechanism of hard scattered particles when compared to the expectation from p+p collisions.

Similar analyses have been performed on charged hadron spectra. So far no direct p+p reference measurement is available. PHENIX has scaled the measured neutral pion spectrum in p+p to account for non-pions. The nuclear modification factor as displayed on the right hand side of Fig. 2 is slightly larger than the one for neutral pions, but both are compatible within errors. The other RHIC experiments have used a parameterization of UA1 data as their reference for $`p_T<6\mathrm{GeV}/c`$. The curves included in Fig. 2 show fits extracted from the presented data, the systematic errors, which are not shown, are of similar size as for PHENIX. All results show qualitatively similar features: $`R_{AA}`$ increases at low $`p_T`$, has a maximum around $`p_T=22.5\mathrm{GeV}/c`$ and decreases for higher $`p_T`$. There are considerable differences in the magnitude of the observed suppression for the different experiments, although probably not very significant in view of the systematic errors. For BRAHMS the relatively small value of the number of collisions used in the calculation may lead to an overestimate of $`R_{AA}`$. Part of the discrepancies may be due to the different reference distributions used.

This is in line with the observation, that the collision-normalized ratio of central to peripheral spectra is in much better agreement between PHENIX  and STAR . Such a ratio is one possibility to investigate the centrality dependence of the observed suppression. The ratio central to peripheral has the advantage that no p+p reference is needed, however, it suffers from the larger uncertainty of the estimate of the number of collisions in peripheral reactions. While also in this representation a suppression is observed, the new features of the collisions at RHIC are not as striking here. Similar ratios for SPS energies by the WA98 experiment  show no enhancement, but also a suppression, which is qualitatively similar, though weaker than at RHIC.

The centrality dependence of the neutral pion suppression has been investigated by PHENIX , there is a gradual transition from no suppression in peripheral collision to a strong suppression in very central without any indication of threshold effects. The centrality dependence of the charged hadron spectra has been studied in detail by STAR  and PHENIX . A significant change in shape is observed when going from peripheral to central collisions. This can be best illustrated by looking at the truncated $`p_T`$ as obtained by PHENIX : For $`p_T<2\mathrm{GeV}/c`$ the $`p_T`$ increases with increasing number of participants, just like the $`p_T`$-broadening known from lower energies which may be attributed to multiple scattering or collective flow, which would be expected to get more important for larger systems. For $`p_T>2\mathrm{GeV}/c`$ the $`p_T`$ decreases with increasing number of participants.

## 4 FLAVOR COMPOSITION AT HIGH $`𝐏_𝐓`$

Differences in the suppression for charged hadrons and neutral pions may be partially due to a flavor dependence of the suppression mechanism. Moreover, if the particle production at high $`p_T`$ is actually due to incoherent hard scattering processes, the flavor composition of hadronic spectra should approach values known from p+p collisions and should be calculable in pQCD. PHENIX has extended its previously reported baryon/pion ratios at 130 GeV to measurements at 200 GeV . The same trend is observed: The proton- and antiproton-to-pion ratios increase with increasing $`p_T`$ reaching values close to one at high $`p_T`$ in central collisions, as seen for antiprotons in Fig. 3 on the left side. This is very different from the expectation of much smaller values seen in p+p and also in peripheral Au+Au reactions. Other ratios, which may be calculated for hard processes, have been looked at, like e.g. the antiproton/proton ratio, which is also expected to decrease at high $`p_T`$ for hard scattering production. PHENIX results are compatible with a constant, relatively large value at high $`p_T`$ , while STAR reports an indication of a decrease at the highest $`p_T`$ . But even taking this possible decrease into account, the (anti-)proton/pion ratios indicate a still unexpected behavior in the $`p_T`$ range, where charged hadrons can presently be identified.

The strongest hint of the remaining puzzle comes again from the neutral pion measurement in PHENIX. They have compared the neutral pion yield to the charged hadron yield in minimum bias collisions up to $`p_T=8\mathrm{GeV}/c`$ , and report that even at very high $`p_T`$ pions seem to make up only about $`50\%`$ of the total charged hadron yield. Other hadrons, possibly baryons, need to contribute there in contrast to the expectations from p+p collisions. The right side of Fig. 3 tries to illustrate the current situation. The charged hadron to neutral pion ratio has been estimated from fits to the spectra presented by PHENIX for central collisions. The identified charged hadron to pion ratios have then been used to successively build up this ratio for the total charged hadrons. It can be seen that the total sum of pions, kaons, protons and antiprotons is consistent with the charged hadrons up to intermediate $`p_T`$. At high $`p_T`$ still a considerable non-pionic contribution is apparently needed, and the measurement of identified hadron spectra at these higher $`p_T`$ will be of great importance.

## 5 ELLIPTIC FLOW

A lot of new and improved results on elliptic flow have been presented. A detailed summary is given in , so I will not discuss this in any detail. It should, however, be mentioned that, while azimuthal asymmetries for low and intermediate $`p_T`$ appear to be dominated by hydrodynamical effects, the persistence of a finite elliptic asymmetry $`v_2`$ out to very high $`p_T`$ indicates that modifications of hard scattering production are likely relevant for these analyses. This is nicely demonstrated in Fig. 4, which shows $`v_2`$ as measured by STAR  out to beyond $`p_T=10\mathrm{GeV}/c`$. It will be interesting to see at which momenta the asymmetry disappears, and how much of the $`v_2`$ is actually due to partial jet quenching.

## 6 JET STRUCTURES FROM AZIMUTHAL CORRELATIONS

While the suppression of high $`p_T`$ hadron production as seen in inclusive spectra is certainly established and will yield important constraints on the property of the hot and dense matter created in these collisions, it is even more interesting to investigate jet structures themselves. Analyses searching for jet patterns in azimuthal correlations have been performed by STAR  and PHENIX . Both experiments see small angle correlations of particles relative to high $`p_T`$ hadrons or photons, which in turn originate predominantly from pions. The magnitude and shape of this correlation in Au+Au collisions is very similar to the one in p+p. This is the first observation of jet structures in heavy ion collisions.

Also large angle correlations are seen by both experiments. STAR has performed a detailed analysis of these correlation phenomena . As shown in Fig. 5 they attempt to describe the correlation function in heavy ion collisions by a superposition of a flat background, a component of elliptic flow and the jet correlation as measured in p+p. In peripheral collisions (left side of Fig. 5) both the trigger-jet ($`\mathrm{\Delta }\varphi 0`$) and the counter-jet ($`|\mathrm{\Delta }\varphi |\pi `$) are very similar to the expectations from p+p. In central collisions (right side of Fig. 5), the trigger-jet remains unaltered, but the counter-jet has almost completely disappeared. The existence of the trigger-jet ensures that a hard scattering has really taken place, such that the suppression of the balancing counter-jet is a very direct indication of jet quenching.

STAR has also presented the centrality dependence of the relative strength of the two jet structures compared to p+p. As can be seen in Fig. 6, the strength of the trigger-jet shows even a small increase towards more central collisions, which is surprising and should be further investigated. The counter-jet strength exhibits a gradual decrease with increasing number of participants, qualitatively very similar to the centrality dependence of the high $`p_T`$ neutral pion suppression. This measurements provides a very important step towards understanding jet quenching, more detailed systematic investigation of observed first trends in the data and comparisons to theory are now required.

## 7 SUMMARY

A lot of exciting results on hard probes have been presented at this conference. The high $`p_T`$ hadron suppression in central Au+Au collisions relative to p+p collisions has been established, most notably through the neutral pion measurements from PHENIX. Detailed theoretical calculations are now eagerly awaited. Elliptic azimuthal asymmetries persist at very high $`p_T`$, which may be related to partial jet quenching. Correlation structures due to jets have been observed by STAR and PHENIX. The most important highlight of the conference is the suppression of the counter-jet in triggered central events as seen by STAR, which provides the most direct observation of jet quenching to date. The most urgent open question concerns the explanation of the large non-pionic contribution to hadron spectra at very high $`p_T`$ as reported by PHENIX.

I would like to sincerely thank all speakers on high $`p_T`$ and numerous other colleagues from the RHIC and SPS experiments for the help and support in preparing my talk and these proceedings.


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# Multiple flux jumps and irreversible behavior of thin Al superconducting rings

## I Introduction

Recently, Pedersen et al. Pedersen  observed jumps in the magnetization of superconducting rings which corresponds to changes of the vorticity larger than unity. This is in contrast to the behavior of superconducting disks where only changes in the value of the vorticity of unit size were observed GeimN . In some respect the observed behavior in rings is similar to vortex avalanches which were observed in superconductors with strong bulk pinning Zieve ; Behina  or to jumps in the magnetization when several vortices (in the form of a chain) enter in a superconducting film of width comparable to the coherence length Bolech ; Vodolazov . The occurrence of such jumps in a defect free superconducting ring originates from the fact that several metastable states with different vorticity $`L`$ are possible for a given magnetic field. However the existence of such multiple stable states is not a sufficient condition to explain changes in the vorticity larger than unity (e.g. they also exist in the case of superconducting disks). An additional important requirement is to find the stability condition and finally the state to which the system relaxes to. This requires the study of the transition process from one state to another, i.e. it requires the analysing the time-dependent process.

The stability condition was studied numerically in Ref. Fink  for the case of a hollow cylinder, and in a number of works (see for example Ref. Baelus ; Berger  and references therein) for superconducting disks and rings by using the static Ginzburg-Landau (GL) equations. Unfortunately no analytical results were presented due to the rather general character of the studied systems in the above works.

Recently, we studied the transition process our1  using the time-dependent Ginzburg-Landau equations. It was shown that transitions between different metastable states in a mesoscopic superconducting ring are governed by the ratio between the time relaxation of the phase of the order parameter $`\tau _\varphi `$ (which is inversely proportional to the Josephson frequency) and the time relaxation of the absolute value of the order parameter $`\tau _{|\psi |}`$. We found that if the ratio $`\tau _{|\psi |}/\tau _\varphi `$ is sufficiently large the system will always transit from a metastable state to the ground state. This leads to an avalanche-type variation of $`L`$ when the vorticity of the metastable state differs appreciably from the vorticity of the ground state. In contrast to the case of a superconducting film, in a ring the ’vortex’ entry occurs through a single point and the vorticity increases one by one during the transition. In low-temperature superconductors like In, Al, Sn the ratio $`\tau _{|\psi |}/\tau _\varphi `$ is very large for temperatures far below the critical temperature $`T_c`$ and hence, if such systems are driven far out of equilibrium they will always relax to the ground state.

In this work we investigate the conditions under which a state with a given vorticity becomes unstable in a finite width ring and we find how the supeconducting order parameter in the ring changes with increasing applied magnetic field. We are able to find an analytical expression for the dependence of the order parameter on applied magnetic field, and hence for the upper critical field at which superconductivity vanishes in such a sample. We provide a direct comparison between the theoretical and experimental results on aluminium rings. Our theoretical calculations are based on a numerical solution of the time-dependent Ginzburg-Landau equations.

The paper is organized as following. In section II the theoretical formalism is presented and the two-dimensional time-dependent GL equations are solved. In Section III the experimental results are presented and compared with our theory. In Section IV we present our conclusions and our main results.

## II Theory

We consider sufficient narrow rings such that we can neglect the screening effects. This is allowed when the width of the ring $`w`$ is less than $`\mathrm{𝑚𝑎𝑥}\lambda ,\lambda ^2/d`$, where $`\lambda `$ is the London penetration length and $`d`$ is the thickness of the ring. In order to study the response of such a ring on the applied magnetic field we use the time-dependent Ginzburg-Landau equations

$`u\left({\displaystyle \frac{\psi }{t}}+i\phi \psi \right)`$ $`=`$ $`(\mathrm{i}𝐀)^2\psi +(1|\psi |^2)\psi ,`$ (1a)
$`\mathrm{\Delta }\phi `$ $`=`$ $`\mathrm{div}\left(\mathrm{Im}(\psi ^{}(\mathrm{i}𝐀)\psi )\right),`$ (1b)
where all the physical quantities (order parameter $`\psi =|\psi |e^{i\varphi }`$, vector potential $`A`$ and electrostatical potential $`\phi `$) are measured in dimensionless units: the vector potential $`A`$ is scaled in units $`\mathrm{\Phi }_0/(2\pi \xi )`$ (where $`\mathrm{\Phi }_0`$ is the quantum of magnetic flux), and the coordinates are in units of the coherence length $`\xi (T)`$. In these units the magnetic field is scaled by $`H_{c2}`$ and the current density, $`j`$, by $`j_0=c\mathrm{\Phi }_0/8\pi ^2\lambda ^2\xi `$. Time is scaled in units of the Ginzburg-Landau relaxation time $`\tau _{GL}=4\pi \sigma _n\lambda ^2/c^2`$, the electrostatic potential, $`\phi `$, is in units of $`c\mathrm{\Phi }_0/8\pi ^2\xi \lambda \sigma _n`$ ($`\sigma _n`$ is the normal-state conductivity). Here the time-derivative is explicitly included which allows us to determine the moment at which the state with given vorticity $`L`$ becomes unstable. It is essential to include the electrostatic potential (which is responsible for the appearance of the Josephson time or frequency) in order to take into account the multi-vortex jumps. In some previous studies (see for example Refs. McCumber ; Tarlie ) $`\phi =0`$ was assumed and as a consequence only transitions with unit vorticity jumps, i.e. $`\mathrm{\Delta }L=1`$, are possible in the ring our1 . The coefficient $`u=48`$ was chosen such that after the transition the system is in the thermodynamically equilibrium state our1 . We assume that the width ($`w`$) of the ring is less than two coherence length $`\xi `$, because: i) all experimental results presented here were performed for such type of samples; and ii) only in this case it is possible to obtain simple analytical expressions. For instance, the dependence of the order parameter on the applied magnetic field and the upper critical field $`H_{max}`$.

For $`w2\xi `$ the order parameter is practically independent of the radial coordinate. This is demonstrated in Fig. 1 where the dependence of the order parameter in the middle of the ring is compared with its value at the inner and outer boundary of the ring, i.e. $`r=R\pm w/2`$ ($`R`$ is the mean radii of the ring), for two different rings. Notice that these two numerical examples corresponds already to relative thick mesoscopic rings, i.e. $`R/w12`$. For the field $`H_{max}`$ we are able to fit our numerical results to the expression

$$H_{max}=3.67\frac{\mathrm{\Phi }_0}{2\pi \xi w}.$$
(2)
For rings with $`w2\xi `$ and $`w/R<1`$ this analytical expression is within $`2\%`$ of the numerical results. It is interesting to note that $`H_{max}`$ does not depend on the radii of the ring. But the value of the vorticity of the system depends on $`R`$. For example, for $`R=5.5\xi (16.5\xi )`$ $`L=55(501)`$ for $`w=\xi `$ at $`H=H_{max}`$.

Note that Eq. (2) has the same dependence on the superconducting parameters as in the case of a thin plate with thickness $`d<\sqrt{5}\lambda `$ placed in a parallel magnetic field Ginzburg ; Douglass . Even the numerical coefficient is quite close, i.e. for a thin plate it is equal to $`2\sqrt{3}3.46`$. Furthermore, we found that the transition to the normal state of our rings at the critical field $`H_{max}`$ is of second order as is also the case for a thin plate. A possible reason for this close similarity is that for a thin plate with thickness $`d<\sqrt{5}\lambda `$ the screening effects are also very small. In the calculations of Refs. Ginzburg ; Douglass  an averaged value for the order parameter was used independent of the coordinate. Note that this is similar to our $`|\psi |`$ which is practically independent on the radial coordinate (see Fig. 1).

The absolute value of the order parameter (in the middle of the ring) is, too a high accuracy, given by the expression

$$|\psi |^2=1(H/H_{max})^2p(L,H)^2,$$
(3)
with $`p(L,H)=L/RHR/2`$, where the vorticity $`L`$ depends on the history of the system. This result is similar to the one obtained in Refs. Ginzburg ; Douglass  with the exception of the last term in Eq. (3) which appears due to the closed geometry of the ring and hence leads to a nonzero $`L`$.

All the above results were obtained for a ring which is in the ground state at any value of the magnetic field. However such a system can exhibit several metastable states at a given magnetic field, and consequently this may lead to hysteretic behavior when one sweeps the magnetic field up and down. Furthermore, with changing field the vorticity may jump with $`\mathrm{\Delta }L>1`$. An important question which arises is the condition of stability of the state with given vorticity. This question was studied earlier for one-dimensional rings Tarlie ; our2 , i.e. rings with zero width. It turns out that the system transits to a state with another vorticity when the value of the gauge-invariant momentum $`𝐩=\varphi 𝐀`$ reaches the critical value

$$p_c=\frac{1}{\sqrt{3}}\sqrt{1+\frac{1}{2R^2}}.$$
(4)
At this condition it is easy to find the value of the field for the first ’vortex’ entry

$$H_{en}/H_{c2}=2p_c/R=\frac{2}{\sqrt{3}R}\sqrt{1+\frac{1}{2R^2}}.$$
(5)
We will now generalize the results of Refs. Tarlie ; our2  to the case of finite width rings with $`w2\xi `$. First we will neglect the dependence of $`\psi `$ on the radial coordinate in which case the GL equations reduce to one-dimensional expressions. But in order to include the suppression of the order parameter by an external field for a finite width ring we add the term $`(H/H_{max})^2\psi `$ to the RHS of Eq. (1a), where $`H_{max}`$ is given by Eq. (2). Using the stability analysis of the linearized Ginzburg-Landau equations near a specific metastable state as presented in Ref. our2  we obtain the modified critical momentum

$$p_c=\frac{1}{\sqrt{3}}\sqrt{1\left(\frac{H}{H_{max}}\right)^2+\frac{1}{2R^2}}.$$
(6)
Note that now $`p_c`$ decreases with increasing magnetic field. This automatically leads to a decreasing value of the jump in the vorticity $`\mathrm{\Delta }L`$ at high magnetic field, because in Ref. our1  it was shown that

$$\mathrm{\Delta }L_{max}=\mathrm{Nint}(p_cR),$$
(7)
where $`\mathrm{Nint}(x)`$ returns the nearest integer to the argument.

In order to check the validity of Eq. (6) we performed a numerical simulation of the two-dimensional Ginzburg-Landau equations, Eqs. (1a,b), for a ring with $`R=5.5\xi `$ and $`w=1.5\xi `$ (for these parameters the theoretical findings fit the experimental results - see section below). In Fig. 2 the magnetization, the order parameter and the gauge-invariant momentum $`p`$ are shown as function of the applied magnetic field. The magnetic field was cycled up and down from $`H<H_{max}`$ to $`H>H_{max}`$. The condition (6) leads to an hysteresis of $`M(H)`$ and to a changing value of the jump in the vorticity in accordance with the change in $`p_c`$. The main difference between our theoretical prediction (6) and the results of our numerical calculations appears at fields close to $`H_{max}`$. Apparently it is connected with the fact that for the considered ring the distribution of the order parameter along the width of the ring is appreciably nonuniform at $`HH_{max}`$ and as a consequence the one-dimensional model breaks down (see Fig. 1).

Finally, we also considered the same ring with a defect. The effect of the defect was modelled by introducing in the RHS of Eq. (1a) the term $`\rho (s)\psi `$ ($`s`$ is the arc-coordinate) where $`\rho (s)=1`$ inside the defect region with size $`\xi `$ and $`\rho (s)=0`$ outside. This leads to the results shown in Fig. 3 for $`M(H)`$, $`|\psi |(H)`$ and $`p(H)`$. Due to the presence of the defect, $`p_c`$ differs from Eq. (6) already at low magnetic field ($`p_c(H=0)0.33`$ at given ”strength” of the defect) and as a result only jumps with $`\mathrm{\Delta }L=1`$ are possible in such a ring. In this case the $`p_c`$ and $`|\psi |`$ also depend on the applied magnetic field with practically the same functional dependence on $`H`$ as Eq. (6).

## III Comparison with experiment

The measurements were performed on individual Al superconducting rings by using ballistic Hall micromagnetometry Geim1 ; Geim2 . The techniques employs small Hall probes microfabricated from a high-mobility two-dimensional electron gas (2DEG). The rings - having radii $`R1\mu m`$ and width $`w`$ ranging from $`0.1`$ to $`0.3\mu m`$ \- were placed directly on top of the microfabricated Hall crosses, which had approximately the same width $`b`$ of about $`2\mu m`$ (see micrograph in Fig. 4 for a ring with an artificial defect). These experimental structures were prepared by multi-stage electron-beam lithography with the accuracy of alignment between the stages better than $`100nm`$. The rings studied in this work were thermally evaporated and exhibited a superconducting transition at about 1.25K. The superconducting coherence length was $`\xi (T=0)0.18\mu m`$. The latter was calculated from the electron mean free path $`l25nm`$ of macroscopic Al films evaporated simultaneously with the Al rings. The Hall response, $`R_{xy}`$, of a ballistic cross is given by the amount of magnetic flux $`B𝑑s`$ through the central square area $`b\times b`$ of the cross Geim1 ; Peeters . For simplicity, one can view the ballistic magnetometer as an analogue of a micro-SQUID, which would have a square pick-up loop of size $`b`$ and superconducting rings placed in its centre. We present our experimental data in terms of the area magnetization $`M=<B>H`$ which is the difference between the applied field $`H`$ and the measured field $`<B>R_{xy}`$. Previously, we have studied individual superconducting and ferromagnetic disks and found excellent agreement with the above formula Geim2 ; Novoselov . For further details about the technique, we refer to our earlier work Geim1 ; Geim2 ; Peeters .

Rings with and without an artificial defect were studied. Let us consider first the ring without artificial defect. In Fig. 5(a) the full magnetization loop of such a ring with parameters $`R=1.0\pm 0.1\mu m`$ and $`w=0.25\pm 0.05\mu m`$ is shown. In Fig. 6 (solid curve) the low field part of the virgin curve is presented. From the virgin trace $`M(H)`$ we can find the magnetic field for the first vortex entry, $`H_{en}`$, and hence we estimate $`\xi 0.19\mu m`$ at the given temperature ($`T0.4K`$) using Eq. (5) (this value of $`\xi `$ is in agreement with the above experimental value $`\xi (0)0.18\mu m`$ obtained from the mean free path). Furthermore, we know from Fig. 5(a) that the vorticity changes with $`\mathrm{\Delta }L=3`$ for $`H0`$. This agrees with the fact that the radii of the ring is larger than $`4.6\xi `$ (see Eq. (7)). Another important information which may be extracted from the virgin curve is that at the first vortex entry the magnetization drops considerably but it does not change sign. If we recall that at every vortex entry $`p`$ decreases on $`1/R`$ (and hence the current density $`j`$ and $`M[𝐣\times 𝐫]𝑑V`$ also changes proportionally) we can conclude that the radii of our ring should be in the range $`5.5\xi R6.5\xi `$. This agrees with the experimental value $`R/\xi 5.3\pm 0.5`$.

If we take the above value for $`\xi `$ and $`w1.5\xi `$ we obtain the maximum field of $`H_{max}223`$ G. This value is slightly smaller than the value obtained from Figs. 2 and 3 $`H_{max}240G`$ which we attribute to the large coordinate step which we used in our numerical calculations of Eq. 1(a,b). The value is also larger than the experimental value $`H_{max}185`$ G. This disagreement between theory and experiment is most likely connected to the semi-quantitative applicability of the Ginzburg-Landau equations in the considered temperature range. The range of applicability of the Ginzburg-Landau equations (even stationary ones) for this specific superconductor is very narrow. Nevertheless based on previous comparison between experiments and theory for mesoscopic superconducting disks Deo1 ; Deo2  it was found that the GL equations provided a rather good description of the superconducting state even deep inside the $`(H,T)`$ phase diagram.

Figs. 2(a) and 5(a) are qualitatively very similar. For example our theory describes: i) the hysteresis; ii) the non-unity of the vorticity jumps, i.e. $`\mathrm{\Delta }L=3`$ in the low magnetic field region, $`\mathrm{\Delta }L=2`$ in the intermediate H-region, and $`\mathrm{\Delta }H=1`$ near $`H_{max}`$. Theoretically (experimentally) we found 6(5), 13(21), 22(18) jumps with respectively $`\mathrm{\Delta }L=3`$, $`2`$, $`1`$; and iii) the non symmetric magnetization near $`\pm H_{max}`$ for magnetic field sweep up and down.

In the ring with approximately the same mean radii and width but containing an intentionally introduced artificial defect, jumps with $`\mathrm{\Delta }L=1`$ are mostly observed (see Fig. 5(b)). The reason is that an artificial defect considerably decreases the critical value $`p_c`$ (and hence the field $`H_{en}`$ \- see dotted curve in Fig. 6). From Figs. 2(c), 3(c) it is clear that the maximum value $`p_c^{id}0.54`$ for a ring without defect and $`p_c^d0.35`$ for a ring with a defect. The ratio $`p_c^d/p_c^{id}0.65`$ is close to the ratio of the field of first vortex entry $`H_{en}^d/H_{en}^{id}0.67`$ obtained from experiment (see Fig. 6). From Fig. 2(c) it is easy to see that for a ring without a defect at $`p0.35`$ there are only jumps with $`\mathrm{\Delta }L=1`$. But if we slightly increase $`p`$ then jumps with $`\mathrm{\Delta }L=2`$ can appear in the system. So we can conclude that $`p=0.35`$ is close to the border value which separates regimes with jumps in vorticity of $`\mathrm{\Delta }L=1`$ and $`\mathrm{\Delta }L=2`$. From our experimental data it follows that the maximum value of $`p_c`$ is very close to this border. Thermal fluctuations may influence the value of $`\mathrm{\Delta }L`$, in particular for a $`p_c`$ value close to this border value. This is probably the reason why in the experiment (Fig. 5(b)) occasional jumps with $`\mathrm{\Delta }L=2`$ are observed which are absent in our simulation (Fig. 3(a)).

## IV Conclusion

We studied multiple flux jumps and irreversible behavior of the magnetization of thin mesoscopic Al superconducting rings. We have shown experimentally and theoretically that at low magnetic fields and for rings with sufficiently large radii the vorticity may change by values larger than unity. With increasing magnetic field the order parameter gradually decreases and thus leads to a decrease of the size of the jumps in the vorticity. For rings with width less than $`2\xi `$ analytical expressions were obtained for the dependence of the order parameter on the applied magnetic field. We have found that a state with a given vorticity becomes unstable when the value of the gauge-invariant momentum reaches a critical value $`p_c`$ which decreases with increasing magnetic field. This is responsible for the fact that $`\mathrm{\Delta }L`$ decreases with increasing $`H`$. The introduction of an artificial defect in the ring leads to a decrease of $`p_c`$ in comparison to the case of a ring without a defect and also results in a decrease of $`\mathrm{\Delta }L`$.

###### Acknowledgements.

This work was supported by the Flemish Science Foundation (FWO-Vl), the ”Onderzoeksraad van de Universiteit Antwerpen”, the ”Interuniversity Poles of Attraction Program - Belgian State, Prime Minister’s Office - Federal Office for Scientific, Technical and Cultural Affairs”, EPSRC (UK), and the European ESF-network on Vortex Matter. One of us (D.Y.V.) was supported by FWO-Vl.


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# Violation of the Minimum H-H Separation “Rule” for Metal Hydrides

## Abstract

Using gradient-corrected, all-electron, full-potential, density-functional calculations, including structural relaxations, it is found that the metal hydrides $`RT`$InH1.333 ($`R`$ = La, Ce, Pr, or Nd; $`T`$ = Ni, Pd, or Pt) possess unusually short H$``$H separations. The most extreme value (1.454 Å) ever obtained for metal hydrides occurs for LaPtInH1.333. This finding violates the empirical rule for metal hydrides, which states that the minimum H$``$H separation is 2 Å. Electronic structure, charge density, charge transfer, and electron localization function analyses on $`RT`$InH1.333 show dominant metallic bonding with a non-negligible ionic component between $`T`$ and H, the H$``$H interaction being weakly metallic. The paired, localized, and bosonic nature of the electron distribution at the H site are polarized towards La and In which reduces the repulsive interaction between negatively charged H atoms. This could explain the unusually short H$``$H separation in these materials. Also, $`R`$$``$$`R`$ interactions contribute to shielding of the repulsive interactions between the H atoms.

The most attractive aspect of metal hydrides from a technological point of view is their potential use as energy-storing materials. Hydrogen as energy carrier and other visions of the “hydrogen society” are especially attractive from an environmental point of view, but since hydrogen is a low-density gas at STP, the storage of the large quantities required for most applications is a challenge. High-pressure-compressed-gas storage is energy intensive if high volume efficiency is desired, liquid or solid hydrogen storage even more so, and all involve certain hazards. Storage of hydrogen in the form of solid metal hydrides, from which it can readily be recovered by heating, is safe and volume efficient.

The amount of hydrogen per volume unit in metal hydrides is very high; in some cases higher than in liquid or solid hydrogen, e.g., VH2 stores more than twice the amount of hydrogen than solid H2 at 4.2 K. It is unfortunate, however, that most metal hydrides are heavy in relation to the amount of hydrogen they contain. FeTiH2 and LaNi5H7, e.g., only contain 1.9 and 1.6 wt.$`\%`$ hydrogen, respectively. Therefore, efforts in hydride research have over the past 25$``$30 years been concentrated on designing new, or modifying known, intermetallic hydrides to increase the storing capacity and simultaneously adjusting their properties to make them capable of delivering hydrogen at useful pressures ($`>`$0.1 MPa) and acceptable temperatures ($`<`$ 425 K) maelan01 . These aspects are particularly important for most mobile applications where hydrogen would be used directly in combustion engines or indirectly via fuel cells. It has proven difficult to exceed 2 wt.$`\%`$ of stored hydrogen and it remains a challenge to increase this figure if metal hydrides are to become a viable source for the transportation sector.

The search for efficient hydrogen-storage metal hydrides schlapbach94  has to some extent been hampered by the mental barriers which empirical rules have put on the thinking. For example, the interstitial hole size where hydrogen is expected to occupy should be $`>`$ 0.40 Å. Switendick switendick79  observed from a compilation of experimental structure data that the minimum H$``$H separation in ordered metal hydrides is $`>`$2Å (“the 2-Å rule”). This empirical pattern is later rao85  supported by band-structure calculations which ascribe the effect to repulsive interaction generated by the partially charged hydrogen atoms. A practical consequence of this repulsive H$``$H interaction in metal hydrides is that it puts a limit to the amount of hydrogen which can be accommodated within a given structural framework. So, if H$``$H separations less than 2 Å would be possible this could open for new efforts to identify potential intermetallics for higher hydrogen storing capacity. However, there are indeed metal hydrides which do violate “the 2-Å rule” and we have here identified the origin for such behavior.

$`R`$NiIn ($`R`$ = La, Ce, Pr, and Nd) crystallizes in the ZrNiAl-type structure (space group $`P\overline{6}2m`$) and can formally be considered as a layered arrangement with a repeated stacking of two different planar nets of composition $`R_3`$Ni2 and NiIn3 along  of the hexagonal unit cell. If the hydrides of these materials obey the hole-size demand and “the 2-Å rule” one would expect H to occupy the interstitial $`2d`$ site within $`R_3`$Ni2 trigonal bipyramid. However, proton magnetic resonance (PMR) studies suggest ghoshray92 ; sen96  that H occupies both the 4$`h`$ and 6$`i`$ sites or either of them with H$``$H distances in the range 1.5$``$1.8 Å. Recent powder X-ray and neutron diffraction studies yartys  on $`R`$NiInD1.333-x (ideally $`R_3`$Ni3In3D4) show that deuterium occupies the 4$`h`$ site located on three-fold axis of $`R_3`$Ni tetrahedra that share a common face to form trigonal bipyramid (Fig. 1). This configuration gives rise to extraordinary short H$``$H separations of around 1.6 Å yartys . As the diffraction techniques generally determine the average structure, neglect of partial H-site occupancies and local lattice distortions may lead one to conclude with shorter H$``$H separations than actually present in the real structure yvon88 . Hence, it is of interest to perform structural optimization theoretically.

The present full-potential LMTO wills  calculations are all electron, and no shape approximation to the charge density or potential has been used. The basis functions, charge density and potential were expanded in spherical harmonic series inside the muffin-tin spheres and in Fourier series in the interstitial regions. The ratio of interstitial to unit cell volume is around 0.42. The calculations are based on the generalized-gradient-corrected-density-functional theory as proposed by Perdew et al. pw96  Spin-orbit terms are included directly in the Hamiltonian matrix elements for the part inside the muffin-tin spheres. The basis set contained semicore $`5p`$ and valence $`5d`$, $`6s`$, $`6p`$, and $`4f`$ states for La (for Ce the $`4f`$ electrons are treated alternatively as valence and localized core electrons, whereas the Nd-$`4f`$ and Pr-$`4f`$ electrons are treated as localized electrons using open core approximation), $`3s`$, $`3p`$, $`4s`$, $`4p`$, and $`3d`$ for Ni, $`4s`$, $`4p`$, $`5s`$, $`5p`$, and $`4d`$ for Pd, $`5s`$, $`5p`$, $`6s`$, $`6p`$, and $`5d`$ for Pt, $`5s`$, $`5p`$, and $`5d`$ for In and $`1s`$, $`2p`$, and $`3d`$ states for H. All orbitals were contained in the same energy panel. To ensure well-converged wave functions a so-called multi basis was included, implying the use of different Hankel or Neuman functions each attaching to its own radial functions. This allows reliable description of the higher-lying unoccupied states and low-lying semicore states. The self consistency was obtained with 105 k points in the irreducible part of the Brillouin zone. Test calculations were made for 210 k points to check for convergence, but the optimized $`c/a`$ ratio for 105 and 210 k points for LaNiInH1.333 is essentially the same. To gauge the bond strength and nature of bonding we have used crystal orbital Hamiltonian population (COHP) and electron localization function (ELF) analyzes, as is implemented in TBLMTO-47 cohp .

All calculations relate to ideal and fully saturated hydrides with composition $`R_3T_3`$In3H4 ($`RT`$InH1.333; $`R`$ = La, Ce, Pr, or Nd, $`T`$ = Ni, Pd, or Pt). For (trivalent) $`R`$ the $`4f`$ electrons were treated as core electrons (except for La; 4$`f`$). As Ce-$`4f`$ electrons are known to take different valence states in intermetallic compounds, different possibilities delin98  for the valence states of Ce were considered in both the hydrides and intermetallic phases during the structural optimization. For this optimization all atom positions were relaxed by force minimization and equilibrium $`c/a`$ and volume were obtained by total energy minimization. Optimized structural parameters for the Ce compounds are in good agreement with experimental values (only) when Ce atoms are assumed to be in the trivalent state. The calculated equilibrium lattice parameters and the changes between the intermetallic and corresponding hydride phases are given for selected compounds along with experimental parameters in Table 1.

In general, the calculated lattice parameters are in good agreement with the experimental values, and the small differences found may partly be attributed to hydrogen non-stoichiometry (around 10$`\%`$) in the experimental studies. The hydrogen-induced lattice expansion is strongly anisotropic (Table 1); a huge expansion along  ($`\mathrm{\Delta }c/c`$ = 14$``$20%) and a smaller intralayer contraction ($`\mathrm{\Delta }a/a`$ = 0$``$5.8%). The calculated cohesive energy and heat of formation for the hydrides are larger than for the corresponding intermetallic phases indicating that it might be possible to synthesize all these hydrides. The electronic structure studies show that all considered phases are in the metallic state consistent with experimental findings. The calculated $`R`$H, $`T`$H, and H$``$H distances are given in Table 2 along with experimentally available values.

An interesting observation is that all $`RT`$InH1.333 materials have unusually short H$``$H distances. Two explanations have been proposed. Pairing of the hydrogen atoms (either by molecular H2-like bonding or by bonding mediated by the intermediate $`T`$ atom) has been advanced to explain the anomalous PMR spectrum of CeNiInH1.0 ghoshra93 . The second explanation focuses on the significantly shorter La$``$La distance in LaNiInH1.333 than in closely related phases yartys , whereby the La atoms (generally $`R`$) may act as a shielding that compensates the repulsive H$``$H interaction.

In order to evaluate these possibilities we have calculated the total energy for (hypothetical) LaPtInH1.333 as a function of H$``$H separation according to three different scenarios: (1) Keeping La, Pt, and In fixed in their equilibrium positions, (2) moving La 0.08 Å out of the equilibrium position toward H, and (3) moving La 0.08 Å out of the equilibrium position away from H. The obtained results are illustrated in Fig. 2. When La, Pt, and In are in their optimized equilibrium position, the equilibrium H$``$H separation is 1.454 Å. This scenario corresponds to a lower total energy than the two alternatives. For scenario 3 we obtain a shorter H$``$H separation (1.438 Å) than for the ground state configuration, and for scenario 2 a correspondingly larger separation (1.462 Å).

As the total energy curves increase steadily on reduction of the H$``$H separations, the possibility of stabilization of hydrogen in the form of molecular H2-like units seems completely ruled out. The total energy increases drastically also for increased H$``$H separation beyond the equilibrium value. This is due to increasing repulsive $`T`$H interaction and decreasing attractive H$``$H interaction. The considerable changes in the equilibrium H$``$H distance on $`R`$ displacement indicate that $`R`$ in the $`R_3T_2`$ trigonal bipyramidal configuration (Fig. 1) acts as a shielding that to some extent compensates repulsive H$``$H interactions. When the $`R`$H separation is reduced the H atoms are allowed to approach each other more closely.

Owing to charge transfer from metal to hydrogen the repulsive H$``$H interaction in metal hydrides are generally larger than that within the H2 molecule and this may be the physical basis for “the 2-Å rule”. Another example of violation of “the 2-Å rule” is found for Th2AlH4 vaji1 , but here the minimum H$``$H separation (1.945 Å) within the Th5 trigonal bipyramids is much larger than the bond distance in the H2 molecule and the H$``$H separations in $`RT`$InH1.333. In order to quantify the bonding interaction between the constituents in the $`RT`$InH1.333 series the integrated crystal orbital Hamilton population (ICOHP) were calculated. For example, the ICOHP values up to $`E_F`$ for LaNiInH1.333 are $``$3.44, $``$0.14, $``$0.72, $``$0.85, $``$0.86, $``$1.21, and $``$0.61 eV for Ni(2c)$``$H, H$``$H, La$``$H, Ni(2c)$``$In, La$``$Ni(1b), Ni(1b)$``$In, and Ni(2c)$``$La, respectively. This indicates that the strongest bonds are those between Ni(2c) and H. Another important observation is that the bonding interaction between the hydrogens is small, which further confirms that the short H$``$H separation in these materials are not rooted in hydrogen pairing or formation of H2-like molecular units.

In order to substantiate this observation further we have calculated the valence-charge-density distribution in (100) of LaNiInH1.333 (Fig. 3a). From this figure, it is apparent that Ni and H form an NiH2 molecule-like structural subunit. Moreover, Fig. 3a demonstrates that there is no substantial charge density distributed between the H atoms. In order to depict the role of charge transfer we have displayed the charge transfer (the difference in the electron density of the compound and that of constituent atoms superimposed on the lattice grid) for LaNiInH1.333 within (100) in Fig. 3b. From Fig. 3b it is clear that electrons are transfered from La, In, and Ni to the H site. So, there is considerable ionic bonding component between H and the metallic host lattice. The transferred electrons from the metallic host lattice to the H2-like subunit of the structure enter the antibonding $`\sigma ^{}`$ levels and gives rise to repulsive interaction. This repulsive interaction between the negatively charged H atoms could explain why the H-H separation in these materials are larger than that in the H2 molecule. If there was strong covalent bonding between Ni and H one should expect a significant (positive) value of charge transfer distribution between these atoms (contributed by both atoms). The absence of such a feature rules out this possibility. The ELF is an informative tool to distinguish different bonding interactions in solids elf  and ELF for LaNiInH1.333 in (100) is given in Fig. 3c. The large value of ELF at the H site indicates strongly paired electrons with local bosonic character. Another manifestation of covalent bonding between Ni and H should have been paired electron distribution between these atoms. The negligibly small ELF between Ni and H indicates that the probability of finding parallel spin electrons close together is rather high (correspondingly small for antiparallel spin pairs) in this region confirm metallic bonding consistent with the result obtained from charge transfer analysis and the detailed analysis show that delocalized metallic Ni(2c)-$`d`$ electrons are distributed in this region. Even though the charge distribution between Ni and H looks like a typical covalent bonding the charge transfer and ELF analyzes clearly show that the electron distribution between Ni and H are having parallel spin alignment and purely from Ni site. Hence, chemical bonding between Ni and H is dominated by metallic components with considerable ionic weft. The partial density of state analysis also show that the H-$`s`$ states are well separated from the Ni-$`d`$ states in the whole valence band indicates the presence of ionic bonding between Ni and H. Due to the repulsive interaction between the negatively charged H electrons, the ELF contours are not spherically shaped but polarized towards La and In. The localized nature of the electrons at the H site and their polarization towards La and In reduce significantly the H$``$H repulsive interaction and this can explain the unusually short H$``$H separation in this compound. The ELF between the H atom takes a significant value of 0.35. Considering the small charge density, this indicates a weak metallic type of interaction between the hydrogen atoms.

$`RT`$InH1.333 constitutes a series with much shorter H$``$H separations than other known metal hydrides. We have shown that the short distances between the H atoms in such metal hydrides are governed primarily by the polarization of negative charges on H towards the electropositive La and In. We believe that this conclusion is of more general validity, and may be utilized to search for other metal hydrides of potential interest as hydrogen storage materials.

The authors are grateful to the Research Council of Norway for financial support and for computer time at the Norwegian supercomputer facilities.


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# Precise measurement of hyperfine intervals using avoided crossing of dressed states

## Abstract

We demonstrate a technique for precisely measuring hyperfine intervals in alkali atoms. The atoms form a three-level $`\mathrm{\Lambda }`$ system in the presence of a strong control laser and a weak probe laser. The dressed states created by the control laser show significant linewidth reduction. We have developed a technique for Doppler-free spectroscopy that enables the separation between the dressed states to be measured with high accuracy even in room-temperature atoms. The states go through an avoided crossing as the detuning of the control laser is changed from positive to negative. By studying the separation as a function of detuning, the center of the level-crossing diagram is determined with high precision, which yields the hyperfine interval. Using room-temperature Rb vapor, we obtain a precision of 44 kHz. This is a significant improvement over the current precision of $``$1 MHz.

There has been much excitement in recent times in the use of atomic coherences to modify the properties of light beams passing through an atomic vapor. For example, atomic coherences have been used to slow light to low velocities and even to stop and “store” light . In electromagnetically induced transparency (EIT) experiments, an initially absorbing medium becomes transparent to a probe beam when a control laser is applied to an auxiliary transition . The control laser creates atomic coherences that shift the absorption away from the line center. EIT techniques have several practical applications in probe amplification , lasing without inversion  and suppression of spontaneous emission . In many of these experiments, the atoms form a three-level system and the control laser strongly drives two of these levels. As is well known, the strong driving creates dressed states of the system . It is the coherence between the dressed states that is the basis for the phenomena mentioned above. Experimental observations of these phenomena have been facilitated by the advent of low-cost tunable diode lasers which can be used to access transitions in alkali atoms such as Rb and Cs. Alkali atoms have convenient energy levels with strong oscillator strengths which form almost ideal three-level systems.

In this paper, we show that such “coherent control” techniques can be adapted to make precise measurements of hyperfine intervals in alkali atoms. There are two properties of the dressed states that are important for this measurement. First, the coherence between the dressed states results in linewidth narrowing well below the natural linewidth . Hence it is possible to measure small shifts in the location of the dressed state. Second, the dressed states have opposite symmetry. Therefore, as the detuning of the control laser is changed from positive to negative, the dressed states go through a characteristic avoided crossing. These two features can be combined to determine the exact center of the level-crossing diagram, which yields the hyperfine interval. In our case, we work with room-temperature Rb vapor. The linewidth of the hyperfine peaks is about 27 MHz, but the technique allows us to extract the hyperfine interval with a precision of 44 kHz.

To understand our technique, let us first consider the three-level $`\mathrm{\Lambda }`$-type system in Rb in some detail. The measurements are done on the $`D_2`$ line in 87Rb ($`5S_{1/2}5P_{3/2}`$ transition). As shown in Fig. 1, 87Rb has two hyperfine levels in the ground state with $`F=1`$ and 2. The excited state splits into four hyperfine levels, of these the $`F^{}=2`$ level couples to both ground levels and can be used to form the $`\mathrm{\Lambda }`$ system. The control laser drives the $`F=1F^{}=2`$ transition with Rabi frequency of $`\mathrm{\Omega }_R`$ and detuning from resonance of $`\mathrm{\Delta }_c`$. The weak probe laser measures absorption on the $`F=2F^{}=2`$ transition at a detuning $`\mathrm{\Delta }`$. The spontaneous decay rate from the excited level is $`\mathrm{\Gamma }`$, which is $`2\pi \times 6.1`$ MHz in Rb.

The absorption of the weak probe in the presence of the control laser has been derived previously . As is well known, the strong control laser creates two dressed states due to the ac Stark shift . The probe absorption gets modified due to this and shows peaks at the location of the two dressed states (Autler-Townes doublet), given by

$$\mathrm{\Delta }_\pm =\frac{\mathrm{\Delta }_c}{2}\pm \frac{1}{2}\sqrt{\mathrm{\Delta }_c^2+\mathrm{\Omega }_R^2}.$$
(1)
Here $`\mathrm{\Delta }_+`$ and $`\mathrm{\Delta }_{}`$ are the values of the probe detuning where the peaks occur. The corresponding linewidths ($`\mathrm{\Gamma }_\pm `$) of these peaks are different because of the coherence between the two dressed states, and given by

$$\mathrm{\Gamma }_\pm =\frac{\mathrm{\Gamma }}{2}\left(1\frac{\mathrm{\Delta }_c}{\sqrt{\mathrm{\Delta }_c^2+\mathrm{\Omega }_R^2}}\right).$$
(2)
It is clear from the above expression that, if $`\mathrm{\Delta }_c=0`$, the two peaks are symmetric and have identical linewidths of $`\mathrm{\Gamma }/2`$. However, for any non-zero detuning, the peaks have asymmetric linewidths. The first peak has larger linewidth while the second peak has smaller linewidth by precisely the same factor, in such a way that the sum of the two linewidths is equal to the unperturbed linewidth, $`\mathrm{\Gamma }`$.

The above analysis shows how the three-level system is useful in many applications. For example, probe absorption at line center ($`\mathrm{\Delta }=0`$) is strongly suppressed in the presence of a resonant control laser because the dressed states created by the control laser are shifted by the Rabi frequency. This is the basis for EIT experiments. Similarly, it is clear from Eq. 2 that the linewidth $`\mathrm{\Gamma }_+`$ of the second dressed state can be much below the natural linewidth when the control-laser detuning is large. The basic idea for our experiment is also contained in the above analysis. From Eq. 1, the separation between the dressed states is $`\sqrt{\mathrm{\Delta }_c^2+\mathrm{\Omega }_R^2}`$. As the detuning of the control laser is varied from negative to positive, the states exhibit an avoided crossing, so that the separation at zero detuning is not zero but equal to the Rabi frequency. Thus, by studying the variation of the separation with detuning, it is possible to determine the location of the level crossing precisely.

However, observing the Autler-Townes doublet in room-temperature vapor is complicated by effects due to Doppler broadening. The above expressions are valid for a stationary atom; in room-temperature vapor they have to be corrected for the thermal velocity distribution of the atoms. One consequence of this is that the linewidth appearing in Eq. 2 is not the natural linewidth but the Doppler width, which is 560 MHz for room-temperature Rb atoms. We have solved the problem of Doppler broadening in the following manner. A part of the probe laser is split off as a “pump” beam and sent through the vapor cell so that it is counter-propagating with respect to the probe and control beams. The intensity of the pump beam is chosen to be about 4 times higher than the probe. In this configuration, the zero-velocity group of atoms preferentially absorbs from the pump and the probe gets transmitted. This is a standard technique used in Doppler-free saturated-absorption spectroscopy  which we have adapted to the three-level case.

The experimental schematic for the hyperfine measurements in Rb is shown in Fig. 2. The probe and control beams are obtained from two frequency-stabilized diode laser systems operating near the $`D_2`$ line in 87Rb. The linewidth of the lasers after stabilization has been measured to be below 1 MHz. The two beams co-propagate through a room-temperature vapor cell containing Rb. The absorption through the cell is about 25%. The counter-propagating pump beam discussed above is generated from the probe laser using a beamsplitter. To set the frequency of the control laser, a part of the control beam is tapped off for saturated-absorption spectroscopy in a vapor cell. It can be potentially locked to any of the hyperfine peaks or crossover resonances in the spectrum. We lock it to the $`F=1F^{}=(1,2)`$ crossover resonance. The remaining frequency offset (of about 78 MHz) to bring it close to the $`F=1F^{}=2`$ is obtained using an acousto-optic modulator (AOM). The frequency shift in the AOM is varied to get different detunings and the value of the AOM frequency at which the level-crossing occurs gives the hyperfine interval between the $`F=(1,2)`$ crossover resonance and the $`F^{}=2`$ level. Note that the only absolute frequency entering the measurement is the frequency of the AOM, all other frequencies such as the separation of the dressed states or the Rabi frequency of the control laser are only important in their relative values.

The transmission of the probe laser as it is scanned across the $`F=2F^{}=2`$ transition is shown in Fig. 3. In the first trace, the control laser is turned off. The pump-probe configuration results in the appearance of a Doppler-free peak as for standard saturated-absorption spectroscopy. Ideally, the linewidth of the peak should be the natural linewidth of 6.1 MHz. The linewidth obtained in our case is about 27 MHz. There are many reasons for this broadening, the main two being misalignment between the counter-propagating beams, and power broadening due to the pump beam. However, as we will see below, the large linewidth does not seriously affect the measurement.

In the presence of the control laser, the $`F^{}=2`$ peak splits into two peaks exactly as predicted by the above analysis. This is shown in the middle trace of Fig. 3. The two peaks have asymmetric linewidths because of the non-zero detuning of the control laser, with the peak on the right having smaller linewidth. The detuning for this spectrum is +13.5 MHz. In the lowest trace of Fig. 3, we show the same spectrum when the detuning has been changed to $`13.5`$ MHz. Notice that now it is the peak on the left that has the smaller linewidth, showing that the symmetry of the dressed states changes as the detuning changes from positive to negative. Furthermore, the sum of the linewidths of the two peaks in both cases is equal to the unperturbed linewidth, as predicted by Eq. 2. However, as mentioned before, the unperturbed linewidth is 27 MHz and not the natural linewidth of 6.1 MHz.

The variation of the separation of the Autler-Townes doublet as a function of AOM frequency is shown in Fig. 4. Since the frequency of the control laser is first shifted using the AOM, and then locked to the $`F=1F^{}=(1,2)`$ crossover resonance, the AOM frequency at which the separation reaches a minimum yields the hyperfine interval to the $`F^{}=2`$ level. The solid line in Fig. 4 is the expected variation in separation as a function of control-laser detuning from Eq. 1. The best fit yields a value of 78.433(44) MHz for this hyperfine interval. Note that the absolute values of the control-laser Rabi frequency and the separation of the peaks are not important. Any scaling error in obtaining these numbers from the measured experimental parameters will not affect the determination of the minimum. The only absolute number of consequence is the AOM frequency and this is measured very precisely using a frequency counter.

The accuracy of 44 kHz we obtain is significantly better than the accuracy with which hyperfine intervals in alkali atoms are currently known . The values in Ref.  are obtained by fitting to all the available data on alkali atoms with measurements from a range of techniques such as optical double resonance, cascade radiofrequency and level crossing. The typical error in Ref.  for hyperfine intervals in the $`5P_{3/2}`$ state of Rb is about 1 MHz. There is a more recent measurement in Rb  using stabilized diode lasers similar to the lasers we have used in this work. Absolute frequencies of the different hyperfine levels are obtained using a Fabry-Perot interferometer and a stabilized HeNe laser as the frequency reference. The accuracy quoted in Ref.  is 0.4 MHz. The frequency stability of the diode lasers is a limitation in obtaining higher accuracy with such an interferometric technique.

The most precise measurements in 87Rb to date have been reported in Ref.  with a quoted error of only 4–9 kHz. The extremely small error in this work has been achieved using optical heterodyning of two ultra-stable tunable Ti-sapphire lasers locked to different hyperfine transitions. Several experimental advancements were used to bring down errors to this level. The linewidth of the hyperfine transitions was reduced to 7 MHz in the vapor cell using magnetic shielding and careful control of pump and probe intensities. The cells themselves were specially constructed to ensure ultra-high purity. The lasers were locked with 3 kHz precision to the line center using third-harmonic lock-in detection at the modulation frequency. Ultra-stable frequency standards were used to achieve stability of AOMs. By contrast, we have used standard locking of a low-cost diode laser to the hyperfine transition. The transition is broadened to a linewidth of 27 MHz in the vapor cell. We have therefore not really pushed the limits of precision for our technique. It is conceivable that, by using some of the advanced techniques mentioned in Ref. , we can reduce our errors by a factor of 5 to 10. However, even at the level of 44 kHz, the technique is useful since hyperfine intervals in the other isotope of Rb, 85Rb, or in other alkali atoms are known only with $``$MHz precision.

In conclusion, we have demonstrated a new technique for measuring hyperfine intervals in alkali atoms. The atoms form a three-level $`\mathrm{\Lambda }`$ system with an excited level coupled to a ground level by a strong control laser, and the same excited level coupled to a different ground level by a weak probe laser. The control laser creates dressed states that show significant linewidth reduction when the control laser is detuned from resonance. In addition, the states go through an avoided crossing as the sign of the detuning is changed from positive to negative. Even though we work with room-temperature vapor, we have adapted a technique of using a counter-propagating pump beam that allows us to overcome the Doppler effect and measure the separation of the dressed states very accurately. By studying the separation as a function of detuning, we determine the line center of the level-crossing diagram with high precision. We work with room-temperature Rb atoms, where we obtain a precision of 44 kHz. This is already a useful level of precision since typical accuracy for hyperfine intervals in alkali atoms is of order 1 MHz. However, we think that with foreseeable improvements, the error can be brought down to the few kHz level. The technique is easily extended to other alkali atoms such as Li, K, and Cs, where the transitions are accessible with low-cost tunable diode lasers.

The authors thank Anusha Krishna for help with the experiments. This work was supported by a research grant from the Department of Science and Technology, Government of India.