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# Aging, rejuvenation and memory effects in re-entrant ferromagnets

## I Introduction

Disordered magnetic systems have been intensively studied in the last decades. Among them, the systems with competing magnetic interactions are of particular interest. When the contributions of ferromagnetic and antiferromagnetic interactions are comparable, conventional long range order is not stable and a spin glass behavior is obtained. If the ferromagnetic interactions are preponderant, the system displays a re-entrant behavior, with, for decreasing temperatures, a transition from the paramagnetic phase to a ferromagnetic phase, followed by a transition to a spin glass phase.

Experimentally, in some compounds the amount of ferromagnetic and antiferromagnetic interactions can be continuously varied by changing the concentration of a magnetic ion Maletta ; Nogues ; Nogues2 . One such example is the $`CdCr_{2x}In_{22x}S_4`$ thiospinel Nogues , a frustrated magnetic insulator with ferromagnetic nearest neighbor and antiferromagnetic next nearest neighbor interactions. The $`x=0.85`$ compound is a model spin glass in which aging has been extensively studied Sitges . The interest in aging phenomena has been revived by experiments on the effect of temperature changes, which have revealed non trivial rejuvenation and memory effects MemChaos , also identified later on in many disordered systems KTN ; Weissman ; Ciliberto ; Parker . While these features are well accounted for in hierarchical pictures where one assumes a hierarchical organization of the metastable states of the spin glass as a function of temperature Hierarchy , their interpretation in the physical space Domains  is less clear and is currently the subject of many efforts, both on the theoretical and experimental sides Review ; 2dXY ; Lemaitre ; NumRecent ; SGFerro .

In this paper, we present a comparative study of spin-glass type phenomena, and in particular of the rejuvenation and memory phenomena, in the ferromagnetic phases of the $`CdCr_{2x}In_{22x}S_4`$ system for several concentrations $`x`$ of the magnetic ions ($`x>0.85`$). Our motivation for studying these ferromagnetic phases is the fact that since they are conceptually simpler than spin glasses (spins are organized in domains), the rejuvenation and memory phenomena should be more easily described in terms of geometrical spin arrangements. This argument already led us to study the ferromagnetic phase of the weakly diluted $`x=0.95`$ compound SGFerro  in which we could observe some rejuvenation and memory effects. The latter were discussed in terms of pinning and reconformations of ferromagnetic domain walls in the dilution-induced disorder. The work that we present here, involving the study of a more diluted sample ($`x=0.90`$), complements the previous investigation and provides further insights on the role of disorder in these out-of-equilibrium phenomena.

The paper is organized as follows. First, we present the phase diagram of the $`CdCr_{2x}In_{22x}S_4`$ system, the general behavior of the magnetization and the low frequency ac susceptibility of the studied samples with $`x>0.85`$. Then we analyse the results of isothermal ac susceptibility relaxations at various temperatures both in the ferromagnetic phases and in the re-entrant spin glass phases. This allows us, for example, to highlight the effect of disorder on isothermal aging. We describe experiments in which we have investigated the effect of temperature changes on aging. The comparison of the results for different concentrations $`x`$ shows that the ability of a disordered ferromagnet to memorize aging at a given temperature is strongly dependent on the disorder strength. Whereas for weak disorder ($`x`$ = 0.95), the memory of an isothermal aging is easily erased by a short low temperature excursion (below the temperature at which the system was aged) SGFerro , for stronger disorder ($`x`$ = 0.90), this memory is preserved and can only be erased by an excursion down to the re-entrant spin glass phase. Finally, we discuss the whole set of results in terms of pinning and reconformations of the ferromagnetic domain walls in their disordered environment and raise the question of the relevance of this wall dynamics for explaining the rejuvenation and memory phenomena in spin glasses.

## II Characterization of the system

The investigated samples are chromium thiospinels of formula $`CdCr_{2x}In_{22x}S_4`$ for $`x=1.00`$, $`x=0.95`$, $`x=0.90`$ and $`x=0.85`$ prepared by M. Noguès at the CNRS Meudon-Bellevue laboratory. They have been well characterized in the past by various techniques Nogues  including neutron diffraction Pouget  and display behaviors ranging from pure ferromagnet, to re-entrant ferromagnet and spin glass for decreasing $`x`$. The samples are polycrystalline powders and the measurements reported here were performed with a commercial $`Cryogenic^{Ltd}`$ S600 SQUID magnetometer.

### II.1 Structure and phase diagram

The phase diagram of the $`CdCr_{2x}In_{22x}S_4`$ is shown in Fig. 1. The pure compound $`CdCr_2S_4`$ is a normal spinel, i.e. all the Cr3+ ions occupy octahedral (B) sites of the lattice whereas the tetrahedral (A) sites are occupied by Cd2+ ions only. The Cr3+ ions are in a $`3d^3`$ electronic state, leading to a magnetic moment of spin only type with S=$`\frac{3}{2}`$. The main magnetic interactions between a Cr3+ ion and its six nearest neighbors are positive Pouget  ($`J_1/k_B=13.25\pm 0.12K`$) and induce ferromagnetism below $`T_C=84.8K`$. The existence of super exchange antiferromagnetic interactions Dwight67  between the twelve third nearest neighbors ($`J_3/k_B=0.915\pm 0.015K`$) induces frustration in the magnetic lattice that can be quantified by the weighted interaction ratio $`R=\frac{z_3\times J_3}{z_1\times J_1}=0.138`$, to be compared to the critical ratio for the stability of ferromagnetism $`R_C=0.25`$ in the spinel structure Balt66 . The dilution of the Cr3+ ions by non magnetic In3+ ions enhances this frustration as the antiferromagnetic couplings via the In3+ orbitals $`J_L`$ are amplified by a factor $`R_{In}=J_L/J_39.0`$ Veill86 ; Mery85  . This large enhancement explains quantitatively the absence of a percolating ferromagnetic cluster for dilutions ($`1x`$) greater than about 15% Nogues . The dilute samples ($`0.15<x<0.85`$) therefore undergo a unique phase transition towards a spin glass phase at low temperatures.

For higher concentrations in chromium ions ($`0.85<x<1`$), the sequence of phase transitions upon cooling down is as followed: a para-ferromagnetic phase transition first occurs at a critical temperature $`T_c`$, followed by the onset of spin glass type irreversibilities, at a lower critical temperature $`T_g`$. This phenomenon is usually referred to as reentrance.

### II.2 Field Cooled and Zero Field Cooled magnetizations

Fig. 2 displays the Field Cooled (FC) and Zero Field Cooled (ZFC) magnetizations (normalized to the value of the applied field) vs. temperature for the studied samples. The ZFC measurements have been performed after cooling the samples in zero field (at $`80mK/s`$) to 3K, applying the field at 3K, and recording the data upon slowly re-heating (at $`3mK/s`$). The FC data have been taken in the same manner (but cooling with the field on). The amplitude of the small probing field was typically of $`10Oe`$ in order to remain in the linear response regime. We have applied demagnetizing field factor corrections to the data to take into account the different geometries of the samples demagnet . The results are presented for a spherical shape factor.

While at high temperatures, all samples are paramagnetic, two types of behavior appear at lower temperatures.

In the pure ($`x=1.00`$) and the weakly diluted ($`x=0.95`$) samples, a transition from the disordered paramagnetic state to a long range ferromagnetic ordered state is signalled by a sharp increase of both the ZFC and FC magnetizations above the Curie temperature $`T_c`$. This transition is confirmed by neutron diffraction measurements which evidence spontaneous magnetization, magnetic Bragg peaks and characteristic spin waves Pouget . Below $`T_c`$, magnetic irreversibilities are observed in the separation of the FC and ZFC curves: the magnetization becomes history dependent. The slow increase of the FC magnetization as the temperature is decreased is accounted for by a small extra polarization of the sample when cooled in a field and can be related to the temperature dependence of the spontaneous magnetization. On the other hand, the plateau of the ZFC magnetization, at a level equal to the inverse of the demagnetizing field factor, indicates that the spins are well organized in ferromagnetic domains.

The behavior of the strongly diluted ($`x=0.90`$) sample is markedly different. The increase of the FC and ZFC magnetizations upon cooling from the paramagnetic phase is less pronounced than in the less diluted samples. Neutron diffraction measurements reveal only short range ferromagnetism with no magnetic Bragg peaks nor a true divergence of the spin-spin correlations Pouget . We can still define for convenience a ‘transition’ temperature $`T_c`$ at the inflection point of the magnetization increase but it is important to note that this is not a true transition to a long range ordered state. With this definition, we see that, just below $`T_c`$, no clear separation of the FC and ZFC curves is found within experimental accuracy. Nevertheless, we observe a rounded magnetization plateau at a level corresponding to the expected demagnetizing field factor which suggests that the magnetic moments in the sample are still organized in ferromagnetic domains.

At lower temperatures, while nothing special happens in the pure sample, the FC magnetization of the $`x=0.95`$ and $`x=0.90`$ samples decreases and tends to saturate. In parallel, we observe a sharp drop of the ZFC magnetization. This change of behavior corresponds to the transition from the ferromagnetic state to the strongly frozen re-entrant spin glass state and is to be compared with the reference spin glass behavior of the more diluted $`x=0.85`$ sample also shown in Fig. 2.

### II.3 Low frequency ac susceptibility

To complete the previous analysis, we have measured the low frequency ac susceptibility $`\chi =\chi ^{}i\chi ^{\prime \prime }`$ of the samples as a function of temperature. Here again, the data has been taken while re-heating at $`12mK/s`$, after cooling to 3K at $`80mK/s`$, using a probing field of weak amplitude (typically 1.7 Oe peak value) in order to remain in the linear response regime. We have used the paramagnetic phase response (assuming $`\chi ^{\prime \prime }=0`$) to correct a slight frequency dependent phase shift in the detection setup. In the following, we focus on the out-of-phase component $`\chi ^{\prime \prime }`$ which is directly related to the dissipation processes.

Fig. 3 shows $`\chi ^{\prime \prime }`$ at $`0.4Hz`$ vs. temperature for all the studied samples. The onset of ferromagnetism is signalled by a sharp increase in $`\chi ^{\prime \prime }`$ when cooling from high temperatures. This increase in the dissipation indicates that the characteristic relaxation times of the system have reached a value comparable to the macroscopic measurement time (equal here to the inverse of the ac field frequency). This is the standard scenario expected at a second order phase transition where the average relaxation time diverges. We can define a transition temperature $`T_c`$ at the inflection point of the $`\chi ^{\prime \prime }`$-increase. We find that $`T_c`$ slightly decreases for decreasing frequencies, in agreement with the expectation from dynamic scaling arguments. Below $`T_c`$, $`\chi ^{\prime \prime }`$ keeps a non zero value, roughly temperature independent in the whole ferromagnetic region meaning that there are still dissipation processes at the time scale of the experiments in the ferromagnetic phase of the studied samples, even in the pure one. The stronger the dilution, the higher this plateau value of $`\chi ^{\prime \prime }`$. The primary effect of an increase in the disorder strength is therefore an increase of the level of low frequency dissipation.

At lower temperatures, sharp peaks with a critical frequency dependence Tholence ; Mydosh  are observed in the out-of-phase susceptibility $`\chi ^{\prime \prime }`$ of the diluted samples ($`x=0.95`$ and $`x=0.90`$) and signal the transition from the ferromagnetic state to the re-entrant spin glass state. The corresponding transition temperatures estimated from the inflection points at low frequency ($`0.4Hz`$) are about the same as the ones at which strong irreversibilities are observed in FC-ZFC measurements. Curiously, a small peak in $`\chi ^{\prime \prime }`$ is also observed at low temperatures in the pure $`x=1.00`$ sample where no existence of a re-entrant spin glass phase has ever been reported. However, while the frequency dependence of the peaks observed in the diluted samples is characteristic of critical slowing down (in the frequency range explored \[0.04Hz-8Hz\]), we have found that the position of the peak in the pure sample has an Arrhenius type frequency dependence, evocative of a dynamical freezing of the spins. Even if the origin of this peak is at this moment not completely clear, it does not seem to correspond to a phase transition as in the diluted samples.

## III Slow dynamics and aging at constant temperature

We have investigated the isothermal slow dynamics and aging of the $`CdCr_{2x}In_{22x}S_4`$ samples in the following way. The samples were cooled from their paramagnetic phase down to various successive aging temperatures $`T_m`$, in both the ferromagnetic and the re-entrant spin glass phases (with a cooling rate of typically $`1mK/s`$). At each fixed aging temperature, the time evolution of the ac susceptibility was recorded for three different frequencies: $`0.04Hz`$, $`0.4Hz`$ and $`4Hz`$.

In all cases, we observe a slow time decay (aging) of the ac susceptibility $`\chi (\omega ,t)`$ towards an asymptotic frequency dependent value $`\chi _0(\omega )`$ (stationary susceptibility). The relaxation is more important in relative value on the out-of-phase component than on the in-phase component and in the following we focus on $`\chi ^{\prime \prime }`$.

The influence of temperature on aging is illustrated in table I, in which we report, for the $`x=0.95`$ and $`x=0.90`$ samples, the amplitude of the $`\chi ^{\prime \prime }`$ relaxations (in absolute and relative values) at fixed frequency, observed at various temperatures and for a given waiting time $`t_w=15000s`$. The trend is the same for both samples. The relaxations are always weaker in the ferromagnetic phase than in the re-entrant spin glass phase. Moreover, in the ferromagnetic phase, the relaxation is mainly important near $`T_c`$ and tends to disappear in the experimental background noise at lower temperatures.

Concerning the frequency dependence of the relaxation, we observe that the lower the frequency $`\omega `$, the greater the relaxation amplitude observed in the experimental time window. This result is in agreement with a previous investigation of the $`x=0.95`$ sample SGFerro , where a qualitative $`\omega t`$ scaling (characteristic of spin glasses Sitges ) of the non stationary part of the susceptibility was found both in the re-entrant spin glass and in the ferromagnetic phases. Here, we have studied this scaling behavior of the isothermal ac susceptibility relaxation in a more quantitative way. We have recorded the relaxation of the ac susceptibility of the $`x=0.90`$ sample following a quench ($`80mK/s`$) to a temperature $`T_m=42K`$ in the ferromagnetic phase for $`8`$ frequencies $`\omega `$ of the ac field in the range \[$`0.04Hz`$-$`4Hz`$\]. Fig. 4 shows the resulting relaxation curves for the out-of-phase component $`\chi ^{\prime \prime }`$ as a function of the reduced variable $`\omega t`$. As we can see in the figure, the scaling works pretty well over nearly five decades. All the relaxation curves, after subtraction of a constant which corresponds to the stationary part $`\chi _0^{\prime \prime }(\omega )`$, lie on a unique master curve which is a function of $`\omega t`$ and can be nicely fitted by a power law with an exponent of order $`0.2`$ (same value as commonly observed in spin glasses Sitges ).

## IV Rejuvenation and memory effects

In conventional spin glasses, such as the $`x=0.85`$ compound, it is known that decreasing the temperature from T to T-$`\mathrm{\Delta }`$T in the spin glass phase, after having isothermally aged the sample at T, strongly restarts the dissipation processes. This is the rejuvenation effect MemChaos , the system seems to forget its previous equilibration stage at T. For a sufficiently large $`\mathrm{\Delta }`$T, the system rejuvenates completely and the relaxation of the ac susceptibility at T-$`\mathrm{\Delta }`$T is identical to that obtained after a direct quench from the paramagnetic phase. The other striking feature happens when the system is re-heated to the initial temperature T after a given low temperature history. No restart of aging is found and the relaxation is the exact continuation of the one that occurred before going to low temperatures. This is the memory effect MemChaos , aging at T-$`\mathrm{\Delta }`$T had no influence on aging at T. These effects have been interpreted as an evidence for a hierarchical organization (tree-like for example) as a function of temperature of the metastable states of the spin glass Hierarchy .

In order to reach a better understanding of these non trivial rejuvenation and memory effects in terms of geometrical spin arrangements, we have previously investigated the pure and weakly disordered ferromagnetic phase of the $`x=1.00`$ and $`x=0.95`$ compounds SGFerro . We found clear rejuvenation effects coexisting with a very weak memory of aging, which was easily erased by an excursion at lower temperature. Here, we report similar investigations of the rejuvenation and memory phenomena in the short range ferromagnetic phase of the $`x=0.90`$ sample. Our results shed light on the role of disorder in the rejuvenation and memory phenomenology.

In a first experiment, we have studied the rejuvenation and memory phenomena in the temperature dependence of the ac susceptibility. Fig. 5 shows the out of phase susceptibility $`\chi ^{\prime \prime }`$ of the $`x=0.90`$ sample at $`0.4Hz`$ vs. temperature. All along the experiment a sweeping rate $`|dT/dt|`$ of $`3mK/s`$ was used. The sample was cooled down to a measurement temperature $`T_m=42K`$ where it was isothermally aged during $`8h`$ (full symbols). After this aging stage, the cooling was resumed down to a final temperature $`T_0`$ (two cases, $`T_0=38K`$ and $`T_0=20K`$, were studied) and finally, the sample was slowly re-heated from $`T_0`$ to the paramagnetic phase (open symbols). For comparison, a reference curve, recorded with the same protocol but without the aging stage, is also plotted on this graph (dotted and solid lines for cooling and re-heating).

Aging is clearly visible in the downward relaxation with time of $`\chi ^{\prime \prime }`$ at $`T_m`$. When cooling is resumed after the aging stage at $`T_m`$, a rejuvenation effect is evidenced by the increase of $`\chi ^{\prime \prime }`$ back to the reference cooling curve. Considering now the re-heating process, we see that in the experiment with a short excursion down to $`T_0=38K`$, a memory of the aging at $`T_m`$ is found as $`\chi ^{\prime \prime }`$ departs from the heating reference curve on approaching $`T_m`$ and displays a characteristic dip around $`T_m`$ before merging back with the reference curve. In contrast, in the experiment with a longer excursion down to $`T_0=20K`$, the re-heating curve remains superimposed onto the re-heating reference curve and no memory dip is found. Let us mention that in another experiment made with the same protocol but with $`T_0=30K`$, we observed a memory effect identical to the one observed with $`T_0=38K`$.

In a second experiment, we have studied the rejuvenation and memory phenomena as a function of time. Fig. 6 shows the out of phase susceptibility $`\chi ^{\prime \prime }`$ at $`0.4Hz`$ vs. observation time measured with a negative temperature cycling protocol : the sample was quenched from high temperatures down to the measurement temperature $`T_m=42K`$, aged there during $`t_1=17000s`$, cooled then to $`T_0`$ , aged at this temperature another $`t_2=17000s`$ then heated back to $`T_m`$ and finally aged there again for $`t_3=17000s`$. Three values were used, $`T_0=38K`$, $`30K`$ and $`20K`$.

Just after the quench, $`\chi ^{\prime \prime }`$ relaxes downwards with time (it is the same kind of relaxation as in the exp. of Fig. 5). Cooling from $`T_m`$ to $`T_0`$ induces a restart of aging for $`T_0=38K`$ and $`T_0=30K`$: it is the rejuvenation effect observed here as a function of time. Heating back to $`T_m`$ reveals the memory of the previous aging stage at $`T_m`$: except for a short transient regime, the relaxation at $`T_m`$ is the exact continuation of the one that occurred before the cycle. However, in the experiment going down to $`T_0=20K`$ (that is, in the border region between the ferromagnetic and spin-glass phases), the relaxation at $`T_0=20K`$ does not show any upturn signing up a rejuvenation effect. We do not have a reference curve of a relaxation at $`20K`$ after a direct quench for comparison; further studies in this temperature region would be of interest. A strong restart of aging is observed when coming back to $`T_m`$ from $`T_0=20K`$ after the negative cycle (in agreement with the absence of memory in the experiments of Fig. 5). We have checked that this restart of aging is not a long transient which would yield to a memory at a longer observation time as the data points cannot be superposed onto a reference isothermal relaxation curve.

In summary, the experiments reported above show that the rejuvenation effect is a characteristic feature of disordered ferromagnetic phases, as was already observed in SGFerro ; FerroUppsChaos . It is not influenced by the amount of disorder. In contrast, the ability of a ferromagnet to store and retrieve a memory of a previous aging strongly depends on the disorder strength. Whereas the memory is weak and rapidly erased by a low temperature excursion for the weakly disordered $`x=0.95`$ sample, it is much more robust in this more disordered $`x=0.90`$ sample. For the latter, the memory of aging is not much affected by a low temperature excursion below $`T_m`$ as long as the lowest temperature reached during the experiment remains sufficiently above the re-entrant spin glass transition temperature.

While performing the previous experiments on the $`x=0.90`$ sample, we observed a surprising behavior of the ac susceptibility which may be related to the mechanism responsible for the erasure of the memory. When recording the cooling/re-heating reference curves of Fig. 5 for $`T_0=20K`$, we found that in the region \[20K,35K\], the cooling curve was always below the re-heating curve. This means that the state which progressively develops in the short range ferromagnetic phase while cooling from the paramagnetic phase is less dissipative than the one obtained when re-heating from the low temperature re-entrant spin glass phase. This rather unusual phenomenon is displayed in Fig. 7. We have investigated the aging properties of these two states which we call for convenience the cooled state and the re-heated state. Fig.7 shows $`\chi ^{\prime \prime }`$ vs. temperature at $`0.4Hz`$ measured along the following procedure: slow cooling from high temperatures to $`3K`$ with an aging stop at $`30K`$ during $`4h`$ (full circles), slow cooling to $`3K`$ and re-heating with an aging stop at $`30K`$ for $`6h`$ (open circles) during the re-heating.

In the figure, the hysteresis between cooling and re-heating is clearly evidenced. If we consider now the relaxations, we find a larger relaxation amplitude in the re-heated state than in the cooled state. This extra dissipation gained in the vicinity of the re-entrant spin glass transition indicate some incompatibility between the short range ferromagnetic correlations that develop while cooling the sample from the paramagnetic phase and those that develop in the vicinity of the re-entrant spin glass phase. The region where we observe a large hysteresis between cooling and re-heating may be a region where the two types of correlations coexist in proportions that depend on the thermal history. In the cooled state, this region corresponds mainly to a ferromagnetic pattern whereas in the re-heated state, it corresponds mainly to a spin glass pattern. We believe that the development of these spin glass correlations at low temperature is responsible for the erasure of the memory of any previous aging in the short range ferromagnetic state.

## V Discussion

The series of experiments presented in this paper illustrates how the static and dynamic properties of a ferromagnet, the $`CdCr_2S_4`$ are influenced by the introduction of site disorder. In a non-disordered ferromagnet, the susceptibility is mainly related to the domain pattern in the sample via the demagnetizing field, and the out-of-phase ac susceptibility gives more specific informations on the stiffness and the density of the domain walls. In this case, dynamic properties simply reflect the growth of the domains with time, which mainly proceeds by wall displacements. This phenomenon which is only related to the surface tension of the walls is a fast process.

The introduction of pinning disorder, such as site dilution or structural defects, changes drastically this picture Balents . The frustration which arises from the competition between the elastic energy associated with the wall deformation (which tends to favor a smooth interface) and the pinning energy associated with the disorder (which favors a rough interface) results in a drastic slowing down of dynamical processes. A domain wall has now many configurations between which it can make thermally activated hops. The wall displacements hindered by the frustration then proceed by reconformations of some parts of the wall which roughly correspond to jumps from one pinning site to another. In the presence of a driving magnetic field which forces the domain growth (a field ramp for exemple), this phenomenon is commonly known as the Barkhausen noise. In contrast, without any driving field, the overall domain growth can be extremely slow and one can observe the slow reconformations of the domain walls in a static pinning disorder without any notable growth of the domains.

Actually, the dynamics of pinned elastic interfaces has many similarities with that of spin-glasses. Theoretical arguments Balents  suggest that their energy landscape is hierarchical with small length scale $`l`$ reconformations corresponding to hoping of small energy barriers $`E(l)\mathrm{{\rm Y}}l^\theta `$. In spin glasses, the rejuvenation effect upon cooling and the memory when re-heating are usually ascribed to a hierarchical organization of the metastable states Hierarchy . When the temperature is lowered, the system remains in a deep well (memory effect), while new subwells appear, inducing new aging processes (rejuvenation effect). A similar hierarchical scheme is expected for the dynamics of a pinned domain wall. As time elapses at fixed temperature, the wall equilibrates on longer and longer length scales (aging), while shorter length scale processes are fluctuating in equilibrium. When the temperature is lowered, the conformation of the wall on large length scale freezes (allowing for the memory upon re-heating) and the equilibration now restarts on shorter length scales, which are no longer in equilibrium because their Boltzmann weight has changed (rejuvenation). In parallel with these hierarchical reconformation processes of the walls, the average domain size may grow with time. In that case, the disorder seen by the domain wall is changing with time and obviously, this net motion tends to erase the memory of the reconformations.

The above scenario accounts well for the observed behavior in the pure $`x=1.00`$ and weakly diluted $`x=0.95`$ samples SGFerro , and also that of some disordered dielectric crystals Levelut . In both $`x=1.00`$ and $`x=0.95`$ samples, aging and rejuvenation are clearly found in parallel with a weak memory of aging which is erased by domain growth during a long excursion to lower temperatures. The case of the more disordered $`x=0.90`$ sample, described here in details, is interesting since it shows that the memory effect is stabilized by the disorder and supports the scenario described above. The stronger the pinning of the domain walls, the slower their overall displacement, the better the memory of the domain wall reconformations. This memory can nevertheless be erased by a low temperature excursion close to the reentrant spin glass transition, which indicates that the spin glass order establishing at low temperature is incompatible with the short range ferromagnetic order developing above the re-entrant spin glass transition temperature.

It is tempting to extend this scenario of hierarchical wall reconformations in a pinning disorder to the case of spin glasses, because it provides us with a simple explanation for the rejuvenation and memory phenomena in the real space of spins without invoking temperature chaos arguments Domains ; Lemaitre  (see 2dXY ; Berthier ). In a spin glass, the nature of these walls is not as clear as in a ferromagnet, and remains an open question. They may be related to the non trivial sponge-like excitations recently discussed from the results of 3d spin-glass simulations Martin . It would be interesting to test the effect of temperature changes on such excitations.

Finally, let us mention that our results are consistent with other investigations on the re-entrant ferromagnet $`(Fe_{0.20}Ni_{0.80})_{75}P_{16}Al_3`$ and also on the disordered manganite $`Y_{0.7}Ca_{0.3}MnO_3`$ FerroUppsChaos . The former sample ressembles our $`x=0.90`$ compound regarding the temperature dependence of the susceptibility (rounded plateau in the ferromagnetic region); the absence of memory effect is probably due to the proximity of the re-entrant spin glass phase transition.

## VI Conclusion

In this article, we have studied the slow dynamics of the ferromagnetic phases of the $`CdCr_{2x}In_{22x}S_4`$ system for $`x=1.00`$, $`x=0.95`$ and $`x=0.90`$ by means of ac susceptibility and magnetization measurements. We found that increasing the disorder strength induces a slowing down of the ac response of the ferromagnetic phases resulting in an increase of the low frequency dissipation. Using relaxation procedures developed for the study of the out of equilibrium dynamics of spin glasses, we have found an aging behavior of the low frequency ac susceptibility both in the ferromagnetic phases and in the re-entrant spin glass phases, with the same qualitative features as in conventional spin glasses .

We have searched for rejuvenation and memory phenomena in the ferromagnetic phases of the studied samples. Whereas the weakly disordered $`x=0.95`$ compound displays only a weak memory of aging (rapidly erased by an excursion at lower temperatures), the more disordered $`x=0.90`$ compound shows a more robust memory of aging which can only be erased by the growth of spin glass correlations in the vicinity of the re-entrant spin glass transition. Our results support a scenario in which, aging, rejuvenation and memory are described in terms of hierarchical reconformations of elastic walls in a random pinning disorder. In this picture, the memory is contained in the large length scale conformation of the walls and is erased by the growth of the domains. Our results show that an increase in the disorder strength tends to reduce the domain growth and allows to observe clear rejuvenation and memory effects. The extension of this wall reconformation scenario to the case of spin glasses raises interesting questions such as the nature of the domains and the walls.

Acknowledgements

We are grateful to X. Colson for his active participation to this work. We also wish to thank J.-P. Bouchaud, F. Bert, D.Hérisson, M. Ocio for stimulating discussions during this work, L. Berthier and M. Noguès for important remarks on the manuscript, and L. Le Pape for his technical assistance.


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# Moving discrete breathers in a Klein–Gordon chain with an impurity

## I Introduction

A nonlinear phenomena which has been paid a lot of attention during recent years concerns to the localisation of oscillations in discrete nonlinear Klein–Gordon lattices. Since the discovery of intrinsic localised modes or *discrete breathers* by Sievers and Takeno Sievers and Takeno (1988), they have been found in a great number of systems. MacKay and Aubry MacKay and Aubry (1994) proved the existence of discrete breathers in Klein–Gordon lattices and established a method for calculating them as exact solutions of the dynamical equations (for a review, see Flach and Willis (1998); Aubry (1997)). In addition, these localized oscillations, under certain conditions, can move and transport energy and they are usually called *moving breathers* Chen et al. (1996); Aubry and Cretegny (1998); Cuevas et al. (2002a); Ibañes et al. (2002); Cuevas et al. (2002b).

A method used for calculating discrete breathers in Klein–Gordon lattices consists in approximating the dynamical equations by a Nonlinear Schrödinger Equation (NLS) and the moving breather by an envelope soliton. One problem that had been studied using the NLS limit concerned to the interaction of moving breathers with an impurity supposing that the breather has a small amplitude Forinash et al. (1994). However, moving breathers involve oscillations of large amplitude, which implies that the NLS approximation may not be as accurate as expected. The aim of this paper is to study the influence of an impurity in the movement of discrete breathers in a Klein–Gordon chain, i.e. using the dynamical equations without any approximation, a problem which has not been yet undertaken.

In Klein–Gordon lattices, the local modes due to an impurity and the localized modes due to the nonlinearity of the lattice can be considered equivalent entities Archilla et al. (1999); Cuevas et al. (2001). This fact suggests that a moving breather can exhibit an interesting behaviour when interacts with an impurity. As a matter of fact, we have found that the moving breather can cross the impurity, can be reflected by it (being able to let the impurity excited), or can be trapped, generating a local depository of energy. The results obtained in our study show that it is necessary the resonance of the moving breather with a nonlinear local mode (i.e. a discrete static breather centred in the impurity site) in order to generate a trapped breather.

This behaviour is qualitatively similar to the observed in the NLS approximation Forinash et al. (1994). However, the ranges of the values for which the different phenomena occur are rather different. Furthermore, the most remarkable difference between their approximation and our results is that in they obtained that the trapping is due to a resonance with a linear local mode, whereas in our case, the resonance must involve a nonlinear local mode.

In addition, we have observed the non existence of trapping phenomena even though resonance with the nonlinear local mode occur. We have also observed that in this case the tails of the nonlinear local mode and the lineal local mode have different vibration patterns. As a consequence, we conjecture that both tails must have the same vibration pattern in order that the trapping occur.

## II Model and solutions generation

### II.1 Formulation of the model

In order to study the effects of impurities on breather mobility, we consider a simple model where moving breathers can be generated, that is, a Klein–Gordon chain with nearest neighbours attractive interaction Chen et al. (1996); Aubry and Cretegny (1998), whose Hamiltonian is given by:

$$H=\underset{n}{}\left(\frac{1}{2}\dot{u}_n^2+V_n(u_n)+\frac{1}{2}C(u_nu_{n1})^2\right),$$
(1)
where $`u_n`$ represents the displacement of the n-th particle with respect to its equilibrium position, $`C`$ is a coupling constant and $`V_n(u_n)`$ is the on–site potential at the n-th site. We choose $`V`$ as the Morse potential, i.e., $`V_n(u)=D_n(e^u1)^2`$, which proves to be a very suitable one to obtain moving breathers Aubry and Cretegny (1998); Cuevas et al. (2002a, b). $`D_n`$ represents the well depth in the n-th site. An impurity will be introduced in the chain by means of an inhomogeneity in the 0-th well, i.e., $`D_n=D_o(1+\alpha \delta _{n,0})`$, with $`\alpha `$ being a parameter which gives account of the magnitude of the impurity. It takes its values in the interval $`[1,\mathrm{})`$. Hereafter, we will consider $`D_o=1/2`$. Notice that the impurity can be also introduced in the coupling. We have checked that the results are qualitatively the same and will be published elsewhere.

This kind of chain has been used as a simple model of DNA dynamics; in that context it is usually referred to as Peyrard-Bishop model Peyrard and Bishop (1989). In the framework of this model, the variables $`u_n`$ represents the transverse stretching of the hydrogen bonds connecting the two bases, $`D`$ is the dissociation energy of a base pair, and $`C`$ is the stacking coupling constant.

This Hamiltonian leads to the dynamical equations

$$F(\{u_n\})\ddot{u}_n+V_n^{}(u_n)+C(2u_nu_{n+1}u_{n1})=0.$$
(2)
These equations have two kinds of solutions, linear ones, which correspond to oscillations of small amplitude, and nonlinear ones, which correspond to intrinsic localised modes (discrete breathers).

### II.2 Linear modes

The dynamical equations can be linearised if the amplitude of the oscillations is small. Thus, the equations (2) can be written as:

$$\ddot{u}_n+\omega _\mathrm{n}^2u_n+C(2u_nu_{n+1}u_{n1})=0,$$
(3)
where $`\omega _\mathrm{n}`$ is the natural frequency of the n-th oscillator in the harmonic limit. It is related to the well depth of the Morse potential in the form $`\omega _\mathrm{n}^2=2D_n`$, which implies that $`\omega _\mathrm{n}^2=\omega _\mathrm{o}^2(1+\alpha \delta _{n,0})`$, with $`\omega _\mathrm{o}=1`$ as $`D_o`$ has been chosen to be $`1/2`$.

Thus, this equation has $`N1`$ solutions (being $`N`$ the number of particles) corresponding to linear extended modes (LEMs) and one localised solution, which corresponds to a linear local mode (LLM) whose origin lies in the introduction of the impurity.

The frequencies of the LEMs can be calculated supposing that they are plane waves ($`u_n(t)=e^{i\omega (q)tnq}`$) and that the LLM decays in the space following a dependence of the form $`u_n(t)=e^{i\omega _\mathrm{L}t}r^n`$ Forinash et al. (1994). Thus, the frequencies of the LEMs are given by:

$$\omega (q)=\sqrt{\omega _o^2+4C\mathrm{sin}^2\frac{q}{2}},$$
(4)
where $`q`$ is the LEM wave vector and takes its value in the interval $`(0,\pi ]`$ if $`\alpha <0`$ and in $`[0,\pi )`$ if $`\alpha >0`$.

The frequency of the LLM is given by the relation Forinash et al. (1994):

$$\omega _L^2=\omega _\mathrm{o}^2+2C+sgn(\alpha )\sqrt{\alpha ^2+4C^2}.$$
(5)
It is worth remarking that LLMs with $`\alpha <0`$ have wave vector $`q=\pi `$ (the particles vibrate in zigzag) while the solution for $`\alpha >0`$ corresponds to $`q=0`$ (the particles vibrate in phase). Figure 1 shows the dependence of the frequencies of the linear modes with $`\alpha `$, where the isolated frequencies corresponds to the LLMs.

The knowledge of the frequency of the LLM is very important in order to explain the properties of moving breathers, because discrete breathers and local modes can be viewed as equivalent entities when the interplay between nonlinearity and inhomogeneity is considered Archilla et al. (1999); Cuevas et al. (2001).

### II.3 Static and moving breathers

A static breather can be obtained solving the full dynamical equations. It can be done using common methods based on the anticontinuous limit Marín and Aubry (1996). The implementation of these methods basically consists in calculating the orbit of an isolated oscillator at a fixed frequency $`\omega _\mathrm{b}`$, and using this solution as a seed for solving the complete dynamical equations by means of a Newton–Raphson continuation method.

If the oscillator initially chosen is the corresponding to the impurity, a static breather centred in the impurity is obtained. It will be called *nonlinear local mode* (NLLM), in analogy to the linear local modes (LLMs) that appear in the spectrum of linear modes (equation 5).

Once a static breather is calculated, it can be moved under certain conditions. There exists a systematic method to calculate moving solutions Chen et al. (1996); Aubry and Cretegny (1998) which consists in adding to the velocities of the static breather a perturbation of magnitude $`\lambda `$ colinear to the direction of the pinning mode, and letting the system evolve in time. This perturbation breaks the shift translational symmetry of the system. In addition, the coupling of the static breather must be strong enough Cuevas et al. (2002a).

In this paper, we have studied breathers with a frequency $`\omega _\mathrm{b}=0.8`$ and a coupling $`C=0.13`$ although this value has been increased in order to make some comparisons. These values of the parameters provide moving breathers with low phonon radiation for values of the perturbation $`\lambda 0.2`$. We have considered different impurities given by different values of parameter $`\alpha `$ in the range $`1\alpha 1`$.

## III Interaction of moving breathers with impurities

### III.1 Numerical observations

We have studied the behaviour of moving breathers when they interact with an impurity. This study is performed varying the value of the magnitude of the impurity $`\alpha `$, and shows an interesting behaviour. We have found some critical values of parameter $`\alpha `$ ($`\alpha _1<\alpha _2<\alpha _3<0`$) which separate the different regimes (see figure 2):

1. *The impurity acts as a potential barrier*. It occurs whenever $`\alpha >0`$ and $`\alpha (1,\alpha _1)`$ with $`\alpha _1<0`$. The breather rebounds when reaches the impurity and let it excited during a brief time lapse. The amplitude of this excitement decreases when the impurity is higher, i.e., when $`|\alpha |`$ increases. Note that if $`\alpha 0`$, the potential barrier can be observed, i.e., the breather can cross the impurity provided the translational velocity is high enough, as it occurred in Cuevas et al. (2002b).
2. *The impurity is excited and the breather rebounds*. It occurs for $`\alpha (\alpha _1,\alpha _2)`$. The energy of the excited impurity is higher than the energy of the NLLM for the considered value of $`\alpha `$ and whose frequency is the same as the incident moving breather, $`\omega _\mathrm{b}`$. It implies that the excited impurity will vibrate with a frequency smaller than $`\omega _\mathrm{b}`$ because the on–site potential is soft. This behavior is shown in figure 3.
3. *The breather is trapped by the impurity*. It occurs in the interval $`\alpha (\alpha _2,\alpha _3)`$. When the breather is near the impurity, it is absorbed and remains trapped while its center oscillates between the neighbouring sites. The trapping of the breather is shown in figure 4. Furthermore, the trapped breather is quasi-periodic, as can be deduced from its Fourier spectrum (Figure 5), and, as a consequence, it emits a great amount of phonon radiation.
4. *The impurity acts as a potential well*. It occurs when $`\alpha _3<\alpha <0`$ and manifests as an acceleration of the breather when reaches a site near the impurity, and a deceleration when the impurity is crossed.

All of these cases have been studied using a breather with $`\omega _\mathrm{b}=0.8`$ and $`C=0.13`$. The translational velocity of the moving breathers has been chosen small so as not to have high phonon radiation. The critical values of $`\alpha `$ cannot be determined because the transition between the different behaviours are diffuse. An estimation of the critical values for $`\omega _\mathrm{b}=0.8`$ and $`C=0.13`$ are: $`\alpha _10.54`$, $`\alpha _20.49`$ and $`\alpha _30.02`$. These regimes have also been found for different values of the frequency, although the value of $`\alpha _2`$ decreases with $`\omega _\mathrm{b}`$.

If the coupling is higher, the phonon radiation is not so low and can mask some of the effects.

### III.2 Justification of some results

Some of the results exposed in the last subsection can be explained from the properties of the NLLMs. Concretely, if a continuation of the static breathers is performed varying the parameter $`\alpha `$, a bifurcation appears for $`\alpha \alpha _c>0`$ and another one for $`\alpha \alpha _{res}<0`$. The first one is originated by a localized Floquet eigenmode which abandons the unit circle. In the second case, the breather bifurcates with the stationary solution through a pitchfork (figure 6). In this bifurcation, the outer branches correspond to NLLMs either with $`u_n>0`$ for $`t=0`$ and with $`u_n<0`$ for $`t=0`$, while the central branch corresponds to the stationary solution, i.e. all the oscillators at rest. This kind of bifurcation is different to the broken pitchforks obtained in disordered systems Archilla et al. (1999); Cuevas et al. (2001); Kopidakis and Aubry (1999). It is due to the fact that, even thought an isolated impurity breaks the shift translational symmetry of the system, it does not break the mirror symmetry. Consequently, the pitchforks are not broken.

The value $`\alpha _{res}`$ coincides with the point at which the frequency of a LLM is the same as the frequency of the NLLM, i.e., $`\omega _\mathrm{L}=\omega _\mathrm{b}`$. This value can be calculated from the equation 5 as a function of $`\omega _\mathrm{b}`$ and $`C`$:

$$\alpha _{res}=\sqrt{(\omega _\mathrm{b}^2\omega _\mathrm{o}^2)(\omega _\mathrm{b}^2\omega _\mathrm{o}^24C)}$$
(6)
Thus, for $`C=0.13`$ and $`\omega _\mathrm{b}=0.8`$, $`\alpha _{res}=0.5628`$ which is lower than $`\alpha _1`$. We have also checked for different values of the frequency and coupling and we have found that there are situations where $`\alpha _1`$ is slightly smaller that $`\alpha _{res}`$ but always $`\alpha _{res}<\alpha _2`$. However, the trapped breather does not exist for $`\alpha >0`$. It indicates that $`\alpha (\alpha _{res},0)`$ is a necessary condition for the existence of the trapped breather.

A conjecture for the existence of trapped breathers when $`\alpha <0`$ is the following: in this case, the LLM has $`q=0`$, and also all the particles of the NLLM vibrates in phase; this vibration pattern indicates that the NLLM bifurcates from plane waves with $`q=0`$ Flach (1996), i.e., the NLLM bifurcates from the LLM and it will be the only localized mode that exists when the impurity is excited for $`\alpha >\alpha _{res}`$. In fact, we have performed successful a continuation from the NLLM to the LLM at constant action and disorder Archilla et al. (1999); Cuevas et al. (2001). Thus, when the moving breather reaches the impurity, it can excite the NLLM. However, Doppler effect makes the NLLM ‘see’ the moving breather with a frequency different from $`\omega _\mathrm{b}`$ so that when they interact, they merge into an entity (the trapped breather) with two frequencies.

When $`\alpha _{res}<\alpha <\alpha _2`$, the NLLM is unable to create a trapped entity. It is observed that the energy of the NLLM decreases with $`|\alpha |`$, so, there must be threshold for the energy of the NLLM in order that the trapped breather can exist. The narrow window of impurity excitements observed in the interval $`(\alpha _1,\alpha _2)`$ can be due to a resonance of the moving breather with the NLLM of frequency slightly smaller that $`\omega _\mathrm{b}`$ and, therefore, the excited impurity has a higher energy than the NLLM of frequency $`\omega _\mathrm{b}`$, as we are considering a soft potential.

For $`\alpha <\alpha _{res}`$, the trapped breather cannot be generated, and the moving breather always rebounds. In addition, the NLLM does not exist. Therefore, there must be connection between both facts, i.e., the existence of the NLLM will be a necessary condition in order to obtain a trapped breather.

If $`\alpha >0`$, the scenario is different. In this case, the LLM has $`q=\pi `$ but the NLLM’s particle vibrate again in phase, that is, the NLLM will not bifurcate from the LLM. Thus, there are two different localized modes for $`\alpha >0`$: the LLM and the NLLM. But, actually, the equations that govern the system are nonlinear, so the linear modes can only correspond to low-amplitude oscillations. In the case of the NLLM, the linear regime corresponds to the tails. Thus, if the moving breather reaches the impurity site, it will excite the NLLM, its tails and also the tails of the LLM. But the latter vibrate in zigzag. As a consequence, there will be two different linear localized entities: the tails of the LLM (vibrating in zigzag) and the tails of the NLLM (vibrating in phase). Therefore, we conjecture that the existence of both linear localized entities at the same time may be the reason why the impurity is unable to trap the breather when $`\alpha >0`$.

To summarize, the existence of a NLLM for a certain value of $`\alpha `$ is necessary for the existence of trapped breathers. However, if there exists a LLM with a different vibration pattern to the NLLM, the trapped breather does not exist.

## IV Conclusions

We have studied the interaction of a moving discrete breather in a Klein–Gordon chain with an impurity at rest. A rich behaviour is observed when the breather reaches the impurity. It can be summarized as follows: a) the impurity can act as a potential barrier or a potential well; b) the breather can be reflected by the impurity which is let excited; c) the impurity can trap the breather, making it quasi-periodic.

A previous work made using the NLS approximation Forinash et al. (1994) showed that moving breathers interacting with an impurity have qualitatively the same behaviour as the observed by us. There is, however, a very important difference between this work and ours. It relies in the fact that in the NLS approximation, a resonance between the frequencies of the moving breather and the linear local mode created by the impurity is needed whereas in our case, this resonance prevents the breather from being trapped. In our case, the trapping phenomena is owed to the resonance between the moving breather and a nonlinear localised mode.

The model used in our study is the same as the studied by Peyrard and Bishop to explain DNA denaturation Peyrard and Bishop (1989). It indicates that our results can be applied to study some properties of DNA chains. For instance, if a moving breather is generated in a DNA chain, it can be trapped by an impurity, and act as a precursor of the transcription bubble Ting and Peyrard (1996). This trapped breathers can interact with another breathers and collect energy Bang and Peyrard (1996).

The impurity in DNA can have two different origins. The first one consists in a modification of the well depth due to the action of a transcription enzyme through a chemical effect, as explained in Ting and Peyrard (1996). The second one relies in the fact that the A-T base pairs have 2 hydrogen bonds whereas the C-G base pairs have 3 hydrogen bonds. So, it can be supposed that in the first case, the well depth of the Morse potential is 2/3 of the second case. From the results of this paper, trapping does not occur when the well depth in the impurity is higher than in the homogeneous area. It implies that trapping can occur in a chain of C-G pairs with an impurity of A-T. Nevertheless, the main fault of these mechanisms is the assumption of homogeneity in DNA, where the role of the inhomogeneity due to the genetic code is known to be crucial in the dynamics Salerno and Kivshar (1994). However, the study of the effects of impurities is the first step to understand the dynamics of moving breathers in DNA sequences.

## Acknowledgments

This work has been supported by the European Commission under the RTN project LOCNET, HPRN-CT-1999-00163. We acknowledge PG Kevrekidis for his useful comments. JC acknowledges an FPDI grant from ‘La Junta de Andalucía’.


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# Lepton flavor violation decays with the fourth generation neutrino 𝜈'

## Acknowledgments

This research is supported by the the Chinese Postdoctoral Science Foundation and CAS K.C. Wong Postdoctoral Research Award Fund. We are grateful to Prof. X.M Zhang for useful discussions.


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# Unusually Weak Diffuse Interstellar Bands toward HD 62542

## 1 Introduction

Following the first reported detection of diffuse interstellar bands (DIBs) some 80 years ago (Heger 1922), several different approaches were made to the task of identifying the carriers (see Herbig 1995 or Snow 1995, 2001 for recent reviews). During the era of photographic spectroscopy, the principal approach was to examine correlations of the strengths of the DIBs with other interstellar quantities, but such studies rarely led to definitive conclusions (Snow, York, & Welty 1977). With the advent of electronic detectors in the 1970s, however, it became possible to measure the strengths and profiles of the DIBs more accurately. Differences in profile shape among the DIBs and differences in relative DIB strength in different interstellar environments strongly suggest that the DIBs are due to a variety of carriers (Krełowski & Walker 1987; Josafatsson & Snow 1987; Krełowski & Sneden 1993; Cami et al. 1997). Some uncertainties remain, however, as to which of the DIBs are more closely related, because of differences both in the sightlines and DIBs considered and in how the DIBs are defined and measured in the various studies.

The breadth of the DIBs has often been ascribed to broadening by predissocation, but this requires the DIB carriers to be continually replenished at a rapid rate to maintain the necessary density of absorbers. Douglas (1977) and Smith, Snow, & York (1977) proposed a solution for this dilemma: the DIB carriers could be large molecules undergoing internal conversion, a process routinely seen in laboratory spectra. Laboratory and theoretical studies of small and large ($`>`$10 atomic nuclei) molecules are now producing specific predictions of DIB candidate lines (e.g., Foing & Ehrenfreund 1994 and Galazutdinov et al. 2000 for C60+; Tulej et al. 1998 for C$`{}_{}{}^{}{}_{7}{}^{}`$; McCarthy et al. 1997, 2000 for carbon chains; Guthe et al. 2001 for l-C3H$`{}_{}{}^{}{}_{2}{}^{}`$; Krełowski et al. 2001 for naphthalene cations). Ultra-high resolution spectra of several DIBs have revealed structure in the profiles suggestive of the rotational structure expected for large molecules (Sarre et al. 1995; Kerr et al. 1996; Ehrenfreund & Foing 1996; Krełowski & Schmidt 1997). Astrophysical studies, together with the laboratory studies, thus have shown that large molecules may well be present in interstellar clouds and must be considered as possible candidates for some of the DIBs (Salama & Allamandola 1992a,b; Snow et al. 1998; Sonnentrucker et al. 1997, 1999).

We are currently assembling an extensive dataset of DIB information of much higher quality than has previously been available (Thorburn et al., in prep.). For most of the 60 stars in this survey, our optical spectra cover the range from 3700 to 10,500Å, at a signal to noise ratio $``$1000 between 5780 and 7000Å. For some Southern stars (including the one discussed in this paper), the spectra have less complete spectral coverage and lower S/N, however. Our goal is to assemble a high-quality dataset — including DIB strengths and many other interstellar parameters — for a set of sightlines specifically selected to sample a wide variety of environments. Our hope is that with sufficient data quality (allowing us to measure very weak DIBs and fine details of the DIB profiles), careful consideration of the continua near the DIBs, and more complete coverage of the other interstellar parameters, we may be able to identify definite dependences and relationships among the DIBs, between the DIBs and other interstellar species, and between the DIBs and specific physical or chemical factors characterizing the interstellar clouds.

In this paper, we report results for one particular line of sight with very unusual dust extinction properties and explore, by comparison with other lines of sight, the possible interpretations of the DIBs in this case. In the next section, we summarize what is known about the star (HD 62542) and its line of sight. In Section 3, we describe the observations and our results, while in Section 4 we discuss possible implications for understanding the DIBs.

## 2 The Line of Sight toward HD 62542

The star HD 62542 lies behind material associated with the Gum Nebula (Cardelli & Savage 1988; Cardelli et al. 1990; Whittet et al. 1993; Churchwell et al. 1996). Whittet et al. estimated a spectroscopic distance of 405 pc, based on an adopted B3 V spectral type. The distance estimate from Hipparcos — 246 pc, with a one-$`\sigma `$ uncertainty range from 212 to 294 pc — is more consistent with the slightly later B5 V type adopted by Cardelli & Savage, however.

Allowing for the uncertainties in spectral type, the color excess $`E(BV)`$ = 0.33–0.37, the total visual extinction AV = 1.07–1.20 mag, and the ratio of total to selective extinction RV = 2.90–3.24 (Cardelli & Savage 1988; Whittet et al. 1993; Rachford et al. 2002). The total hydrogen column density $`N`$(H I) + 2$`N`$(H2) is about 2.2 $`\times `$ 1021 cm-2 (Rachford et al. 2002).

This star has one of the most extreme ultraviolet extinction curves known, featuring a very broad, shortward-displaced 2175Å bump and an extremely steep far-UV rise — similar to that of another extreme case, HD 29647 (Snow & Seab 1980; Cardelli & Savage 1988). Those extinction curve properties are often interpreted as indicating a preponderance of small dust grains. Snow & Seab (1980), Mathis & Cardelli (1992), and Mathis (1994) have speculated that such extinction curves are produced by the addition of a thin mantle overlying the small carbonaceous grains thought to be responsible for the bump and the far-UV extinction. While a strong water ice feature has been observed toward the more heavily reddened HD 29647 (AV = 3.6 mag; Goebel 1983), water ice mantles may not significantly affect the 2175Å bump (Mathis 1994). Given the much smaller value of AV toward HD 62542, we think detection of water ice in this sightline is unlikely — but would still recommend looking for it.

High resolution spectra of Na I and K I suggest that most of the interstellar material in this line of sight is concentrated in a single cloud at $`v_{}`$ = 14 km s-1; additional weaker components are seen in Na I and Ca II (D. Welty et al., in prep.). The column densities of CH, CN, and C2 in the main cloud are quite high for the amount of reddening; CH+ is not detected, however (Cardelli et al. 1990; Gredel, van Dishoeck, & Black 1993). Various diagnotics, interpreted via theoretical models, have suggested total hydrogen (H + H2) densities $`n_\mathrm{H}`$ ranging from several hundred per cm3 (Black & van Dishoeck 1991) to 10,000 cm-3 (Cardelli et al.) in the main cloud. The C2 rotational level populations and the relative weakness of the mm-wave CN emission, however, suggest $`T`$ $``$ 50 K and $`n_\mathrm{H}`$ in the range 500–1000 cm-3 (Gredel et al. 1991, 1993) — also rather high for a cloud with such moderate extinction. Spectra obtained with FUSE indicate a molecular hydrogen column density of 5.9 $`\times `$ 1020cm-2, with a corresponding hydrogen molecular fraction $`f`$(H2) = 2$`N`$(H2)/\[$`N`$(H I) + 2$`N`$(H2)\] = 0.60, averaged over the line of sight (Rachford et al. 2002). The molecular fraction is somewhat uncertain, however, owing to uncertainties in $`N`$(H I). If the density of the cloud is of order 500–1000 cm-3, then the extent of the cloud along the line of sight is only about 0.5–1.0 pc. This cloud thus may be viewed as a small, dense knot within the filamentary structure associated with the Gum nebula. Cardelli & Savage (1988) and Cardelli et al. (1990) proposed that the more diffuse outer layers of the cloud may have been stripped by the passage of stellar winds and/or shocks within the Gum nebula.

## 3 Observations and Results

Table 1 lists the stars compared in this paper, with spectral type, V magnitude, color excess, and a general characterization of the UV extinction curve. Kappa Cas was chosen because it has nearly the same $`E(BV)`$ and AV as HD 62542. It was the obvious difference between the DIBs toward $`\kappa `$ Cas and those toward HD 62542 that led us to write this paper — the bands discussed in this paper are weaker in HD 62542 by factors of at least 4–8, despite the very similar $`E(BV)`$ and AV. Rho Oph D and $`\theta ^1`$ Ori C were chosen for comparison because they belong to the class of stars with shallow far-UV extinction curves (Fitzpatrick & Massa 1990) noted for having weak DIBs. HD 183143 is included because it has frequently been cited in the literature as a standard for strong DIBs, for example in the compilations of Herbig (1975), Jenniskens & Désert (1994), and Tuairisg et al. (2000); HD 215733 is included as a lightly reddened star observed with the same instrument as HD 62542.

The spectra of HD 62542 and HD 215733 were obtained using the University College London Echelle Spectrograph (UCLES; Walker & Diego 1985) on the Anglo-Australian Telescope in 1998 September. Sections of 23 orders, giving incomplete coverage of the spectrum between 5075 and 10,295Å, were recorded on the MIT/LL2 CCD (2048$`\times `$4096; 15$`\mu `$m pixels). While the primary motivation for these observations was to obtain spectra of the interstellar Na I D and K I $`\lambda `$7698 lines, a number of DIBs also lie within the spectral coverage. The spectra were extracted from the raw CCD images using standard procedures within IRAF. The spectral resolution is 5 km s-1; for both stars, the S/N is of order 70 between about 5700 and 8800Å.

The spectra of $`\kappa `$ Cas, $`\theta ^1`$ Ori C, $`\rho `$ Oph D, and HD 183143 were obtained at Apache Point Observatory (APO) with the Astrophysical Research Consortium (ARC) echelle spectrograph (ARCES). The ARCES spectra are recorded at a resolution of 8 km s-1, using a 1.6 arcsecond slit. The CCD is a 2048$`\times `$2048 Site/Tektronix device with 24$`\mu `$m pixels. Multiple spectra, with exposure times $``$30 min, were obtained to achieve S/N $``$ 1000 at 5780Å. For reddened stars, the S/N is greater than 100 throughout the entire range between 3600 and 10,000Å. The spectra were extracted using IRAF, with special settings to accommodate the narrow (FWHM $``$ 3.3 pixels), closely spaced ($``$10 pixels, center to center) spectral orders and the aliasing caused by the fact that not all orders can be simultaneously lined up along the rows of CCD pixels. All of the spectral orders passed by the system fit on the CCD. Identical spectral regions from adjacent orders were weighted and co-added, after standard wavelength calibrations and one-dimensional flat field corrections were applied, to produce a blazeless spectrum covering the range 3600–10,000 Å. Details of the spectrograph and the routine observing procedures are discussed by York, Hildebrand, Hobbs et al. (in prep.).

Figures 12, and 3 show regions from 5725–5815Å, 6200–6300Å, and 6570–6670Å. These wavelength regions are the only ones included in the UCLES spectra that contain strong, well-studied DIBs. The top two spectra in each figure are noiseless atlas spectra (model representations of a flat continuum and Gaussian components designed to yield features comparable in strength to those seen toward HD 183143) from Jenniskens & Désert (1994; hereafter JD94) and Tuairisg et al. (2000; hereafter T00). The atlases represent averages over several stars, with lines scaled in strength by the ratio of $`E(BV)`$ in HD 183143 to that for each of the other stars. The stellar spectra have been binned to a resolution of 8 km s-1, shifted so that the interstellar K I lines are at 0 km s-1, and plotted in order of increasing AV (top to bottom). The dots on either side of the DIBs in the spectra of HD 183143 denote the end points of the linear continua used for measuring equivalent widths. The sharp features that occur in all stellar spectra at nearly the same wavelengths are telluric lines. While there are many weak DIBs seen in common between JD94, T00, and our spectrum of HD 183143, there are also features that do not match up. Some of these features are stellar lines (e.g., at 6579 and 6582Å) which, of course, do not appear in the atlases; others are weak DIBs that are not well represented in the two atlases. In addition, since the relative strengths of the DIBs can vary from star to star (Herbig 1995, and references therein), the averaged atlas spectra do not necessarily match the actual spectrum of HD 183143 itself. A more complete list of DIBs, which resolves discrepancies between previous atlases and our new spectra, is in preparation (York et al., in prep.).

The DIB at 6284Å deserves special mention, since it is partially blended with a telluric band of O2, and has long been recognized as a difficult DIB to measure cleanly. In our data, however, the spectral resolving power is sufficient to clearly separate the narrow O2 band features from the much broader DIB, and there was thus no difficulty in excising the telluric absorption in order to measure the equivalent width of the diffuse band.

The equivalent widths of five relatively strong, well-known DIBs for all six lines of sight are listed in Table 2, together with the ratio of total to selective extinction (RV), the total visual extinction (AV), and the column densities of H I, H2, K I, and various molecular species. Several footnotes to the table list measurements of the strengths of those DIBs from selected recent references, for comparison; a more thorough comparison of our new DIB measurements with previous values will be given by York et al. (in prep.).

## 4 Discussion

It is apparent from Table 2 and from Figures 1– 3 that the strengths of the 5780, 5797, 6270, 6284, and 6614Å DIBs do not increase monotonically with AV — at least for this small (and likely biased) sample of six lines of sight. As noted earlier, HD 2905 ($`\kappa `$ Cas) and HD 62542 have essentially identical AV, but the equivalent widths of all five DIBs are weaker toward HD 62542 by factors of at least 4–8. None of those bands is detected toward HD 62542, given the S/N in our data, and we can list only upper limits in Table 2.111 Several other, weaker DIBs identified in the literature (e.g., those at 6203 and 6660Å) also are absent toward HD 62542, with upper limits similar to those for the other narrow DIBs. The nearly 70% increase in AV between HD 62542 and $`\rho `$ Oph D is accompanied by increases in the strengths of all five DIBs by factors of at least 2–6. The bands toward $`\rho `$ Oph D are about half as strong as those toward $`\kappa `$ Cas, even though AV is higher toward $`\rho `$ Oph D by a factor of almost 1.7. The DIBs toward $`\theta ^1`$ Ori C are even weaker (except 6284), even though AV is slightly higher than toward $`\rho `$ Oph D. On the other hand, AV is greater by a factor of almost 3.9 toward HD 183143 than toward $`\kappa `$ Cas, and the five DIBs are stronger by factors of 2.5–3.4 — more consistent with a nearly linear relationship.

Krełowski et al. (1999) have compared the equivalent widths of the DIBs at 5780 and 5797Å with those of the strongest lines from the diatomic molecules CH (4300Å) and CH+ (4232Å). In Figure 4, we plot the strengths (log Wλ) of these two DIBs versus the column density of CH. The DIB strengths are primarily from our survey, but with some values from Josafatsson & Snow (1987), Herbig (1993), and Krełowski et al. (1999); the values for $`N`$(CH) are from various references (see the appendix to Welty & Hobbs 2001), from fits to new high-resolution spectra of translucent sightlines (Welty et al., in prep), and from our survey. There is at best a weak correlation between the strength of the 5780Å DIB and $`N`$(CH); the relationship between the strength of the 5797Å DIB and $`N`$(CH) is somewhat tighter, with steeper slope. Toward HD 62542, however, both DIBs are clearly much weaker than for other sightlines with comparable $`N`$(CH). The DIBs toward HD 62542 are also anomalously weak when compared with the column densities of C2 and CN, but such comparisons cannot be made with $`N`$(CH+), as only an upper limit is available.

In view of the similarities in UV extinction toward HD 62542 and HD 29647, comparisons of other interstellar properties for these two lines of sight are of interest. It is difficult to assess the atomic and molecular abundances toward HD 29647, due to its later spectral type (B8 V), its confusing spectrum (Hg-Mn), the near-perfect velocity match between the star and the main interstellar cloud in the line of sight (Adelman et al.2001), and the star’s very low $`v`$sin$`i`$, which makes stellar lines appear nearly as narrow as interstellar lines in most currently available spectra (e.g. Crutcher 1985). There is insufficient far-UV flux for FUSE observations, and it can be difficult to interpret, or even to identify unambiguously, some of the interstellar lines. Owing to the breadth of the DIBs, however, it is possible to determine the DIB strengths toward this star. It was previously established that the 5780 and 5797Å DIBs toward HD 29647 are unusually weak, but might be present with very narrow profiles (Snow & Seab 1991). More comprehensive data to be presented by Snow et al. (in prep.) cover all the DIBs in Figs. 13 here, and yield the following results: the 5780 and 5797Å DIBs are present, with 5780 strongly dominant over 5797; the 6284Å band is weakly present, with normal width; and the 6614Å band is present but very weak. The DIBs toward both stars thus are markedly weak relative to extinction, when compared to the DIBs in most diffuse cloud lines of sight reported in the literature (note that AV = 3.6 mag for HD 29647).

There is longstanding evidence in the literature that the generically strongest DIBs tend to be relatively weak in dense clouds (e.g., Wampler 1966; Snow & Cohen 1974; Adamson, Whittet, & Duley 1991; Adamson et al. 1991; Snow 1995). The current results for HD 62542 (and for HD 29647) appear to support this trend, in the extreme. The DIBs are also known to be weak, relative to extinction, in environments with intense radiation fields (Jenniskens, Ehrenfreund, & Foing 1994; Snow et al. 1995). This combination of factors — DIB weakness in dense clouds and in regions of high UV flux — leads to a picture in which the DIBs form and survive most readily either in “ordinary” diffuse clouds or in the diffuse outer layers of dense clouds (the “skin effect” discussed by Adamson et al. 1991). The weakness of the DIBs toward HD 62542 and the suggestion of Cardelli et al. (1990) that the more diffuse outer layers of the dense cloud toward HD 62542 have been stripped off are consistent with this scenario.

Of the sightlines considered in this paper, the three with “normal” DIB strengths per unit $`E(BV)`$ (HD 215733, $`\kappa `$ Cas, HD 183143) all have a number of interstellar components — of roughly comparable strength and spread out in velocity — in C I, Na I, and/or K I (Fitzpatrick & Spitzer 1997; Welty & Hobbs 2001; McCall et al. 2002). Toward $`\kappa `$ Cas and HD 183143, $`N`$(CN)/$`N`$(CH) $`<`$ 0.05 and $`N`$(CH+)/$`N`$(CH) $``$ 1.0 (Table 2) — both suggestive of relatively low densities in an ensemble of “normal” diffuse clouds. The sightlines with weak DIBs (HD 62542, $`\rho `$ Oph D, $`\theta ^1`$ Ori C), however, are characterized by somewhat different structures and/or atomic and molecular abundances. While there are a number of Na I components toward $`\theta ^1`$ Ori C, the overall $`N`$(Na I) is quite low, relative to $`N`$(H) (Welty & Hobbs 2001), and CH, CN, and CH+ have not been detected — all suggesting that those components correspond to diffuse clouds bathed in a strong ambient radiation field. The available high resolution Na I and K I spectra of HD 62542 and $`\rho `$ Oph D indicate, however, that those lines of sight are each dominated by a single strong component \[or perhaps several narrow, closely blended components for $`\rho `$ Oph D, as seen in higher resolution spectra of $`\rho `$ Oph A (Welty & Hobbs 2001)\]. The molecular column densities toward HD 62542 imply the presence of much denser gas: $`N`$(CN)/$`N`$(CH) $``$ 1.0 and $`N`$(CH+)/$`N`$(CH) $`<`$0.02; $`\rho `$ Oph D represents an intermediate case, with $`N`$(CN)/$`N`$(CH) $``$ 0.1 and $`N`$(CH+)/$`N`$(CH) $``$ 0.3.

The carriers of the DIBs considered here thus seem to require a relatively low density and/or (at most) a moderately intense radiation field (Cami et al., 1997; Sonnentrucker et al. 1997). Correlations between the strengths of the 5780 and 5797Å DIBs, $`N`$(H), $`N`$(Na I), and $`N`$(K I) suggest that the DIB carriers generally behave like dominant ions — though the weakness of those DIBs toward stars in Sco-Oph and in the Orion Trapezium region is reminiscent of the weakness of the trace neutral species there (Herbig 1993; Welty & Hobbs 2001). There also are indications that the carrier of the 5797Å DIB may be more readily destroyed (ionized?) than that of the 5780Å DIB where the radiation field is stronger (Sonnentrucker et al. 1997; Krełowski, Galazutdinov, & Musaev 1998; Welty & Hobbs 2001). Such patterns are consistent with suggestions that the DIB carriers are molecular ions — which are destroyed (through electron attachment) in dense environments (e.g., toward HD 62542) or which are not formed or maintained in clouds with weak radiation fields (e.g., Leger & d’Hendecourt 1985; Crawford, Tielens, & Allamandola 1985; van der Zwet & Allamandola 1985; Salama et al. 1996, 1999; see LePage, Snow, & Bierbaum 2001 for a recent overview and model). No specific molecule or family of molecules can be firmly identified at the present time, however. The DIB behavior argues strongly against molecular anions as the DIB carriers — at least for the stronger, more well-studied DIBs — consistent with the recent rejection of the C$`{}_{}{}^{}{}_{7}{}^{}`$ hypothesis (McCall et al. 2001; Galazutdinov et al. 2001; Sarre & Kendall 2000).

While we are tempted to associate the weakness of the DIBs toward HD 62542 with the low UV field intensity and high molecular content of the main cloud at 14 km s-1, we note that the hydrogen molecular fraction is not extremely high. The value $`f`$(H2) = 0.60 (if verified once a more accurate H I column density can be obtained) is comparable to, but not greater than, the values found for other diffuse or translucent clouds such as the main clouds toward $`\zeta `$ Oph. We hypothesize instead that the part of the main cloud toward HD 62542 that is conducive to the formation and survival of DIBs is unusually thin, sandwiched between the dense cloud that dominates the molecular absorption and the hot, low-density gas of the Gum nebula in which that cloud is immersed. In this view, the more extended diffuse neutral region where the DIB carriers would normally reside is essentially absent in this line of sight. The main cloud toward HD 29647, with somewhat stronger DIBs than those toward HD 62542, appears to be in a more quiescent region (Cardelli & Savage 1988), and thus may have a more normal outer structure.

## 5 Summary/Conclusions

A number of the diffuse interstellar bands (at 5780, 5797, 6270, 6284, and 6614 Å) commonly seen even in relatively lightly reddened lines of sight appear to be essentially absent toward the moderately reddened star HD 62542, previously known to exhibit both strong interstellar molecular lines and an unusually steep far-UV extinction curve with a weak, shifted 2175Å bump. The line of sight appears to be dominated by a single small, very dense cloud, whose more diffuse outer layers may have been stripped by stellar winds and/or shocks within the Gum nebula.

Comparisons of those five moderately strong DIBs in six lines of sight indicate that the strengths of the DIBs are not well correlated with AV, but must depend on other (as yet undetermined) properties of the interstellar clouds. For this small sample, the bands are weaker, per unit AV, for sightlines with strong CN and weak CH+, relative to CH (HD 29647, HD 62542), and are stronger for sightlines with weak CN and strong CH+ ($`\kappa `$ Cas, HD 183143) — consistent with reduced abundances of the carriers of these DIBs in denser gas. \[We note that our larger sample suggests that different DIBs can show somewhat different dependences on $`N`$(CH+)/$`N`$(CN), however.\] Moreover, the DIBs are weaker when the far-UV extinction is either very steep, and the radiation fields not enhanced (HD 62542, HD 29647) or very shallow, with a strong ambient field ($`\theta ^1`$ Ori C); the other sightline with relatively weak DIBs ($`\rho `$ Oph D) has moderately shallow far-UV extinction and (probably) a somewhat enhanced radiation field. Thus, too little or too much UV flux removes the DIB absorbers from the gas — accounting qualitatively for the very large variations in DIB strengths with AV seen in Table 2. The results presented in this paper thus extend the similar conclusions of Cami et al. (1997) to higher densities and molecular abundances. The absence of DIBs toward HD 62542, combined with similar behavior seen in other sightlines with similar interstellar conditions, suggests that molecular ions, or other species having a similar response to ambient density and radiation, are the most likely carriers of the DIBs.

We are assembling a data base for 60 lines of sight — with data on H2, CH, CH+, CN, C2, AV, $`f`$(H2), T01(H2), T35(H2); detailed component structures from high-resolution spectra of K I, Na I, CH, CH+, and CN (Welty & Hobbs 2001; D. Welty et al., in prep.); abundances of H$`{}_{}{}^{+}{}_{3}{}^{}`$ and CO (McCall et al. 2002); strengths of interstellar IR emission and absorption bands; and element abundances/depletions measured with HST and FUSE (Sonnentrucker et al., in prep.) — in order to search for correlations between the DIB strengths and other interstellar properties.

TPS acknowledges NASA grant NAG5-6758 and NASA contract 2430-60020, both to the University of Colorado. DEW acknowledges support from NASA grant NAG5-3228 to the University of Chicago. BJM acknowledges support from the Fannie and John Hertz Foundation and the Miller Institute for Basic Research in Science. PS acknowledges support from NASA contract NAS5-32985 to Johns Hopkins University. This work is based in part on observations obtained with the Apache Point Observatory 3.5 m telescope, which is owned and operated by the Astrophysical Research Consortium.


text:
# Glory Oscillations in the Index of Refraction for Matter-Waves

## Abstract

We have measured the index of refraction for sodium de Broglie waves in gases of Ar, Kr, Xe, and N2 over a wide range of sodium velocities. We observe glory oscillations—a velocity-dependent oscillation in the forward scattering amplitude. An atom interferometer was used to observe glory oscillations in the phase shift caused by the collision, which are larger than glory oscillations observed in the cross section. The glory oscillations depend sensitively on the shape of the interatomic potential, allowing us to discriminate among various predictions for these potentials, none of which completely agrees with our measurements.

A singularity in the classical differential scattering cross section $`\frac{d\sigma }{d\mathrm{\Omega }}=\frac{b}{\mathrm{sin}\theta }|\frac{d\theta }{db}|^1`$ arises when $`\theta (b_{\mathrm{glory}})=0`$ or $`\pi `$ at finite non-zero impact parameter, $`b_{glory}`$. This was named glory scattering by B. Cellini who observed the resulting circle of back-scattered light around the shadow of his head on the dewy grass. An even brighter glory can be observed surrounding the shadow of one’s airplane on the clouds of spherical water droplets below gen .

Glory scattering is not just an optical phenomenon. Interatomic potentials are attractive at long range but have repulsive cores. Hence there is an impact parameter just beyond the potential minimum for which $`\theta (b_{\mathrm{glory}})=0`$. Quantum mechanics demands that atom-atom scattering be treated as a wave phenomenon, but when the de Broglie wavelength is much smaller than the potential, the semiclassical approximation can be used Ford and Wheeler (1959) in which the incident wave is viewed as traveling along classical paths. There are then two possible paths to scatter into the forward direction—a long range diffractive component from large $`b`$, and the aforementioned path near the potential minimum. Waves from these paths contribute to the scattering amplitude in the forward direction, $`f(k,\theta =0)`$, for which the partial wave treatment reads:

$$f(k,0)=\underset{l=0}{\overset{\mathrm{}}{}}\frac{2l+1}{2k}\mathrm{sin}2\delta _l+i\underset{l=0}{\overset{\mathrm{}}{}}\frac{2l+1}{k}\mathrm{sin}^2\delta _l,$$
(1)
where the sums are both real.

The behaviors of the real and imaginary parts of $`f(k,0)`$ are different. $`\text{Im}f`$ (the second sum in Eq. 1) has a large value owing to the fact that $`\mathrm{sin}^2\delta `$ averages to $`\frac{1}{2}`$ where the scattering is strong ($`\delta \pi `$). The contributions from large $`l`$ and $`l_{glory}`$ add on top of this large value, making $`\text{Im}f`$ less sensitive to the shape of the potential. On the other hand, the strong scattering region contributes zero on average to $`\text{Re}f`$, and the long range and glory contributions can either add or subtract, making it easier to discern effects from each region as well as their relative phase.

The ratio,

$$\rho (k)\frac{\text{Re}f(k,0)}{\text{Im}f(k,0)},$$
(2)
has been shown to give information about the rate of increase of the interatomic potential $`V(r)`$ for large $`r`$ independently of the strength of $`V(r)`$ Berman ed. (1997). Also, oscillations in $`\rho `$ depend sensitively on the potential near the well bottom. This sensitivity has motivated several theoretical predictions for $`\rho `$ based on possible interatomic potentials Audouard et al. (1995); Forrey and et al. (1996); Champenois and et al. (1997); Forrey and et al. (1997).

We have measured $`\rho (k)`$ in an atom interferometer using a technique that parallels out previous measurement at fixed $`k`$ Schmiedmayer and et al. (1995); Berman ed. (1997). $`\rho `$ is found by measuring $`\text{Re}f`$, which is related to the phase shift caused by the collision, as well as $`\text{Im}f`$, which is related via the optical theorem to the absorption cross section rot . An atom interferometer determines the phase shift and attenuation of the de Broglie wave in one arm of the interferometer that passes through a “target gas” by interfering with the other arm which does not. Specifically, propagation through a gas of length $`L`$ modifies the wavefunction by a factor $`\mathrm{exp}[i(n1)k_{lab}L]`$ where $`n`$ is the complex index of refraction, $`n=1+2\pi n_df(k,0)/k_{lab}k`$, with $`n_d`$ the target gas density and $`k`$ and $`k_{lab}`$ the Na wavevectors in the center-of-mass and lab frames.

The interferometer is composed of three nanofabricated diffraction gratings forming a Mach-Zehnder geometry Keith and et al. (1991). A gas cell exposes one path of the interferometer to a gas while leaving the other path undisturbed (Fig. 1). A beam velocity of 0.7–3.0 km/s (with $``$5% rms spread) is chosen by changing the carrier gas mixture in the supersonic oven. The velocity is measured to $`\pm `$30 m/s from the atom diffraction pattern of a grating.

Several apparatus improvements were necessary in order to study the velocity-dependent index of refraction. New 100 nm period gratings Savas and et al. (1996) double the path separation—and hence the maximum usable velocity in the interferometer—compared to the old 200 nm gratings Rooks and et al. (1995). These gratings, developed by Tim Savas and Hank Smith, have already lead to a number of advances in atomic and molecular physics gra .

A thinner gas cell wall Hammond (1997) also allows the atom paths to be closer together and hence allows higher velocities. The wall of the gas cell is a 10 $`\mu `$m thick Si wafer which is anodically bonded to a glass substrate. Channels cut into the glass create the volume of the cell and allow the beam to enter and exit (Fig. 1).

The gas cell can be filled and emptied with a time constant of 1–2 sec ($``$10 times faster than before) using computer-controlled valves and wider supply lines. Faster cycle times reduce errors due to phase drift caused by thermal and mechanical motion of the gratings. This drift has been further reduced by mounting the interferometer on a rigid optical breadboard suspended by a vibration isolation system inside of the vacuum chamber.

$`\rho `$ is measured by comparing the interference pattern with and without gas in the cell. In the absence of gas, we observe an interference pattern in the detected signal $`I_0`$ that depends on the position $`x`$ of one of the gratings,

$$I_0(x)=N_0+A_0\mathrm{cos}(\varphi _0+k_gx),$$
(3)
where $`N_0`$ is the average detected flux of atoms (ranging from 5–100 kHz depending on beam velocity), $`A_0`$ is the amplitude of the interference pattern (typically 5–20% of $`N_0`$), and $`k_g`$ is the grating wavevector. $`\varphi _0`$, the phase of the interference pattern in the absence of gas, is found by a fit to $`I_0(x)`$ which also determines $`N_0`$ and $`A_0`$. When the cell is filled with gas, the interference pattern becomes

$$I_{gas}(x)=N_{gas}+A_{gas}\mathrm{cos}(\varphi _{gas}+k_gx)$$
(4)
from which $`\rho `$ can be determined Schmiedmayer and et al. (1995):

$$\rho =\frac{\varphi _{gas}\varphi _0}{\mathrm{ln}A_{gas}\mathrm{ln}A_0}$$
(5)
A feature of this experimental method is that the measurements of attenuation and phase shift are relative measurements, eliminating problems due to intensity fluctuations and phase drift. Furthermore, measuring the ratio of attenuation vs phase eliminates the dependence on the target gas pressure (which may fluctuate), and obviates the need to know it absolutely. It also cancels out the $`v^{2/5}`$ dependence of cross section and phase shift that can obscure the glory oscillations in $`f`$.

In Fig. 2, $`\rho (v)`$ is plotted as a function of Na beam velocity $`v`$ for target gases of Ar, Kr, Xe, and N2. Each data point represents an average of 1–3 hours of data taken at one to three different pressures at a single beam velocity on a single night. Our previous index of refraction measurement Schmiedmayer and et al. (1995) taken at a beam velocity of 1 km/s is shown for comparison.

The improvements to the experimental apparatus mentioned above have allowed us to acquire the large range of data in Fig. 2 with smaller statistical error than our previous measurements. We have also been more careful to consider possible systematic errors, correcting for these effects where feasible.

The biggest source of systematic uncertainty is interference from unwanted paths that reach the detector—for instance, the two paths that form the mirror image of the interferometer shown in Fig. 1, or from paths of Na2 molecules composing 25% of the intensity of the beam Chapman and et al. (1995). To avoid molecule interference, we deliberately misalign the gas cell wall at low velocities so that it appears wider than the Na2 path separation. The 50 $`\mu `$m-wide detector is positioned to avoid the other orders, but because of beam alignment error and thermal drift, there is occasionally some detection of the wrong interference pattern, contributing as much as 5% to the interfering amplitude, $`A_0`$, except at higher velocities where it can be 50%. The resulting error in $`\rho `$ is typically $`+3`$/$`0`$% but as much as $`+20`$/$`0`$% at the highest velocities of both the 100 and 200 nm data. This accounts for the asymmetrical systematic error bars in Fig 2.

Another systematic effect is the attenuation of the path outside the gas cell due to gas leaking from the ends of the cell. The integrated density of gas along the path inside the cell relative to the path outside is $`120\pm 20`$ which results in a $`+1.7`$(0.3)% correction to the measured $`\rho `$.

Another source of error arises from measuring the interference pattern while the gas cell pressure hasn’t fully equilibrated after filling or evacuating. We do this to reduce the cycle time to $``$20 sec leaving only 3 sec of dead time for filling or emptying. The resulting error in fitting to the time-averaged interference pattern, up to 0.5% uncertainty in $`\rho `$, is included in the systematic error bars.

Contaminants in the target gas must also be avoided. One such contaminant caused a 3% uncertainty in $`\rho `$ for the 200 nm Ar data before it was fixed.

Error bars on the new data points in Fig. 2 include the sum of statistical and systematic errors. Because the only non-negligible systematic comes from beam alignment and drift, we have an independent check of this error by examining the repeatability of data taken on different nights. We expect that the error in alignment or drift may exceed our estimates on some nights, but this can be recognized: $`\rho `$ will be artificially low compared to other nights, we will see this deviation in all the gases measured, and the measurement will have larger statistical error bars as the ratio changes due to drift. An example of these features can be seen in the severely outlying data points measured at 1450 m/s for Kr, Xe, and N2.

Another check of systematics can be made by comparing the 100 and 200 nm data where they overlap. At this velocity, unwanted interference is seven times larger for the 200 nm data than for the 100 nm data, yet the agreement between the two is well within the error estimates.

The data are also consistent with older measurements taken at $`v=1`$ km/s Schmiedmayer and et al. (1995), with the exception of Xe, which disagrees dramatically. However, no care was taken in that experiment to consider systematic errors, which we estimate were $`+30`$/$`10`$% in $`\rho `$ due to the unwanted interference of Na2 molecules and could have been worse for this particular measurement if thermal drift was excessive.

To compare our measurements with a prediction for $`V(r)`$, the sum in Eq. (1) must be computed. The Na wavelength is much smaller than the range of the interatomic potentials we are considering, so hundreds of partial waves contribute to the sum and we are justified in replacing it with an integral:

$$\text{Re}f(k)=k_0^{\mathrm{}}b\mathrm{sin}2\delta (b)𝑑b$$
(6a)
$$\text{Im}f(k)=k_0^{\mathrm{}}2b\mathrm{sin}^2\delta (b)𝑑b$$
(6b)
where $`b(l+\frac{1}{2})/k`$ is the classical impact parameter.

Because the kinetic energy is much greater than the well depth of the interatomic potential, we can find $`\delta (b)`$ using the Eikonal approximation—that $`\delta `$ is the accumulated phase shift of the atom traveling at constant speed along a straight-line path with impact parameter $`b`$:

$$\delta (b)=\frac{\mu }{2k\mathrm{}^2}_{\mathrm{}}^{\mathrm{}}𝑑zV(\sqrt{b^2+z^2}),$$
(7)
where $`\mu `$ is the reduced mass. Predictions using this approach are valid to 6% in $`\rho `$ for the Na-Ar system and 3% for the Na-Kr and Na-Xe systems in comparison to an exact quantum treatment Forrey (2001). Predictions for $`\rho `$ must also average over the room-temperature distribution of target gas velocities in our experiment, which damps the glory oscillations somewhat at lower beam velocities Champenois and et al. (1997); Forrey and et al. (1997).

Fig. 2 also shows calculations of $`\rho (v)`$ based on predictions of $`V(r)`$ for Na-Ar zim ; Duren and Groger (1978); Forrey and et al. (1997); Tellinghuisen and et al. (1979); Tang and Toennies (1977), Na-Kr zim ; Duren et al. (1968), and Na-Xe Baumann et al. (1992); Duren et al. (1968); Buck and Pauly (1968) derived from spectroscopic measurements and beam scattering experiments. The oscillations in these curves are glory oscillations, and are evident in the data. Even after allowing for statistical and systematic errors, our data disagree with these predictions. We believe this is because our measurements are very sensitive to the shape of the potential near the minimum (see examples in Roberts (2002)), where the transition from the repulsive core to the Van der Waals potential is poorly understood, even though the well depth and location of the minimum are fairly well known. The N2 data are remarkable as well for showing a large variation in $`\rho `$ without any evidence of an oscillation, unfortunately, the potential is not understood in enough detail to explain this behavior Habitz (1980); Nefedov et al. (1999).

Because there is good agreement on the location and depth of the potential minima, we can use this knowledge to scale our measurements of $`\rho `$ in a way that is sensitive to the shapes of all three Na-rare-gas potentials, independent of the well location and depth. We can write any potential as $`V(r)=D_eg(r/r_e)`$ where $`D_e`$ and $`r_e`$ are the depth and location of the minimum and $`g(x)`$ is a dimensionless function with a minimum $`g(1)1`$. In the Eikonal approximation $`\rho `$ depends only on $`g(x)`$ and the dimensionless parameter $`\alpha D_er_e/\mathrm{}v`$. $`\alpha `$ is approximately the phase shift in radians accumulated along the glory path. Changing the well depth or location of a potential without changing its shape $`g(x)`$ is equivalent to changing the velocity scaling of $`\rho (v)`$.

In Fig. 3 we have plotted measurements of $`\rho `$ for Ar, Kr, and Xe verses the dimensionless parameter $`\alpha `$, using values of $`D_e`$ and $`r_e`$ taken from Champenois and et al. (1997). Because of thermal averaging, the values of $`\rho `$ we measure also depend weakly on the ratio of $`v`$ to the mean speed of the scatterer, but differences in $`\rho (\alpha )`$ due to thermal averaging would be at most of 5%. Also included are data for Ne, with new systematic error estimates, which were taken with the older apparatus Schmiedmayer and et al. (1995); Forrey and et al. (1996). Plotted in this manner, the combined data clearly show a full glory oscillation, as well as a hint of a second. For comparison we show $`\rho `$ as derived from the Lennard-Jones potential, $`g(x)=x^{12}2x^6`$, and the Morse potential $`g(x)=e^{2\beta (x1)}2e^{\beta (x1)}`$ using $`\beta =4.7`$ which is appropriate for the Na-Ar system Forrey and et al. (1997). The continuity of the data plotted together in this fashion demonstrates the similarity of Na-rare-gas potentials for these four systems and shows that Lennard-Jones and Morse potentials are too simplistic to accurately model the data here.

In conclusion, we have measured $`\rho `$ to a typical accuracy of 9% at various Na velocities in gases of Ar, Kr, Xe, and N2. The consistency of our scaled data for different gases suggests that the shape $`g(x)`$ of different Na-rare-gas potentials is similar. However, discrepancies in the comparison to predictions of $`\rho `$ suggest that the shape of the potential is not well understood theoretically. Unfortunately, the difficulty of the inverse scattering problem Newton (1966); Chadan and Sabatier (1989) prevents us from deriving the potential based on knowledge of $`f(k)`$. However, our explorations of modifications to suggested interatomic potentials do indicate that they would agree better with our measurements if $`V(r)`$ were modified such that $`V(r_0)=0`$ occurs at smaller $`r_0`$ and the well were made less deep in the range $`r_e<r<2r_e`$ Roberts (2002). Our measurements should be useful in evaluating future refinements of the relevant interatomic potentials.

We would like to extend our grateful thanks to Tim Savas and Hank Smith for fabricating gratings for our use. We thank Edward Smith for the invention of the gas cell, and Peter Finin for his technical assistance. This work was supported by the Army Research Office Contracts DAAG55-97-1-0236 and DAAG55-98-1-0429, Naval Research Contract N00014-96-1-0432, and National Science Foundation Grant PHY98-77041. TR acknowledges the support of a National Defense Science and Engineering Graduate Fellowship.