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# A nonplanar Peierls-Nabarro model and its applications to dislocation cross-slip

## Abstract

A novel semidiscrete Peierls-Nabarro model is introduced which can be used to study dislocation spreading at more than one slip planes, such as dislocation cross-slip and junctions. The strength of the model, when combined with ab initio calculations for the energetics, is that it produces essentially an atomistic simulation for dislocation core properties without suffering from the uncertainties associated with empirical potentials. Therefore, this method is particularly useful in providing insight into alloy design when empirical potentials are not available or not reliable for such multi-element systems. As an example, we study dislocation cross-slip and constriction process in two contrasting fcc metals, Al and Ag. We find that the screw dislocation in Al can cross-slip spontaneously in contrast with that in Ag, where the screw dislocation splits into two partials, which cannot cross-slip without first being constricted. The response of the dislocation to an external stress is examined in detail. The dislocation constriction energy and the critical stress for cross-slip are determined, and from the latter, we estimate the cross-slip energy barrier for straight screw dislocations.

The past decades have witnessed a growing interest towards a quantitative understanding of deformation and strength of materials and, in particular, the effect of impurities and alloying elements on dislocation properties. While continuum elasticity theory describes well the long-range elastic strain of a dislocation for length scales beyond a few lattice spacings, it breaks down near the singularity in the region surrounding the dislocation center, known as the dislocation core. There has been a great deal of interest in describing accurately the dislocation core structure on an atomic scale because of its important role in many phenomena of crystal plasticity Duesbery1 ; Vitek . The core properties control, for instance, the mobility of dislocations, which accounts for the intrinsic ductility or brittleness of solids. The core is also responsible for the interaction of dislocations at close distances, which is relevant to plastic deformation. For example, by integrating the local rules derived from atomistic simulations of core interactions into dislocation-dynamics simulations, a connection between micro-to-meso scales can be established to study dislocation reactions and crystal plasticity Nature .

Cross-slip, the process by which a screw dislocation moves from one glide plane to another, is ubiquitous in plastic deformation of materials. For example, cross-slip is considered to be responsible for the onset of stage III in the stress-strain work-hardening curves. Furthermore, cross-slip can result in the formation of glide plane obstacles (sessile segments) in hcp metals and in L12-, B2- and L10\- based intermetallic alloys, responsible for the anomalous high-temperature yield stress peak. However, theoretical studies of alloying and impurity effects on dislocation cross-slip have proved to be particularly difficult because one has to deal with both long-ranged elastic interactions (between dislocation segments) and short-ranged atomic interactions (due to the constriction process) that are inherent in a cross-slip process.

There are currently two theoretical approaches to study cross-slip. One is based on the line tension approximation which completely ignores atomic interactions, therefore it is not reliable Friedel ; Escaig . The other approach is direct atomistic simulations employing empirical potentials Rasmussen ; Rao . Although the second approach is quite powerful in determining cross-slip transition paths and estimating the corresponding activation energy barriers, it is time-consuming and, more importantly, it critically depends on the accuracy and availability of the empirical potentials employed in the simulations. For example, reliable interatomic potentials usually are not available for multi-elements materials. As a consequence, the possible hardening mechanisms due to alloying for most materials are still uncertain, and the design of new materials based on favorable cross-slip properties lacks guidance. Thus, the understanding at an atomic level of the chemistry effect on the dislocation core properties and cross-slip mechanisms is of great importance in predicting and controlling plastic deformation in structural materials, since the deformation behavior is often associated with the presence of substitutional or interstitial alloying elements. The ultimate goal of theoretical studies is then to use this information to direct alloying design for new materials with desired mechanical properties by tailoring the dislocation properties - in close collaboration with experimental efforts.

In this paper, we introduce a novel model based on the Peierls-Nabarro (P-N) framework which allows the study of dislocation cross-slip employing ab initio calculations. In fact, there has been a resurgence of interest recently in applying the simple and tractable P-N model to study dislocation core structure and mobility in conjunction with ab initio $`\gamma `$-surface calculations Joos ; Juan ; Bulatov ; Hartford ; Lu1 ; Lu3 . This approach represents a combination of an atomistic (ab initio) treatment of the interactions across the slip plane and an elastic treatment of the continua on either side of the slip plane. Therefore, this approach is particularly useful for studying the interaction of impurities with dislocations when empirical potentials are either not available or not reliable to deal with such multi-element systems. Furthermore, it allows to study general trends in dislocation core properties and to correlate them with specific features of the underlying electronic structure. However, to date, all models based on the P-N framework are applicable only to a single slip plane while the important cross-slip process requires at least two active intersecting slip planes, i.e., the primary and cross-slip planes. In this work the semidiscrete variational P-N modelBulatov ; Lu1 ; Lu3  is extended so as to take into account two intersecting slip planes. We shall apply this new model to study the dislocation constriction and cross-slip process in two fcc metals, Al and Ag, exhibiting different deformation properties. We are particularly interested in the evolution of the dislocation core structure under external stress and the interplay between the applied stress and the cross-slip process.

We begin by developing an appropriate energy functional for the Peierls dislocation at two intersecting slip planes. To facilitate presentation, we adopt the following conventions: In Fig. 1, a screw dislocation placed at the intersection of the primary (plane I) and cross-slip plane (plane II) is allowed to spread into the two planes simultaneously. The $`X`$ ($`X^{}`$) axis represents the glide direction of the dislocation at the plane I (II). For an fcc lattice, the two slip planes are (111) and ($`\overline{1}11`$), forming an angle $`\theta `$ 71. The dislocation line is along the \[10$`\overline{1}`$\] ($`Z`$ axis) direction and $`L`$ represents the outer radius of the dislocation beyond which the configuration independent elastic energy is ignored.Lu1  In the spirit of the P-N model, the dislocation is represented as a continuous distribution of infinitesimal dislocations with densities of $`\rho ^\mathrm{I}(x)`$ and $`\rho ^{\mathrm{II}}(x^{})`$ on the primary and cross-slip planes, respectively, where, $`x`$ and $`x^{}`$ are the coordinates of the atomic rows at the two planes. Following the semidiscrete Peierls framework developed earlier Bulatov ; Lu1 , the total energy of the dislocation is

$$U_{tot}=U_\mathrm{I}+U_{\mathrm{II}}+\stackrel{~}{U}.$$
(1)
Here, $`U_\mathrm{I}`$ and $`U_{\mathrm{II}}`$ are the energies associated with the dislocation spread on planes I and II, respectively, and $`\stackrel{~}{U}`$ represents the elastic interaction energy between the dislocation densities on planes I and II. The expressions for $`U_\mathrm{I}`$ and $`U_{\mathrm{II}}`$ are identical to that given earlier for the single glide plane case Bulatov ; Lu1 , while the new term $`\stackrel{~}{U}`$ can be derived from Nabarro’s equation for general parallel dislocations Nabarro ,

$`U_{\mathrm{I}(\mathrm{II})}`$ $`=`$ $`{\displaystyle \underset{i,j}{}}{\displaystyle \frac{1}{2}}\chi _{ij}\{K_e[\rho _1^{\mathrm{I}(\mathrm{II})}(i)\rho _1^{\mathrm{I}(\mathrm{II})}(j)+\rho _2^{\mathrm{I}(\mathrm{II})}(i)\rho _2^{\mathrm{I}(\mathrm{II})}(j)]+K_s\rho _3^{\mathrm{I}(\mathrm{II})}(i)\rho _3^{\mathrm{I}(\mathrm{II})}(j)\}`$
$`+{\displaystyle \underset{i}{}}\mathrm{\Delta }x\gamma _3(f_1^{\mathrm{I}(\mathrm{II})}(i),f_2^{\mathrm{I}(\mathrm{II})}(i),f_3^{\mathrm{I}(\mathrm{II})}(i)){\displaystyle \underset{i,l}{}}{\displaystyle \frac{x(i)^2x(i1)^2}{2}}\rho _l^{\mathrm{I}(\mathrm{II})}(i)\tau _l^{\mathrm{I}(\mathrm{II})}+Kb^2\mathrm{ln}L,`$
$`\stackrel{~}{U}`$ $`=`$ $`{\displaystyle \underset{i,j}{}}K_s\rho _3^\mathrm{I}(i)\rho _3^\mathrm{p}(j)A_{ij}{\displaystyle \underset{i,j}{}}K_e[\rho _1^\mathrm{I}(i)\rho _1^\mathrm{p}(j)+\rho _2^\mathrm{I}(i)\rho _2^\mathrm{p}(j)]A_{ij}`$
$`{\displaystyle \underset{i,j}{}}K_e[\rho _2^\mathrm{I}(i)\rho _2^\mathrm{p}(j)B_{ij}+\rho _1^\mathrm{I}(i)\rho _1^\mathrm{p}(j)C_{ij}\rho _2^\mathrm{I}(i)\rho _1^\mathrm{p}(j)D_{ij}\rho _1^\mathrm{I}(i)\rho _2^\mathrm{p}(j)D_{ij}].`$
Here, $`f_1^{\mathrm{I}(\mathrm{II})}(i)`$, $`f_2^{\mathrm{I}(\mathrm{II})}(i)`$ and $`f_3^{\mathrm{I}(\mathrm{II})}(i)`$ represent the edge, vertical and screw component of the general dislocation displacement at the $`i`$-th nodal point in plane I(II), respectively, while the corresponding component of dislocation density in plane I(II) is defined as $`\rho ^{\mathrm{I}(\mathrm{II})}(i)=\left(f^{\mathrm{I}(\mathrm{II})}(i)f^{\mathrm{I}(\mathrm{II})}(i1)\right)/\left(x(i)x(i1)\right)`$. The projected dislocation density $`\rho ^\mathrm{p}`$(i) is the projection of the density $`\rho ^{\mathrm{II}}`$(i) from plane II onto plane I in order to deal with the non-parallel components of the displacement. The $`\gamma `$-surface, $`\gamma _3`$, which in general includes shear-tension coupling can be determined from ab initio calculations. $`\tau _l^{\mathrm{I}(\mathrm{II})}`$ is the external stress component interacting with the corresponding dislocation densities, $`\rho _l^{\mathrm{I}(\mathrm{II})}(i)`$ ($`l`$ = 1,2,3). This term represents the contribution to the total energy from the elastic work done by the applied stress Bulatov ; Lu1 . The response of a dislocation to an applied stress is achieved by the minimization of the energy functional with respect to $`\rho _l^{\mathrm{I}(\mathrm{II})}(i)`$ at the given value of $`\tau _l^{\mathrm{I}(\mathrm{II})}`$. The dislocation core energy is defined as the configuration-dependent part of the total energy, which includes the density-dependent part of the elastic energy and the entire misfit energy, in the absence of stress Lu1 . $`K_e`$ and $`K_s`$ are the edge and screw components of the general prelogarithmic elastic energy factor $`K`$ Bulatov ; Lu1 , while $`\chi _{ij}`$, $`A_{ij}`$, $`B_{ij}`$, $`C_{ij}`$ and $`D_{ij}`$ are double-integral kernels defined by

$`\chi _{ij}`$ $`=`$ $`{\displaystyle \underset{x_{j1}}{\overset{x_j}{}}}{\displaystyle \underset{x_{i1}}{\overset{x_i}{}}}\mathrm{ln}|xx^{}|𝑑x𝑑x^{},`$
$`A_{ij}`$ $`=`$ $`{\displaystyle \underset{x_{j1}^{}}{\overset{x_j^{}}{}}}{\displaystyle \underset{x_{i1}}{\overset{x_i}{}}}{\displaystyle \frac{1}{2}}\mathrm{ln}(x_0^2+y_0^2)𝑑x𝑑x^{},`$
$`B_{ij}`$ $`=`$ $`{\displaystyle \underset{x_{j1}^{}}{\overset{x_j^{}}{}}}{\displaystyle \underset{x_{i1}}{\overset{x_i}{}}}\mathrm{ln}{\displaystyle \frac{x_0^2}{x_0^2+y_0^2}}𝑑x𝑑x^{},`$
$`C_{ij}`$ $`=`$ $`{\displaystyle \underset{x_{j1}^{}}{\overset{x_j^{}}{}}}{\displaystyle \underset{x_{i1}}{\overset{x_i}{}}}\mathrm{ln}{\displaystyle \frac{y_0^2}{x_0^2+y_0^2}}𝑑x𝑑x^{},`$
$`D_{ij}`$ $`=`$ $`{\displaystyle \underset{x_{j1}^{}}{\overset{x_j^{}}{}}}{\displaystyle \underset{x_{i1}}{\overset{x_i}{}}}\mathrm{ln}{\displaystyle \frac{x_0y_0}{x_0^2+y_0^2}}𝑑x𝑑x^{},`$
where $`x_0=Lx+x^{}\mathrm{cos}\theta `$, and $`y_0=x^{}\mathrm{sin}\theta `$. The equilibrium structure of the dislocation is determined by minimizing the total dislocation energy functional energy with respect to the dislocation density.

In order to compare and understand the different cross-slip behavior in Al and Ag, we have carried out ab initio calculations for their $`\gamma `$-surfaces. In both calculations, we used a supercell containing six layers of atoms in the  direction. The ab initio calculations are based on the pseudopotential plane-wave method Payne  within the local density approximation. Owing to the planar nature of the dislocation core structure in fcc metals, we disregard in the $`\gamma `$-surface calculations the displacement perpendicular to the slip planes and consider partially the shear-tension coupling by performing volume relaxation along the  direction. The complete $`\gamma `$-surface for Al and Ag is shown in Fig. 2(a) and 2(b) respectively. The most striking difference between the two $`\gamma `$-surfaces is the large difference in intrinsic stacking fault energy, which is 165 mJ/m2 for Al and 14 mJ/m2 for Ag. This dramatic difference in $`\gamma `$-surface gives rise to very different dislocation core structures and cross-slip behavior that we are going to explore. The ab initio calculated Burgers vector, $`b`$, of a perfect 1/2 dislocation in Al and Ag is 2.85 and 2.83 Å, respectively.

The model calculation is set up by introducing a screw dislocation at the intersection of the two slip planes without applying external stress to the system at first. The initial configuration of the dislocation is specified by a step function for the screw displacement $`f_3^\mathrm{I}(x)=0`$ for $`x<L`$ and $`f_3^\mathrm{I}(x)=b`$ for $`xL`$. All other displacement components including those on the cross-slip plane are set initially to zero. This corresponds to a pure screw dislocation with a zero width “spread” on the primary plane. We then relax the dislocation structure according to the energy functional. The results of the dislocation density $`\rho (x)`$ in the primary and cross-slip planes for Al and Ag are presented in Figs. 3(a) and 3(b), respectively. The screw dislocation in Al which starts out at the primary plane spontaneously spreads into the cross-slip plane, as the density peak at the cross-slip plane indicates. As expected, the edge component of the density is zero at the cross-slip plane because only the screw displacement can cross-slip. On the other hand, the screw dislocation in Ag dissociates into two partials, separated by 7.8 $`b`$ ($``$ 22 Å), in excellent agreement with the experimental value of 20 Å in TEM measurements Cockayne . The left (right) partial has a positive (negative) edge component of the Burgers vector represented by the positive (negative) density. The integral of the edge density over all atomic sites is zero, corresponding to a pure screw dislocation. These partial dislocations cannot cross-slip, as the arrows in Fig. 3(a) indicate, without first annihilating their edge components, and the dislocation density on the cross-slip plane is essentially zero. Apparently, the lack of obvious dissociation in Al stems from the fact that Al has a much higher intrinsic stacking fault energy than Ag. The absence of obvious dissociation into partials in Al is also consistent with experiment Duesb0 .

Next we apply an external Escaig stress to the dislocations and examine the evolution of the dislocation core structure under stress with the emphasis on the effect of stress on the dislocation cross-slip. The Escaig stress, defined as the edge component of the diagonal stress tensor, interacts only with the edge displacement of a dislocation, extending or shrinking its stacking fault width depending on the sign of the stress. We apply the Escaig stress only on the dislocation at the primary plane, and the stress components projected on the cross-slip plane are removed. The evolution of the dislocation core structure in Ag, represented by its displacement density distribution, is presented in Fig. 4 as the Escaig stress is varied. Upon application of positive (stretching) stress of $`\tau _1^\mathrm{I}`$ = 0.32 GPa, the separation of the partials rises rapidly from 7.8 $`b`$ (equilibrium separation in the absence of applied stress) to 12 $`b`$ (Fig. 4(a)). In Fig. 4(a) we show only the density at the primary plane, as the density at the cross-slip plane is essentially zero. For stress higher than 0.32 GPa, the partials move to the two ends of the simulation box and the lattice breaks down. To activate cross-slip, however, one needs to apply a negative (compressive) Escaig stress to the dislocation in order to annihilate the edge components of the partials’ displacement, known as a constriction process. Upon application of negative stress, the partials move towards each other and reduce the width of the stacking fault. During this process, the edge components of the displacement from the two partials annihilate each other at the primary plane while the screw component is being built up at both planes. One example of such structure is shown in Fig. 4(b). The left and right density peaks represent the original two partial dislocations, while the third peak at the center corresponds to the build-up of the screw density from the overlapping partials. Interestingly, the screw component of the dislocation density at the cross-slip plane is also accumulating, indicating the inception of the cross-slip process. However, further increasing the negative Escaig stress does not yield smaller separation between the partials. We find that the lower limit for the partials separation in Ag is 1.7 $`b`$, which is in agreement with the atomistic simulation result for Cu, reporting a corresponding value of 1.6 $`b`$ Duesbery . In other words, no complete constriction can be achieved for a straight dislocation. The critical configuration in which the constriction is most developed is shown in Fig. 4(c). In this case, three partial dislocations with the same amount of screw component of the Burgers vector are formed. The cross-slipped screw dislocation density is about one third of the remaining screw density at the primary plane. In order to complete the cross-slip, either thermal fluctuations or other type of external stress have to be present. This is because the remaining edge component of the partials interacts with the Escaig stress, and as a result the partials exchange signs and move away from each other. For example, as shown in Fig. 4(d), the left partial now acquires a negative edge density and the right partial a positive edge density. Associated with the inversion of the edge component of the density for the partials, a run-on stacking fault is formed between them, with an energy of about 1.0 J/m2. The run-on stacking fault is the most unstable stacking fault in an fcc lattice, with atoms from the neighboring (111) planes sitting right on top of each other. The distance between the two partials is more than 10 $`b`$. It is interesting to note that in the wake of the (partial) constriction process, a pure screw dislocation segment is formed at the intersection of the two planes, with an appreciable amount of cross-slip.

Next we examine the situation of Al. We first apply positive Escaig stress to the complete screw dislocation. We find that the screw dislocation remains unsplit until the stress reaches the threshold value of 0.96 GPa, required to separate the overlapping partials. The dislocation core structure corresponding to such a stress-driven dissociation is shown in Fig. 5(a). We find that the screw density component at the cross-slip plane is only reduced by a few percent due to the small splitting, leaving the density at the cross-slip plane approximately equal to that in the primary plane. Increasing the positive stress will further separate the partials and reduce cross-slip. The maximum positive Escaig stress, however, that the dislocation can sustain is 1.92 GPa (Fig. 5(b)). In this configuration, the partials are separated by 5 $`b`$. The central peak in the screw density plot corresponding to the original complete dislocation is reduced significantly, and the cross-slipped screw density amounts to only 1/3 of the screw density at the primary plane. Therefore, the application of positive Escaig stress in Al corresponds to an “inverse cross-slip” process that transfers displacement from the “cross-slip” plane to the “primary plane”. Interestingly, applying negative Escaig stress to the dislocation has no effect on the dislocation splitting or core width. The dislocation remains unsplit all the way until the stress is great enough to break down the lattice. Finally, it is important to point out that for all cases studied here in Al and Ag, upon removal of the applied external stress, the dislocation returns spontaneously to its equilibrium configuration.

We have also estimated the critical energetics that are relevant to cross-slip. For example, we calculated the constriction energy, defined as the difference in dislocation core energy between the normal and constricted states. By approximating the state with 1.7 $`b`$ separation between the partials as the constricted state, we were able to estimate the constriction energy for Ag to be 0.14 eV/$`b`$. A similar approach has been used to evaluate the constriction energy for a screw dislocation in Cu based on atomistic simulations, reporting a value of 0.17 eV/$`b`$, which is in a good agreement with our model calculations Duesbery . Obviously, the constriction energy for Al is zero because its normal state is fully constricted. We have also calculated the critical stress for cross-slip, which is defined as the glide stress in the cross-slip plane to move a partially constricted dislocation from the primary to the cross-slip plane Duesbery . We find that the critical stress for cross-slip in Ag is 1.68 GPa, compared to 0.32 GPa in Al. Finally, we estimated the cross-slip energy barrier, which in the context of our calculations, is defined as the difference in dislocation core energy before and after cross-slip takes place under the application of the above mentioned critical stress for cross-slip. In other words, we calculate the core energy difference for the dislocation between its normal state and the state that the dislocation just starts to cross-slip under the critical cross-slip stress. We find that the cross-slip energy barrier in Ag is 0.14 eV/$`b`$, much larger than that of 0.05 eV/$`b`$ in Al. One needs to be cautious when comparing our results for the cross-slip energy barrier directly with experiment, since the dislocations are assumed to be straight in our current implementation of the Peierls-Nabarro model. However, it is possible to extend the present formalism to deal with an arbitrarily curved dislocation where a more realistic cross-slip energy barrier can be obtained. Nevertheless, the present model is still capable to provide reliable energetics for straight dislocations.

In summary, we have presented a novel model based on the semidiscrete Peierls-Nabarro framework that allows the study of dislocation cross-slip and constriction. The $`\gamma `$-surface entering the model is determined from ab initio calculations which provide reliable atomic interactions across the slip plane. We find that the screw dislocation in Al can spontaneously spread into the cross-slip plane, while in Ag it dissociates into partials and can not cross-slip. We have also examined in detail the response of the dislocation core structure to an external Escaig stress and the effect of negative Escaig stress on the constriction of the Shockley partials. We find that one can not achieve 100% constriction for the case of straight partial dislocations considered in this work. By computing the dislocation core energy under stress we estimate the dislocation constriction energy for Al and Ag. The calculated values of the critical stress and the energy barrier for dislocation cross-slip demonstrate that dislocation cross-slip is much easier in Al than in Ag. Since our ab initio based model is much more expedient than direct ab initio atomistic simulations, it can serve as a powerful and efficient tool for alloy design, where the goal is to select the “right” elements with the “right” alloy composition to tailor desired mechanical, and in particular, dislocation properties, such as cross-slip properties.

###### Acknowledgements.

Two of us (G.L. and N.K.) acknowledge the support from Grant No. DAAD19-00-1-0049 through the U.S. Army Research Office. G.L. was also supported by Grant No. F49620-99-1-0272 through the U.S. Air Force Office for Scientific Research.


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# Effect of spin orbit scattering on the magnetic and superconducting properties of nearly ferromagnetic metals: application to granular Pt

## Abstract

We calculate the effect of scattering on the static, exchange enhanced, spin susceptibility and show that in particular spin orbit scattering leads to a reduction of the giant moments and spin glass freezing temperature due to dilute magnetic impurities. The harmful spin fluctuation contribution to the intra-grain pairing interaction is strongly reduced opening the way for BCS superconductivity. We are thus able to explain the superconducting and magnetic properties recently observed in granular Pt as due to scattering effects in single small grains.

The recent observation of superconductivity in Pt grains of $`1\mu `$m size at $`1`$mK  motivated this theoretical study of the superconducting and magnetic properties of small grains taking account of the spin-orbit (s-o) scattering by external and internal surfaces. The importance of the s-o interaction at surfaces has been shown by Merservey and Tedrow from a number of different measurements on superconductors. In Pb, for example,the probability that a conduction electron will change its spin direction in a surface collision is of the order 1. Taking into account s-o scattering, we show that the interplay between incipient magnetism and superconductivity in Pt is tilted towards BCS superconductivity because s-o scattering is inimical to magnetism and reduces the paramagon effects that inhibit singlet pairing in the late transition metals.

Why can s-o scattering generate superconductivity (sc) in Pt or other nearly ferromagnetic metals? In bulk Pt, no sc is observed despite a strong electron-phonon coupling; the BCS parameter is $`\lambda _{Ph}^{Pt}0.4`$ . The reason for the absence of sc in bulk Pt is due to the strong exchange interactions between the itinerant 5d electrons. The resulting paramagnon effects suppress BCS s-wave sc. The Pt grains are small enough to have a large surface to volume ratio but are sufficiently large ($`100\AA `$) that the Bloch representation applies and we can ignore the Rashba effect . Although the ”lattice softening” near surfaces may enhance $`\lambda _{Ph}^{Pt}`$, more importantly, the s-o scattering at rough surfaces strongly reduces the harmful paramagnon effects. In the case of Pt grains, the extremely weak impurity magnetism observed at mK temperatures clearly points to an important role of the changed magnetic behavior for the occurence of sc . Independently of whether the sc extends throughout the grain or is restricted to a surface shell of thickness small compared with the grain size, s-o scattering at surfaces and defects will be important for the sc and magnetic properties. If shells exist in the compacted granules, they may (as in a thin film) consist of small crystallites large enough for bulk superconductivity but sufficiently small to limit the mean free path for s-o scattering. We find that, with reasonable values for the exchange and scattering parameters, sc in granular Pt is possible at the observed temperatures.

We first address the magnetic properties of small grains by calculating the static susceptibility $`\chi (q)`$ in the presence of ordinary and s-o scattering, taking the exchange enhancement effects into account as in Ref. . The Stoner factor $`S`$ accounts for the average exchange and the spin correlation range $`\sigma `$ measures the spatial range of the inter-atomic exchange. Scattering is included by considering the effect on $`\chi _0`$, the susceptibility without exchange enhancements. We find a significant effect of s-o scattering on $`\chi _0`$ that affects both $`S`$ and $`\sigma `$.

The susceptibility $`\chi (r)`$ is then calculated to determine how scattering as well as exchange enhancement affects the the RKKY (Ruderman-Kasuya-Kittel-Yoshida) oscillations occuring in $`\chi _0(r)`$. The short range and long range parts of $`\chi (r)`$ determine the two pertinent magnetic properties observed in dilute magnetic systems , namely, the magnitude of the giant moment $`\mu _{gm}`$ and the scale of the spin glass freezing temperature, $`T_f/x`$, in, e.g., $`\text{PtFe}_x`$. The exchange effects suppress the RKKY oscillations at small r yielding the ferromagnetic correlations responsible for $`\mu _{gm}`$; s-o scattering reduces $`\mu _{gm}`$. The spin glass transition observed in the bulk $`\text{PtFe}_x`$ systen is due to the long range oscillations of $`\chi (r)`$ relevant for the interaction between two impurity moments at a distance $`ra(=\text{lattice constant})`$ in the absence of scattering effects. With scattering $`\chi (r)`$ at large $`r`$ is so strongly reduced that spin glass freezing would not be expected in the Pt grains where $`x=4`$ppm.

We consider first the magnetic properties. The static q-dependent, exchange enhanced susceptibility $`\chi (q)`$ in the presence of ordinary and s-o scattering is appropriate to describe the giant moments and spin glass freezing. We assume a susceptibility of the RPA form:

$$\chi (q)=\frac{2\mu _B^2\chi _0(q)}{1\chi _0(q)\frac{1}{3}\left[U+2J_H+3J^{}(q)\right]},$$
(1)
where $`\chi _0(q)=N(0)u(q)`$, $`N(0)`$ is the density of states (DOS) per spin for all three 5d sub bands at the Fermi level, and $`u(q)`$ reduces to the Lindhard function for free electrons with no impurity scattering. $`U`$ is the intra-atomic self-exchange and $`J_H`$ is Hund’s rule exchange. Including up to second nearest neighbors we can define the inter-atomic exchange interaction $`J^{}(q)J^{}(0)(qa)^2J_{eff}^{}`$ where $`a`$ is the lattice constant. We also define $`\overline{U}=N(0)U/3`$, $`\overline{J}_H=N(0)J_H/3`$, $`\overline{J}^{}(q)=N(0)J^{}(q)/3`$, $`\overline{U}_{eff}=\overline{U}+2\overline{J}_H+3\overline{J}^{}(0)`$, and $`\overline{J}_{eff}^{}=N(0)J_{eff}^{}`$ . Now $`\chi (0)=2\mu _B^2Su_0`$, where $`S=1/(1\overline{U}_{eff}u_0)`$ and $`u_0=u(0)`$.

To define the spin correlation range, $`\sigma `$, we first expand Eq. (1) for small q . With $`u(q)u_0+u_2(qa)^2`$, Eq. (1) becomes

$$\chi (q)=\frac{2\mu _B^2Su_0}{1+\sigma ^2q^2},$$
(2)
which yields a factor $`\frac{1}{r}e^{r/\sigma }`$ where $`\sigma ^2/a^2=S\left[u_0\overline{J}_{eff}^{}u_2\overline{U}_{eff}\right]u_2/u_0`$, in agreement with Clogston .

For arbitrary q we model the suceptibility with

$$\chi (q)=\frac{2\mu _B^2\chi _0(q)}{1I(q)\chi _0(q)},$$
(3)
where $`I(q)`$ is a two parameter phenomenological interaction which is determined so that Eq.(1) reduces to Eq.(2) for small $`q`$. This yields $`\overline{I}(q)=N(0)I(q)=\overline{U}_{eff}/\left[1+(qa)^2(\overline{J}_{eff}^{}/\overline{U}_{eff})\right]`$. $`\overline{U}_{eff}`$ is determined directly by $`S`$. We take $`S=3.8`$ for Pt  and find $`\overline{U}_{eff}=0.737`$. We fix $`\overline{J}_{eff}^{}`$ to provide a reasonable value for the spin fluctuation induced effective mass enhancement $`\lambda _{SF}`$ . As in the case of Pd, the problem here is to divide the effective mass enhancement $`m^{}/m=1+\lambda _{SF}+\lambda _{Ph}`$ between the phonon and spin fluctuation contributions. We assume that $`\lambda _{Ph}`$ is about the same in Pt as in Pd and take the Pd value of $`\lambda _{Ph}^{Pd}=0.41`$ . Assuming $`m^{}/m1=0.63`$ for Pt  we have $`\lambda _{SF}^{Pt}=0.22`$. Employing the standard calculation of $`\lambda _{SF}`$,

$$\lambda _{SF}=\frac{3}{2}_0^{2k_F}\frac{qdq}{2k_F^2}\frac{[\overline{I}(q)]^2u(q)}{1\overline{I}(q)u(q)},$$
(4)
we find $`\overline{J}_{eff}^{}=0.163`$ which yields $`\sigma =3.21\text{Å}`$. Physically, $`\overline{J}_{eff}^{}`$ is a measure of the range of $`\overline{I}(r)`$ in position space. Increasing $`\overline{J}_{eff}^{}`$ increases $`\sigma `$ and the range of $`\overline{I}(r)`$ but decreases the range of $`\chi (q)`$ in q-space yielding a smaller $`\lambda _{SF}`$ from Eq. (4).

Assuming the RPA form of Eq. (1) is not changed by the presence of scattering centers, one need only consider the effect of scattering on $`\chi _0`$. This was first done by de Gennes  for ordinary scattering alone. He showed that $`\chi _0(q)`$ is not affected for $`q=0`$. Fulde and Luther (FL1)  calculated $`\chi (q,\omega )`$ for small $`q`$ and Jullien  extended this work to arbitrary $`q`$ and $`\omega `$. Spin-orbit scattering was later added to the ordinary scattering in FL2 . We use the result of FL2 for the effect of s-o scattering on $`\chi _0`$. As FL2 were primarily interested in obtaining approximate analytic expressions for the $`\omega `$-dependent susceptibility we employ however the formalism of Julien  which is more suitable for computations. Equation (9) of Jullien for $`\chi _0`$ with ordinary scattering alone, can be generalized to include s-o scattering by comparison with Eq.(14) of FL2. The result is

$$\chi _0(𝐪,\omega _0)=\frac{i}{2\pi }_0^{\mathrm{}}𝑑\omega \frac{Z(\omega )\left[1\pi k_F\gamma _1Z(\omega )/3\right]}{1\pi k_F\gamma _0Z(\omega )\left[1\pi k_F\gamma _1Z(\omega )/3\right]},$$
(5)
where $`Z(\omega )=\frac{d^3k}{(2\pi )^3}G(𝐤,\omega )G(𝐤+𝐪,\omega +\omega _0)`$, $`\gamma _0=1/k_F\mathrm{}_0`$ and $`\gamma _1=1/k_F\mathrm{}_1`$ with $`\mathrm{}_0`$ and $`\mathrm{}_1`$ the mean free paths for ordinary and s-o scattering, respectively. The single particle propagator $`G`$ contains the scattering rates in the combination $`\gamma =\gamma _0+\gamma _1`$. We set $`\omega _0=0`$ and consider from now on only $`\chi (q)`$. In their small-q approximation FL2 set $`\chi _0(q)/N(0)=1`$. By doing this they neglected the $`\gamma _1`$ corrections to $`\chi _0(0)`$ that are crucial in the following considerations. The computation of $`\chi `$ proceeds as in Ref.  leading to the results shown in Fig. (1) where we take for Pt, $`k_F=0.642\text{ cm}^1`$ and $`a=3.923\AA `$. Fig. (1a) shows the large effect of s-o scattering on $`\chi _0(0)`$. In Fig. (1b) $`S`$, $`u_0`$, and $`\sigma `$ are shown vs $`\gamma _1`$. $`S`$ and $`u_0`$ do not depend on $`\gamma _0`$ and the dependence of $`\sigma `$ on $`\gamma _0`$ arises only through $`u_2`$ and is negligible.

We need the Fourier transform of $`\chi (r)`$ at small r to calculate the induced spin polarization around an impurity moment and at large r for the RKKY interaction responsible for spin glass transition. For $`\chi (q)\chi _0(q)`$ the Fourier transform can be done analytically yielding the usual RKKY oscillations. Integrating $`\chi (r)`$ over $`d^3r`$ leads directly to the sum rule

$$d^3r\chi (r)=\chi (q=0)=2\mu _B^2N(0)Su_0.$$
(6)
$`\chi _0`$ alone does not provide a reasonable induced moment since the RKKY oscillations do not yield the necessary short range ferromagnetic correlations. This problem does not occur in our two parameter model for $`\chi `$ as can be seen from Fig. (2a). Here we plot the dimensionless susceptibility $`\overline{\chi }(r)`$ which is defined by $`\chi (r)=2\mu _B^2N(0)(\mathrm{\Omega }/a^3)\overline{\chi }(r)`$, where $`\mathrm{\Omega }`$ is the atomic volume ($`a^3/4`$ for the fcc lattice). The first effect of $`U_{eff}`$ is to shift the curve to larger r increasing the spin correlation range $`\sigma `$, an effect discussed by Giovannini, Peter, and Schrieffer . Further increasing $`U_{eff}`$ pushes the curve above the axis for small r. Increasing $`\overline{J}_{eff}^{}`$ has a similar effect. The solid curve for the Pt parameters provides both the ferromagnetic short range correlations and the long range oscillations necessary for spin glass freezing. The effect of scattering at small r is shown in Fig. (2b). Ordinary scattering (dash curve) tends to smooth out the oscillations with little change in the area under the curve consistent with the sum rule, Eq. (6). Spin orbit scattering (dot-dash curve) on the other hand reduces the magnitude of $`\chi (r)`$.

The giant moments observed in the bulk PtFex  are not seen in the Pt powders  although, according to susceptibility measurements, the granules contain $`x=(4\pm 1)`$ ppm of magnetic impurities. The giant moment consists of two parts, $`\mu _{gm}=\mu (i)+\mu (h)`$, where $`\mu (i=\text{impurity})`$ is the local moment of the 3d electrons of the Fe impurity atom and $`\mu (h=\text{host})`$ is the spin polarization of the 5d electrons of the Pt host matrix. We assume that $`\mu (i)`$ of Fe in Pt has approximately the same value as in Pd and take $`\mu (i)3\mu _B`$. Using the experimental susceptibility value , $`\mu _{gm}8\mu _B`$, leads to $`\mu (h)5\mu _B`$. We have

$$\mu (h)=4\pi _0^{r_{gm}}r^2𝑑r\sigma _s(r),$$
(7)
where $`r_{gm}`$ is the giant moment radius and $`\sigma _s(r)`$ is the isotropic spin polarization induced by the Fe moment at $`𝐫=0`$ due to the exchange interaction $`V_{ex}`$ between the 3d electrons of the impurity and the 5d electrons of the Pt host, $`\sigma _s(r)=(V_{ex}/4)N(0)\mu _B\overline{\chi }(r)`$. N(0) is the DOS per spin and $`\text{eV}\text{cm}^3`$. In order to calculate $`\mu (h)`$ we need the parameters $`r_{gm}`$ and $`V_{ex}`$. $`\mu (h)`$ is not particularly sensitive to $`r_{gm}`$ and an upper limit can be obtained from the sum rule, Eq.(6): $`\mu (h)_{r_{gm}\mathrm{}}=V_{ex}N(0)a^3Su_0\mu _B/4`$ . We take $`r_{gm}2.5a10\text{Å}`$ as in Pd and then fix the value of the local exchange coupling $`V_{ex}`$ by requiring that Eq. (7) yield $`\mu (h)=5\mu _B`$. We find $`V_{ex}=2.504\text{eV}`$ which is somewhat large but still seems reasonable. Here we have used $`N(0)=0.386(m_b^{}/m)`$ states/eV/atom with band mass $`m_b^{}/m=3.36`$. The effect of s-o scattering on $`\mu (h)`$ is shown in Fig. (3), where $`\mu (h)`$ from Eq. (7) (solid curve) and for $`r_{gm}\mathrm{}`$ (dash curve) are shown versus the s-o scattering parameter $`\gamma _1`$. It turns out that $`\mu (h)`$ is practically independent of ordinary scattering, $`\gamma _0`$. This can be seen from the sum rule result, $`r_{gm}\mathrm{}`$, since $`S`$ and $`u_0`$ are only affected by s-o scattering. Due to the rapid decrease of $`\chi (r)`$ in the presence of scattering the sum rule is approximately exhausted for the experimental $`r_{gm}`$. The decrease of $`\chi (r)`$ at small r seen in Fig. (2b) leads to a reduction of $`\mu (h)`$ by a factor 2 for $`\gamma _10.2`$ and can explain why giant moments are not observed in the Pt granules.

The spin glass freezing temperature $`T_f`$ in dilute impurity systems is determined by the long range spin polarization that provides the RKKY coupling between two magnetic impurities. At large $`r`$ and in the absence of scattering, $`\chi (r)`$ and $`\chi _0(r)`$ are nearly the same and proportional to $`\mathrm{cos}(2k_Fr)/r^3`$. The scale of $`T_f`$ is set by the average RKKY coupling energy of a typical impurity atom pair. Although a correct calculation of $`T_f`$ requires evaluation of the second moment of the distribution of the couplings, an estimate can be obtained from the envelope of $`\chi (r)`$ determined by the peaks of the oscillations. Denoting this quantity by $`<\overline{\chi }(r_{avg})>`$ we take for Fe impurities in Pt

$$k_BT_f\mu _{\text{Fe}}^2\left(\frac{V_{ex}}{2\mu _B}\right)^2\mathrm{\hspace{0.17em}2}N(0)\frac{\mathrm{\Omega }}{a^3}<\overline{\chi }(r_{avg})>,$$
(8)
where $`\mu _{\text{Fe}}`$ is the bare Fe moment. Without scattering, $`k_BT_f=\mu _{\text{Fe}}^2(V_{ex}/2\mu _B)^2\mathrm{\hspace{0.17em}2}N(0)x/4\pi `$, where $`x=n_{\text{Fe}}/n_{\text{Pt}}`$ with $`n_{\text{Fe}}=1/r_{avg}^3`$ and $`n_{\text{Pt}}=4/a^3`$. Using this equation with $`x5`$ppm and $`\mu _{\text{Fe}}=3\mu _B`$, we obtain for bulk Pt a value for $`T_f`$ ($`2.1\text{mK/ppm}`$) that is almost an order of magnitude greater than the observed $`0.26\text{mK/ppm}`$. Our rather large value of $`V_{ex}`$ presumably contributes to this discrepency. Here however, we are concerned with the effect of scattering on $`T_f`$, Eq. (8). In the presence of either ordinary or s-o scattering, $`\overline{\chi }(r)`$ falls off rapidly at large r. A rough numerical fit gives $`\overline{\chi }(r)\mathrm{exp}(5\gamma _ir/a)`$ for $`r/a>\mathrm{\hspace{0.17em}1}/\gamma _i`$ where $`\gamma _i=\gamma _0\text{ or }\gamma _1`$. Although a power law cannot be ruled out, the decrease is in any case much faster than $`1/r^3`$. We can thus conclude that the contributions to $`\chi (r)`$ we have calculated do not lead to a measurable $`T_f`$ in the presence of scattering in granular Pt. However, at large r, diffusion-type diagrams for $`\chi `$ may be dominant leading to a contribution proportional to $`1/r^3`$ and independent of ordinary scattering. In Ref.  it was shown that these contributions are exponentially small in the presence of s-o scattering. Thus it seems quite reasonable that no spin glass transition was observed in the Pt granules.

The single grain superconducting transition temperature $`T_c`$ is affected by scattering only through the indirect effect on the spin fluctuation part pair interaction, $`\lambda _{SF}`$. There is no direct effect for ordinary scattering due to Anderson’s theorem which also holds for s-o scattering , for other scattering processes that obey time-reversal symmetry, and in zero magnetic field. In order to estimate the indirect effect we calculate $`T_c`$ for s-wave pairing with the standard weak-coupling equation:

$$T_c=\mathrm{\Theta }_D\mathrm{exp}\left[\frac{1+\lambda _{Ph}+\lambda _{SF}}{\lambda _{Ph}\lambda _{SF}\mu ^{}}\right].$$
(9)
Here $`\lambda _{SF}`$ is given by Eq. (4) but now with scattering included. We take $`\mathrm{\Theta }_D(Pt)=234K`$ and $`\mu ^{}=0.1`$ which is a standard estimate. We assume $`\lambda _{Ph}0.41`$ is not affected by scattering and it turns out that $`\lambda _{SF}`$ is practically independent of $`\gamma _0`$, yielding a decrease of only a few percent in $`T_c`$. In Fig. (3) we plot $`T_c`$ versus $`\gamma _1`$ for $`\gamma _0=0.01`$. It is seen that the $`T_c`$’s observed in Pt powders  are reached for a s-o scattering rate $`\gamma _1`$ less than 0.1 and that $`T_c`$ increases strongly with increasing $`\gamma _1`$.

In conclusion, we have shown that ordinary and s-o scattering affect the exchange enhanced magnetic properties of the itinerant d electrons so that $`\mu _{gm}`$ and $`T_f`$ of Pt$`\text{Fe}_x`$, e.g., are reduced. On the other hand, s-o scattering weakens the spin fluctuations to the extent that the phonons dominate and superconductivity with $`T_c1`$ mK can occur in single Pt granules. This is possible with moderate s-o scattering since the effective electron-electron interaction in bulk Pt is very close to zero . Of the effects not considered here that could change $`T_c`$, phonon softening is probably the most important. To control surface phonon effects and to complement the studies of grains an experimental search for superconductivity in thin films of Pt is of interest. In films one must distinguish between thick ($`>100\AA `$) films where s-o scattering accounts for the surface effects on the 3D electron states and thin films with smooth surfaces where the Rashba s-o splitting occurs throughout the film thickness. How the spin fluctuations in very thin films of nearly ferromagnetic metals affect (spoil?) the Rashba effect is an open question. It would also be interesting to investigate thin films where the surface roughness suppresses the Rashba effect and s-o scattering reduces $`\lambda _{SF}`$. Finally, the films can become so thin, or the grains so small, that size quantization of electron states occurs that may lead to new effects in the interplay between magnetism and superconductivity.

###### Acknowledgements.

We would like to thank P. Hertel for helpful discussions.


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# Untitled Document

Resonant Absorption between Moving Atoms

due to Doppler Frequency Shift and Quantum Energy Variation

Ching-Chuan Su

Department of Electrical Engineering

National Tsinghua University

Hsinchu, Taiwan

Abstract – By taking both the Doppler frequency shift for electromagnetic wave and the quantum energy variation of matter wave into consideration, a resonant-absorption condition based on the local-ether wave equation is presented to account for a variety of phenomena consistently, including the Ives-Stilwell experiment, the output frequency from ammonia masers, and the Mössbauer rotor experiment. It is found that in the resonant-absorption condition, the major term associated with the laboratory velocity is a dot-product term between this velocity and that of the emitting or absorbing atom. This term appears both in the Doppler frequency shift and the transition frequency variation and then cancels out. Thereby, the experimental results can be independent of the laboratory velocity and hence comply with Galilean relativity, despite the restriction that the involved velocities are referred specifically to the local-ether frame. However, by examining the resonant-absorption condition in the Mössbauer rotor experiment to a higher order, it is found that Galilean relativity breaks down.

1. Introduction

It is well known that the Doppler effect due to the relative motion between a transmitter and a receiver causes a shift in the received frequency of electromagnetic or acoustic wave. The Doppler effect has been applied by Ives and Stilwell to deal with the frequency shift in the light emitted from a fast-moving hydrogen atomic beam . However, it was found that the observed frequency shift agrees with the Doppler effect only to the first order of the atom speed normalized to the speed of light $`c`$. In order to account for the observed shift correctly to the second order, a hypothesis of Larmor and Lorentz was adopted, which states that the frequency of a wave radiated from a moving source of speed $`v`$ is altered by a factor of $`\sqrt{1v^2/c^2}`$ . It is noted that this speed-dependent factor is identical to the one in the famous Lorentz mass-variation law. Presently, an almost unanimously accepted explanation of this additional frequency shift is provided by Einstein’s special relativity, whereby a second-order Doppler effect has been derived based on the Lorentz transformation of space and time . Thus it seems to imply that the frequency shift to the second order between a transmitter and a receiver in relative motion is purely a kinematical property. And, for the case of resonant absorption between moving atoms or ions, it seems to assume tacitly that the transition frequencies of the emitting or the absorbing atoms in motion remain unchanged, in spite of the well-known fact that the electronic quantum states in atoms depend on the mass of electron, which in turn depends on the particle speed. Furthermore, in the common understanding the speed $`v`$ which determines the second-order Doppler frequency shift by the mass-variation factor is the relative speed between the transmitter and the receiver. However, in the Hafele-Keating experiment with circumnavigating atomic clocks and in the GPS (global positioning system) with atomic clocks onboard the orbiting satellites, it has been demonstrated with a high precision that the speed which determines the transition frequency and clock rate by the mass-variation factor is referred uniquely to an ECI (earth-centered inertial) frame . Thus there seems to exist a discrepancy in the reference frame for the speed in the mass-variation factor.

Recently, we have presented the local-ether model of propagation of electromagnetic wave . It is supposed that electromagnetic wave propagates via a medium like the ether. However, the ether is not universal. Specifically, it is supposed that in the region under sufficient influence of the gravity due to the Earth, the Sun, or another celestial body, there forms a local ether which as well as the associated gravitational potential moves with the respective body. Within each local ether, it is proposed that as in the classical propagation model, electromagnetic wave propagates at the speed of light $`c`$ with respect to the associated local ether, independent of the motions of source and receiver. Thereby, for earthbound or interplanetary waves, the propagation is referred specifically to a geocentric or a heliocentric inertial frame, respectively. This local-ether model has been adopted to account for the effects of earth’s motions in a wide variety of propagation phenomena, particularly the Sagnac correction in GPS, the time comparison via intercontinental microwave link, and the echo time in interplanetary radar. As examined within the present accuracy, the local-ether model is still in accord with the Michelson-Morley experiment which is known to make the classical ether notion obsolete. Furthermore, by modifying the speed of light in a gravitational potential, this simple propagation model leads to the deflection of light by the Sun and the increment in the interplanetary radar echo time which are important phenomena supporting the general theory of relativity. Moreover, based on this new classical model, the first-order Doppler frequency shift has been derived to account for the anisotropy in antenna temperature of CMBR (cosmic microwave background radiation), the shift in the spectrum of light radiated from a moving star, and the seasonal variation of eclipse intervals in Roemer’s observations of Jupiter’s moons .

Further, the matter wave associated with a particle has been supposed to follow the local-ether model and be governed by a wave equation incorporating a natural frequency and the electric scalar potential . From the local-ether wave equation, a first-order time evolution equation similar to Schrödinger’s equation is derived. From the electrostatic force derived from this evolution equation, it has been found that the rest mass of a particle is just the natural frequency, aside from a scaling factor. That is, the inertial mass of a particle originates from the natural frequency and hence from the temporal variation of the associated matter wave. Furthermore, due to the dispersion of matter wave, it has been derived that the mass of the particle and the angular frequency of the matter wave increase with the particle speed by the famous Lorentz mass-variation factor, except that the speed is referred specifically to the associated local-ether frame. A feature different from Schrödinger’s equation is that the time derivative in the local-ether evolution equation incorporates an extra multiplying term of the ratio of the speed-dependent angular frequency to the natural frequency. As a consequence, it has been found that the energies of quantum states of the matter wave bounded in an atom decrease with the inverse of the speed-dependent mass . Thus the transition frequency and the atomic clock rate decrease with the atom speed by the mass-variation factor. Thereby, the frequency variation associated with the speed-dependent mass-variation factor has been derived as an intrinsic quantum property of the matter wave bounded in atom. Similarly, the gravitational redshift has been derived as an effect of the gravitational potential on the quantum energy. Anyway, the dependence of quantum energy on speed can be expected at least for hydrogen-like atoms. Since it is well known in standard textbooks on quantum mechanics that the electronic quantum states in such an atom depend on the mass of electron, which in turn has been known to depend on speed. However, according to the local-ether model, the atom speed that determines the mass variation is referred uniquely to an ECI (earth-centered inertial) frame for earthbound atoms. Thus the quantum energy and hence the atomic clock rate tend to depend on earth’s rotation, but is entirely independent of earth’s orbital motion around the Sun or others. This consequence has been used to account for the east-west directional anisotropy in the Hafele-Keating experiment, the synchronism among GPS atomic clocks, and for the spatial isotropy in the Hughes-Drever experiment .

In this investigation, based on the local-ether propagation model, a higher-order Doppler frequency shift for electromagnetic wave is derived. Further, by taking the speed-dependent variation of quantum energy of matter wave into account, we present a resonant-absorption condition between moving emitting and absorbing atoms. Then this frequency relation is applied to deal with various experiments consistently, including the Ives-Stilwell experiment, the output frequency from ammonia masers, and the Mössbauer rotor experiment. Moreover, we examine the spatial isotropy, Galilean relativity, and their breakdowns in these experiments.

2. Higher-Order Doppler Frequency Shift

In this section, based on the local-ether model of wave propagation, the Doppler frequency shift is given to higher orders. Consider the case where both the source and the receiver are located within the same local ether and are moving at velocities $`𝐯_s`$ and $`𝐯_e`$ with respect to this local-ether frame, respectively. According to the classical propagation model, the propagation time $`\tau `$ is the propagation range $`R`$ divided by the isotropic speed $`c`$ as $`\tau =R/c`$. It is important to note that the propagation range is the distance from the position of the source at the instant of wave emission to the one of the receiver at the instant of reception, as viewed in the local-ether frame. Thus the propagation range and hence the propagation time depend on the velocity $`𝐯_e`$ and the acceleration $`𝐚_e`$ of the receiver with respect to the local-ether frame. Quantitatively, when $`\tau `$ is short, the propagation range is given implicitly by

$$R=\left|𝐑_t+𝐯_e\frac{R}{c}+𝐚_e\frac{R^2}{2c^2}\right|,$$
$`(1)`$
where $`𝐑_t`$ is the directed propagation-path length from the source to the receiver both at the instant of emission. It can be shown that to the second order of normalized speed, the propagation range can be given explicitly in terms of the path length $`R_t`$ by

$$R=R_t\left\{1+\frac{1}{c}u_e+\frac{1}{2c^2}\left(u_e^2+v_e^2+𝐚_e𝐑_t\right)\right\},$$
$`(2)`$
where radial speed $`u`$ ($`=𝐯\widehat{R}_t`$) is the component of velocity $`𝐯`$ along $`𝐑_t`$ and the unit vector $`\widehat{R}_t=𝐑_t/R_t`$.

Consider the Doppler effect for the case where the source is emitting wave periodically and is moving with respect to the receiver. Due to the motions of the transmitter and receiver, the rate of reception tends to be different from the one of emission. As discussed in , the received time difference $`\mathrm{}t`$ between two signals transmitted with a differential time difference $`\mathrm{}t^{}`$ can be given in terms of the difference in the propagation range by

$$\mathrm{}t=\mathrm{}t^{}+\frac{R(t^{}+\mathrm{}t^{})}{c}\frac{R(t^{})}{c},$$
$`(3)`$
where $`R(t)`$ denotes the propagation range for the wave emitted at an arbitrary instant $`t`$. Then the received frequency $`f_r`$ and the transmitted frequency $`f_t`$ are related by

$$\frac{f_t}{f_r}=\frac{\mathrm{}t}{\mathrm{}t^{}}=1+\frac{dR}{cdt},$$
$`(4)`$
where the time derivative of the propagation range is evaluated at the instant of wave emission.

The second-order Doppler effect can be given if the first-order formula of the propagation range is used. By so doing, the Doppler frequency relation becomes

$$\frac{f_t}{f_r}=1+\frac{dR_t}{cdt}+\frac{d}{c^2dt}(𝐯_e𝐑_t).$$
$`(5)`$
Due to the relative motion between source and receiver, $`d𝐑_t/dt=𝐯_{es}`$ and hence $`dR_t/dt=u_{es}`$, where $`𝐯_{es}`$ ($`=𝐯_e𝐯_s`$) is the Newtonian relative velocity between receiver and source at the instant of emission and $`u_{es}`$ ($`=u_eu_s`$) is the radial speed of the receiver with respect to the source. Thus, as given in , the second-order Doppler frequency relation becomes

$$\frac{f_t}{f_r}=1+\frac{u_{es}}{c}+\frac{𝐯_e𝐯_{es}}{c^2}+\frac{𝐚_e𝐑_t}{c^2}.$$
$`(6)`$
It is noted that the transverse components of velocities are also involved in the second-order Doppler shift. To the second order of normalized speed, the inverse frequency ratio reads

$$\frac{f_r}{f_t}=1\frac{u_{es}}{c}\frac{𝐯_e𝐯_{es}}{c^2}\frac{𝐚_e𝐑_t}{c^2}+\frac{u_{es}^2}{c^2}.$$
$`(7)`$
When the third-order Doppler effect needs to be considered, the second-order formula of the propagation range should be used, as discussed later.

3. Quantum Energy Variation and Resonant-Absorption Condition

Based on the local-ether wave equation, it has been found that the mass of a particle increases with its speed by the famous Lorentz mass-variation factor, except that the speed is referred specifically to an ECI frame for earthbound particles . From this wave equation a first-order time evolution equation is derived, which is similar to Schrödinger’s equation except that the time derivative is referred specifically to the local-ether frame and incorporates an extra multiplying term of the mass-variation factor. Thereby, a quantum-mechanical approach has been presented to show that the energies of quantum states of the matter wave bounded in an atom or a molecule decrease with the inverse of the speed-dependent mass. It is known that the frequency of light emitted from or absorbed by an atom is equal to the transition frequency, which in turn corresponds to the difference in energy between two involved quantum states. Thus the state transition frequency $`f`$ of a moving atom decreases with its speed by the speed-dependent mass-variation factor as

$$f=f_0\sqrt{1v^2/c^2},$$
$`(8)`$
where $`v`$ is the atom speed referred to the local-ether frame which is an ECI frame for earthbound atoms, $`f_0`$ is the rest transition frequency of an identical atom stationary in the local-ether frame, and the frequency $`f`$ is observed in the atom frame (with respect to which the atom is stationary) such that no Doppler shift is involved.

The atomic clock rate depends on the transition frequency of the associated atom and hence decreases with the atom speed by the mass-variation factor. The preceding speed-dependent frequency-variation formula has been adopted in  to account for the east-west directional anisotropy in the clock rate demonstrated in the Hafele-Keating experiment with cesium atomic clocks onboard an aircraft undergoing circumnavigation . In this experiment the observed clock rate is determined from the number of the atomic clock ticks which in turn are detected and counted by a device which is comoving with the clock without relative motion. Thus the clock rate is associated with the quantum energy variation, but has nothing to do with the Doppler frequency shift. Moreover, it has been used to account for the synchronism and the clock-rate adjustment in GPS atomic clocks onboard earth’s satellites in circular orbits.

A speed-dependent frequency of the form of (8) (but of different physical origin and reference frame of speed) was first introduced by Fitzgerald, Lorentz, and Larmor before the advent of the special relativity  and was later derived by assuming the length contraction  or the time dilation . In the local-ether model, the frequency-variation formula due to the quantum effect is not expected to hold in all energy states in all atoms and other forms of the speed-dependence are not precluded. This is in view of the complication that the interactions which affect energy states are versatile, such as electronic or nuclear, electric or magnetic, spin or orbital, and intrinsic or external. In , the frequency-variation formula is verified only for electronic states due to the electric scalar potential in an atom or a molecule. Nevertheless, it is assumed that this formula holds in the experiments examined in this investigation.

Then we proceed to consider the case where the source atom $`s`$ and the receiver atom $`e`$ are located within the same local ether but are moving respectively at velocities $`𝐯_s`$ and $`𝐯_e`$ with respect to the local-ether frame. Due to the motions of the source and receiver, the Doppler effect also causes a frequency shift. Suppose $`f_{0s}`$ and $`f_{0e}`$ are the rest transition frequencies of atoms $`s`$ and $`e`$, respectively. The transmitted frequency $`f_t`$ of the wave emitted from the moving atom $`s`$ is related to the rest transition frequency $`f_{0s}`$ as

$$f_t=f_{0s}\sqrt{1v_s^2/c^2}.$$
$`(9)`$
On the other hand, in order for the wave being resonantly absorbed by the moving atom $`e`$, the rest transition frequency $`f_{0e}`$ should be related to the received frequency $`f_r`$ as

$$f_r=f_{0e}\sqrt{1v_e^2/c^2}.$$
$`(10)`$
The received frequency $`f_r`$ and the transmitted frequency $`f_t`$ in turn are related to each other by the Doppler effect as shown in (6) or (7).

Thus, by taking both the Doppler frequency shift for electromagnetic wave and the quantum energy variation of matter wave into account, we arrive at the resonant-absorption condition in terms of the rest transition frequencies $`f_{0s}`$ and $`f_{0e}`$, which to the second order of normalized speed is given by

$$f_{0e}\sqrt{1v_e^2/c^2}=f_{0s}\sqrt{1v_s^2/c^2}\left\{1u_{es}/c(𝐯_e𝐯_{es}+𝐚_e𝐑_tu_{es}^2)/c^2\right\}.$$
$`(11)`$
For the case where the receiver is comoving with the source ($`𝐯_e=𝐯_s`$) without acceleration, the resonant-absorption condition becomes trivially as $`f_{0e}=f_{0s}`$. This resonant-absorption condition made its debut in .

When the resonant-absorption condition is not met, the off-resonance absorption tends to be much weaker. The deviation in frequency from the resonant-absorption condition is given by the difference between the received frequency and the transition frequencies of the absorbing atoms in motion. That is,

$$\delta f=f_rf_{0e}\sqrt{1v_e^2/c^2}.$$
$`(12)`$
By using (9), the frequency deviation can be written as

$$\delta f=\mathrm{}f_D\mathrm{}f_Q,$$
$`(13)`$
where $`\mathrm{}f_D`$ and $`\mathrm{}f_Q`$ denote the frequency shifts due to the Doppler and the quantum effects and are given by

$$\mathrm{}f_D=f_rf_t$$
$`(14)`$
and

$$\mathrm{}f_Q=f_{0e}\sqrt{1v_e^2/c^2}f_{0s}\sqrt{1v_s^2/c^2},$$
$`(15)`$
respectively. In words, $`\mathrm{}f_Q`$ is the difference in the speed-dependent transition frequency between the receiver and source atoms in motion. From (4) it is seen that the fractional Doppler frequency shift is given by

$$\frac{\mathrm{}f_D}{f_r}=\frac{dR}{cdt}.$$
$`(16)`$
The resonant-absorption condition corresponds to the deviation $`\delta f=0`$, which means that the frequency shift due to the Doppler effect for electromagnetic wave propagating in free space exactly cancels the one due to the quantum effect of matter wave bounded in atom.

4. Reexamination of Resonant-Absorption Experiments

Based on the local-ether model, we reexamine the resonant-absorption experiments reported in the literature. Thereby, we present reinterpretations of the Ives-Stilwell experiment, the output frequency from ammonia masers, and of the Mössbauer rotor experiment and explore the associated spatial isotropy, Galilean relativity, and their breakdowns. The first experiment is associated with a radial relative motion ($`u_{es}\pm v_{es}`$) and the last two are with a transverse relative motion ($`u_{es}=0`$).

4.1. Ives-Stilwell experiment

Consider the case where the source is moving at a velocity $`𝐯_s`$ and the receiver is stationary, both with respect to the local-ether frame. Thus $`a_e=0`$, $`v_e=0`$, and $`u_{es}=u_s`$. Then the second-order resonant-absorption condition becomes a simpler form of

$$f_{0e}=f_{0s}\frac{\sqrt{1v_s^2/c^2}}{1u_s/c}.$$
$`(17)`$
For this case $`f_r=f_{0e}`$ and thus this formula is identical to that derived in different ways based on the transformation of four-vectors  or on the time dilation , except the difference in reference frame of velocity $`𝐯_s`$. According to the local-ether model, the term $`(1u_s/c)`$ in the preceding formula is due to the Doppler frequency shift to the second order, while the term $`\sqrt{1v_s^2/c^2}`$ is due to the quantum energy variation.

A similar frequency shift has been demonstrated in the Ives-Stilwell experiment, where light is emitted from fast-moving hydrogen atoms in an excited state and is absorbed by a spectrograph used to measure the received frequency . The radiation from the moving atoms is reflected from two mirrors and then the two reflected light beams are guided to a photographic plate where the frequencies are recorded for measurement and comparison. The two mirrors are arranged in such a way that the atoms are moving toward one of them and away from the other . Due to the Doppler effect with the relative motions between the emitting atoms and the mirrors, the light beams reflected from the mirrors tend to shift in frequency. However, by virtue of no relative motions among the mirrors, the spectrograph, and the other components of experimental setup, no further Doppler effect is introduced after the reflection.

Note that even for a geostationary experimental setup, the receiver is not stationary with respect to the associated local-ether frame due to earth’s rotation. Consider the laboratory frame in which the setup and the receiver are stationary. Suppose that the emitting atoms are moving at a velocity $`𝐯_t`$ with respect to the laboratory frame, which in turn moves at a velocity $`𝐯_0`$ with respect to an ECI frame. Thus $`𝐯_e=𝐯_0`$, $`𝐯_s=𝐯_t+𝐯_0`$, and $`𝐯_{es}=𝐯_t`$. In the experiment the atoms move nearly in the radial direction and the directions of the two propagation paths are antiparallel. Thus $`u_{es}=v_t\mathrm{cos}\theta `$, where $`\theta `$ denotes the small angle of $`𝐯_t`$ from $`\widehat{R}_t`$, $`\pm \widehat{R}_t`$ represents the direction from the emitting atoms to the reflecting point on either mirror, and the upper or the lower sign applies for the light beam reflected from the mirror which the atoms approach or recede from, respectively. Then the resonant-absorption condition (11) leads to that the received frequencies for the two reflected light beams are

$$f_{r\pm }=f_{0s}\sqrt{1(𝐯_t+𝐯_0)^2/c^2}\left\{1\pm v_t\mathrm{cos}\theta /c+(𝐯_0𝐯_t+v_t^2\mathrm{cos}^2\theta )/c^2\right\}.$$
$`(18)`$
It is noted that the first-order term is independent of the laboratory velocity $`𝐯_0`$. If the velocity $`𝐯_0`$ is neglected, the preceding formula reduces to (17).

To the second order of normalized speed, the received frequencies become

$$f_{r\pm }=f_{0s}\left\{1v_t\mathrm{cos}\theta /c+(v_t^2+v_0^2)/2c^2\right\}^1.$$
$`(19)`$
Both the Doppler and the quantum effects contribute to the second-order terms. It is noted that the dot-product term $`𝐯_0𝐯_t`$ appears both in the Doppler and the quantum effects and then cancels out. In the Ives-Stilwell experiment the speed $`v_t`$ of hydrogen atoms is of the order of 10<sup>6</sup> m/sec, which is achieved by electrostatically accelerating hydrogen ions with a voltage of tens of kV. Thus the atom speed $`v_t`$ is much higher than the laboratory speed $`v_0`$ which is due to earth’s rotation and, perhaps, to the motion of a vehicle carrying the experimental setup. Thus the preceding frequency formula can be substantially independent of the laboratory velocity $`𝐯_0`$.

The first- and the second-order fractional frequency shifts are associated with the difference between and with the sum of the two received frequencies, respectively. Thus, in terms of wavelengths, the normalized speed and its square can be given by

$$\frac{v_t}{c}=\frac{1}{2\mathrm{cos}\theta }\frac{\lambda _R\lambda _B}{\lambda _0}$$
$`(20)`$
and

$$\frac{v_t^2}{c^2}=\left(\frac{\lambda _R+\lambda _B}{\lambda _0}2\frac{v_0^2}{c^2}\right),$$
$`(21)`$
where $`\lambda _B=c/f_{r+}`$, $`\lambda _R=c/f_r`$, and $`\lambda _0=c/f_{0s}`$. By measuring $`\lambda _R`$ and $`\lambda _B`$, the first- and the second-order fractional shifts can be calculated and compared, with a knowledge of $`\theta `$, $`\lambda _0`$, and $`v_0`$. This provides a crucial means to test the minor second-order frequency shift. It can be expected that the deviation of the sum $`\lambda _R+\lambda _B`$ from $`2\lambda _0`$ is quite small. By using a high-precision spectrograph, it has been measured that $`\lambda _R=6618.808`$ (in angstrom) and $`\lambda _B=6507.253`$ . Meanwhile, it is known that $`\lambda _0=6562.793`$ and $`\theta =0.075`$ (in rad). Then formulas (20) and (21) lead to $`v_t^2/c^2=7.26\times 10^5`$ and 7.24$`\times 10^5`$, respectively, where the term $`v_0^2/c^2`$ is as small as 10<sup>-12</sup> and hence is omitted. The agreement between the two data is quite good, since the discrepancy is as small as the round-off in the calculation. According to the local-ether model, the wavelength $`\lambda _0`$ corresponds to a transition frequency of a hydrogen atom stationary with respect to an ECI frame. This seems to be in accord with the description that $`\lambda _0`$ is the wavelength of the H<sub>α</sub> line of the Balmer series observed in a reference frame at rest with respect to the radiating atom . However, the value of $`\lambda _0`$ could be actually measured from geostationary atoms in a geostationary laboratory. Even so, the fractional discrepancy in $`\lambda _0`$ due to the difference in reference frame is also of the order of $`v_0^2/c^2`$. Thus the local-ether model is in accord with the self-consistency between the first- and the second-order frequency shifts demonstrated in the Ives-Stilwell experiment.

4.2. Output frequency from ammonia masers

Next, we consider the case where the source is moving transverse to the propagation path. In the ammonia maser, the molecular beam is injected into a resonant cavity and emits microwave due to quantum state transition . The output of the microwave comes through a waveguide coupled to the cavity via a small aperture. Suppose that the cavity and the receiver are stationary in the laboratory frame of velocity $`𝐯_0`$ and that the emitting ammonia molecular beam moves at a velocity $`𝐯_t`$ with respect to the cavity. Moreover, suppose that the output waveguide is thin and long and is positioned with its longitudinal axis being perpendicular to the direction of molecular beam represented by $`𝐯_t`$. Thus the direction of the propagation path of the microwave is virtually parallel to the longitudinal axis of the output waveguide and hence is transverse to the molecule velocity, that is, $`𝐯_t\widehat{R}_t=0`$.

Thus $`𝐯_e=𝐯_0`$, $`𝐚_e=0`$, $`𝐯_s=𝐯_t+𝐯_0`$, $`𝐯_{es}=𝐯_t`$, and $`u_{es}=0`$. Then the resonant-absorption condition (11) leads to the received frequency

$$f_r=f_{0s}\sqrt{1(𝐯_t+𝐯_0)^2/c^2}\left\{1+𝐯_0𝐯_t/c^2\right\}.$$
$`(22)`$
The Doppler effect is presented by the dot-product term $`𝐯_0𝐯_t`$. Thus, by taking both the Doppler and the quantum effects into account, the resonant-absorption condition leads to that the received frequency at the output waveguide of the maser is given by

$$\frac{f_r}{f_{0s}}=1\frac{v_t^2+v_0^2}{2c^2}.$$
$`(23)`$
It is noted again that the dot-product term $`𝐯_0𝐯_t`$ appears both in the Doppler and the quantum effects and then cancels out. Consequently, the output frequency from the maser is independent of the directions of velocities $`𝐯_t`$ and $`𝐯_0`$. Moreover, the resonant-absorption condition leads to

$$\frac{f_{0e}}{f_{0s}}=1\frac{v_t^2}{2c^2}.$$
$`(24)`$
It is seen that this frequency relation is even independent of the laboratory velocity $`𝐯_0`$.

It is noticed that a term quite similar to the second-order Doppler effect in (22) has been derived alternatively from a classical approach, aside from the reference frame of the laboratory velocity . Further, a similar cancellation of the terms associated with $`𝐯_0`$ has been accounted for by an alternative approach, where a speed-dependent frequency based on the time dilation is used . Anyway, it has been demonstrated experimentally that the beat frequency between two masers with molecular beams moving in opposite directions is substantially zero and is almost independent of earth’s motions . Thus the local-ether model is in accord with the experiments with ammonia masers.

4.3. Mössbauer rotor experiment

Then we consider the case where both the source and the absorber are moving in the laboratory frame. The Mössbauer rotor experiment is based on the recoilless gamma-ray nuclear resonance absorption known as the Mössbauer effect \[13-17\]. The source and the absorber of gamma ray are placed separately on a rotating rod. Both the quantum energy variation of nuclear states and the Doppler frequency shift of wave propagation cause the frequency shift. A frequency deviation from the resonant-absorption condition exhibits itself with an increase in the scattering of gamma ray, which in turn can be measured by counters fixed at the laboratory or at the rod.

Suppose that the absorber and the source atoms in the Mössbauer rotor experiment rotate about an axis with linear velocities $`𝐯_r`$ and $`𝐯_t`$, respectively, where the axis is stationary in a laboratory frame which in turn moves at a velocity $`𝐯_0`$ with respect to the local-ether frame. In the rotor experiment, the directed path length $`𝐑_t`$ from the source to the absorber is always perpendicular both to $`𝐯_r`$ and $`𝐯_t`$. Moreover, the path length $`R_t`$ is fixed, while the direction $`\widehat{R}_t`$ is changing with time. Thus $`dR_t/dt=0`$ and $`d𝐑_t/dt=𝐯_{rt}`$, where $`𝐯_{rt}=𝐯_r𝐯_t`$.

To the second order of normalized speed, the fractional Doppler frequency shift (16) due to the motions of the source and receiver becomes

$$\frac{\mathrm{}f_D}{f_r}=\frac{d}{cdt}\left(R_t+\frac{1}{c}𝐯_0𝐑_t\right)=\frac{𝐯_0𝐯_{rt}}{c^2},$$
$`(25)`$
where the orthogonality $`𝐯_r𝐑_t=0`$ has been made use of and the derivative $`d𝐯_0/dt`$ is omitted. It is seen that this frequency shift depends on the laboratory velocity $`𝐯_0`$. It is noted that due to the path length $`R_t`$ being a constant, the first-order term of normalized speed vanishes in the preceding formula. Thus, to the third order of normalized speed, the fractional shift $`\mathrm{}f_D/f_{0e}`$ is identical to the preceding formula of $`\mathrm{}f_D/f_r`$.

Consider the case where the source and the absorber have the identical rest transition frequency $`f_0`$. Thus the fractional frequency shift due to the quantum effect is

$$\frac{\mathrm{}f_Q}{f_0}=\sqrt{1(𝐯_r+𝐯_0)^2/c^2}\sqrt{1(𝐯_t+𝐯_0)^2/c^2}\frac{1}{2c^2}(2𝐯_{rt}𝐯_0v_r^2+v_t^2).$$
$`(26)`$
It is noted that the dot-product term $`𝐯_{rt}𝐯_0`$ appears again. Consequently, by taking both the Doppler and the quantum effects into account to the second order of normalized speed, the fractional frequency deviation from the resonant absorption is

$$\frac{\delta f}{f_0}=\frac{v_r^2v_t^2}{2c^2}.$$
$`(27)`$
It is noted that the dot-product term $`𝐯_0𝐯_{rt}`$ cancels out and hence the frequency deviation is independent of the directions of velocities $`𝐯_r`$ and $`𝐯_t`$. Furthermore, this frequency deviation is independent of the laboratory velocity $`𝐯_0`$.

It is noticed again that a term quite similar to the second-order Doppler effect in (25) has been derived alternatively from a classical approach, aside from the reference frame of the laboratory velocity . Further, a similar cancellation of the terms with $`𝐯_0`$ has been accounted for by an alternative approach, where a speed-dependent frequency based on the length contraction is used . Anyway, this fractional frequency deviation has been demonstrated in experiments with various rotation rates and various positions of the source and the absorber at the rod \[13-15\]. Moreover, it has been found that between the two geostationary counters oriented to detect the gamma rays propagating south- and northward, respectively, there is no substantial difference in the measured frequency deviation . Thus the frequency deviation can be independent of the orientation of counter. Based on these, the local-ether model is also in accord with the Mössbauer rotor experiment.

4.4. Spatial isotropy, Galilean relativity, and their breakdowns

According to the local-ether model, the speed of an earthbound atom is referred to an ECI frame. Thus the quantum energy in an atom is entirely independent of earth’s orbital motion around the Sun or whatever. Further, the quantum energy can even be independent of earth’s rotation, if the atom speed remains a constant during the rotation. Such a constant-speed condition is met by a geostationary atom, by an atom moving at a fixed velocity with respect to ground at a substantially fixed latitude, or by an atom moving in a circular satellite orbit around the Earth. For an atom satisfying the constant-speed condition, the energies of quantum states and hence the transition frequency between two states are independent of the orientation and position of the Earth in space, whatever the dependence of quantum energy on the speed. This spatial isotropy of transition frequency with respect to earth’s motions has been adopted in  to account for the hourly and daily frequency stability in geostationary atoms in the Hughes-Drever experiment  and for the high synchronism among the various GPS atomic clocks moving in circular orbits . On the other hand, for two atomic clocks moving even at an identical speed but in different directions with respect to the ground, their speeds with respect to an ECI frame tend to be different. Thereby, this isotropy breaks down, as demonstrated in the east-west directional anisotropy in atomic clock rate in the Hafele-Keating experiment .

The applicability of the aforementioned spatial isotropy can be extended to the cases where electromagnetic wave as well as matter wave is involved. According to the local-ether model, the results of an earthbound experiment are entirely independent of earth’s orbital motion. Further, the results can be independent of earth’s rotation, so long as the atom speeds $`v_e`$, $`v_s`$, $`u_e`$, and $`u_s`$ along with the terms $`𝐯_e𝐯_s`$ and $`𝐚_e𝐑_t`$ are invariant under earth’s rotation. Thereby, the frequency-variation formula (8), the propagation-range formula (2), and the resonant-absorption condition (11) remain unchanged under earth’s rotation and hence the associated phenomena exhibit the spatial isotropy. In the Ives-Stilwell experiment and the ammonia maser, it is seen that the speeds $`v_e`$ and $`v_s`$ are invariant under earth’s rotation and the acceleration $`𝐚_e`$ is zero. Moreover, the terms $`u_e`$, $`u_s`$, and $`𝐯_e𝐯_s`$ are invariant under earth’s rotation, since $`𝐯_e`$, $`𝐯_s`$, and $`𝐑_t`$ all change in a coordinated way with earth’s rotation. Thus the spatial isotropy can be expected in these experiments and has been demonstrated in the hourly and daily stability of the output frequency from ammonia masers .

The spatial isotropy with respect to earth’s motions can be generalized with a step forward. As the velocities $`𝐯_e`$ and $`𝐯_s`$ are written in the laboratory frame of velocity $`𝐯_0`$, the terms $`𝐯_r𝐯_0`$, $`𝐯_t𝐯_0`$, and $`v_0^2`$ emerge in the relevant formulas. It has been indicated that the dot-product term $`𝐯_r𝐯_0`$ or $`𝐯_t𝐯_0`$ can be common in the Doppler and the quantum effects and then cancels out. Consequently, the results of the experiment are independent of the orientation of the setup with respect to the ground. Thus the experiment possesses a spatial isotropy with respect to the setup orientation as well as to earth’s motions. This kind of spatial isotropy is observed in the three experiments examined so far. Thereby, the output frequency from the ammonia maser is independent of the direction of the molecule velocity and hence no observable beat frequency between masers with different orientations can be expected, as demonstrated experimentally in . Moreover, the frequency deviation from the resonant absorption in the Mössbauer rotor experiment can be expected to be stable under earth’s rotation and be identical for counters with different orientations, as demonstrated experimentally in .

Further, the squared term $`v_0^2/c^2`$ in some frequency formulas cancels out or is too small to detect. As a consequence, the experimental results become independent of the laboratory velocity $`𝐯_0`$ and hence comply with Galilean relativity, in spite of the restriction on the reference frame of the particle and the propagation velocities. Thus, when the whole experimental setup is put on a vehicle moving smoothly with respect to the ground, the measurement results can be independent of the ground velocity of the vehicle, as well as of the setup orientation and earth’s motions. Thereby, the spatial isotropy is generalized to the compliance with Galilean relativity. In this way, it is seen that the Mössbauer rotor experiment complies with Galilean relativity. Moreover, Galilean relativity can also be observed in the Ives-Stilwell experiment and in the output frequency from the ammonia maser, as the minute squared term is difficult to detect. Anyway, these experiments preserve the spatial isotropy with respect to the setup orientation and earth’s motions.

However, when the measurement precision is improved such that higher-order effects can be detected, some minute terms may emerge to make Galilean relativity or even the spatial isotropy break down. The just-mentioned squared term $`v_0^2/c^2`$ in the Ives-Stilwell experiment and the ammonia maser is an example. For another, we reexamine the Mössbauer rotor experiment to a higher order. In order to derive the Doppler effect to the third order of normalized speed, the second-order propagation-range formula (2) is needed, which for the Mössbauer rotor experiment becomes

$$R(t)=R_t\left\{1+\frac{1}{c}u_0+\frac{1}{2c^2}[u_0^2+(v_r^2+v_0^2+2𝐯_r𝐯_0)+𝐚_e𝐑_t]\right\}.$$
$`(28)`$
For a rotation at a fixed angular velocity, the terms of $`v_r`$ and $`𝐚_e𝐑_t`$ as well as $`v_0`$ are constants during rotation. Thus the time rate of change of the propagation range $`R`$ is given by

$$\frac{dR(t)}{dt}=R_t\frac{d}{dt}\left\{\frac{1}{c}u_0+\frac{1}{2c^2}[u_0^2+2𝐯_r𝐯_0]\right\}.$$
$`(29)`$
Then, to the third order of normalized speed, the fractional Doppler frequency shift due to wave propagation can be given from (16) as

$$\frac{\mathrm{}f_D}{f_0}=\frac{dR}{cdt}=\frac{1}{c^2}𝐯_{rt}𝐯_0\frac{1}{c^3}[(𝐯_{rt}𝐯_0)u_0v_rv_{rt}u_0],$$
$`(30)`$
where we have made use of $`d𝐯_r/dt=\widehat{R}_tv_rv_{rt}/R_t`$ and of $`\mathrm{}f_D/f_0=\mathrm{}f_D/f_r`$ to the third order. It is seen that $`\mathrm{}f_D=0`$ when $`v_0=0`$.

By taking both the Doppler and the quantum effects into account to the third order of normalized speed, the fractional frequency deviation from the resonant absorption is

$$\frac{\delta f}{f_0}=\frac{1}{2c^2}(v_r^2v_t^2)\frac{1}{c^3}(𝐯_{rt}𝐯_0v_rv_{rt})u_0.$$
$`(31)`$
It is noted that the dot-product term $`𝐯_{rt}𝐯_0`$ survives in the third-order effect, although it cancels out in the second-order one. The presence of this term then makes the spatial isotropy with respect to the setup orientation and hence Galilean relativity break down, although it is quite small in magnitude. Accordingly, the frequency deviations tend to be different as measured in counters with different orientations with respect to the ground, when they can be measured to the third order. Thereby, a directional anisotropy in the frequency deviation is predicted. On the other hand, the spatial isotropy with respect to earth’s rotational and orbital motions is preserved.

5. Conclusion

Based on the local-ether wave equation for matter wave, the energies of quantum states and hence the state transition frequency in an atom decrease with the atom speed by the mass-variation factor, where the speed is referred to the associated local-ether frame. Further, for the situation where the source and the receiver atoms move at different velocities, the local-ether resonant-absorption condition is presented by taking both the Doppler frequency shift for electromagnetic wave and the quantum energy variation of matter wave into account. It is shown that the resonant-absorption condition accounts for the Ives-Stilwell experiment, the output frequency from ammonia masers, and the Mössbauer rotor experiment in a consistent way.

Based on the local-ether model, it is evident that the phenomena due both to electromagnetic and matter waves do not at all depend on earth’s orbital motion around the Sun or others. This immediately accounts for the null effect of earth’s orbital motion in various earthbound phenomena. Further, for a geostationary experimental setup, the results can be independent of earth’s rotation. This accounts for the spatial isotropy found in the stability of frequency in the Hughes-Drever experiment and the ammonia maser. The spatial isotropy also holds for the atomic clocks onboard earth’s satellites moving in circular orbits and hence accounts for the high synchronism among the various GPS atomic clocks. Further, in the formula of the Doppler or the quantum effect, it is seen that the major term associated with the laboratory velocity is a dot product between this velocity and that of the emitting or absorbing atom. This term appears both in the Doppler frequency shift and the transition frequency variation and then cancels out. Thus the experimental results become invariant with respect to the setup orientation, as well as to earth’s motions. This spatial isotropy has been demonstrated in the ammonia maser where the output frequency is independent of the direction of the molecule velocity and in the Mössbauer rotor experiment where the frequency deviation from the resonant absorption is independent of the orientation of the counter. Further, the frequency deviation is independent of the laboratory velocity and hence the Mössbauer rotor experiment complies with Galilean relativity.

However, the aforementioned dot-product term with the laboratory velocity may survive in some formulas. Thus the spatial isotropy with respect to the setup orientation and hence Galilean relativity break down. This breakdown is in accord with the east-west directional anisotropy in atomic clock rate demonstrated in the Hafele-Keating experiment. By examining the resonant-absorption condition in the Mössbauer rotor experiment to the third order, such a breakdown is also found. Thereby, it is expected that the frequency deviation tends to be different as measured in counters with different orientations. This predicted directional anisotropy in the frequency deviation may provide a mean to test the local-ether model, if the measurement precision can be raised to the third order of normalized speed.

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