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# 1 The angular power spectrum with correlated mixture of the adiabatic and isocurvature perturbations in the baryonic sector (solid line), in the CDM sector (long-dashed line), and in the baryonic and CDM sectors (dot-dashed line). (See Eqs. (), (), and (), respectively.) We also show the CMB angular power spectrum in the purely adiabatic (short-dashed line) and isocurvature density perturbations (dotted line). We consider the flat universe with Ω_𝑏ℎ²=0.019, Ω_𝑚=0.3, and ℎ=0.65, where Ω_𝑏 and Ω_𝑐 are the (present) density parameters for the baryon and the CDM, respectively, and ℎ is the Hubble constant in units of 100 km/sec/Mpc. The overall normalizations are taken as [𝑙(𝑙+1)𝐶_𝑙/2𝜋]_{𝑙=10}=1.

In supersymmetric models, it is known that there are various light scalar fields which play important roles in cosmology. In particular, in many class of scenarios, there exists a scalar field (other than the inflaton) which once dominates the universe and decays at a later stage of the evolution of the universe. Indeed, this is the case in, for example, Affleck-Dine baryogenesis  and sneutrino-induced leptogenesis . In addition, if the modulus field acquires a large amplitude at the beginning of the universe, it is expected to decay after the big-bang nucleosynthesis (BBN) and spoils the success of the BBN if their masses are of $`O(100\mathrm{GeV}1\mathrm{TeV})`$ . One solution to this cosmological difficulty is to push up the mass of the modulus field and make it decay before the BBN starts . Although these scenarios have been attracted many attentions, it is very difficult to observe the consequence of the late-decaying scalar condensations.

One of the most important consequences of such scenarios is that the cosmic microwave background (CMB) radiation we observe today originates to the late-decaying scalar field (denoted as $`\varphi `$ hereafter) rather than the inflaton field. Thus, if there exists a primordial fluctuation in the amplitude of $`\varphi `$, it becomes a new source of the cosmic density perturbations and affects the CMB anisotropy. In particular, recently the observation of the CMB power spectrum is being greatly improved and hence it may be possible to observe some signal in the CMB anisotropy from the late-decaying scalar condensations. Thus, it is very important to discuss the CMB anisotropy taking account of the effects of the late-decaying scalar condensations, which is the subject of the study here. We will see that, if the scalar condensation acquires a primordial fluctuation, it may significantly affect the CMB angular power spectrum. In particular, we will emphasize that the conventional constraints on the inflation models can be greatly relaxed if such a scalar field exists. In addition, in some case, correlated mixture of the adiabatic and isocurvature density fluctuations can be generated in such a scenario and the on-going MAP  experiment may observe the signal of the late-decaying scalar condensations.

Let us start our discussion with introducing the scenario we have in mind. Here, we consider the thermal history with a scalar field $`\varphi `$ which decays and produces a large amount of entropy at a late stage of the evolution of the universe. In this study, we assume inflation to solve horizon, flatness, and other cosmological problems. Then, after the inflation, the universe is reheated and the radiation dominated universe is realized. We call this epoch as the RD1 epoch.

If the potential of $`\varphi `$ is dominated by the parabolic term, $`\varphi `$ changes its behavior depending on the relative size of $`H`$ and $`m_\varphi `$, where $`m_\varphi `$ is the mass of $`\varphi `$ and $`H`$ is the expansion rate of the universe. In the very early universe, the total energy density of the universe is extremely large and hence the relation $`Hm_\varphi `$ holds. In this case, the slow-roll condition is satisfied and $`\varphi `$ takes (almost) constant value. On the contrary, as the universe expands, $`H`$ becomes smaller than $`m_\varphi `$ at some point. Then, $`\varphi `$ oscillates and the energy density of $`\varphi `$ decrease as $`\rho _\varphi a^3`$. Consequently, the energy density of the radiation decreases faster than $`\rho _\varphi `$ if $`H_{}^<m_\varphi `$. Thus, if the initial amplitude of the scalar field, denoted as $`\varphi _{\mathrm{init}}`$, is large enough, the universe is once dominated by the scalar field $`\varphi `$ after the RD1 epoch. (We call this epoch as $`\varphi `$D epoch.) In the following, we assume that $`\varphi _{\mathrm{init}}`$ is large enough so that the $`\varphi `$D epoch is realized. Then, $`\varphi `$ decays when $`H\mathrm{\Gamma }_\varphi `$ with $`\mathrm{\Gamma }_\varphi `$ being the decay rate of $`\varphi `$. After the decay of $`\varphi `$, the radiation-dominated universe is realized. We call this epoch as RD2 epoch.

In this framework, the CMB radiation we observe today originates to the scalar field $`\varphi `$, not to the inflaton field. Thus, if $`\varphi `$ has an primordial fluctuation, it also affects the CMB anisotropy. Such a fluctuation is expected to be generated during the inflation; for the Fourier mode with comoving momentum $`k`$, the initial value of the fluctuation of $`\varphi `$ is given by $`\delta \varphi (t,\stackrel{}{k})=\left[H_{\mathrm{inf}}/2\pi \right]_{k=aH_{\mathrm{inf}}}`$, where $`H_{\mathrm{inf}}`$ is the expansion rate of the universe during the inflation. (Here, we assumed $`m_\varphi H_{\mathrm{inf}}`$.)

In this class of scenario, there are two independent sources of the cosmic density perturbations; one is the primordial fluctuation of the inflaton field $`\chi `$ and the other is the primordial fluctuation of the scalar field. Since we use the linear perturbation theory, their effects can be discussed separately. The effect of the inflaton-field fluctuation $`\delta \chi `$ is parameterized by the metric perturbation $`\mathrm{\Psi }^{(\delta \chi )}`$ generated by the inflaton fluctuation. (The superscript $`(\delta \chi )`$ is for perturbations from the inflaton fluctuation.) It is well-known that inflaton fluctuation provides the adiabatic density fluctuations, i.e., no entropy perturbation is generated from $`\delta \chi `$. Thus, in the following, we study the effects of the primordial fluctuation of the scalar field $`\varphi `$.

Since we are interested in the CMB anisotropy, it is crucial to understand the relations among the density fluctuations of each components, like photon, CDM, baryon, and so on, after the decay of the scalar field $`\varphi `$. For this purpose, we define the perturbed line element (in the Newtonian gauge) as

$`ds^2`$ $`=`$ $`(1+2\mathrm{\Psi })dt^2+a^2(1+2\mathrm{\Phi })\delta _{ij}dx^idx^j.`$ (1)
In addition, from the density fluctuations of each components in the Newtonian gauge, we define

$`\delta _X=\delta \rho _X/\rho _X,`$ (2)
where $`X=r`$, $`c`$, and $`b`$, corresponding to radiation,#1#1#1We assume that there is no entropy between the photon and the neutrinos. CDM, and baryon, respectively.

To parameterize the density fluctuations of each components after the decay of $`\varphi `$, it is convenient to consider the “entropy” between the $`\varphi `$ field and the components generated from the decay product of the inflaton field before the decay of $`\varphi `$:

$`S_{\varphi \chi }^{(\delta \varphi )}(k)={\displaystyle \frac{\delta \rho _\varphi (t,k)}{\rho _\varphi (t)}}\delta _\chi (t)={\displaystyle \frac{2\delta \varphi _{\mathrm{init}}(k)}{\varphi _{\mathrm{init}}}},`$ (3)
where $`\delta \varphi _{\mathrm{init}}`$ is the initial fluctuation of $`\varphi `$ and the superscript “$`(\delta \varphi )`$” is for perturbations generated from the primordial fluctuation of $`\varphi `$.

Density (and other) fluctuations in the RD2 epoch are generally parameterized by using $`S_{\varphi \chi }^{(\delta \varphi )}`$. If a component $`X`$ is generated from the decay product of $`\varphi `$, then there is no entropy between the photon and $`X`$. On the contrary, if the component $`X`$ has some source other than $`\varphi `$, the entropy between the photon and $`X`$ is the same as $`S_{\varphi \chi }^{(\delta \varphi )}`$. Thus, if all the components in the universe are generated from $`\varphi `$, the density fluctuations become purely adiabatic and

$`\left[\delta _\gamma ^{(\delta \varphi )}\right]_{\mathrm{RD2}}={\displaystyle \frac{4}{3}}\left[\delta _b^{(\delta \varphi )}\right]_{\mathrm{RD2}}={\displaystyle \frac{4}{3}}\left[\delta _c^{(\delta \varphi )}\right]_{\mathrm{RD2}}=2\mathrm{\Psi }_{\mathrm{RD2}}^{(\delta \varphi )},`$ (4)
where the subscripts $`\gamma `$, $`b`$, and $`c`$ are for the photon, baryon, and CDM, respectively. In this case, the isocurvature perturbation in the $`\varphi `$ field is converted to the purely adiabatic density perturbation after the decay of $`\varphi `$ . On the contrary, if the baryon asymmetry does not originate to the decay product of $`\varphi `$, the entropy between the radiation and the baryon becomes $`S_{\varphi \chi }^{(\delta \varphi )}`$ and hence

$`\left[\delta _\gamma ^{(\delta \varphi )}\right]_{\mathrm{RD2}}={\displaystyle \frac{4}{3}}\left[\delta _c^{(\delta \varphi )}\right]_{\mathrm{RD2}}=2\mathrm{\Psi }_{\mathrm{RD2}}^{(\delta \varphi )},\left[\delta _b^{(\delta \varphi )}\right]_{\mathrm{RD2}}={\displaystyle \frac{3}{4}}\left[\delta _\gamma ^{(\delta \varphi )}\right]_{\mathrm{RD2}}+{\displaystyle \frac{9}{2}}\mathrm{\Psi }_{\mathrm{RD2}}^{(\delta \varphi )},`$ (5)
and in the case where all the components other the CDM are generated from the decay product of $`\varphi `$,

$`\left[\delta _\gamma ^{(\delta \varphi )}\right]_{\mathrm{RD2}}={\displaystyle \frac{4}{3}}\left[\delta _b^{(\delta \varphi )}\right]_{\mathrm{RD2}}=2\mathrm{\Psi }_{\mathrm{RD2}}^{(\delta \varphi )},\left[\delta _c^{(\delta \varphi )}\right]_{\mathrm{RD2}}={\displaystyle \frac{3}{4}}\left[\delta _\gamma ^{(\delta \varphi )}\right]_{\mathrm{RD2}}+{\displaystyle \frac{9}{2}}\mathrm{\Psi }_{\mathrm{RD2}}^{(\delta \varphi )}.`$ (6)
In addition, if the baryon and the CDM are both generated from sources other than $`\varphi `$, we obtain

$`\left[\delta _\gamma ^{(\delta \varphi )}\right]_{\mathrm{RD2}}=2\mathrm{\Psi }_{\mathrm{RD2}}^{(\delta \varphi )},\left[\delta _b^{(\delta \varphi )}\right]_{\mathrm{RD2}}=\left[\delta _c^{(\delta \varphi )}\right]_{\mathrm{RD2}}={\displaystyle \frac{3}{4}}\left[\delta _\gamma ^{(\delta \varphi )}\right]_{\mathrm{RD2}}+{\displaystyle \frac{9}{2}}\mathrm{\Psi }_{\mathrm{RD2}}^{(\delta \varphi )}.`$ (7)
It is important to notice that, for the cases given in Eqs. (5) $``$ (7), the entropy perturbations are correlated with the adiabatic perturbation.#2#2#2Here, we assumed that the baryon number asymmetry and/or the CDM is generated before the $`\varphi `$ field starts to oscillate. In other case, the size of the correlated entropy perturbation may change. For details, see .

Now, we are at the point to discuss the CMB anisotropy. The CMB anisotropy is characterized by the angular power spectrum $`C_l`$ which is defined as

$`\mathrm{\Delta }T(\stackrel{}{x},\stackrel{}{\gamma })\mathrm{\Delta }T(\stackrel{}{x},\stackrel{}{\gamma }^{})_\stackrel{}{x}={\displaystyle \frac{1}{4\pi }}{\displaystyle \underset{l}{}}(2l+1)C_lP_l(\stackrel{}{\gamma }\stackrel{}{\gamma }^{}),`$ (8)
with $`\mathrm{\Delta }T(\stackrel{}{x},\stackrel{}{\gamma })`$ being the temperature fluctuation of the CMB radiation pointing to the direction $`\stackrel{}{\gamma }`$ at the position $`\stackrel{}{x}`$ and $`P_l`$ is the Legendre polynomial. As we mentioned, there are two sources of the density perturbations; the primordial fluctuations of the scalar fields $`\chi `$ and $`\varphi `$. Since there is no correlation between these fields, the CMB anisotropies from these fluctuations are uncorrelated and the resultant CMB power spectrum is given in the form

$`C_l=C_l^{(\delta \chi )}+C_l^{(\delta \varphi )},`$ (9)
where $`C_l^{(\delta \chi )}`$ and $`C_l^{(\delta \varphi )}`$ are contributions from the primordial fluctuations of the inflaton field $`\chi `$ and the $`\varphi `$ field, respectively. The inflaton contribution $`C_l^{(\delta \chi )}`$ is known to be the adiabatic result.

The new contribution $`C_l^{(\delta \varphi )}`$ depends on the properties of the density perturbations of each components. If all the components in the universe (i.e., the photon, baryon, CDM, neutrino, and so on) are dominantly generated from the decay product of $`\varphi `$, there is no entropy between any of two components. In this case, $`C_l^{(\delta \varphi )}`$ is from adiabatic perturbations. This fact has an important implication. In general, the scale dependences of $`\mathrm{\Psi }^{(\delta \chi )}`$ and $`S_{\varphi \chi }^{(\delta \varphi )}`$ are different. In the slow-roll inflation scenario, $`\mathrm{\Psi }^{(\delta \chi )}`$ is given by

$`\mathrm{\Psi }_{\mathrm{RD2}}^{(\delta \chi )}={\displaystyle \frac{4}{9}}\left[{\displaystyle \frac{H_{\mathrm{inf}}}{2\pi }}{\displaystyle \frac{3H_{\mathrm{inf}}^2}{V_{\mathrm{inf}}^{}}}\right]_{k=aH_{\mathrm{inf}}},`$ (10)
where $`V_{\mathrm{inf}}^{}V_{\mathrm{inf}}/\chi `$ with $`V_{\mathrm{inf}}`$ being the inflaton potential. On the contrary, $`S_{\varphi \chi }^{(\delta \varphi )}`$ is related to the fluctuation of the amplitude of $`\varphi `$, as seen in Eq. (3), and hence

$`S_{\varphi \chi }^{(\delta \varphi )}={\displaystyle \frac{2}{\varphi _{\mathrm{init}}}}\left[{\displaystyle \frac{H_{\mathrm{inf}}}{2\pi }}\right]_{k=aH_{\mathrm{inf}}}.`$ (11)
In many models of slow-roll inflation, the expansion rate $`H_{\mathrm{inf}}`$ is almost constant during the inflation. On the contrary, the slope of the inflation potential $`V_{\mathrm{inf}}^{}`$ may significantly vary. As a result, $`S_{\varphi \chi }^{(\delta \varphi )}`$ becomes (almost) scale independent while $`\mathrm{\Psi }^{(\delta \chi )}`$ may have significant scale dependence. Since the currently measured CMB power spectrum suggests (almost) scale invariant primordial density perturbation in the conventional scenario, inflation models are excluded if $`\mathrm{\Psi }^{(\delta \chi )}`$ has too strong scale dependence .

If the $`\varphi `$ field exists, however, the situation may change . Since $`S_{\varphi \chi }^{(\delta \varphi )}`$ is expected to be (almost) scale invariant, we can relax the constraint on the inflation models if $`C_l^{(\delta \varphi )}`$ becomes significantly large, which happens when $`S_{\varphi \chi }^{(\delta \varphi )}{}_{}{}^{>}\mathrm{\Psi }^{(\delta \chi )}`$. As shown in Eq. (3), $`S_{\varphi \chi }^{(\delta \varphi )}`$ is inversely proportional to $`\varphi _{\mathrm{init}}`$. Thus, if the initial amplitude of $`\varphi `$ is small, this may happen and the CMB power spectrum may become consistent with the observational data in a larger class of models of inflation.

Now, we study effects of the correlated entropy fluctuations. We first plot the angular power spectrum with the correlated mixture of the adiabatic and isocurvature perturbations in the baryonic and/or CDM sector, i.e., the cases with the relations given in Eqs. (5) $``$ (7). For comparison, we also plot the angular power spectrum for the purely adiabatic and isocurvature cases. As one can see, the CMB angular power spectrum strongly depends on properties of the primordial density perturbations. If there exists correlated entropy between the baryon and other components with the relation (5), negative interference between the adiabatic and isocurvature perturbations suppresses $`C_l`$ at lower multipole while the effect of the isocurvature perturbation becomes too small to affect the structure at high multipole. As a result, the angular power spectrum is enhanced at the high multipole rather than at the low multipole. If the effect of the entropy perturbation becomes more efficient, then $`C_l^{(\delta \varphi )}`$ at high multipole is suppressed relative to that at low multipole like in the purely isocurvature case. This happens when the entropy perturbation is in the CDM component with the condition given in Eq. (6). In addition, with the relation given in Eq. (7), the correlated entropy becomes more effective than the case where only the CDM sector has the correlated entropy. Then, the acoustic peaks are more suppressed relative to the Sachs-Wolfe (SW) tail.

As mentioned before, the actual CMB angular power spectrum is given by the sum of the inflaton contribution $`C_l^{(\delta \chi )}`$ and the contribution from the primordial fluctuation of the late-decaying scalar field $`C_l^{(\delta \varphi )}`$. (See Eq. (9).) To parameterize their relative size, we define

$`R_bS_{b\gamma }^{(\delta \varphi )}/\mathrm{\Psi }_{\mathrm{RD2}}^{(\delta \chi )},R_cS_{c\gamma }^{(\delta \varphi )}/\mathrm{\Psi }_{\mathrm{RD2}}^{(\delta \chi )},`$ (12)
where $`S_{b\gamma }^{(\delta \varphi )}`$ ($`S_{c\gamma }^{(\delta \varphi )}`$) is the entropy between the baryon and the photon (between the CDM and the photon) generated from the primordial fluctuation of $`\varphi `$. (We adopt Eqs. (5) and (6), and hence $`S_{b\gamma }^{(\delta \varphi )}`$ and $`S_{c\gamma }^{(\delta \varphi )}`$ are equal to $`\frac{9}{2}\mathrm{\Psi }_{\mathrm{RD2}}^{(\delta \varphi )}`$ if they are non-vanishing.) The shape of the CMB angular power spectrum depends on the values of these parameters.

Using Eqs. (10) and (11), the $`R`$-parameters are given as

$`R_{b,c}={\displaystyle \frac{3}{2}}\left[{\displaystyle \frac{V_{\mathrm{inf}}^{}}{\varphi _{\mathrm{init}}H_{\mathrm{inf}}^2}}\right]_{k=aH_{\mathrm{inf}}}.`$ (13)
Hence $`R_{b,c}`$ is model- and scenario-dependent; it depends on the scale of inflation, shape of the inflaton potential, and initial amplitude of $`\varphi `$. For example in the chaotic inflation model with the parabolic potential $`V_{\mathrm{inf}}=\frac{1}{2}m_\chi ^2\chi ^2`$, the above expression becomes

$`\left[R_{b,c}\right]_{\mathrm{chaotic}}=\left[{\displaystyle \frac{9M_{}^2}{\varphi _{\mathrm{init}}\chi }}\right]_{k=aH_{\mathrm{inf}}}.`$ (14)
Using the fact that the inflaton amplitude at the time of the horizon crossing of the COBE scale is $`\chi 15M_{}`$ in the chaotic inflation model, $`\left[R_{b,c}\right]_{\mathrm{chaotic}}0.6M_{}/\varphi _{\mathrm{init}}`$. Of course, the values of $`R_b`$ and $`R_c`$ depend on the model of inflation, and they vary if we consider different class of inflation models.

In Fig. 2, we plot the resultant angular power spectrum with several values of $`R_b`$. As expected, $`C_l`$ at the high multipole is more enhanced relative to that at low ones as the $`R_b`$-parameter increases. It is important to note that the effect of the uncorrelated entropy fluctuation always suppresses $`C_l`$ at high multipole relative to that at low multipole. Thus, if the on-going experiments, like MAP , observes the enhancement of the $`C_l`$ at high multipole, it can be regarded as a unique signal of the late-decaying scalar condensation. In fact, if the $`R_b`$-parameter is too large, the angular power spectrum at high multipole is too much enhanced, which becomes inconsistent with the currently available data. We checked that $`R_b4.5`$ is excluded at 95 % C.L. even adopting the most conservative constraint.

We also studied the effects the correlated entropy perturbation in the CDM. If $`R_c`$ is non-vanishing, $`C_l`$ at high multiple is suppressed compared to the SW tails. Thus, too large $`R_c`$ is also excluded from the current data of the observations of the CMB power spectrum; $`R_c`$ is constrained to be smaller than $`2.0`$ for $`R_b=0`$.

In summary, we have discussed the effects of the late-time entropy production due to the decay of the scalar-field condensations on the cosmic density perturbations. If the universe is reheated by the decay of the scalar field $`\varphi `$, many of the components in the present universe are generated from the decay products of the $`\varphi `$ field. In such a case, cosmic density perturbations are affected by the primordial fluctuation of $`\varphi `$ which may be generated during the inflation.

If all the components in the universe originate to the decay product of $`\varphi `$, density perturbations generated from the primordial fluctuation of $`\varphi `$ becomes adiabatic. In this case, the CMB angular power spectrum from the fluctuation of $`\varphi `$ becomes the usual adiabatic ones with (almost) scale-invariant spectrum. If this becomes the dominant part of the cosmic density perturbations, then we have seen that the constraints on inflation models from observations of the CMB angular power spectrum are drastically relaxed .

If the baryon or the CDM is not generated from $`\varphi `$, on the contrary, correlated mixture of the adiabatic and isocurvature perturbations may arise. In this case, the CMB angular power spectrum may be significantly affected and the shape of the resultant power spectrum depends on which component has the correlated isocurvature perturbation. In particular, if the baryonic component has the correlated isocurvature perturbation, $`C_l`$ at high multipole is more enhanced relative to that at low multipole, which may be observed by the MAP experiment and regarded as a unique signal of the late-time entropy production.

Acknowledgment: This work is supported by the Grant-in-Aid for Scientific Research from the Ministry of Education, Science, Sports, and Culture of Japan, No. 12047201 and No. 13740138.


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# Dominance of excitation continuum in the longitudinal spectrum of weakly coupled Heisenberg 𝑆=1/2 chains.

## Abstract

A low-field spin flop transition in the quasi one-dimensional antiferromagnet BaCu2Si2O7 is exploited to study the polarization dependence of low-energy magnetic excitations. The measured longitudinal spectrum is best described as single broad continuum, with no sharp “longitudinal mode”, in apparent contradiction with the commonly used chain-MF/RPA theories. The observed behavior is also quite different than that previously seen in the related KCuF3 material, presumably due to a large difference in the relative strength of inter-chain interactions. The results highlight the limitations of the chain-MF/RPA approach.

The physics of weakly-interacting spin chains is of great fundamental interest, as it represents the crossover from quantum to semi-classical spin dynamics. Excitations in conventional three-dimensional magnets are single-particle spin wave states. These can be described as precessions of magnetic moments around their equilibrium orientation, and are necessarily polarized perpendicular to the order parameter. In contrast, the excitation spectrum of one-dimensioanl (1D) quantum-disordered antiferromagnets (AFs) is isotropic. In particular, in the $`S=1/2`$ Heisenberg model, the spectrum is a polarization-independent multi-spinon continuum Fadeev and Takhtajan (1981); Hal ; KCU ; Tennant et al. (1995); Dender et al. (1996). Arbitrary weak inter-chain interactions in quasi-1D $`S=1/2`$ AFs restore long-range order (LRO) Sca ; Affleck et al. (1994); Wang (1997); Affleck and Halperin (1996), break rotational invariance and reinstate the transverse spin waves at low frequencies Sch ; Ess . The continuum persists in the high-frequency regime.

A counter-intuitive novel feature of weakly-interacting Heisenberg $`S=1/2`$ chains is the longitudinal mode (LM), a long-lived “spin wave” polarized parallel to the direction of ordered moment Sch ; Ess . This new type of excitation was recently discovered in the KCuF3 compound Lake et al. (2000); Nag , where it is seen as a single symmetric broad peak in the longitudinal spectrum.Lake et al. (2000) Such behavior is not fully understood within the commonly used chain-Mean-Field Sca  and Random Phase Approximation (MF/RPA) theories Sch ; Ess  that predict a sharp (long-lived) LM and a separate broad longitudinal continuum (LC). To further probe the limitations of the MF/RPA approach, and learn more about the exotic LM, we performed a polarization-sensitive inelastic neutron scattering study of BaCu2Si2O7. The advantage of this material is a considerably smaller ratio of inter-chain and in-chain interactions, as compared to KCuF3. This brings us closer to the idealized weak-coupling limit, where the MF/RPA theory can be expected to work best. Surprisingly, the measured longitudinal spectrum substantially deviates from theoretical predictions. Contrary to expectation, the LM in BaCu2Si2O7 is altogether ill-defined, and the low-energy longitudinal spectrum is best described as a single broad continuum feature. Thus, for longitudinal polarization, there is no analogue of the separation of single-particle and continuum states, that was previously seen in the transverse spectrum Zhe (a, b).

The magnetism of BaCu2Si2O7 is by now very well characterized using bulk methods Tsu ; Tsukada et al. (2001), neutron diffraction Tsu ; Zheludev et al. (2002) and inelastic neutron scattering Tsu ; Zhe (a); Ken ; Zhe (b). The material is orthorhombic (space group $`Pnma`$, $`a=6.862`$ Å, $`b=13.178`$ Å, $`c=6.897`$ Å) with slightly zigzag AF $`S=1/2`$ chains of Cu2+ ions running along the $`c`$ axis. The in-chain exchange constant is $`J=24.1`$ meV. Interactions between the chains are much weaker, and the characteristic badwidth of spin wave dispersion perpendicular to the chain direction (“mass gap” in the terminology of Ref. Ess ) is $`\mathrm{\Delta }=2.51`$ meV. BaCu2Si2O7 orders antiferromagnetically at $`T_N=9.2`$ K$`=0.033J/k_\mathrm{B}`$ with a zero-$`T`$ saturation moment of only $`m_0=0.15`$ $`\mu _\mathrm{B}`$. For comparison, for KCuF3, $`J=37`$ meV, $`T_N=39`$ K$`=0.09J/k_\mathrm{B}`$, $`m_0=0.54`$ $`\mu _\mathrm{B}`$ (Ref. S. K. Satija and Hirakawa (1980); KCU ; Tennant et al. (1995) and references therein). Due to a weak easy-axis aniso1tropy in BaCu2Si2O7, the ordered staggered magnetization is aligned along the $`c`$ axis.

The most direct way to determine the polarization of magnetic excitations is by using polarized neutrons. Such measurements are typically associated with severe intensity losses in the polarizing monochromator and analyzer. Given the size of currently available single-crystal samples, and the expected scattering cross section for longitudinal excitations in BaCu2Si2O7, this type of experiment does not appear feasible. Fortunately though, even for an unpolarized neutron beam, the scattering intensity is polarization dependent. Only spin components perpendicular to momentum transfer contribute to the cross section. One commonly used strategy is to measure the inelastic signal at equivalent wave vectors in different Brillouin zones (BZs). Comparing such data sets can provide polarization information, but relies heavily on the exact knowledge of the spectrometer resolution function. The latter can be estimated quite accurately, but an error of only a few percent can ruin the polarization analysis. This was the main problem in previous inconclusive attempt to apply this technique to longitudinal excitations in BaCu2Si2O7, as described in Ref. Zhe (b).

In the present work the problem was overcome by using the “reverse” approach. The same inelastic scan (always in the same BZ) was performed for different orientations of the ordered moment in the system. Polarization information was then extracted in a point-by-point data analysis that is robust and insensitive to any resolution effects. As described in detail below, to change the direction of ordered moment we exploited one of the recently discovered field-induced spin-re orientation transitions in BaCu2Si2O7 Zheludev et al. (2002). A 5 mm diameter and 40 mm long cylindrical single crystal sample was mounted on the the thermal 3-axis spectrometer PONTA (5G) at the JRR3-M reactor at Japan Atomic Energy Research Institute at Tokai. The sample cylinder axis is close to the $`(1,1,0)`$ reciprocal-space direction and was oriented vertically in the experiment. The $`(0,0,1)`$ and $`(0.5,1.86,0)`$ reciprocal-lattice vectors determined the horizontal scattering plane. Sample environment was a horizontal-field 6 T cryomagnet. The field was at all times applied along the $`c`$ axis of the crystal. The data were collected in an energy scan close to the 1D AF zone-center $`(0,0,1)`$. The design of the horizontal-field magnet imposes stringent constraints on experimental geometry, allowing only narrow $`\pm 15^{}`$ windows for the incident and scattered beams. For this reason, each data set was collected while simultaneously scanning the energy transfer $`\mathrm{}\omega `$ and momentum transfer perpendicular to the chain axis $`𝐪_{}`$, at a constant momentum transfer along the chains $`q_{}=2\pi /c`$, which is the 1D AF zone-center. Figure 1 shows the trajectory of the scan relative to the previously determined spin wave dispersion in BaCu2Si2O7. Also shown is the evolution of the instrument resolution ellipsoid, calculated in the Cooper-Nathans approxomation Cooper and Nathans (1967); Popovici (1975).

The scan was repeated in three independent measurements. The first measurement (Fig. 2, solid circles) was performed in a magnetic field $`H_1=1.2`$ T at $`T=2`$ K. Under these conditions, just as at $`H=0`$, the ordered moment in BaCu2Si2O7 is parallel to $`c`$ Ken ; Zheludev et al. (2002). The measured intensity is related to the longitudinal (parallel to the ordered moment) and transverse (perpendicular to the ordered moment) dynamic structure factors $`S^{}(𝐪,\omega )`$ and $`S^{}(𝐪,\omega )`$ through $`I_1(𝐪,\omega )S^{}(𝐪,\omega )(1+\mathrm{cos}^2\alpha )+S^{}(𝐪,\omega )\mathrm{sin}^2\alpha +(𝐪,\omega ).`$ Here $`\alpha `$ is the angle between the momentum transfer $`𝐪`$ and the chain axis, and $`(𝐪,\omega )`$ is the background, assumed to be of non-magnetic origin. In our particular case $`\alpha 15^{}`$ through the entire scan, and it is mostly the transverse spin fluctuations that are observed. In the a second measurement the same scan was repeated at $`H_2=2.2`$ T, which exceeds the critical field $`H_c=2.0`$ T of a spin-flop transition Tsukada et al. (2001); Zheludev et al. (2002). These data are plotted with open symbols in Fig. 2. In the spin-flop state the ordered staggered moment is perpendicular to the field direction and therefore lies within the crystallographic $`(a,b)`$ plane. The measured inelastic intensity can be written as $`I_2(𝐪,\omega )S^{}(𝐪,\omega )(1+\mathrm{sin}^2\alpha )+S^{}(𝐪,\omega )\mathrm{cos}^2\alpha +(𝐪,\omega ).`$ For small $`\alpha `$ one observes an equal mixture of longitudinal and transverse spin fluctuations. In the final measurement, performed at zero field, the sample was removed from the magnet and sample holder. The same scan was repeated to directly measure the extrinsic background $``$, mainly due to spurious scattering in the sample environment (triangles in Fig. 2). The intrinsic background (from scattering in the sample itself) was previously shown to be negligible Zhe (b). At each $`(𝐪,\omega )`$-point the equations for $`I_1`$ and $`I_2`$ were then solved to extract the dynamic structure factors for different polarizations, as plotted in Fig. 3.

Using this method to determine the polarization of spin fluctuations is based on several assumptions. The first is that the spin structure rotates as a whole when going through the spin-flop transition, but is otherwise unaffected. For BaCu2Si2O7, such behavior was confirmed by previous neutron diffraction studies in magnetic fields up to 5 T Zheludev et al. (2002). In particular, upon crossing $`H_c`$, the magnitude of the ordered moment remains almost constant, and the change in relative alignment of nearby spins is insignificant. The second requirement is that magnetic anisotropy and Zeeman effects are negligible on the experimentally relevant energy scales, as defined by the gap $`\mathrm{\Delta }`$ and the experimental energy resolution (typically 1.7 meV FWHM). In our measurements this condition is also satisfied. Indeed, at $`H=H_2=2.2`$ T the Zeeman energy per spin is an order of magnitude smaller: $`gS\mu _\mathrm{B}H0.25`$ meV. Performing differential measurements at $`H_1`$ and $`H_2`$, with $`gS\mu _\mathrm{B}\delta H`$ of only 0.13 meV, further minimizes the effect, as shown by arrows in Fig. 2. The magnitude of magnetic anisotropy in BaCu2Si2O7 is also negligible, the associated spin wave gap being only about 0.2 meV Zhe (b). In summary, the spin flop transition only changes the coordinate system in which the terms “longitudinal” and “transverse” are defined, but should not affect the nature of the excitation spectrum.

Previous measurements of transverse spin fluctuations in BaCu2Si2O7 Zhe (a, b) were found to be in remarkably good quantitative agreement with MF/RPA theory Sch ; Ess . In this approach each individual spin chain is viewed as subject to an effective staggered exchange field $`𝐇_\pi `$, generated by LRO neighboring chains. The staggered field in turn generates an attractive potential between spinons, producing 2-spinon bound states. Two components of the spin-triplet bound state are polarized perpendicular to $`𝐇_\pi `$. These are analogues of conventional spin waves, and have a gap $`\mathrm{\Delta }H_\pi ^{2/3}`$. The third component is the longitudinal mode with a gap $`\mathrm{\Delta }_{}=\sqrt{3}\mathrm{\Delta }`$. Regardless of polarization, a multi-magnon continuum, the remains of the spinon-continuum, has a gap of $`\mathrm{\Delta }_c=2\mathrm{\Delta }`$. Starting from this MF solution the RPA is used to calculate the spin wave dispersion perpendicular to the chains. For BaCu2Si2O7 the MF/RPA dynamic structure factor for transverse spin waves is explicitly written out in Eqs. 4–7 in Ref. Zhe (b). The continuum part is well approximated by the “truncated Muller ansatz” functional form, as given by Eqs. 10 and 11 in the same reference. As an important consistency check, this model cross section function, after a numerical convolution with the spectrometer resolution, was fit to the transverse spectrum measured in this work. Since all parameters of the model were previously determined with very good accuracy Ken ; Zhe (b), the only parameter varied in the present data analysis was an overall intensity scaling factor. An excellent fit was obtained, and is shown in a solid line in Fig. 3a. Continuum and single mode parts are shown a hatched and greyed areas, respectively.

We now turn to discussing the main result of this work, namely the measured longitudinal spectrum. As shown in Fig. 3b, the scattering is a broad asymmetric peak with a maximum around 4 meV energy transfer, and an extended “tail” on the high-energy side. As a first step, we analyzed the data using a model cross section based on MF/RPA theory, as for transverse excitations. The corresponding dynamic structure factor for the LM is given by Eqs. 12 and 13 in Ref. Zhe (b). At the particular wave vector, the MF/RPA predicts the LM at 4.2 meV, quite close to the observed intensity maximum. Given the shape of the observed peak, in our fits the LM was allowed to have a non-zero intrinsic energy width. The corresponding $`\delta `$-function in Eq. 12 of Ref. Zhe (b) was replaced with a Lorenzian profile of FWHM $`\mathrm{\Gamma }`$. In addition, the prefactor $`\gamma `$ that chracterizes the energy-scaled intensity of the longitudinal mode relative to that of transverse spin waves was treated as an adjustable parameter. Continuum scattering was assumed to be exactly as for transverse polarization. This model, when convoluted with the spectrometer resolution function, yields a reasonably good two-parameter fit to the data with $`\gamma =2.2(1)`$ and $`\mathrm{\Gamma }=2.4(7)`$ meV (heavy solid line in Fig. 3b).

The obtained parameter values clearly indicate the failure of the MF/RPA model to describe longitudinal excitations in BaCu2Si2O7. First, the refined intensity coefficient $`\gamma `$ is about 4.5 times larger, than the MF/RPA prediction Ess . Second, to obtain a good fit, we had to assume a substantial intrinsic width for the LM. In contrast, the LM in the MF/RPA model is infinitely sharp. For weakly-coupled chains like those in BaCu2Si2O7, this damping effect has a particularly important consequence: the LM becomes altogether ill-defined. Indeed, in this case, the continuum is relatively strong, and comparable in intensity to single-mode scattering. In the MF/RPA the LC has a (pseudo)gap at $`2\mathrm{\Delta }`$, and the LM is centered at about $`1.73\mathrm{\Delta }`$. At the same time, our analysis shows that in BaCu2Si2O7 the intrinsic FWHM of the LM is itself be about $`\mathrm{\Delta }`$. Given these numbers, the LM and the LC are too close to be separated, and constitute a single continuum feature. To illustrate this fact, in Fig. 3b we also show a fit to the longitudinal data using only the truncated Muller ansatz (heavy dotted line), with no single mode contribution. With a continuum gap $`\mathrm{\Delta }_c=1.4(1)\mathrm{\Delta }`$ (smaller than the expected MF/RPA value of $`2\mathrm{\Delta }`$), this empirical function describes the data at least as well as the cross section that also includes a damped LM. The situation is quite different for materials with inter-chain interactions of intermediate strength, such as KCuF3. Here the LC, which is the high-energy “tail” seen in constant-$`q`$ scans, is relatively weak. As a result, even though the LM is broadened, it is seen as a well-defined symmetric inelastic peakLake et al. (2000).

Comparing the spectra measured in BaCu2Si2O7 and KCuF3, we conclude that the MF/RPA picture based on distinct LM and LC contributions does not become more accurate in the weak-coupling limit. The width of the LM peak normalized by $`\mathrm{\Delta }`$ in the weaker-coupled BaCu2Si2O7 system is even greater, than in the KCuF3 compound. This counter-intuitive behavior may be related to the critical nature of spin correlations in isolated $`S=1/2`$ chains. Quantum criticality implies that there is no characteristic energy scale in the chains, and therefore any inter-chain coupling is to be considered as strong. Strictly speaking, the RPA is well justified only for inter-chain interactions small compared to the energy gap in individual chains. In our case, the chains are intrinsically gapless. The gap $`\mathrm{\Delta }`$ only emerges in the MF theory and is necessarily of the same order of magnitude as inter-chain coupling itself Sch . The problem is therefore only marginally suited for the RPA for intrinsic reasons.

In summary, despite a small ratio of inter-chain and in-chain interactions, the low-energy longitudinal spectrum of BaCu2Si2O7 is dominated by a broad excitation continuum, and there appears to be no distinct “longitudinal mode”. Further theoretical calculations beyond the MF/RPA are needed to better understand this behavior.

Work at the University of Tokyo was supported in part by the Grant-in-Aid for COE Research “SCP coupled system” of the Japanese Ministry of Education, Culture, Sports, Science, and Technology. Oak Ridge National Laboratory is managed by UT-Battelle, LLC for the U.S. Department of Energy under contract DE-AC05-00OR22725. We would like to thank F. Essler, S. Maslov and A. Tsvelik (BNL) for iluminating discussions.


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# References

WHY EVERYTHING GETS SLOWER ?

D.Stauffera,b and K.Kułakowskia

a Faculty of Physics & Nuclear Techniques, University of Mining & Metallurgy

al.Mickiewicza 30, 30-059 Kraków, Poland

b visiting from Inst. for Theor. Physics, Cologne Univ., D-50923 Köln, Euroland

## Abstract

A social system is represented by the Barabási-Albert model. At each node of the graph, an Ising spin is placed, $`S=\pm 1`$, with antiferromagnetic interaction between connected nodes. The time to reach equilibrium via Glauber kinetics does not depend on the system size. The average energy associated with the rare spin flips in equilibrium oscillates with the number $`m`$ of edges of new nodes. The conclusions are illustrated with events from recent European history, where after some strong change a rather immobile society evolved.

Keywords: sociophysics, stability, Barabasi-Albert, Ising antiferromagnet

Some of us wonder sometimes why it is so difficult to reorganize a social system . There are many examples in history when a society prevents changes just by means of inertia. A commonly accepted example is provided by the history of Soviet Union in 60’s, when reforms of Khrushchev failed despite apparent lack of objections. In fact, the famous ’perestrojka’ in 80’s could happen only because members of the Politburo in Moscow were pretty sure that Gorbachev does not talk seriously .

Here we are interested in the time dependence of a flexibility of a social system, described in possibly simplest way. We profit from recent works of Barabási and Albert , where social connections are modeled as edges of graphs. A special algorithm was introduced in Ref. to construct the so-called scale-free networks of nodes connected by edges. The resulting systems were proven to show qualitative similarities with networks known from different branches of knowledge, as biology, ecology or linguistics. For a review of this new subject see Ref..

A social system is represented by a scale-free Barabási-Albert network, with the number $`m`$ of edges of successively added nodes as the only parameter. Ising spins $`S=\pm 1`$ are assigned to all nodes. The interaction is chosen to be antiferromagnetic and it is limited to the nodes directly connected by edges. This choice can be motivated heuristically as follows. There is a natural tendency of social units (people, enterprises or political fractions) to differ and to compete. As a result of the competition, one unit of each two becomes more self-concentrated, egoistic and powerful than the other - and it wins. In this sense, a stable state of each pair of units is: one up (positive, subordinated) and one down (negative, prevailing). At the initial state of a newly created system, however, all units are idealistic and claim to serve to the community. A stable state of the whole system is attained by a gradual evolution of the units, which is composed from local competitions between members of interacting pairs. A similar splitting of an evolving society into performers of two opposite strategies was described by Mitchell et al. in terms of rules of cellular automata .

Our time evolution accords with the Monte-Carlo Glauber dynamics . However we believe that in our problem, the character of the evolution rule is of secondary importance. The relevant feature is the existence of the working function - energy in the Ising model - which is minimized apart from thermal fluctuations. As it was proven by Derrida , in this case a local equilibrium state is well defined, and the length of the limit cycle is at most 2. In fact, we need only the existence of an absorbing state, which is stable against existing disturbances. This condition seems to be fulfilled also in the world of social phenomena, at least until a Great Disturbance appears.

In contrast to spin glass simulations since a quarter of a century, we do not discuss here phase transitions, ordering below the phase transition temperatures, or ground states. Instead we look at the initial nonequilibrium dynamics as a model for the development of social rigidity.

We used the program employed already by Aleksiejuk et al  and replaced ferromagnetic by antiferromagnetic couplings. The Barabási-Albert network started with $`m`$ mutually connected sites and then was grown to $`N+m`$ sites according to the standard rule that a newly added site selects $`m`$ neighbours from the already existing network sites, with a selection probability proportional to the number $`k`$ of neighbours the selected site had before. The Ising spins, initially all up, where flipped with heat bath (Glauber) dynamics, i.e. up with probability $`x/(1+x)`$ and down with probability $`1/(1+x)`$, where $`x=\mathrm{exp}(nJ/k_BT)`$ is the Boltzmann thermal probability and $`n=_jS_j`$ is the sum over all $`k(i)`$ neighbours of spin $`i`$, with $`S_j=\pm 1`$ and a positive exchange energy $`J`$. One iteration $`tt+1`$ is one Monte Carlo step per spin. During each iteration we counted the total number of spins which are flipped, the total energy change ($`|n|`$ summed over all spin flips), and the magnetization $`M=_iS_i`$.

Fig.1 for $`m=5`$ shows that the magnetization decays weakly with time, the total energy changes strongly, while the number of flipped spins is mostly in between. Changing the network size $`N`$ from 2 million to 20,000 gives similar results, Fig.2. Figs.3 and 4 show a slightly faster equilibration with $`m=1`$ or 2, instead of 5, and Fig.5 summarizes this trend for $`m=2`$, 4, 6, 8, 10.

In Fig.2 we see that for $`m=5`$ the energy change stabilizes in about 100 timesteps, and this characteristic time does not depend on the system size. (It alse remains about the same if we use lower temperatures.) The stable value is a small fraction of the number of nodes, i.e. about $`0.005N`$. Similarly, the number of spin flips stabilizes near $`0.015N`$. The magnetization changes reveal two stages; after a short transient, it decreases with time $`t`$ proportionally to $`t^\beta `$, with $`\beta `$ less than 0.1.

The $`m`$ dependence of the results, Fig.6, reveals some kind of oscillations with amplitude decreasing with $`m`$. This effect can be assigned to the difference between $`m`$ even and odd, which is expected to alter the density of frustration in the system: A cycle with an even number of antiferromagnetic edges allows all spins to be antiparallel to their neighbours on this cycle; for an odd number of edges this is impossible and leads to frustrated edges connecting parallel spins even at zero temperature.

In the above results, the flexibility of the modeled system is measured by the number of spins flipped at a given iteration step, and by the energy change during these flips. Continuing our allegorical interpretation, we assign the number of personnel changes to the number of spin flips. This is justified by our every-day experience that it is easier to change a person than his/her attitude. Even more important is the change of energy, which can be seen as a measure of a social cost of changes. An exchange of a politician without a resulting change in the problems of the society corresponds to a spin flip with zero energy change, $`n=0`$. These flips dominate at long times in our simulations.

For social systems, two conclusions can be drawn from our results. First, after a big (external) disturbance, the ability of a system to change decreases with time and soon it becomes very small. Actually, this result follows as a simple consequence of our model of a social system as an interacting medium with the energy as a work function which is minimized during the time evolution. With this assumption, the proof of Derrida  holds. Our second conclusion is more subtle. If the above interpretation is valid, personnel changes or even changes of attitude of the administration are not equivalent to changes of the social structure, which can remain unharmed. A real change demands a new initial state far from equilibrium, when most units agree.

These conclusions can be easily illustrated by examples from recent history of Europe. In years 1989-91 the reforms of the democratic Polish government transformed the life in the country much more than the changes in the ten following years. The characteristic time can then be evaluated as one or two years. The moral is: once you can change something, do it quickly. On the other hand, there is a continuity of the so-called ’national interests’ of many countries, and they are present in political strategies through centuries. At the reverse of the same effect we find that the amounts of unemployed people in several countries (including ours) seem to be very resistant with respect to changes of governments and parliaments, not to mention a ”New Politics” claimed frequently during elections.


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# Nanometer-Scale Metallic Grains Connected with Atomic-Scale Conductors

## I introduction

Fabrication of nanometer scale devices has recently become a subject of intensive study. In nanometer-scale metallic devices, discrete electronic energy levels can be resolved at low temperatures. The effects of discrete electronic levels on quantum transport in small metallic samples have been observed in atomic contacts and in nanometer scale grains.

Atomic contacts have been created using scanning probe microscopes During et al. (1990) and mechanically controlled break junctions Moreland and Ekin (1985); Muller et al. (1992). In these techniques, a metallic contact is broken, for example by elongation, and one measures the conductance versus elongation. The combination of two effects, conductance quantization van Wees et al. (1988); Wharam et al. (1988) and sudden rearrangements of the atomic structure Landman et al. (1990); Sutton and Pethica (1990), cause the conductance to decrease in discrete steps while the contacts are stretched to the breaking point. The steps are on the order of the conductance quantum $`G_0=2e^2/h`$.

In metallic grains, a single grain has been placed in weak tunneling contact with source and drain leads, Ralph et al. (1995); Davidović and Tinkham (1999) creating a single electron transistor (SET). Fulton and Dolan (1987) At dilution refrigerator temperature, discrete energy levels of the grain are measured from the I-V curve. The discrete energy spectra are analogous to those in artificial atoms. Kastner (1992); Ashoori (1996); Kouwenhoven et al. (1997)

Study of both atomic scale contacts and grains has led to major advances in understanding quantum transport in metals. For an extensive review of quantum properties of atomic-scale conductors and grains see Refs. Agrait et al.  and Delft and Ralph (2001), respectively.

In this paper, we describe a technique to connect one gold grain to drain and source by atomic scale contacts. The samples that we generate demonstrate behaviors of both atomic contacts and metallic grains. We show that the contact conductances can be changed in discrete steps of size comparable with $`G_0`$, showing that the conductance channels are well transmitting. This property differentiates our new devices from previously studied grains. Delft and Ralph (2001) We investigate the Coulomb blockade of a grain as a function of the contact conductance. We identify a regime of intermediate Coulomb blockade, where the sample resistance is close to the resistance quantum.

## II Experimental setup

The samples are created by combining metal deposition and electric field induced surface migration of gold. Recently, an electromigration technique has been implemented in fabrication of metallic electrodes with nanometer separation by Park et al. Park et al. (1999) In this technique a gold nanowire had been made by electon-beam lithography, then broken by passing large current through it. The current flow had caused the electromigration of gold atoms, and the nanowire to break. An electromigration technique was subsequently applied at cryogenic temperatures, Park et al. (2002) which lead to the fabrication of atomic scale transistors.

Our technique is different from that of Park et al., in that a strong electric field is applied to create a connection between two separate gold leads; it is based on electric field induced surface migration, T.M.Mayer et al. (1999) which is different from electromigration.

A $`5N`$ purity gold film is deposited on to two insulating $`Si_3N_4`$ substrates separated by a 70 nm slit, as shown in Fig. 1, in vacuum of $`10^6`$ torr. The slit has a large undercut in $`SiO_2`$, which prevents electrical contact between the films. The exposed length of the slit is $`0.1`$ mm.

Electric current across the slit is monitored during the deposition. The applied voltage is $`U`$ and the voltage source impedance is $`R_S`$. When the thickness of the film is near $`80nm`$, an electric contact between drain and source appears abruptly.

The contact between the drain and the source forms at a random location along the exposed length of the slit. The nature of the contact depends on $`R_S`$, $`U`$, the amount of gold deposited after the contact is detected, vapor pressure and temperature. The devices that can be obtained by this technique are metallic point contacts, tunneling junctions, and grains.

## III Metallic point contacts

To create a metallic point contact, we set $`R_S=0`$ and $`U0.1`$ V. Once the slightest conductance is detected, deposition is stopped. With further gold deposition the conductance would increase rapidly and display discrete steps in conductance versus time, of size $`G_0`$.

In some samples, stable contacts with conductance comparable with $`G_0`$ can be obtained by stopping the metal deposition at the right time. These contacts are stable for minutes or longer.

Frequently, it is impossible to stop the deposition when the contact conductance is near $`G_0`$, because the contact conductance jumps to a value of $`100G_0`$. In addition, the contacts that have conductance of order $`G_0`$ often suddenly jump into this $`100G_0`$ state or they disconnect.

## IV Planar Tunneling Barriers

Intuition suggests that if two gold surfaces are in mechanical contact, then there should also exist a good electrical contact. In this section, we show that mechanical contact does not necessarily imply a good electrical contact. It is possible to create a stable planar tunneling junction between two gold surfaces, with large tunneling resistance. This tunneling barrier is created if the gold surface contains adsorbates.

Planar tunneling barriers between gold surfaces have been first proposed by Hansen et al. Hansen et al. (2000a, b) The authors observe that gold metallic contacts of conductance $`G_0`$ grown in ultrahigh vacuum are much less stable than intentionally contaminated contacts with the same conductance. The enhanced stability is explained by a tunneling barrier composed of adsorbates, which has a mechanical contact area much larger than that for a metallic contact with the same conductance. The dimensions of these barriers are obtained by fitting the I-V curves. They vary from $`12nm`$ to $`50nm`$. The thickness of the barrier is of order several $`\AA `$.

We confirm this proposal in our experimental setup and clarify the conditions under which different types of contacts form. Since the pressure during the metal deposition is $`10^6`$ Torr, the surfaces contain adsorbates. The nature of the contact that forms at this pressure depends on the applied voltage.

If the applied voltage is weak ($`U<0.1`$ V), then the contacts are metallic, as described in the previous section. If the voltage is large, ($`U>5`$ V and $`R_S=0`$), the device contains a planar tunneling barrier and there is no direct metallic connection between drain and source.

If the applied voltage is between $`1`$ V and $`3`$ V, the contacts are mixed between the above two cases. They contain a large tunneling barrier and a small metallic contact somewhere inside the barrier. These contacts have the advantage of having high stability and high channel transmittance. They are described in a separate section.

We discuss the high voltage regime first. We return to the deposition process in Fig. 1 with $`U=10`$ V and $`R_S=0`$. When the $`Au`$ film thickness reaches $`80`$ nm, the current suddenly jumps to a nonzero value.

The conductance $`(I/V)`$ strongly fluctuates in time. The average $`I/V`$ is much smaller than $`G_0`$. As soon as the contact is detected, we stop metal deposition and reduce the bias voltage close to zero. We minimize the time that the devices are exposed to $`10`$ V to about one second.

While reducing the voltage, at a rate of one volt in ten millisecond, we measure the I-V curve. A typical I-V curve is shown in Fig. 2-A. It is relatively well modeled by the I-V curve of a single tunneling junction Wolf (1989) with the barrier height comparable to the gold work function $`W_{Au}=5.1`$ eV. The diameter of the barrier is $`10`$ nm, consistent with ref. Hansen et al. (2000a, b).

The barrier height is slightly larger than $`W_{Au}`$. This is explained by significant contamination of the junctions with adsorbates, such as $`H_2O`$111 In a separate publication, we examine the effect of water molecules on the I-V curve in Fig. 2-A in detail. We find that water is an excellent insulator: when water vapor pressure is increased, the barrier height increases, increasing the sample resistance by orders of magnitude.

We image the contacts by the scanning electron microscope (SEM). Transferring the sample from the deposition chamber to another instrument almost certainly leads to a sudden increase in resistance to an undetectably high value, despite being grounded at both ends during transfer. In most samples, the electrical contact can be reestablished by applying a one second long voltage pulse at 10 V (or sometimes higher) in high vacuum. The sample returns to the high resistance tunneling barrier.

Figure 3-A shows one gold grain in mechanical contact with the source. The sample disconnected spontaneously while transferring to the SEM as described above. We apply the voltage pulse, while imaging and measuring the current simultaneously. The current starts to flow during the pulse duration. After the pulse, the sample resistance at low bias is $`1G\mathrm{\Omega }`$ or higher.

Figure 3 B shows the device after the voltage pulse. We verify through microscopy that no additional connections are formed outside the slit in Figure 3. The mechanical contact area is of order $`10`$ nm, confirming the proposal by Hansen et al.

Under the influence of voltage, the grain pulled a Au protrusion from the right lead, establishing contact. This protrusion forms because of a process known as electric field induced surface migration, see Ref. T.M.Mayer et al. (1999) and references therein.

It is understood that the protrusion grows because of a force acting on surface gold atoms. When the electric field exceeds a certain threshold, it leads to migration of surface gold atoms toward the region of the strongest electric field, creating a protrusion. The protrusion increases the electric field gradient, which in turn accelerates its growth. When the protrusion reaches the other side, a planar junction is formed. This junction is stable after the voltage is reduced.

## V Formation of grains in electric breakdown

Consider a metallic point contact with resistance less than $`10\mathrm{\Omega }`$. We apply a voltage pulse of 10 V in vacuum. The contact breaks down, and after the pulse the resistance is immeasurably large.

We observe the break-down by the SEM. Fig. 4-A shows an area near the contact after the break down. Evidently, a relatively wide region around the point contact melts under the influence of the voltage pulse. The molten gold retracts away from the slit, presumably in order to reduce surface energy.

In addition, a large number of electrically isolated grains is left behind on the substrate surface. This is shown in fig. 4-B. The image indicates a broad distribution of grain diameters. The particles have nearly circular shape. This suggests that the particles have been molten (in the liquid state, minimizing the surface energy in contact with the substrate leads to circular grains).

## VI Planar Tunneling Barriers - Revisited

In Fig. 3-B, there is a grain between drain and source. The majority of devices fabricated with a 10 V pulse, as in fig. 3-B, have I-V curves that exhibit the Coulomb staircase at low temperatures. Since the staircase is conditional on $`R_L,R_R>h/e^2`$, where $`R_L`$ and $`R_R`$ are the contact resistances between the grain and the leads, this shows that there are at least two contacts in series between drain and source. In later sections, when we discuss Coulomb Blockade, we infer from the I-V curves that there is only one grain between the drain and the source. Figure 3-B supports this conclusion.

We propose the following scenario for grain formation. We suggest that the very first contact at 10 V bias voltage is metallic. It lasts only for a very short time, because it breaks down by melting. During the break down, one or several grains are created analogous to Fig. 4.

## VII Mixed Contacts

After creating a device with a 10 V pulse, as in fig. 3-B, we change the circuit in Fig. 1, so that $`R_S=20k\mathrm{\Omega }`$ and slowly increase $`U`$ from zero, and measure the conductance ($`I/V`$). Note that $`U`$ is the total voltage across the sample in series with $`R_S`$. Figure 2-B shows the resulting conductance traces in 3 different samples.

$`I/V`$ jumps to a significant fraction of $`2e^2/h`$ at roughly $`2.8`$ V. After the jump, the voltage across the sample $`V`$ is reduced below $`U`$ by voltage division with $`R_S`$, and the sample voltage becomes close to $`1.7`$ V. Further increase in $`U`$ results in two effects: there are additional discontinuities in conductance, of amplitude $`0.2`$ to $`2e^2/h`$, and there is a smooth increase in conductance versus $`U`$. The increase in conductance is maintained if the voltage $`U`$ is removed.

The discontinuities in conductance of size $`e^2/h`$ suggest that discrete atomic reconfigurations take place, analogous to those in atomic conductors. Agrait et al.  The steps demonstrate that the contacts contain well transmitting channels. In Fig. 3-B, the atomic scale contacts form somewhere inside the tunneling barrier between the grain and the leads.

The smooth conductance increase suggests that the tunneling contribution is increasing. We confirm through microscopy that the area of the planar barrier is increasing while the contact conductance is increasing smoothly.

As described before, in a strong nonuniform electric field, at room temperature, surface gold atoms move toward the strongest electric field. T.M.Mayer et al. (1999) We propose that when the electric field strength increases beyond a certain point, one atom pushes through the barrier, creating a metallic contact.

Once the first atom is connected, further increase in the electric field adds more gold atoms into the contact, increasing the number of channels and the conductance in steps of size $`e^2/h`$.

These discrete atomic additions occur in both barriers. In fact, since the voltage drop is stronger at the higher resistance junction, and voltage drop drives the conductance increase, it follows that the increase in conductance tends to even out any imbalance between the two resistances. This balancing of the electric field leads to the desired property that the Coulomb blockade at low temperature vanishes in a relatively narrow range of sample resistance.

## VIII Coulomb Blockade

To observe Coulomb Blockade, a sample whose resistance at room temperature is greater than or equal to 20 k$`\mathrm{\Omega }`$ must be cooled to milliKelvin temperatures. However, the evaporator in which each sample is prepared cannot be cooled. So each sample must be moved to a dilution refrigerator where it can be cooled to as low as 10mK.

The samples are very sensitive to electrostatic shock and so a careful grounding procedure must be followed to safely transfer each sample from the chamber to the refrigerator. From outside the chamber, before venting to atmosphere, the voltage on the sample is reduced to zero, and both leads are grounded. After venting, a mobile grounding strap grounds the removable deposition stage, and the sample leads are grounded to the stage, where now the voltage leads to the outside circuitry may be safely removed. The stage may now move to an ESD-safe workstation (table) and the sample dismounted.

To dismount the sample from the stage, a small piece of indium wire is used to shunt the contact pads on the chip. Leads running from the stage to chip may now be disconnected. The chip is free to move to a stage more suitable for the dilution refrigerator. A small chip carrier, designed for use in the tailpiece of the refrigerator will house the sample. Leads from the carrier to the chip are connected by indium pressing to the contact pads. The leads, from the top of the refrigerator to a connector at the tailpiece, are grounded, and the carrier is finally attached to the connector. The indium shunt on the chip is removed. The sample is now available for cool down. Only through this laborious grounding procedure can we move samples and have them survive.

We have recently added the gate to our samples. To this end, the mask is placed back over the chip, but rotated by $`90`$ degrees. Then the sample is returned to the deposition chamber and reconnected to the outside electronics. If the resistance of the sample is infinite, the sample is reconnected in high vacum, as in Fig. 3. Then, we deposit a layer of $`Al_2O_3`$, by reactive evaporation of aluminum. Davidović and Tinkham (1999) Aluminum is deposited at angles of $`\pm 5\mathrm{deg}`$ relative to the substrate normal. For each angle, the deposited thickness is 15nm. Then, we deposit a layer of aluminum metal, 40 nm thick, in the direction parallel with the normal.

The refridgerator is closed and pumped down to $`10^5`$ Torr. Then, the sample resistance is modified (if needed), using the techniques described in previous sections. Finally, the sample is cooled to $`0.015`$ K and the I-V curves are measured.

Standard cryogenic filtering techniques lower the electron temperature. Differential conductance is obtained using a lock-in technique. The applied voltage is a sum of a constant dc-voltage $`V`$ and a weak ac-voltage $`v(t)=v_{AC}\mathrm{sin}(2\pi ft)`$, where $`v_{AC}=1\mu `$ V and $`f=500`$ Hz. Current $`I`$ is measured with an Ithaco current preamplifier. To obtain the differential conductance, the output of the amplifier is connected to the input of a lock-in amplifier.

The effects of the gate voltage on differential conductance are shown in fig 5, at $`T=0.015K`$ in sample 3. The differential conductance near zero bias voltage is strongly suppressed. If the bias voltage aproaches a certain threshold from below, the differential conductance rapidly increases by several orders of magnitude.

The voltage threshold displays quasiperiodic modulation with the gate voltage. By applying the gate voltage, the voltage threshold can be reduced to zero. If the gate voltage is chosen so that the voltage threshold is at maximum, then the conductance at zero bias voltage is four orders of magnitude smaller than the conductance at large bias voltage.

This proves unambiguously that the sample consists of a metallic grain connected to drain and source, rather than a single junction. The diamonds in Fig. 5 are symmetric around zero bias voltage, showing that $`C_LC_R`$, where $`C_{L,R}`$ are the effective capacitances determined from the fit to the Orthodox theory of single-charge tunneling on a single metallic island. Averin and Likharev (1991) The image is chopped, because of the random switches in the background charge distribution (note that the gate voltage range is rather large compared with the bias voltage).

Figure 6-A shows the I-V curve of sample 1. This I-V curve is typical for our high resistance samples. We fit the I-V curve using the Orthodox theory, Averin and Likharev (1991) and show the corresponding fit by the dashed line. Good fits are generally found in approximately $`50\%`$ of the samples, suggesting that the samples typically consist of a single metallic grain in weak electric contact with the drain and the source.

The charging energy $`82`$ meV extracted from the fitting is relatively large. As a result, the bias voltage can induce jumps in the background charge distribution (also known as $`Q_0`$-shifts in the Orthodox theory). The I-V curve of sample 1 displays a noticeable deviation from the fit at positive bias voltage, see Fig. 6-A. These deviations are not noise. They are hysteretic - they change when sweeping the voltage up and down. At negative voltage bias, the deviations from the fit are weak and we do not observe any hysteresis when repeating the voltage sweep. This behavior is thus far consistent with single charge tunneling.

Among samples, charging energy fluctuates strongly. These fluctuations are explained by the broad distribution of particle diameters possible in such systems, Fig. 4. In addition, there is another source of fluctuations in charging energy, caused by the distribution of contact conductances. This effect will be discussed in the next section.

## IX Intermediate Coulomb Blockade

As $`R_L+R_R`$ decreases, the effective charging energy rapidly approaches zero, as shown in table 1. If the gap in the $`IV`$ curve is well resolved at $`T=0.015K`$, the grains are referred to as closed. The range of conductances of closed grains is indicated in Fig. 2-B. In table 1, samples 1-3 display a clear Coulomb blockade at $`T=0.015K`$. The parameters in these samples are obtained from the fits to the orthodox theory.

Figure 6-B shows $`IV`$ and $`dI/dVV`$ curves in sample 2. This sample displays a sharp Coulomb blockade, similar to that in sample 1. The I-V curve has no hysteresis, which is not surprising, since the charging energy is only $`4.6`$ meV and the bias voltage is too weak to reconfigure the background charge distribution. The Orthodox theory is in good agreement with the linear segments of the I-V curve. We can identify the same threshold voltages at both signs of the bias voltage: (a) corresponds to (d) and (b) corresponds to (c). This confirms there is only one grain in series with drain and source.

The rounding of the I-V curve is larger than expected from the Orthodox theory. A good fit is obtained with identical junction parameters $`R_L=R_R`$ and $`C_L=C_R`$. The first identity, $`R_L=R_R`$, is not as important as the second identity; good fits can be obtained even if $`R_L/R_R1`$. $`C_L=C_R`$ follows directly from the I-V curve, from the fact that the threshold voltages (b) and (c) have the same magnitude. We have noticed this symmetry in contact capacitance in a relatively large number of samples - roughly $`50\%`$ of samples with charging energy less than $`5`$ meV. In samples with $`E_C<1`$ meV, this symmetry is found in nearly every sample studied.

We do not have an explanation for this symmetry at low temperature and low bias voltage. Experimentally, no special care has been taken to make the junctions symmetric. In fact, the parameters are expected to be significantly asymmetric. We note that the symmetry in effective capacitance is broken in a strong magnetic field. The discussion of the magnetic field dependence is beyond the scope of this paper.

Theoretically, one expects that if $`G_L+G_R>G_0`$, where $`G_{L,R}=1/R_{L,R}`$, the system parameters become renormalized near zero temperature and zero bias voltage. The effective charging energy of the grain decays exponentially with contact conductance,

$$E_C^{eff}=E_Ce^{\alpha (G_L+G_R)/G_0},$$
(1)
where $`\alpha `$ is a constant of order 1, dependent on the nature of the contacts ($`\alpha =1`$ in tunneling junction and $`\alpha =\pi ^2/4`$ in a diffusive metallic contact), $`E_C`$ is the bare charging energy. Panyukov and Zaikin (1991); Nazarov (1999) This exponential dependence on $`G_L`$ and $`G_R`$ also explains strong fluctuations in the charging energy among samples.

The suppression of Coulomb blockade have been studied in larger metallic SETs. Joyez et al. (1997); Chouvaev et al. (1999) The connection between the effective charging energy and the bare sample parameters have been established. Joyez et al. (1997) Our samples are different from metallic SETs in that the contacts are metallic, and the grain diameter is small - small enough so that an electron can enter and exit the grain without loosing its phase coherence. 222The traversal time is roughly $`((R_L+R_R)/R_Q)h/\delta `$, where $`\delta `$ is the level spacing and $`R_Q=h/e^2`$. For a grain of diameter 20nm, the traversal time is easily shorter than the dephasing time in pure gold at low temperatures.

No calculation of the $`IV`$ curve in this regime is available. We still fit the $`IV`$ curve using the Orthodox theory, with the notion that the best fit parameters represent effective (renormalized) parameters. In this sense, $`E_C^{eff}=e^2/(2C^{eff})`$. The central result of this paper, beyond describing the new technique, is that $`C_L^{eff}=C_R^{eff}`$, when $`E_C^{eff}E_C`$ and when the applied magnetic field is weak. In table 1, the sample parameters are the effective parameters as defined here. No connection between effective and bare parameters is established in this paper. This connection is the subject of present research in our laboratory.

The observation $`C_L^{eff}=C_R^{eff}`$ has important implications for conversion from bias voltage into grain energy. For example, if the density of states of the grain varies as a function of energy, then this variation can be measured from the I-V curve. The capacitive division prefactor, which converts from bias voltage to energy, is 2.

In instances where the theoretical calculations can be solved exactly, the theory predicts that any asymmetry in the junction’s real parameters is only enhanced by the renormalization at low temperatures and low bias voltage. Furusaki and Matveev (1995) The theoretical model, however, is valid only if there is one electronic mode per contact, which may not apply to our samples. Our data demonstrate the opposite behavior from that predicted theoretically: in a weak magnetic field, the effective capacitances are symmetrized.

## X Weak Coulomb Blockade

We have observed that when the sample resistance at room temperature is less than roughly $`10k\mathrm{\Omega }`$, then the conductance at $`T=0.015K`$ near zero bias voltage remains on the same order of magnitude as the conductance at large bias voltage (asymptotic conductance/resistance). In Fig. 2-B, the grains with this property are referred to as open. Fig. 7 shows $`dI/dV`$ versus $`V`$ in a sample with room temperature resistance $`14k\mathrm{\Omega }`$. We observe that the conductance at $`V=0`$ and $`T=0.015K`$ remains within an order of magnitude from the room temperature conductance. In samples with asymptotic resistance $`10k\mathrm{\Omega }<R_L+R_R<20k\mathrm{\Omega }`$, the depth and the width of the conductance dip fluctuates strongly among samples (in two out of forty samples studied thus far, the conductance dip is significantly less pronounced than that in Fig. 7).

As the temperature increases, the zero-bias dip broadens. While at room temperature, the zero bias conductance dip is no longer resolved; the I-V becomes linear, with the conductance equal to the $`1/(R_L+R_R)`$. Alternatively, this asymptotic conductance is obtained at low temperatures, by applying a large enough bias voltage so that the I-V curve approaches the linear form.

To interpret this result we first try to fit the data in Fig. 7 to the dynamic Coulomb blockade model of a single tunneling junction. Devoret et al. (1990); Girvin et al. (1990) Yeyati et al. have extended this model to include a metallic contact with one channel, Yeyati et al. (2001) showing that the temperature dependence of a metallic contact does not differ from that of a tunneling junction. Fitting to the dynamic Coulomb blockade model does not reproduce the temperature dependence in Fig. 7.

We fit the data in Fig. 7 to the theory of a mesoscopic metallic grain in the strong tunneling limit. Golubev et al. (1997) This theory has already been used in connection with measurements of strong tunneling SETs by Chouvaev et al. Chouvaev et al. (1999) Strictly speaking, the model in Ref. Golubev et al. (1997) is not applicable to our devices because our contacts are metallic. For example, the parameter $`\alpha `$ in Eq. 1 differs between metallic contacts and tunneling contacts by a factor of $`\pi ^2/4=2.46`$. This implies that the Coulomb blockade is much more strongly suppressed with metallic contacts than with tunneling contacts. Nazarov (1999). In the absence of a theory of the I-V curve for a grain with metallic contacts, we use the theory of tunneling contacts. Golubev et al. (1997) The theory is valid only if $`eVE_C^{eff}`$ or $`k_BTE_C^{eff}`$.

The I-V curve is

$`I(V)`$ $`=`$ $`{\displaystyle \frac{V}{R_L+R_R}}{\displaystyle \frac{e}{\pi \mathrm{}}}{\displaystyle \frac{R_LR_R}{(R_L+R_R)^2}}\mathrm{Im}{\displaystyle \underset{r=L,R}{}}`$ (2)
$`\left({\displaystyle \frac{\mathrm{}}{R_0C}}+ieV_r\right)\mathrm{\Psi }\left(1+{\displaystyle \frac{\mathrm{}}{2\pi k_BTR_0C}}+i{\displaystyle \frac{eV_r}{2\pi k_BT}}\right)`$
$`ieV_r\mathrm{\Psi }\left(1+i{\displaystyle \frac{eV_r}{2\pi k_BT}}\right)`$
Here $`R_0=\frac{R_LR_R}{R_L+R_R},`$ $`C=C_L+C_R,`$ $`V_L=\frac{R_L}{R_L+R_R}V,`$ $`V_R=\frac{R_R}{R_L+R_R}V`$ and $`\mathrm{\Psi }(x)`$ is the digamma function. Note that there is a misprint in Ref. Golubev et al. (1997). The corrected expression is given in Ref. Chouvaev et al. (1999).

There are three fitting parameters $`R_L,R_R`$ and $`C`$. We set $`R_L+R_R`$ to be the same as the sample resistance at high temperature/voltage, and vary $`C`$ and $`R_L/R_S`$ to obtain the best fit. We fit the family of $`dI/dV`$ vs $`V`$ curves measured at different temperatures. The best fit is shown by lines in Fig. 7, and the corresponding sample parameters are given in Table 1, for sample 3. The fit reproduces our data quite well in the entire temperature range.

The I-V in Eq. 2 does not depend on on the capacitance ratio $`C_L/C_R`$. It is reasonable to assume that if the conductance at $`V=0`$ and $`T=0.015K`$ is several times smaller than $`1/(R_L+R_R)`$, then the voltage division across the grain is closer to capacitive than resistive. Then, if Eq. 2 holds, it follows that the effective capacitive division is independent on the bare capacitance ratio $`C_L/C_R`$. This may partially explain why the measured capacitances in the intermediate Coulomb blockade regime are identical.

## XI Conclusion

In conclusion, we present a new technique for fabrication of metallic grains in contact with leads. These grains are connected by two metallic atomic-scale point contacts, with well transmitted conduction channels. We show that when the sample resistance at room temperature is above $`h/e^2`$, then the $`IV`$ curve at low temperatures displays the Coulomb blockade. When the sample resistance approaches $`h/e^2`$, the blockade is weakened. We discover an intermediate regime in which the I-V curve is described by the Coulomb staircase with symmetric junction capacitances. As the sample resistance is reduced further, the Coulomb blockade is completely washed out, and only a weak zero bias conductance dip is observed. This regime is well described by the theory of metallic grains with strong tunneling.

###### Acknowledgements.

We thank M. Pustilnik, L. P. Kouwenhoven, D. Golubev for useful discussions. We thank the Georgia-Tech electron microscopy facility where electron transport experiments in combination with sample imaging have been performed. This work was performed in part at the Cornell Nanofabrication Facility, (a member of the National Nanofabrication Users Network), which is supported by the NSF, under grant ECS-9731293, Cornell University and Industrial affiliates. This research is supported by the David and Lucile Packard Foundation grant 2000-13874 and the NSF grant DMR-0102960.