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# Evidence for power-law frequency dependence of intrinsic dielectric response in the CaCu3Ti4O12

## I Introduction

There exists considerable interest in the dielectric behavior of the compound CaCu3Ti4O12. This material in ceramic and single crystalline forms shows colossal dielectric response with relative permittivity $`\epsilon ^{}`$ up to 105 at room temperature, which is practically frequency independent between DC and 106 Hz for the temperature range between 100 and 600 K. The dielectric permittivity abruptly drops down to a value $`100`$ upon lowering the temperature below 100 K. The value $`\epsilon ^{}100`$ is also seen at frequencies of a few$`\times 10^6`$ Hz and higher. Subramanian et al. (2000); Homes et al. (2001) The dielectric response behavior of the material is characteristic of Debye-like relaxation with a single relaxation time.

Apart from the giant values of the dielectric constant, the independence of dielectric properties with frequency and temperature is a property that is highly desirable for all applications of high-K materials. The understanding of the mechanism underlying the behavior of CCTO ceramics and single crystals might lead to engineering of new high-K materials with broadly temperature and frequency independent dielectric response, especially those suitable for applications in thin film form. For this reason, CCTO has been a subject of intensive research. However, the origin of the giant dielectric constant of CCTO ceramics and single crystals is so far not understood. Attempts were made to explain its behavior as an ’intrinsic’ property of the crystal lattice, Subramanian et al. (2000); Homes et al. (2001) or a property arising due to some ’extrinsic’ factors such as lattice defects Ramirez et al. (2002) or Schottky barriers at electrode-sample interfaces. Lunkenheimer et al. (2002) StructuralSubramanian et al. (2000) and spectroscopic Ramirez et al. (2000); Homes et al. (2001); Kolev et al. (2002); Homes et al. (2003) investigations of ceramic and single crystal samples along with first principles calculations He et al. (2002) suggest an extrinsic, Maxwell-Wagner-type, origin for the dielectric response. Subramanian et al., Subramanian et al. (2000) pointed out that non-conducting barrier layers, possibly twin boundaries, separating conducting domains could give rise to the colossal dielectric response of the material through a barrier-layer capacitance mechanism. Similar ideas were expressed also in Ref. He et al., 2002. Based on impedance spectroscopy data, Sinclair et al. Sinclair et al. (2002) later suggested that CCTO ceramics are a single-step Internal Barrier Layer Capacitor where insulating grain boundaries separate semiconducting grains.

In this article we report that the dielectric response of the thin epitaxial CCTO films is strongly dominated by a power law, and they behave as semiconductors with hopping conduction. Experiments on oxygen annealing suggest that the films with lower oxygen content are intrinsically more conducting. The most conducting films show the presence of relatively low conducting capacitive layers in their morphology and significantly larger dielectric constants at low frequencies. Finally, CCTO films can be obtained, which show the intrinsic relative permittivity of the compound $`\epsilon ^{}100`$ at room temperature. The observations provide additional evidence and strongly support the arguments for a barrier layer mechanism of the origin of the colossal dielectric response of CCTO.

## II Experiment

CCTO films were grown by PLD using a KrF laser with a wavelength of 248 nm on LaAlO3 (001) (LAO) substrates of $`h_s=500`$ $`\mu `$m thickness (relative permittivity $`\epsilon _s=24`$) in oxygen atmosphere from CCTO ceramic targets prepared by DuPont. The average fluence across the laser spot on the target was kept equal to $``$2.5 J/cm2. Pulse repetition rates were from 1 Hz to 5 Hz. The film composition and structure were characterized by Rutherford Backscattering Spectroscopy (RBS), X-ray diffractometry, Transmission Electron Microscopy (TEM), Atomic Force Microscopy (AFM), and Scanning Near-Field Microwave Microscopy.Steinhauer et al. (2000) Electrical properties of the films were investigated using Interdigital Electrode (IDE) capacitors lithographically made on top of the films. We have characterized properties of films of thicknesses $`h_f`$ ranging from 80 nm to 1500 nm.

The following growth conditions were found optimal for both crystalline quality of the films and roughness of the film surface: Substrate temperature is 695 C, oxygen pressure is 60–200 mTorr, substrate is slightly immersed in the visible plasma plume. The deposition rate for these conditions is 0.6–1 Å/pulse. After deposition, samples were cooled down at the rate of 5 C/min in oxygen at pressure $`P_{\text{O}_2}750`$ Torr. Films produced under these conditions were found to be rather conducting. Their room temperature conductivity varied in the range 10-7–10-4 $`\mathrm{\Omega }^1`$cm-1. To make more insulating films, we decreased the deposition rate of the films by decreasing the laser repetition rate and/or annealed films in oxygen after deposition. Post-deposition anneals were carried out in flowing oxygen at atmospheric pressure and at a temperature of 695 C.

The conductance of as-deposited films was found to be strongly dependent on deposition conditions and poorly reproducible. Increase of the background oxygen pressure during deposition resulted in less conducting films. Post-deposition annealing in oxygen always decreased the film conductance and created films with similar properties. High-Resolution TEM investigations of the CCTO/LAO interface show a very sharp and clean interface indicating that there is no chemical reaction between the film and substrate during annealing. Table 1 lists parameters of five samples chosen based on their room temperature conductivity and discussed in the paper.

CCTO grows epitaxially with the (00k) direction perpendicular to the substrate surface with a high quality of epitaxy, in agreement with the behavior reported in the literature.Si et al. (2002); Lin et al. (2002) Figure 1 shows a typical result of X-ray diffraction $`\theta `$$`2\theta `$ scan of a CCTO film. The full width at half-maximum of the X-ray diffraction rocking curves around the (004) CCTO peak of as-deposited films was 0.57–0.60. RBS studies of the films showed cation ratios corresponding to that of CCTO. TEM studies showed that the film-substrate lattice mismatch was relaxed by misfit dislocations at the interface.

Interdigital capacitors were made on top of the films after all film fabrication steps. The layout of an interdigital capacitor and notation of its dimensions are shown in Fig. 2. The capacitor fingers were of $`r=25`$ $`\mu `$m width and $`l=700`$ $`\mu `$m length and were separated by gaps of width $`d=15`$ $`\mu `$m. The electrodes consisted either of $``$20 nm thick Pt layer or a $``$10 nm thick Pt adhesion layer followed by a $``$20 nm thick Au layer and were deposited through a photoresist mask by PLD at room temperature with following lift-off. The parasitic resistance of the pure Pt electrodes is much larger than that of Pt/Au electrodes and reaches 180 $`\mathrm{\Omega }`$ for some samples. The parasitic resistance of Pt/Au electrodes does not exceed 15 $`\mathrm{\Omega }`$. The impedance of the IDE capacitors was measured by means of LCR meters HP 4284A (20 Hz – 1 MHz), Agilent 4285A (75 kHz – 30 MHz), and SRS 510 (100 Hz – 100 kHz).

If the film thickness $`h_f`$ is much smaller than the interdigital capacitor dimensions (see Fig. 2): $`h_fr`$, $`d`$, $`d_{\text{end}}`$, $`h_s`$, $`w`$, $`l`$, the number of fingers $`n3`$, and thickness of capacitor electrodes $`tr`$, which was true in our experiments, the following approximate formula can be used to extract the film relative permittivity $`\epsilon ^{}`$ from the measured capacitance $`C_{\text{meas}}`$ and the capacitance $`C_s`$ of the same IDE capacitor made on a bare substrate with a relative permittivity $`\epsilon _s`$:

$$\epsilon ^{}\epsilon _s+\frac{C_{\text{meas}}C_s}{C^{}},$$
(1)
where

$$C^{}=\frac{1}{2}(n3)\epsilon _0lq_n+2\epsilon _0lq_3+n(2+\pi )\epsilon _0rq_{\text{end}}.$$
(2)
In the last expression, $`\epsilon _0`$ is the permittivity of vacuum, and the coefficients are:

$`q_n`$ $`=`$ $`{\displaystyle \frac{\pi }{3\mathrm{ln}2+\pi d/(2h_f)}}`$ (3)
$`q_3`$ $`=`$ $`{\displaystyle \frac{\pi }{4\mathrm{ln}2+\pi d/h_f}}`$ (4)
$`q_{\text{end}}`$ $`=`$ $`{\displaystyle \frac{\pi }{4\mathrm{ln}2+\pi d_{\text{end}}/h_f}}.`$ (5)
Eqs. (1)-(5) follow from expressions for capacitance of IDE capacitors on multilayered substrates derived in Ref. Gevorgian et al., 1996 and approximate the exact formulas with an accuracy of $``$1% under our conditions.

The conductance of the LAO substrate is much smaller than that of the CCTO films as was determined from the loss tangent measurements of the substrate material. The frequency dispersion of the substrate permittivity is negligibly small in the whole frequency range, and the substrate contribution to the frequency dependent part of the capacitance can be neglected.

## III Results and Analysis

### III.1 Room temperature frequency dependence of dielectric response

Figure 3 shows the room temperature frequency dependence of the capacitance $`C`$ and the conductance $`G`$ measured in the CGp representation (parallel C and G) from 20 Hz to 30 MHz for the three most conducting samples listed in Table 1. The open symbols are experimental data and the solid and dashed lines are fits for the measurement data using the capacitor models shown in the lower right panel of Fig. 3. As is seen, the experimental data for the CCTO thin films do not feature the clear Debye-like behavior demonstrated by CCTO ceramics and single crystals. Instead, their dielectric behavior has a strong contribution of a power law. In a log-log representation, the power law is linearized and it can be recognized in the capacitance data for samples 1 and 2, as well as in the conductance data for sample 3.

To analyze details of the dielectric response of our CCTO films, we start with the simplest equivalent circuit model taking into account the power law frequency behavior of the capacitors, model A in Fig. 3. This model includes a capacitance $`C(f)`$ describing the real part of the relative permittivity of the material, conductances $`G_{\text{DC}}`$ and $`G_{\text{AC}}(f)`$ describing the intrinsic DC conductance and the AC conductance of the material, and the parasitic resistance of the capacitor electrodes $`R_s`$. The AC conductance $`G_{\text{AC}}(f)`$ and the capacitance $`C(f)`$ of the model follow the power law (Curie-von Schweidler law, or the universal dielectric response (UDR) law Jonscher (1977, 1983); Lunkenheimer et al. (2002)):

$$G_{\text{AC}}(f)=G_ff^s,$$
(6)
$$C(f)=C_{\mathrm{}}+(2\pi )^1G_f\text{tan}(\pi s/2)f^{(s1)}.$$
(7)
The conductance data of all the three samples can be well fit with this model in the whole frequency range, whereas the capacitance data for samples 1 and 2 can be fit only partially, as shown by solid lines in Fig. 3. The parameters of the fittings are displayed in the corresponding panels. The capacitance data for samples 1 and 2 deviate from the UDR fits at low frequencies, which might indicate a contribution from possible capacitive layers with lower conductivity (blocking layers).

Therefore, we further continue with the analysis of the responses of samples 1 and 2 only. To take the low frequency deviation into account, we add a parallel RC-circuit with frequency independent parameters in series with elements of model A as shown by model B in Fig. 3. Now, very good fits can be obtained for the capacitance response of both samples 1 and 2 in the whole frequency range, however the corresponding conductivity curves significantly deviate from the experimental points (see dashed lines denoted with the letter B in the upper panels of Fig. 3). Addition of one more element, a frequency independent leakage conductance $`\text{G}_{\text{leak}}`$ around the UDR and the blocking components, as shown in model C Fig. 3, makes it possible to fit simultaneously both capacitance and conductance data with one set of parameters (see dashed lines denoted with the letter C in the upper panels of Fig. 3; the conductivity curves for models A and C almost overlap).

We would like to note here that model B both with UDR-dependent and with frequency independent parameters was invoked in the literature to explain the colossal dielectric response of the bulk CCTO. Lunkenheimer et al. (2002); Sinclair et al. (2002); Adams et al. (2002) For a pronounced Debye-like behavior, as demonstrated by bulk CCTO, it is necessary that $`G_{\text{block}}G_{\text{DC}}`$. Note that a capacitor in series with an RC circuit represents systems with Debye dipolar relaxation.Jonscher (1983)

The frequency response of sample 3 is different from that of samples 1 and 2. Model A is sufficient to fit the response of sample 3 (see solid lines in the lower left part of Fig. 3). Moreover, modes B and C cannot satisfactory describe the response of sample 3. An attempt to fit the capacitance data with the use of model C resulted in a very large $`C_{\mathrm{}}59`$ pF, which gives $`\epsilon _{\mathrm{}}^{}460`$, an unrealistically high value. The fit with the use of model A results in $`C_{\mathrm{}}42`$ pF and $`\epsilon _{\mathrm{}}^{}=90`$.

As can be concluded, sample 3 is either missing any insulating blocking layer components that are present in samples 1 and 2 and in bulk materials, or their effect is removed because the intrinsic conductivity of the material dropped below some critical value, and we observe the intrinsic frequency response of the material in the whole frequency range.

The values of $`C_{\mathrm{}}`$ found from the fit for sample 1 using model C is lower than the capacitance of the same IDE capacitor on a bare substrate, which was attributed to a high leakage in the film. The fit for sample 2 resulted in $`\epsilon _{\mathrm{}}^{}=64\pm 20`$. The values of $`\epsilon _{\mathrm{}}^{}`$ for samples 2 and 3 are close to $``$80 found at terahertz frequencies in Ref. Homes et al., 2001 for the dielectric constant of CCTO single crystals. Additionally, measurements at 1.4 GHz made with a microwave microscopeSteinhauer et al. (2000) on sample 3 gave $`\epsilon ^{}=40\pm 20`$. Application of up to $`\pm `$40 V bias voltage to the capacitors did not change the dielectric response of the films, demonstrating the linearity of the dielectric properties of the CCTO films. The parasitic resistance of the capacitor electrodes $`R_s`$ causes a downturn in the capacitance as well as a strong upturn in the conductance data upon increase of frequency at the highest frequencies of the range. These features are more pronounced for samples with larger $`R_s`$ as seen in Fig. 3. The difference in $`R_s`$ of the three samples arises from different electrode materials and different thicknesses of the Pt film. The values of the parameter $`R_s`$ obtained from the fittings of Fig. 3 are consistent with the resistivity of the Au and Pt thin films and with the geometry of the capacitor electrodes.

The capacitance of sample 5 (Table 1), obtained with a long anneal in oxygen, is weakly frequency dependent at room temperature and remains close to a value corresponding to a CCTO film permittivity of $`100`$ in the whole frequency range.

In the present state of our knowledge of CCTO and within the scope of the present study, we cannot identify the nature of conduction in general and the leakage in particular in our CCTO films. CCTO is a Mott-Hubbard insulatorHe et al. (2002) and might become conducting by relatively small deviations from stoichiometry, by doping with oxygen vacancies, or due to defects. A possible scenario consistent with model C can include leakage along grain boundaries due to deviation of stoichiometry and accumulation of defects along them. Then, as follows from model C, the electrodes do not create barriers at interfaces with the leaking component, and the blocking layers should be internal to the less conducting grains. Annealing in oxygen leads to restoration of defects and to oxidation of the material inside the grains and in the grain boundaries. Both these processes result in drop of intrinsic and leakage conductance of the films.

### III.2 Temperature dependence of permittivity and conductivity

Figure 4 shows the temperature dependence of the film relative permittivity at four frequencies logarithmically separated by one decade, and the 100 Hz conductivity for all the five samples listed in Table 1 in the temperature range from 80 to 300 K. The 100 Hz conductivity was obtained from the capacitor loss tangent data. Similar to the bulk materials Subramanian et al. (2000); Homes et al. (2001) and to the thin films of Ref. Si et al., 2002, the permittivity of the CCTO films starts to rise from a value of about 100 with increasing temperature. At the lowest temperatures, the permittivity is independent of frequency within the measurement error. For the sample with the lowest conductivity, the relative permittivity is close to 100 almost independent of temperature and frequency.

To find out whether the power-law behavior found at room temperature is preserved at lower temperatures, we re-plotted the permittivity data of Fig. 4 in the following way. We subtracted values of the relative dielectric constant obtained at a temperature of 80 K $`\epsilon _{\text{80K}}^{}`$ from the data points for each frequency and plotted the difference ($`\epsilon ^{}\epsilon _{\text{80K}}^{}`$) on a log-scale versus temperature. We take into account here that $`\epsilon _{\text{80K}}^{}\epsilon _{\mathrm{}}^{}`$ obtained at room temperature. The result is displayed in Fig. 5. Only data points with a significant signal-to-noise ratio are shown. In the case of sample 1, the value of $`\epsilon _{\text{80K}}^{}`$ for 1000 Hz was used to plot the 100 Hz curve.

We note that the power law is linearized in the log-log representation. Since the four frequencies used for the plots are logarithmically spaced by one decade, this representation immediately shows how close to the UDR the frequency dependence of the permittivity remains upon lowering the temperature. For instance, the curves for sample 3 look like four equally separated parallel lines, which indicates preservation of the UDR frequency response up to at least 170 K with a small temperature dependence of the $`s`$-parameter.

Figure 6(a) shows Arrhenius plots for the 100 Hz conductivity of samples 1–4. According to the fits and model C of Fig. 3, the conductance of the films is strongly dominated by the highly conducting leakage component in the films. Nevertheless, the analysis of temperature dependence of the film conductivity can provide some insight into the conduction mechanisms of CCTO. We assume here that the contribution of the AC part of the UDR conductivity is negligibly small at this frequency, as can be deduced from the room temperature data of Fig. 3. The Arrhenius representation linearizes the thermally activated conduction $`\sigma \text{exp}(E_a/k_\text{B}T)`$. As can be seen after careful consideration, only the data for sample 1 from 80 K to about 130 K and from 170 K to 300 K can be well linearized in this representation, with activation energies of 0.08 eV and 0.16 eV, correspondingly. The behavior of the three other curves deviates from the thermally activated behavior. However, the three curves can be piecewise linearized in the representation $`\text{ln}\sigma `$ versus $`1/T^{1/4}`$, as shown in Fig. 6(b). The latter representation corresponds to the 3D variable-range hopping conduction modelMott and Davis (1979) with $`\sigma \text{exp}(B/T^{1/4})`$. The data for sample 2 can be linearized in this representation in a large temperature range from 180 K to room temperature. The data for sample 3 can be better linearized in the representation $`\text{ln}\sigma `$ versus $`1/T^{1/4}`$ only for lower temperatures. At higher temperatures, both the representation are indistinguishable. And the data for sample 4 can be linearized in the latter representation in the whole temperature range, where the conductivity is measurable, i. e., between about 240 K and room temperature. This analysis suggests that the hoping of localized charge carriers is the dominant mechanism of charge transport in the samples with lower conductivity, whereas thermally activated transport prevails in the conduction of sample 1.

### III.3 Analysis and Discussion

At this stage we can make a preliminary assessment of our results. The most striking feature of the epitaxial CCTO thin films is that their dielectric response is strongly dominated by a power-law in frequency, in contrast to the Debye-like response of the bulk material. Experiments on annealing of the films in oxygen suggest that films with lower oxygen content are intrinsically more conducting. With increase of the oxygen content the room temperature frequency response of the CCTO thin films evolves from the response indicating presence of some relatively low conducting capacitive layers to purely power law, and then towards frequency independent response with $`\epsilon ^{}`$ close to 100. The most conducting films show significantly larger room temperature dielectric constants at low frequencies ($`\epsilon ^{}310^4`$ at $`f=20`$ Hz).

The power-law frequency dependence of dielectric properties is a behavior typical for semiconducting materials with hopping localized charge carriers.Mott and Davis (1979); Jonscher (1977, 1983); Lunkenheimer et al. (2002); Bobnar et al. (2002) This result, along with the observed strong correlation between the temperature behavior of conductivity and permittivity, allow us to conclude that we are dealing with carrier polarization in the CCTO films. The effect of annealing in oxygen on conductivity suggests that oxygen deficit is a cause of the relatively high film conductivity.

The observations described above strongly support arguments in the literature Subramanian et al. (2000); He et al. (2002); Lunkenheimer et al. (2002); Sinclair et al. (2002); Adams et al. (2002) on the role of blocking barrier layers in CCTO and evidence for an extrinsic, Maxwell-Wagner type, origin of the colossal dielectric response of CCTO ceramics and single crystals. They also imply that the blocking layers must be insulating, thus cutting down on the number of possible microscopic morphologies suggested for bulk CCTO by Cohen et al.Cohen et al. (2003) We did not find any significant dependence of film properties on thickness, in contrast to Ref. Si et al., 2002.

It is of interest in this context to directly compare the characteristics of the dielectric responses of thin films and some of the CCTO bulk samples. The room temperature measurement of the response of the ceramic target we used for film deposition (not shown) yielded $`\epsilon _{\text{100Hz}}^{}4000`$ and a pronounced Debye-like response. The fit of the response with model B, Fig. 3, resulted in $`\text{G}_{\text{DC}}/\text{G}_{\text{block}}=510^4`$ with an intrinsic DC conductivity of the ceramic $`\sigma _{\text{DC}}^{\text{int}}310^4`$ $`\mathrm{\Omega }^1\text{cm}^1`$, assuming that the blocking layers are thin and constitute a small fraction of the sample volume. For the thin film sample 1, $`\text{G}_{\text{DC}}/\text{G}_{\text{block}}1`$ and the internal conductivity $`\sigma _{\text{DC}}^{\text{int}}710^6`$ $`\mathrm{\Omega }^1\text{cm}^1`$, again assuming that blocking layers along with leakage paths make up only a small fraction of the sample volume. A comparison of these values suggests that the ceramic material is intrinsically more conducting and its barrier layers block conductivity more efficiently.

It is still an open question as to what microscopic feature(s) produce the blocking layers in CCTO samples. Lunkenheimer et al.Lunkenheimer et al. (2004) recently showed that contacts contribute to the dielectric response of the CCTO bulk ceramic samples, and this contribution can constitute a significant fraction of their response at low frequencies. However, to date there is no unambiguous experiment that demonstrates that the influence of electrodes alone can explain all the behavior of CCTO dielectric response especially in single crystals. Apart from the contribution of electrode-sample interfaces, a microscopic picture of hopping localized charge carriers confined within small domains, whose boundaries make up large energy barriers for hopping, remains plausible. Within this picture, the boundaries of the small domains constitute a dense network without “holes” for conductivity, and the exact morphology and characteristic scales of the network such as domain size are dependent on sample processing conditions. Suggestions for possible domain boundaries include grain boundaries,Sinclair et al. (2002); Adams et al. (2002) twin boundaries,Subramanian et al. (2000) compositional and anti-phase domain boundaries.Cohen et al. (2003) We take this opportunity to examine the microstructure of our films for evidence of (or absence of) any of the proposed blocking layers with focus on possible twinning of the films. The films showing a dielectric behavior suggestive of the presence of some barrier layers, similar to sample 1 discussed above, are of particular interest.

The films are epitaxial, but morphologically they consist of grains separated by grain boundaries. Taking into account the results of fits of the room temperature dielectric response (Fig. 3), most probably the grain boundaries in the films are more conducting than the grains and cannot act as barrier layers. However, one cannot exclude grain boundaries as possible blocking layers in CCTO bulk ceramics based on this fact, because the microstructure of grain boundaries can be different in thin films and ceramics due to significantly different fabrication processes.

To investigate the microstructure of our films, we have performed detailed plan-view and cross-sectional TEM study of the films. Figure 7(a) shows a simulated electron diffraction pattern from the ideal, twin-free, CCTO lattice with the Im3̄ space symmetry group. Note that due to the Im3̄ symmetry of the lattice the diffraction pattern is not symmetric relative to the $`<`$0ll$`>`$ directions of the pattern. Namely, pairs of spots within a set, e.g. sets {013} or {024}, located symmetrically relative to the $`<`$0ll$`>`$ directions have significantly different intensities. As reported in Ref. Subramanian et al., 2000, the Laue group of twinned CCTO single crystals appeared to be m3̄m instead of m3̄. This means that a CCTO lattice containing twins would produce a diffraction pattern where all spots within each set {013}, {024}, etc., are of equal intensity. The spot positions would be the same for both m3̄ and m3̄m Laue groups. The experimental diffraction pattern in Fig. 7(b) does not show the asymmetry in the intensities of the spots seen in the simulated diffraction pattern in Fig. 7(a). At the same time, the relative intensities of the spots in the experimental diffraction pattern are different from those expected for the twinned lattice. A possible explanation for the lack of asymmetry in the intensity of the spots is that the CCTO film is twinned at a scale smaller than the area that the diffraction pattern came from and, since the film consists of slightly misoriented grains, the experimental diffraction pattern of Fig. 7(b) does not posses either a clear m3̄ or m3̄m symmetry. It is possible also that the films are not twinned but the spots in the diffraction pattern have approximately the same intensity due to multiple diffraction. Microdiffraction patterns obtained with a beam of 40 nm in diameter did not show the asymmetric patterns either, indicating that if there are twins in the crystal they must be smaller than 40 nm in size.

To further identify twins in the CCTO films, we implemented dark field imaging with use of diffracted beams corresponding to spots of sets {013} and {024}. Twins contributing differently to spots of these sets should give rise to twining contrast in dark field images. Figure 7(c) shows a dark field image of the CCTO film cross-section taken with the (013) spot. We do observe contrast between grains here. This contrast can be due to slight misorientation between grains and because the grains can be “twins” to each other. Some contrast observed within grains is most probably caused by strain. There is no contrast seen within grains that is consistent with the presence of twinning. Using the highest possible magnification accessible with this technique, we are able to state that the films do not contain twin domains larger than 10 nm. The presence of smaller twins cannot be excluded, however. It is believed that the twins are in the Ti-O sublattice, making their observation by high-resolution TEM difficult. 111Straightforward HRTEM does not reveal any twinning. Modeling of HRTEM images with varying defocus and sample thickness for the two CCTO structures show that there exist certain features which could in principle allow one to distinguish between twinned and untwinned states in the case of nano-twins.

## IV Conclusions

In conclusion, CaCu3Ti4O12 thin films grown epitaxially on LaAlO3 (001) substrates by PLD were found to be semiconducting with frequency response strongly dominated by a power-law, typical of materials with localized hopping charge carriers. The room temperature frequency response of the CCTO thin films converges with increase of the oxygen content from a response indicating the presence of the relatively low conducting capacitive layers, through purely power law, towards frequency independent response with $`\epsilon ^{}`$ close to 100. Films with lower oxygen content are intrinsically more conducting. Lowering the temperature leads to decrease of the film conductance and to decrease of the dielectric response, which remains dominated by the power law. Below $`T80`$ K, the dielectric response of the films was found to be frequency independent with $`\epsilon ^{}`$ close to 100. The observations suggest that we are dealing with carrier polarization in the CCTO films. The results can be considered as additional evidence that the giant dielectric constants of bulk and thin films of CCTO reported in the literature are of extrinsic origin of Maxwell-Wagner type. Detailed plan-view and cross-sectional TEM studies did not reveal twin domains of size larger than 10 nm in our CCTO films.

## V Acknowledgements

We would like to thank J. B. Neaton for valuable discussions, R. P. Sharma and V. Kulkarni for performing RBS measurements. The work was supported by the University of Maryland/Rutgers NSF MRSEC under grant DMR-00-80008.


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# UWThPh-2003-20 UAHEP03010 R Parity Violating Decays of the Gluino

## 1 Introduction

The possibility of the lightest supersymmetric particle (LSP) decaying through R parity violation has been discussed since the early days of supersymmetry , many studies have been made (e.g. ), and many experimental searches have been undertaken (e.g. ). There seem, however, to have been no investigations up to now of the possibility considered here of R parity violating decays of the gluino. Although these would be most relevant if the recent theme of a light or relatively light gluino were to be experimentally confirmed they could also be important in the case of a heavy gluino LSP. In some cases  the phenomenological advantages of a light gluino have as much to do with a large hierarchy between gluino and squark masses as with a light gluino mass per se. Most recent light gluino investigations have concentrated on the mass region around $`12`$ GeV possibly accompanied by a b squark near $`4`$ GeV  , . Alternative possibilities have also been noted . In the minimal supersymmetric standard model (MSSM), a light gluino is typically accompanied by an even lighter photino allowing the decay $`\stackrel{~}{g}q\overline{q}\stackrel{~}{\gamma }`$. In gauge mediated SUSY breaking models, there is often an ultra-light gravitino below the gluino in mass leading to the decay $`\stackrel{~}{g}g\stackrel{~}{G}`$. In some models these channels are closed leading to an absolutely stable gluino or to one decaying through R parity violating processes. In this article we assume the gluino is the lightest supersymmetric particle and we consider lepton number violating gluino decays. In section II we treat the decays $`\stackrel{~}{g}q\overline{q}\nu `$. The fact that the third generation seems, in some respects, special compared to the first two suggests models in which the R parity violation is tied to the third generation.

If the R parity violation is entirely in the third generation and the gluino lies below the $`b\overline{b}`$ threshold, there will be the loop induced decay $`\stackrel{~}{g}g\nu `$. This is treated in section III neglecting the possibility of a right-handed neutrino.

Finally, in the presence of a light right-handed neutrino, there is the possibility, treated in section IV, that the dominant decay could be a two loop process coupling the gluino to gluon plus $`\nu _R`$. It might be expected that such a dominant decay mechanism would lead to an ultra-long-lived gluino.

## 2 The gluino decay to quark-antiquark-neutrino

We assume an $`R`$ parity violating and lepton number violating term in the superpotential of the form

$`W=\lambda _{ijk}^{}L_iQ_jD_k`$ (2.1)
where $`i,j,k`$ are family indices. Then, if the gluino is above a quark-antiquark threshold one will have the gluino decay to $`q\overline{q}\nu `$ corresponding to the graph of fig. 1.

The fact that the third generation seems, in some respects, special compared to the first two suggests models in which the R parity violation involves third generation quarks and squarks only. We, therefore, take as a working assumption that the non-zero quark flavor indices in 2.1 are third generation only. In any case, the experimental limits on R parity violating couplings are much less restrictive  in the third generation so these could well be dominant. A $`\lambda ^{}`$ involving only third generation quarks could be as great as $`0.1`$. Then the gluino decay would be into $`b\overline{b}\nu `$ assuming the gluino mass is above the $`2b`$ threshold. In this case a light gluino pair production could explain the excess b production seen at Fermilab without requiring the light b squarks of .

The signature of such a decay, hadrons plus missing energy, would be identical to the conventional $`q\overline{q}\stackrel{~}{\gamma }`$ decay. The inverse width for this latter decay is

$`\tau (\stackrel{~}{g}q\overline{q}\stackrel{~}{\gamma })\stackrel{~}{m}^4/(m_{\stackrel{~}{g}}^5\alpha _s\alpha )`$ (2.2)
With a light gluino and a squark mass in the $`100GeV`$ range, this typically results in a gluino lifetime in the nanosecond range which is counter-indicated by the $`KTEV`$ search . If, however, the gluino is the LSP and decays through the R parity violating graph of fig. 1, the lifetime could easily be much longer so that the lightest supersymmetric hadron, presumably the gluino-gluon bound state, would not decay in the sensitive region of a $`KTEV`$ type experiment. We have recently become aware of a previous treatment of this decay mode.

$`\tau (\stackrel{~}{g}q\overline{q}\nu )\stackrel{~}{m}^4/(m_{\stackrel{~}{g}}^5\alpha _s\lambda _{}^{}{}_{}{}^{2})`$ (2.3)
The neutrino mass matrix corresponding to the R parity violation of 2.1 is

$`M_{ii^{}}^\nu {\displaystyle \frac{3}{8\pi ^2}}{\displaystyle \underset{jk}{}}\lambda _{ijk}^{}\lambda _{ikj}^{}m_d(j)m_d(k)/\stackrel{~}{m}`$ (2.4)
where $`\stackrel{~}{m}`$ is the assumed degenerate squark mass and $`m_d(k)`$ is the down-type quark mass in the k’th family. We have also made the simplification of neglecting the CKM quark mixing angles and have assumed that $`A_d\mu \mathrm{tan}\beta `$ is of order $`\stackrel{~}{m}`$. If the dominant $`k,j`$ are third generation,  notes that a $`4.5eV`$ $`\nu _e`$ mass would correspond to

$`\lambda _{133}^{}710^4\left({\displaystyle \frac{\stackrel{~}{m}}{100GeV}}\right)^{1/2}`$ (2.5)
although the present indications of a sub-eV neutrino mass would lead to a $`\lambda ^{}`$ an order of magnitude below 2.5. Such a relation substituted into 2.3 would lead to a gluino lifetime depending only on the ratio of gluino mass to squark mass.

$`\tau (\stackrel{~}{g})=.013s\left({\displaystyle \frac{\stackrel{~}{m}}{1000m_{\stackrel{~}{g}}}}\right)^5\left({\displaystyle \frac{0.1}{\alpha _s}}\right)\left({\displaystyle \frac{710^5}{\lambda _{i33}^{}}}\right)^2`$ (2.6)
A gluino-gluon bound state with a lifetime of order $`.013s`$ might have evaded the current searches since it would appear as a quasi-stable particle whose ultimate decay with a missing neutrino could be confused with a neutron knock-on event.

## 3 The gluino decay to gluon plus neutrino

If the gluino mass is less than twice the mass of the quarks appearing in the $`R`$ parity violating couplings, one has the hitherto uninvestigated decay

$`\stackrel{~}{g}g\nu .`$ (3.1)
A recent analyses of constraints from Z decay suggests at 95% confidence level

$`m_{\stackrel{~}{g}}>6.3GeV/c^2.`$ (3.2)
This limit still allows the possibility that the gluino mass is below the b quark pair threshold. The matrix element corresponding to the graph of fig. 2 plus the analogous graph where the gluon is emitted from the squark line is

$`=ϵ_\mu {\displaystyle \frac{\lambda ^{}g_{3}^{}{}_{}{}^{2}m_b}{4}}\overline{u}(p^{}){\displaystyle \frac{d^4k}{(2\pi )^4}\left(\frac{(\mathit{}^{}+\mathit{})\gamma ^\mu +\gamma ^\mu (\mathit{}+\mathit{})}{(p+k)^2m_b^2}+\frac{(2kq)^\mu }{(kq)^2\stackrel{~}{m}^2}\right)}`$
$`(1\gamma _5)u(p){\displaystyle \frac{1}{(p^{}+k)^2m_b^2}}{\displaystyle \frac{1}{k^2\stackrel{~}{m}^2}}`$ (3.3)
where $`p^{}=pq`$ is the final state neutrino momentum.

This amplitude is equivalent to that induced by an effective magnetic moment coupling

$`=i\mu _a\overline{u}_L(\nu )\sigma ^{\mu \nu }q_\nu u(\stackrel{~}{g})ϵ_\mu (g)`$ (3.4)
with

$`\mu _a{\displaystyle \frac{m_b\alpha _s\lambda ^{}}{\stackrel{~}{m}^2}}`$ (3.5)
The corresponding decay rate is

$`\mathrm{\Gamma }(\stackrel{~}{g}g\nu )=\mu _a^2m_{\stackrel{~}{g}}^3{\displaystyle \frac{m_b^2m_{\stackrel{~}{g}}^3\alpha _s^2\lambda ^2}{\stackrel{~}{m}^4}}`$ (3.6)
Nominal values of $`10GeV`$, $`10TeV`$, $`0.1`$, and $`710^5`$ for $`m_{\stackrel{~}{g}}`$, $`\stackrel{~}{m}`$, $`\alpha _s`$, and $`\lambda ^{}`$, would correspond to a gluino lifetime of $`5.210^3s`$.

A two loop graph that would lead to a gluino decay to gluon plus right-handed neutrino is shown in fig. 3. To investigate such two loop effects we consider an extended superpotential containing a right-handed singlet superfield N.

$`W=W_{MSSM}+\lambda ^{}QDL+ϵH^uH^dN+h_\nu LNH^u`$ (3.7)
Here, lepton number and R parity violation comes through a new $`H^uH^dN`$ interaction governed by the coupling constant $`ϵ`$ in addition to the conventional $`\lambda ^{}`$ coupling. $`W_{MSSM}`$ contains the usual Higgs mixing term $`\mu H^uH^d`$. The small Yukawa coupling $`h_\nu `$ is proportional to the neutrino Dirac mass:

$`h_\nu ={\displaystyle \frac{m_\nu ^{Dirac}}{<H^u>}}`$ (3.8)
The effective transition magnetic moment from fig. 3 is

$`\mu _a{\displaystyle \frac{1}{(4\pi )^3}}{\displaystyle \frac{\lambda ^{}h_\nu h_b\alpha _s\mu Bm_b}{\stackrel{~}{m}^2m_H^2}}`$ (3.9)
Here, $`\mu B`$ is the off-diagonal entry in the Higgs mass squared matrix. In the MSSM with electroweak symetry breaking , it is given by $`\mu B=\frac{1}{2}M_A^2sin(2\beta )`$ where $`M_A`$ is the mass of the CP–odd Higgs scalar.

This $`\mu _a`$, however, would be proportional to the neutrino mass and would be negligible compared to the transition magnetic moment of 3.5.

## 4 A dominant gluino decay to gluon plus right-handed neutrino

Even in the absence of the R parity violating quark-squark-lepton coupling of 2.1, the R parity and lepton number violating Higgs-Higgsino-Lepton coupling in 3.7 could lead to a gluino decay into gluon plus right-handed neutrino.

The lowest order graph contributing to gluino decay would be that of fig. 4 as well as those graphs related by attaching the gluon to other colored lines or by changing the flavor of the internal quark (squark) lines. These amplitudes are proportional to the trilinear boson coupling parameters $`A`$, which are induced in the softly broken MSSM thru supergravity. We can entertain the possibility that the $`\lambda ^{}`$ parameters are negligible and that the dominant trilinear coupling is that of the top quark. Then the two loop gluino decays of fig. 4 could be dominant for a gluino LSP of mass up to the minimum of twice the top mass or twice the stop mass:

$`\mu _a{\displaystyle \frac{1}{(4\pi )^3}}{\displaystyle \frac{\mu \mathrm{cos}(2\beta )m_{\chi ^0}Aϵ\alpha _sh_t}{\stackrel{~}{m}^2m_H^2}}`$ (4.1)
where $`m_{\chi ^0}`$ is the mass of the neutralino. However, if the top quark is heavier than the neutralino, then $`m_{\chi ^0}`$ should be replaced by $`m_t`$ in the estimate here.

Depending on the flavor structure, the $`ϵ`$ coupling might be limited only by neutrino mass measurements and might, therefore, be expected to be extremely small. It is clear that the corresponding gluino lifetime could easily be long enough to have cosmological significance. There is, for instance, the possibility that the gluino-gluon bound state could traverse cosmological distance scales before decaying and, if sufficiently energetic, could contribute through its decay products to the ultra-high-energy cosmic rays. We leave delayed calculation of some of the possible effects discussed here to future investigations.

Acknowledgements

This work was supported in part by the US Department of Energy under grant DE-FG02-96ER-40967. One of the authors, (LC), would like to acknowledge the hospitality of the University of Vienna and the High Energy Physics Institute of the Austrian Academy of Sciences where the initial discussion of the ideas presented here occurred. Discussions with Alfred Bartl as well as some conversations on the gluino decay modes of the current paper with Thomas Gajdosik are especially acknowledged. It has been brought to our attention that gluino decays through bilinear R parity violation (as opposed to the trilinear violation treated here) have also been recently considered .


text:
# Double Beta Decay and the Absolute Neutrino Mass Scale11footnote 1 Talk presennted at NuFact 03, 5th International Workshop on Neutrino Factories & Superbeams, 5–11 June 2003, Columbia University, New York.

## Abstract

After a short review of the current status of three-neutrino mixing, the implications for the values of neutrino masses are discussed. The bounds on the absolute scale of neutrino masses from Tritium $`\beta `$-decay and cosmological data are reviewed. Finally, we discuss the implications of three-neutrino mixing for neutrinoless double-$`\beta `$ decay.

The marvelous recent results of neutrino oscillation experiments have given us important information on neutrino mixing. The data of solar neutrino experiments and of the KamLAND long-baseline $`\overline{\nu }_e`$ disappearance experiment show $`\nu _e\nu _\mu ,\nu _\tau `$ transitions generated by the squared-mass difference $`\mathrm{\Delta }m_{\mathrm{SUN}}^2`$ in one of the two ranges hep-ph/0212129

$$5.1\times 10^5<\mathrm{\Delta }m_{\mathrm{SUN}}^2<9.7\times 10^5(\text{LMA-I}),1.2\times 10^4<\mathrm{\Delta }m_{\mathrm{SUN}}^2<1.9\times 10^4(\text{LMA-II}),$$
(1)
at 99.73% C.L., with best-fit value $`\mathrm{\Delta }m_{\mathrm{SUN}}^{2\mathrm{bf}}6.9\times 10^5`$ (we measure squared-mass differences in units of eV2). The effective solar mixing angle $`\vartheta _{\mathrm{SUN}}`$ is constrained at 99.73% C.L. in the interval hep-ph/0212129

$$0.29<\mathrm{tan}^2\vartheta _{\mathrm{SUN}}<0.86,$$
(2)
with best-fit value $`\mathrm{tan}^2\vartheta _{\mathrm{SUN}}^{\mathrm{bf}}0.46`$. The results of atmospheric neutrino experiments and of the K2K long-baseline $`\nu _\mu `$ disappearance experiment indicate $`\nu _\mu \nu _\tau `$ transitions generated by the squared-mass difference $`\mathrm{\Delta }m_{\mathrm{ATM}}^2`$ in the 99.73% C.L. range hep-ph/0303064

$$1.4\times 10^3<\mathrm{\Delta }m_{\mathrm{ATM}}^2<5.1\times 10^3,$$
(3)
with best-fit value $`\mathrm{\Delta }m_{\mathrm{ATM}}^{2\mathrm{bf}}2.6\times 10^3`$. The best-fit effective atmospheric mixing angle $`\vartheta _{\mathrm{ATM}}`$ is maximal, $`\mathrm{sin}^22\vartheta _{\mathrm{ATM}}^{\mathrm{bf}}1`$, with the 99.73% C.L. lower bound hep-ph/0303064

$$\mathrm{sin}^22\vartheta _{\mathrm{ATM}}>0.86.$$
(4)
These evidences of neutrino mixing are nicely accommodated in the minimal framework of three-neutrino mixing, in which the three flavor neutrinos $`\nu _e`$, $`\nu _\mu `$, $`\nu _\tau `$ are unitary linear combinations of three neutrinos $`\nu _1`$, $`\nu _2`$, $`\nu _3`$ with masses $`m_1`$, $`m_2`$, $`m_3`$, respectively (see Ref. BGG-review-98 ). Figure 1 shows the two three-neutrino schemes allowed by the observed hierarchy $`\mathrm{\Delta }m_{\mathrm{SUN}}^2\mathrm{\Delta }m_{\mathrm{ATM}}^2`$, with the massive neutrinos labeled in order to have

$$\mathrm{\Delta }m_{\mathrm{SUN}}^2=\mathrm{\Delta }m_{21}^2,\mathrm{\Delta }m_{\mathrm{ATM}}^2|\mathrm{\Delta }m_{31}^2||\mathrm{\Delta }m_{32}^2|.$$
(5)
The two schemes in Fig. 1 are usually called “normal” and “inverted”, because in the normal scheme the smallest squared-mass difference is generated by the two lightest neutrinos and a natural neutrino mass hierarchy can be realized if $`m_1m_2`$, whereas in the inverted scheme the smallest squared-mass difference is generated by the two heaviest neutrinos, which are almost degenerate for any value of the lightest neutrino mass $`m_3`$.

Solar neutrino oscillations depend only on the first row $`U_{e1}`$, $`U_{e2}`$, $`U_{e3}`$ of the mixing matrix, and the hierarchy $`\mathrm{\Delta }m_{\mathrm{SUN}}^2\mathrm{\Delta }m_{\mathrm{ATM}}^2`$ implies that neutrino oscillations generated by $`\mathrm{\Delta }m_{\mathrm{ATM}}^2`$ depend only on the last column $`U_{e3}`$, $`U_{\mu 3}`$, $`U_{\tau 3}`$ of the mixing matrix. Hence, the only connection between solar and atmospheric neutrino oscillations is due to the element $`U_{e3}`$. The negative result of the CHOOZ long-baseline $`\overline{\nu }_e`$ disappearance experiment implies that electron neutrinos do not oscillate at the atmospheric scale and $`|U_{e3}|`$ is small: $`|U_{e3}|^2<5\times 10^2`$ at 99.73% C.L. Fogli:2002pb . Therefore, solar and atmospheric neutrino oscillations are practically decoupled Bilenky:1998tw  and the effective mixing angles in solar, atmospheric and CHOOZ experiments can be related to the elements of the three-neutrino mixing matrix by (see also Ref. hep-ph/0212142 )

$$\mathrm{sin}^2\vartheta _{\mathrm{SUN}}=\frac{|U_{e2}|^2}{1|U_{e3}|^2}\mathrm{sin}^2\vartheta _{\mathrm{ATM}}=|U_{\mu 3}|^2\mathrm{sin}^2\vartheta _{\mathrm{CHOOZ}}=|U_{e3}|^2.$$
(6)
Taking into account all the above experimental constraints, we have reconstructed the best-fit and allowed ranges for the elements of the mixing matrix (see Ref. hep-ph/0306001  for a reconstruction taking into account the correlations among the mixing parameters):

$$U_{\mathrm{bf}}\left(\begin{array}{ccc}0.83& 0.56& 0.00\\ 0.40& 0.59& 0.71\\ 0.40& 0.59& 0.71\end{array}\right),|U|\left(\begin{array}{ccc}0.710.88& 0.460.68& 0.000.22\\ 0.080.66& 0.260.79& 0.550.85\\ 0.100.66& 0.280.80& 0.510.83\end{array}\right).$$
(7)
Such mixing matrix, with all elements large except $`U_{e3}`$, is called “bilarge”. It is very different from the quark mixing matrix.

The absolute scale of neutrino masses is not determined by the observation of neutrino oscillations, which depend only on the differences of the squares of neutrino masses. Figure 2 shows the allowed ranges (between the dashed and dotted curves) for the neutrino masses obtained from the allowed values of the oscillation parameters in Eqs. (1)–(4), as functions of the lightest mass in the normal and inverted three-neutrino schemes. The solid lines correspond to the best fit values of the oscillation parameters. One can see that at least two neutrinos have masses larger than about $`7\times 10^3\mathrm{eV}`$.

The most sensitive known ways to probe the absolute values of neutrino masses are the observation of the end-point part of the electron spectrum in Tritium $`\beta `$-decay, the observation of large-scale structures in the early universe and the search for neutrinoless double-$`\beta `$ decay, if neutrinos are Majorana particles (see Ref. Bilenky:2002aw ; we do not consider here the interesting possibility to determine neutrino masses through the observation of supernova neutrinos).

Up to now, no indication of a neutrino mass has been found in Tritium $`\beta `$-decay experiments, leading to an upper limit on the effective mass

$$m_\beta =\sqrt{\underset{k}{}|U_{ek}|^2m_k^2}$$
(8)
of $`2.2\mathrm{eV}`$ at 95% C.L. hep-ex/0210050 , obtained in the Mainz and Troitsk experiments. After 2007, the KATRIN experiment hep-ex/0109033  will explore $`m_\beta `$ down to about $`0.20.3\mathrm{eV}`$. Figure 3 shows the allowed range (between the dashed curves) for $`m_\beta `$ obtained from the allowed values of the oscillation parameters in Eqs. (1)–(4), as a function of the lightest mass in the normal and inverted three-neutrino schemes. The solid line corresponds to the best fit values of the oscillation parameters. One can see that in the normal scheme with a mass hierarchy $`m_\beta `$ has a value between about $`3\times 10^3\mathrm{eV}`$ and $`2\times 10^2\mathrm{eV}`$, whereas in the inverted scheme $`m_\beta `$ is larger than about $`3\times 10^2\mathrm{eV}`$. Therefore, if in the future it will be possible to constraint $`m_\beta `$ to be smaller than about $`3\times 10^2\mathrm{eV}`$, a normal hierarchy of neutrino masses will be established.

The analysis of recent data on cosmic microwave background radiation and large scale structure in the universe in the framework of the standard cosmological model has allowed to establish an upper bound of about 1 eV for the sum of neutrino masses, which implies an upper limit of about 0.3 eV for the individual masses Spergel:2003cb ; astro-ph/0303076 . This limit is already at the same level as the sensitivity of the future KATRIN experiment. Let us emphasize, however, that the KATRIN experiment is important in order to probe the neutrino masses in a model-independent way,

A very important open problem in neutrino physics is the Dirac or Majorana nature of neutrinos. From the theoretical point of view it is expected that neutrinos are Majorana particles, with masses generated by effective Lagrangian terms in which heavy degrees of freedom have been integrated out (see Ref. Altarelli:2003vk ). In this case the smallness of neutrino masses is naturally explained by the suppression due to the ratio of the electroweak symmetry breaking scale and a high energy scale associated with the violation of the total lepton number and new physics beyond the Standard Model.

The best known way to search for Majorana neutrino masses is neutrinoless double-$`\beta `$ decay, whose amplitude is proportional to the effective Majorana mass

$$|m|=\left|\underset{k}{}U_{ek}^2m_k\right|.$$
(9)
The present experimental upper limit on $`|m|`$ between about 0.3 eV and 1.3 eV has been obtained in the Heidelberg-Moscow and IGEX experiments. The large uncertainty is due to the difficulty of calculating the nuclear matrix element in the decay. Figure 4 shows the allowed range for $`|m|`$ obtained from the allowed values of the oscillation parameters in Eqs. (1)–(4), as a function of the lightest mass in the normal and inverted three-neutrino schemes (see also Ref. Pascoli:2002qm ). If CP is conserved, $`|m|`$ is constrained to lie in a shadowed region. Finding $`|m|`$ in an unshaded strip would signal CP violation. One can see that in the normal scheme large cancellations between the three mass contributions are possible and $`|m|`$ can be arbitrarily small. On the other hand, the cancellations in the inverted scheme are limited, because $`\nu _1`$ and $`\nu _2`$, with which the electron neutrino has large mixing, are almost degenerate and much heavier than $`\nu _3`$. Since the solar mixing angle is less than maximal, a complete cancellation between the contributions of $`\nu _1`$ and $`\nu _2`$ is excluded, leading to a lower bound of about $`1\times 10^3\mathrm{eV}`$ for $`|m|`$ in the inverted scheme. If in the future $`|m|`$ will be found to be smaller than about $`1\times 10^3\mathrm{eV}`$, it will be established that either neutrinos have a mass hierarchy or they are Dirac particles. Many neutrinoless double-$`\beta `$ decay experiments are planned for the future, but they will unfortunately not be able to probe such small values of $`|m|`$, extending their sensitivity at most in the $`10^2\mathrm{eV}`$ range (see Ref. Bilenky:2002aw ).

In conclusion, we would like to emphasize that, although the recent years have been extraordinarily fruitful for neutrino physics, yielding important information on the neutrino mixing parameters, still several fundamental characteristics of neutrinos are unknown. Among them, the Dirac or Majorana nature of neutrinos, the absolute scale of neutrino masses, the distinction between the normal and inverted schemes and the existence of CP violation in the lepton sector are very important for our understanding of the new physics beyond the Standard Model.

I would like to thank Carlos Peña-Garay for enlightening discussions.


text:
# Electrostatic Engineering of Nanotube Transistors for Improved Performance

## Abstract

With decreasing device dimensions, the performance of carbon nanotube field-effect transistors (CNFETs) is limited by high Off currents except at low drain voltages. We show that an asymmetric design improves the performance, reducing Off-currents and extending the usable range of drain voltage. The improvement is most dramatic for ambipolar Schottky-barrier CNFETs. Moreover, this approach allows a single device to exhibit equally good performance as an n- or p-type transistor, by changing only the sign of the drain voltage. Even for CNFETs having ohmic contacts, an asymmetric design can greatly improve the performance for small-bandgap nanotubes.

The performance of carbon nanotube field-effect transistors (CNFETs) can be greatly improved in many respects by scaling the devices to smaller size . However, the improvements with smaller size are accompanied by the undesired effect of a lowered On-Off ratio at typical drain voltages. This restricts the range of usable drain voltage, which in turn limits the achievable On-currents. Most CNFETs to date operate as Schottky barrier (SB) CNFETs , and the issue has been studied in detail for such devices . But the problem occurs even for ohmic contacts, especially for small-bandgap tubes, as shown below.

Here, we propose a novel device design for CNFETs that can be scaled down in size for good turn-on performance without severe restrictions on the usable drain voltage. The key idea of the new design is to have large electric fields at the source contact but small fields at the drain, to suppress unwanted tunneling. A related approach has recently been demonstrated for Si-based SB-FETs .

For an ambipolar SB-CNFET, the asymmetric design can suppress either the p- or the n-type branch of the ambipolar transport characteristic, depending only on the sign of the drain voltage. Thus the same device can act as an excellent p- or n-type transistor, and the turn-on performance for both types is controlled by the electrostatics (the geometry of the contact and gate) at the source electrode. By choosing metals of different work function for the gates, it should be possible to fabricate complementary SB-CNFETs that have the desired alignment of transfer characteristics ($`I`$ vs. $`V_\mathrm{g}`$) for standard logic applications.

For a SB-CNFET, the asymmetric design solves the problem of Off-current that increases exponentially with drain voltage, so it allows larger On-currents. This is a critical issue as the device dimensions decrease . Moreover, even for a CNFET having ohmic contacts , e.g. to the valence band, suppressing the current into the conduction band can be essential when the nanotube (NT) bandgap is small.

Two examples of possible asymmetric device geometries are shown in Fig. 1. The first design, Fig. 1(a), relies on having a different thickness for the bottom oxide at the source and drain contacts. The second design, Fig. 1(b), employs a top gate close to the source contact but not the drain. Other ways of engineering the electric fields are possible, such as a sharp source electrode to focus the field at the contact, and a blunt drain electrode to reduce the field there.

To study the transport characteristics of these devices, we use a semiclassical model which has been described elsewhere . We assume ballistic transport within the NT (over the short distances of interest here) . For SB-CNFETs, the current is controlled by the rate of thermally assisted tunneling (at room temperature) through the SBs at the source and drain contact. We neglect charge on the NT, which is a good approximation for the Off-state and in the turn-on regime .

For concreteness, we focus on the asymmetric bottom gate device, Fig. 1(a). At the source contact the oxide thickness, $`t_{\mathrm{ox}}`$, is only 2 nm. CNFETs with symmetric source and drain contacts of such low oxide thickness have been fabricated and show very good turn-on performance . We first treat ideally ambipolar devices, where the metal Fermi level falls in the middle of the NT bandgap at each contact. The NT band gap is taken to be $`0.6`$ eV, corresponding to a diameter of $`1.4`$ nm. Other cases are discussed below.

The calculated transfer characteristics for a symmetric CNFET with $`t_{\mathrm{ox}}=2`$ nm are shown as dashed lines in Fig. 2(a). The quality of the turn-on performance can be quantified by the subthreshold slope, defined by $`S=(d\mathrm{log}_{10}I/dV_\mathrm{g})^1`$, where $`I`$ is the device current and $`V_\mathrm{g}`$ is the gate voltage. The value of $`S`$ for the symmetric CNFET of Fig. 2(a) is $`110`$ mV/decade. (This is already within a factor of 2 of the thermal limit of a conventional transistor, $``$60 mV/decade.) However, the ratio between On- and Off-current decreases with increased drain voltage $`V_\mathrm{d}`$. At $`V_\mathrm{d}=+0.7`$ V, the ratio is only two orders of magnitude, well below the range desired for transistors. This drain voltage effect has been investigated in detail for such symmetric CNFETs , where it represents an important limitation.

In contrast, the asymmetric design of Fig. 1(a) allows a high On/Off ratio even at higher $`V_\mathrm{d}`$, while preserving other good features of the behavior. This is shown by the solid lines in Fig. 2(a). At positive $`V_\mathrm{d}`$, the slope in the turn-on regime (e.g. $`V_\mathrm{g}0.3`$) is the same as for the symmetric device. However, the Off-current is much lower than for the symmetric device, and the On-Off ratio is greatly improved, to over 4 orders of magnitude at $`V_\mathrm{d}=+0.7`$ V.

The contributions of electrons and holes to the current are shown separately for one case in Fig. 2(a). For the asymmetric CNFET at positive $`V_\mathrm{d}`$, the hole current is suppressed, changing the behavior from ambipolar for a symmetric device to n-type for the asymmetric device. By merely reversing the sign of $`V_\mathrm{d}`$, one can instead suppress the electron current, making the same asymmetric CNFET behave as a p-type transistor with identical performance, as shown in Fig. 2(b).

The transfer characteristics ($`I`$ vs. $`V_\mathrm{g}`$) of the asymmetric device can be understood based on the calculated band bending shown in Fig. 3(a) for $`V_\mathrm{d}=+0.3`$ V. At large positive $`V_\mathrm{g}`$ ($`+0.5`$ V) the behavior is similar to a symmetric device — the SB at the source is sufficiently thin for electrons to be injected, and there is little or no barrier for them to be collected at the drain. Thus the current is relatively large \[see Fig. 2(a)\]. As $`V_\mathrm{g}`$ is reduced, the source SB becomes wider, until electron injection becomes negligible for $`V_\mathrm{g}+0.1`$ V.

For negative $`V_\mathrm{g}`$, while the electron current remains negligible, holes can be injected at the drain and are then easily collected at the source. This is the origin of the ambipolar characteristic (and of the undesirable Off-current) in symmetric devices . In our asymmetric device, however, the geometry is chosen so that the SB at the drain remains rather wide, suppressing hole tunneling. Thus the device shows purely n-type character.

At negative $`V_\mathrm{d}`$, the argument is reversed — electron transport is suppressed due to the barrier at the drain contact, while the hole current is as for a symmetric device. Thus by simply changing the sign of $`V_\mathrm{d}`$, we can operate the same device as either an excellent p- or n-type transistor, with a turn-on performance controlled by the source contact geometry. This is a key advantage of the new device design. In principle, complementary n- and p-type transistors based on ohmic contacts (to the conduction and valence band respectively) would give even better performance; but the need for both kinds of contacts presents a formidable obstacle to such a design at present.

The output characteristics ($`I`$ vs. $`V_\mathrm{d}`$) of the asymmetric and the symmetric CNFET are compared in Fig. 4. For the asymmetric device, the current starts to rise appreciable only for $`V_\mathrm{d}`$ half the NT bandgap. The lack of a linear regime of $`I`$ vs. $`V_\mathrm{d}`$ for the asymmetric device does not hinder digital/logic applications which rely on the plateau of saturating current. The plateaus are actually greatly improved for asymmetric CNFETs. For symmetric devices, these plateaus are limited by the onset of the drain leakage current .

The output characteristics can be understood by examining the band bending at fixed $`V_\mathrm{g}`$, Fig. 3(b). At $`V_\mathrm{g}=0.5`$ V, the SB at the source is sufficiently thin for high transmission. However, at low $`V_\mathrm{d}`$ ($`=+0.05`$ V) the electrons injected at the source contact cannot enter the drain contact due to the thick potential barrier . By increasing $`V_\mathrm{d}`$ the barrier at the drain contact is lowered and the injected electrons can be collected at the drain. Thus a $`V_\mathrm{d}`$ of about half the NT band gap is required for a significant flow of current (c.f. Fig. 4). With further increase of $`V_\mathrm{d}`$ the current saturates, being limited by the source or channel (both of which are controlled by $`V_\mathrm{g}`$ in the absence of short-channel effects) rather than by the drain.

So far we have focused on ambipolar SB-CNFETs; but ohmic contacts could provide further performance improvements . Ohmic contacts are most readily achieved for NTs having small bandgap , in which case we find that drain leakage current is still an issue, except at very small $`V_\mathrm{d}`$. Figure 5 shows calculations for a device having ohmic contacts to the valence band, and where the NT bandgap is 0.3 eV, as in Ref. . As expected, the subthreshold slope is excellent (65 mV/dec for $`t_{\mathrm{ox}}=2`$ nm). However, for a symmetric CNFET, the SB to the conduction band (i.e. the bandgap) is only $`0.3`$ eV. Thus positive $`V_\mathrm{g}`$ can induce substantial electron tunneling, leading to the behavior shown by dashed lines in Fig. 5. This electron tunneling is significant even for a 20 nm oxide; and for very thin oxides the effect is dramatic, as shown for $`t_{\mathrm{ox}}=2`$ nm.

For a CNFET having ohmic contacts, the leakage current can be suppressed by an asymmetric geometry, just as for the ambipolar devices described above. Thus, without excessively restricting $`V_\mathrm{d}`$, one can achieve a dramatic improvement of the On-Off ratio, suppressing the drain leakage current over a large range of $`V_\mathrm{g}`$. As thin oxides are necessary for high performance CNFETs, the asymmetric device design may play a key role even for devices based on ohmic contacts, and even more so for Schottky barrier transistors.

We thank Marko Radosavljević and Richard Martel for valuable discussions. S. H. thanks the Deutsche Forschungsgemeinschaft for financial support under the Grant number HE3292/2-1.