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# Temperature dependence of current self-oscillations and electric field domains in sequential tunneling doped superlattices

## I Introduction

Manifestations of vertical transport in weakly coupled semiconductor doped superlattices (SLs) include electric field domain formation,  multistability,  self-sustained current oscillations,  and driven and undriven chaos.  Stationary electric field domains appear in voltage biased SLs if the doping is large enough.  When the carrier density is below a critical value, self-sustained oscillations of the current may appear. They are due to the dynamics of the domain wall separating the electric field domains. This domain wall moves through the structure and is periodically recycled. The frequencies of the corresponding oscillation depend on the applied bias and range from the kHz to the GHz regime. Self-oscillations persist even at room temperature, which makes these devices promising candidates for microwave generation.  Numerical calculation of the voltage–doping SL phase diagram shows that only static electric field domains are possible for high enough SL doping. As the doping decreases, voltage windows where current self-oscillations are possible open up.  These windows may coalesce into a single one as doping is further lowered, and oscillations disappear below a critical doping value. Since doping is not a feasible control parameter, other quantities affecting carrier density should be used to observe these behaviors. Feasible control parameters are laser illumination in undoped SLs  (which behaves qualitatively as well doping), transverse magnetic fields,  and temperature  in doped SLs.

Despite its practical and theoretical interest, the effect of temperature on electric field domains  and current self-oscillations is still poorly understood. Early numerical calculations were performed with a fixed drift velocity corresponding to a fixed temperature.  Using the insight provided by these calculations and reasonable expectations on how drift velocity depends with temperature, the fact that oscillatory voltage windows widen as the temperature increases was explained.  More detailed experimental studies dealing with the influence of temperature on self-oscillations have appeared recently.  Experimental data show that raising the temperature is similar to lowering the SL doping. At low temperature a multiplicity of purely static states (corresponding to coexistence of low and high field domains in the SL) was observed. As the temperature increased, voltage windows corresponding to self-oscillations appeared and widened in the SL $`I`$$`V`$ characteristics.  Experimental data were interpreted by using the discrete drift model  with a fitted drift velocity.  These authors concluded that the peak-to-valley ratio in the negative differential mobility region of the drift velocity was crucial to understand the data. A model including both variation of the electron density in the wells and variation of the drift velocity with temperature was therefore needed.

In a recent paper, we have been able to derive discrete drift-diffusion (DDD) models, including boundary conditions, from microscopic sequential tunneling models.  By using our formulas for the field-dependent drift velocity at different temperatures (ranging from 0 to 175 K), we can compare numerical simulations of these simple discrete models with Wang et al’s experimental data. Our results show that increasing temperature facilitates current self-oscillations in the second plateau. Furthermore, our numerical results (based upon microscopically calculated drift velocities) agree with the available experimental data and explain them quantitatively. We explain qualitatively why regions of stationary states alternate with regions of self-oscillations in the temperature–voltage phase diagram. Finally and on the basis of our numerical simulations, we also explain why the frequency may have local maxima in the voltage intervals where self-oscillations occur. That the frequency may increase with voltage, while the average current simultaneously decreases is thus a consequence of our theory, not an anomaly.

The rest of this paper is as follows. Section II contains a brief description of the DDD model and a calculation of its transport coefficients and boundary conditions appropriate for Wang et al’s experimental sample. Results of numerical simulations of this model and comparison with experimental data are reported in Section III. Section IV contains our conclusions. A discussion of the qualitative theoretical analysis included in the experimental papers is presented in Appendix A.

## II Discrete drift-diffusion model

The main charge transport mechanism in a weakly coupled SL is sequential resonant tunneling. The characteristics of the samples experimentally studied in Ref.  are such that the macroscopic time scale of the self-sustained oscillations is larger than the tunneling time (defined as the time an electron needs to advance from one well to the next one). In turn, this latter time is much larger than the intersubband scattering time. Then tunneling across a barrier is a stationary process with well-defined Fermi-Dirac distributions at each well. These distributions depend on the instantaneous values of the electron density and potential drops and vary only on the longer macroscopic time scale. The tunneling current density across each barrier in the SL may be approximately calculated by means of the Transfer Hamiltonian method.  The resulting formulas can be used to calculate the transport coefficients and boundary conditions of the following DDD model:

$`{\displaystyle \frac{\epsilon }{e}}{\displaystyle \frac{dF_i}{dt}}+{\displaystyle \frac{n_iv(F_i)}{}}D(F_i){\displaystyle \frac{n_{i+1}n_i}{^2}}=J(t),`$ (1)
$`F_iF_{i1}={\displaystyle \frac{e}{\epsilon }}(n_iN_D^w).`$ (2)
In these equations, $`\epsilon `$, $`e`$ and $`N_D^w`$ are well permittivity, minus the electron charge and 2D doping in the wells, respectively. $`=d+w`$ is the SL period, where $`d`$ and $`w`$ are the widths of barriers and wells, respectively. Eq. (1) is Ampère’s law establishig that the total current density, $`eJ`$, is sum of displacement and tunneling currents. The latter consists of a drift term, $`en_iv(F_i)/`$, and a diffusion term, $`eD(F_i)(n_{i+1}n_i)/^2`$. We have adopted the convention (usual in this field) that the current density has the same direction as the flow of electrons. Eq. (1) holds for $`i=1,\mathrm{},N1`$. Eq. (2) is the Poisson equation, and it holds for $`i=1,\mathrm{},N`$. $`n_i`$ is the 2D electron number density at well $`i`$, which is singularly concentrated on a plane located at the end of the well. $`F_i`$ is minus an average electric field on a SL period comprising the $`i`$th well and the $`i`$th barrier (well $`i`$ lies between barriers $`i1`$ and $`i`$: barriers 0 and $`N`$ separate the SL from the emitter and collector contact regions, respectively).

Fig. 1 depicts the field-dependent drift velocity at different temperatures for SL parameter values of Ref. : 40 periods of 14 nm GaAs and 4 nm AlAs and well doping $`N_D^w=2\times 10^{11}`$ cm-2. It has been calculated from the microscopic tunneling current density by the procedure explained in Ref. . The only adjustable parameter in the sequential tunneling formulas is the Lorentzian half-width of the scattering amplitudes, $`\gamma `$. To estimate them, we have considered that the voltage difference, $`\mathrm{\Delta }V`$, between the peaks of two consecutive branches on the second plateau of the static $`I`$$`V`$ characteristic is

$`\mathrm{\Delta }Vϵ_{C3}ϵ_{C2}2\eta \gamma .`$ (3)
Here $`ϵ_{Ci}`$ is the $`i`$th energy level of a given well. For $`\gamma =0`$, the field profile on the second plateau corresponds to two coexisting electric field domains with fields $`(ϵ_{C2}ϵ_{C1})/[e(d+w)]`$ and $`(ϵ_{C3}ϵ_{C1})/[e(d+w)]`$. The domain walls corresponding to two adjacent branches in the $`I`$$`V`$ diagram are located in adjacent wells. Then the voltage difference should be $`\mathrm{\Delta }Vϵ_{C3}ϵ_{C2}`$. In the presence of scattering, resonant peaks have finite widths which we take as $`2\eta \gamma `$, thereby obtaining (3). $`2\eta `$ is an adjustable parameter of the order of unity . By using this formula and the measured current in Ref.  (Figs. 1, 2, and 3), we find $`\gamma =18`$ meV at 1.6 K and $`\gamma =23`$ meV at 140 K for $`\eta 0.6`$. Linear interpolation yields the temperature dependence of $`\gamma `$ in the range we are interested in.

Notice that the first peak of the velocity in Fig. 1 rapidly disappears as the temperature increases for this particular sample. This result might change if we assume different scattering amplitudes for each of the two first subbands of the wells. Moreover, the different extrema of the velocity curve shift to lower field values as the temperature increases. Thus formation of electric field domains and current self-oscillations are expected for voltages on the second plateau and higher. Multistable solution branches of the current–voltage characteristic curve should also shift to lower voltages and higher currents as the temperature increases, as observed in experiments.  These effects could not be obtained from the fitted drift velocity in Ref. . As the diffusion coefficient decreases very rapidly with field, we can safely set $`D0`$ in our DDD model for the experimentally observed voltage range. The relevant model is thus the well-known discrete drift model of Refs.  with the drift velocity deduced from a microscopic calculation of the current plus boundary conditions  (see Fig. 1).

To complete the description of our model, we need to specify initial, boundary and bias conditions. The dc voltage bias condition is

$`{\displaystyle \underset{i=1}{\overset{N}{}}}F_i=V.`$ (4)
Given that $`D(F_i)0`$, we need only one boundary condition specifying $`F_0`$ (the field at the contact region). We will assume that there is an excess electron density in the first well due to tunneling from the highly doped contact region,

$`n_1=(1+c)N_D^w.`$ (5)
For an appropriately chosen dimensionless positive constant $`c`$, this condition selects recycling of charge monopole waves as the mechanism for self-sustained oscillations of the current.  The same behavior can be obtained from more elaborated boundary condition for the microscopic tuneling current between the emitter and the neighboring well  provided contact doping is sufficiently high (ohmic behavior). Given the uncertainties inherent to contact specification, we have preferred to use the phenomenological boundary condition (5) instead.

## III Numerical simulations and comparison with experiments

In this Section, we shall numerically simulate the discrete drift model for different values of temperature. From formula (1) and (2), considering D=0:

$`{\displaystyle \frac{\epsilon }{e}}{\displaystyle \frac{dF_i}{dt}}+{\displaystyle \frac{v(F_i)}{}}\left[N_D^w+{\displaystyle \frac{\epsilon }{e}}(F_iF_{i1})\right]=J(t),`$ (6)
$`{\displaystyle \underset{i=1}{\overset{N}{}}}F_i={\displaystyle \frac{V}{}}.`$ (7)
The corresponding drift curves are chosen among those depicted in Fig. 1 and the boundary condition will be (5) with $`c=10^3`$.

A first interesting conclusion can be drawn effortlessly from an analytical upper bound of the critical doping above which there are stable static electric field domain branches:

$`N_{Dc}^w=\epsilon v_m{\displaystyle \frac{F_mF_M}{e(v_Mv_m)}}.`$ (8)
In this formula, $`F_M`$ and $`F_m`$ are the values of the electric field which correspond to the maximum and minimum of the drift velocity ($`v_M`$ and $`v_m`$) on the second plateau. The temperature dependence of this critical doping is plotted in Fig. 2. We observe that the critical doping increases with temperature, indicating that the voltage range for which self-oscillations exist increases as temperature does. In particular, Fig. 2 predicts a transition temperature at around 93 K whereas about 140 K is experimentally measured.  Despite the fact that the bound (8) is only a rough approximation, the agreement is rather good. We shall see below that the agreement improves when complete simulations of the DDD model are carried out.

Results of our simulations are presented in Figures 3 and 4, corresponding to a 40-well SL with $`d=4`$ nm, $`w=14`$ nm, and $`N_D^w=2\times 10^{11}`$cm-2. Fig. 3 shows the time averaged current–voltage characteristics of such a SL for temperatures ranging from 110 to 150 K. In this temperature range, there are voltage intervals (with a flat form) in which the SL current is stationary interspersed in voltage intervals of current self-oscillations corresponding to recycling of charge monopoles. This agrees with experimental results reported by Wang et al.  For temperatures lower than 110 K or higher than 250 K, the ranges of self-oscillations disappear. These figures are similar to those reported in Li et al’s experiments.

We observe that the $`I`$$`V`$ curve presents intervals in which the average current increases with voltage, followed by intervals in which the average current decreases. At lower temperatures the intervals of increasing current are wider whereas the opposite occurs at higher temperatures. Correspondingly, Fig. 4 shows the frequency of the self-oscillations as a function of voltage. The frequency of the self-oscillations in such an interval starts increasing but it drops to a smaller value than the initial one at the upper limit of the interval. The amplitude of the self-oscillations (not shown here) vanishes at the upper and lower limits of each voltage interval. This suggests that the branches of self-oscillations begin and end at supercritical Hopf bifurcations. As the temperature increases, the region of negative differential mobility in Fig. 1 is smoother and the frequency of the self-oscillations increases (see Fig. 4). In the opposite temperature range, at low temperatures, the electric field profiles consist of basically two stationary domains joined by a domain wall. The $`I`$$`V`$ characteristic curve has multiple branches corresponding to stationary domains with the domain wall located at different wells. This situation resembles that obtained as voltage and doping are varied, provided doping and reciprocal of temperature are assimilated. In Ref.  the phase diagram doping–voltage of a doped SL was calculated. At low doping (high temperature), the electric field inside the SL is almost homogeneous and stationary. Above a critical value, branches of self-oscillations appear. In this region, there are voltage intervals of stationary electric field profiles separated by intervals of self-oscillations. The latter arise and disappear (typically) as Hopf bifurcations from stationary states. Above a certain doping (low temperature), the intervals of self-oscillations vanish and only stationary states (consisting of two electric field domains separated by a domain wall) remain. Notice in Fig. 4 that there are voltage intervals where the oscillation frequency increases with voltage, while the average current decreases with voltage. This behavior was dubbed anomalous by Wang et al,  although it is conveniently explained by the discrete drift model equations as shown by our present simulations. A qualitative explanation of this behavior follows.

First of all, it can be observed in the simulations that the maximum current during one oscillation period does not vary too much, while the minimum current drops precipituously with voltage; see the insets in Fig. 5. This rapid drop of the minimum current and the approximate invariance of the maximum current can be understood from an asymptotic analysis:  the current approximately follows part of the velocity curve, $`eN_D^wv(F)/`$, during the motion of a monopole. The monopole is created when the current surpasses the maximum value $`eN_D^wv_M/`$. Then the current decreases with time until either the monopole exits at the receiving contact or the minimum value $`eN_D^wv_m/`$ is reached. The first possibility is attained at low voltages, the second one at high voltages. The current oscillation starts with zero amplitude at the lower end of a voltage interval, so that the current does not depart too much from its maximum value. As the voltage increases, the minima of the current at each oscillation period decrease. What about the dependence of frequency with voltage? It can be shown  that the oscillation period $`T_p`$ may be estimated from the following formula:

$$T_p=\frac{}{v_{mon}}MT_f\left(\frac{v_M}{v_{mon}}1\right).$$
(9)
Here $`M`$ is such that $`NM`$ represents the number of wells traversed by the charge monopole during one oscillation period, $`v_{mon}`$ is its average velocity and $`T_f`$ is the monopole formation time (which is an increasing function of $`M`$ ). Now, $`M`$ decreases with voltage owing to the dc bias condition,  so that the number of wells traversed by a monopole grows as the voltage increases (see Fig. 5). This means that the first term in (9) decreases with voltage and the second one increases with voltage (it becomes less negative). Thus there is a competition between these two mechanisms: the first tries to make the oscillation period decrease with voltage (therefore the oscillation frequency increases with voltage), while the second term has the opposite effect. Near the lowest voltage of an interval for which there are oscillations, $`v_{mon}v_M`$, and the first term of Eq. (9) dominates. As the voltage increases, the oscillation amplitude increases and $`v_{mon}`$ decreases, so that the second term becomes more important. Of course whether the maximum of the frequency is reached immediately or not cannot be said from our rough argument. Still, the results of our simulations show conclusively that the oscillation frequency may reach a single maximum at voltage intervals where the current oscillates.

## IV Conclusions

Starting from a microscopic sequential tunneling model of transport in weakly coupled SL, we have derived the field-dependent drift velocity for a doped 14/4 SL at temperatures ranging from 0 to 175K. We found that the first plateau rapidly disappears as the temperature increases, and therefore we can set the diffusivity to zero in our DDD model to study the second plateau. Our numerical simulations show that stable solutions change from stationary field profiles with two coexisting electric field domains at low temperature to recycling moving monopoles giving rise to current self-oscillations at higher temperature. Voltage windows in the $`I`$$`V`$ diagram appear and widen as temperature increases. We observe as well an intrincate behavior of the oscillation frequency as a function of the DC voltage for different temperatures. These findings agree with and explain the experimental data reported by Wang et al.

## ACKNOWLEDGMENTS

This work was supported by the Spanish DGES through grants PB98-0142-C04-01 and PB96-0875, and by the European Union TMR contracts ERB FMBX-CT97-0157 and FMRX-CT98-0180.

## A Wang et al’s theoretical explanations

Theoretical interpretation of experimental results in Refs.  is based upon a model proposed earlier by X.-R. Wang and Q. Niu (WN).  Their model is mathematically analogous to an earlier model of Laikhtman.  It consists of a system of rate equations:

$`{\displaystyle \frac{dq_i}{dt}}=I_{i1}(V_{i1})I_i(V_i),`$ (A1)
$`V_iV_{i1}=kq_i,`$ (A2)
$`{\displaystyle \underset{i=0}{\overset{N}{}}}V_i=V,`$ (A3)
with $`i=1,\mathrm{}N`$ . Eq. (A1) is charge continuity equation for the excess 2D electron charge density at the $`i`$th well, $`q_i`$ (WN used the notation $`n_i`$ instead of $`q_i`$). $`I_i(V_i)`$ is the tunneling current across the $`i`$th barrier, which depends only on the potential drop there, $`V_i=\mu _i\mu _{i+1}`$, where $`\mu _i`$ is the chemical potential at the $`i`$th well. (A2) is the Poisson equation with $`k=4\pi l^2/\epsilon `$, $`l=d+w`$. Lastly, (A3) is the dc voltage bias condition. The function $`I_i(V_i)`$ is in fact a piecewise linear N-shaped function common for all wells, $`I(V_i)`$; see Fig. 3 of Ref. .

Before commenting on this model, it is convenient to simplify it by eliminating the charge densities, $`q_i`$. Notice that (A1) and (A2) imply the usual Ampère’s law

$`k^1{\displaystyle \frac{dV_i}{dt}}+I_i(V_i)=,`$ (A4)
where $`i=0,1,\mathrm{},N`$ and $`(t)`$ is the total current.  Thus the model consists of $`N+2`$ equations, (A3) and (A4) for $`N+2`$ unknowns, $`V_i`$, $`i=0,1,\mathrm{},N`$ and $``$. The current $``$ can be eliminated by adding all equations (A4) and using that the bias (A3) is independent of time. The result is the following mean-field model:

$`{\displaystyle \frac{dV_i}{dt}}={\displaystyle \frac{k}{N+1}}{\displaystyle \underset{j=0}{\overset{N}{}}}[I_i(V_i)I_j(V_j)],i=0,\mathrm{},N,`$ (A5)
$`={\displaystyle \frac{1}{N+1}}{\displaystyle \underset{j=0}{\overset{N}{}}}I_i(V_i).`$ (A6)
Eq. (A5) is reminiscent of the problem of synchronization of coupled oscillators of zero frequency at zero temperature with the total current playing the role of order,  parameter. The oscillators $`V_i`$ try to achieve a stationary state such that $`I_i(V_i)=`$, given appropriate properties of the functions $`I_i`$ (positive differential conductivity, $`dI_i/dV_i>0`$).

### 1 Critique of the WN model and its analysis

The main physical objection to the WN model is that the sequential tunneling current across a barrier, $`I_i`$, depends explicitly on the electron densities at adjacent wells, as well as on electrostatic potentials. This is made patent by microscopic derivations,  which are conspicuously absent in WN’s paper. One unphysical consequence is that WN’s results do not depend explicitly on well doping \[except that $`I_i(V_i)`$ might change in some unspecified ad hoc form with doping\]. However, experiments and theory show that stable static electric field domains are formed at large doping, whereas self-sustained current oscillations appear for carrier densities below a critical value.  Similarly, doping at the injecting contact (ignored in the WN model) selects the type of charge density wave (monopoles or dipoles) responsible for current self-oscillations.

WN’s mathematical study of their model contains a linear stability analysis of a given unspecified stationary state and several unproven statements (some of which are even incorrect). Let us be specific. WN claim that all eigenvalues $`\lambda `$ corresponding to inserting $`E_i=A_ie^{\lambda t}`$ in the linearized equations are real, which seems reasonable. However, later on, they claim that a time periodic solution (limit cycle) can appear via a Hopf bifurcation from a stationary state. This is an elementary error: a necessary condition of a Hopf bifurcation is that a pair of complex conjugate eigenvalues cross the imaginary axis. The argument they use (illustrated in their Figure 2) to “prove” the existence of a limit cycle rests on unproven assumptions and, anyway, is not valid in more than two dimensions. In fact, they claim that there exists a large enough region about an unstable stationary state which is invariant under the flow, because the potential difference between two adjacent wells cannot exceed the applied bias. But no one has proved that this model (not to be confounded with physical reality!) posesses such desirable property. Furthermore, if there is only one stationary state and it becomes unstable by changing a control parameter, it will typically do so by having one of its eigenvalues changing from negative to positive values. (Recall that all eigenvalues are real). Then the bifurcating solution will typically (codimension one) be stationary. Thus the situation of WN’s figure 2 is unrealistic: inside the attractive region depicted, there should be another stationary (atracting) fixed point. Other more exotic possibilities are that the flow escapes to decidedly unphysical fixed points having some negative $`V_i`$ or that it wanders chaotically between different unstable fixed points.

### 2 Anomalies

Wang et al  gave an explanation for the fact that the self-oscillation frequency may increase with increasing bias while, at the same time, the mean current decreases. This allegedly anomalous behavior has been explained by means of the discrete drift model in Section III. On the other hand, Wang et al’s explanations of the “anomaly” are based on the claim that Equations (A4) with constant total current $``$ can have a limit cycle. They also give an estimate of its frequency. These arguments are clearly erroneous. In fact, all equations in (A4) are uncoupled if $``$ is a constant. Then (A4) is a one-dimensional autonomous dynamical system, which cannot have limit cycles among its solutions.


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# Surfaces with 𝑝_𝑔=𝑞=3

## 1. Introduction

Let $`X`$ be a smooth minimal complex surface of general type. The smallest possible value of the Euler –Poincaré characteristic $`\chi (X)=1+p_g(X)q(X)`$ is $`1`$, and for $`\chi (X)=1`$ one has the bounds $`1K_X^29`$. If, in addition, the surface is irregular, i.e. $`q(X)>0`$, then one also has $`K_X^22p_g(X)`$ (cf. \[De\]), so that $`p_g(X)4`$. The limit case $`p_g(X)=4`$ corresponds to the product of two curves of genus $`2`$ (cf. \[Be2\]). Here we consider the case $`q(X)=3`$ (cf. Theorem 2.2) and prove that $`X`$ is either the symmetric product of a curve of genus $`3`$ ($`K_X^2=6`$) or a free $`_2`$quotient of the product of a curve of genus 3 and a curve of genus 2 ($`K_X^2=8`$). Both surfaces have already been described in \[CCM\], where it is also shown that the former is the only example with $`K_X^2=6`$ and the latter is the only example with a pencil of curves of genus 2.

However, our approach is independent of the results of \[CCM\], and, as far as we know, it is a new one in the classification of surfaces of general type. We are able to identify the surfaces by looking at the locus $`V^1(X):=\{P\text{Pic}^0(X)|h^1(P)>0\}`$, whose properties have been described very precisely by several authors (cf. \[GL1\], \[GL2\], \[Be1\], \[Si\], \[EL\]). Roughly speaking, if $`V^1(X)`$ is $`0`$dimensional we prove that $`X`$ is the symmetric product of a curve of genus 3 by using a cohomological characterization of theta divisors, due to the first author (cf. Theorem 2.9). If instead $`V^1(X)`$ has positive dimension, then we show the existence of a pencil of curves of genus 2 by using the infinitesimal description of $`V^1(X)`$ (cf. \[GL1\]) and the Castelnuovo –de Franchis Theorem. As a byproduct of the classification, we obtain a description of the moduli space of surfaces of general type with $`p_g=q=3`$ (cf. Corollary 2.4) and we determine the degree of the bicanonical map (cf. Corollary 2.3).

### Acknowledgements

Gian Pietro Pirola has informed us that he has also proven our main result Theorem 2.2. His proof (\[Pi\]) uses different methods, based on the techniques and results of \[CCM\].

We are indebted to Margarida Mendes Lopes for drawing our attention to the problem of classifying surfaces of general type with $`p_g=q=3`$, for several useful conversations on this subject and for pointing out some inaccuracies in an earlier version of this paper.

This research originated during a visit to Pisa of the first author, supported by the program “Short term mobility” of G.N.S.A.G.A. of C.N.R.

### Notations and conventions

We work over the complex numbers; all varieties are projective. We use the standard notation of algebraic geometry; we just recall here the notation for the invariants of a surface $`X`$: $`K_X`$ is the canonical class, $`p_g(X)=h^0(X,K_X)`$ the geometric genus and $`q(X)=h^1(X,𝒪_X)`$ the irregularity. An irrational pencil of genus $`g`$ on a surface $`X`$ is a fibration $`p:XB`$ with $`B`$ a smooth curve of genus $`g>0`$.

## 2. The classification theorem

Throughout the paper we make the following assumption:

###### Assumption 2.1.

$`X`$ is a smooth minimal complex projective surface of general type with $`p_g(X)=q(X)=3`$.

We denote by $`A`$ the Albanese variety of $`X`$ and by $`a:XA`$ the Albanese map. We also assume that we have fixed a Kähler metric on $`X`$, so that for every $`P\text{Pic}^0(X)`$ and $`i0`$ there is an antilinear isomorphism $`H^i(X,P)H^0(X,\mathrm{\Omega }_X^i(P))`$ (cf. \[GL1\], 2.5).

Here are two examples of surfaces satisfying Assumption 2.1:

Example 1. Let $`C`$ be a smooth curve of genus $`3`$. Then the symmetric product of $`C`$ is a surface $`X`$ with $`K_X^2=6`$ satisfying Assumption 2.1. Let $`\text{Pic}^2(C)`$ denote the subset of $`\text{Pic}(C)`$ consisting of the line bundles of degree 2 and let $`\beta :X\text{Pic}^2(C)`$ be the map that sends an unordered pair $`\{p,q\}X`$ to the linear equivalence class of $`p+q`$. The image $`D`$ of $`\beta `$ is a principal polarization by \[LB\], Corollary 11.2.2. By the Riemann’s Singularity Theorem (cf. \[LB\], Theorem 11.2.5) $`D`$ is smooth if $`C`$ is not hyperelliptic, while it has a double point at the canonical class if $`C`$ is hyperelliptic. By Riemann–Roch on $`C`$, $`\beta `$ is $`1`$to$`1`$ if $`C`$ is not hyperelliptic, while if $`C`$ is hyperelliptic it contracts to a singular point of type $`A_1`$ the $`2`$curve of $`X`$ corresponding to the canonical series. In either case $`D`$ is the canonical model of $`X`$. It follows that $`A`$ is the Jacobian of $`C`$ and that, up to the choice of an identification of $`\text{Pic}^2(C)`$ with $`\text{Pic}^0(C)`$, $`\beta `$ is the Albanese map of $`X`$.

Example 2. Let $`C_1`$ be a curve of genus $`2`$ with an elliptic involution $`\sigma _1`$ and $`C_2`$ a curve of genus $`3`$ with a free involution $`\sigma _2`$. We write $`B_1:=C_1/<\sigma _1>`$ and $`B_2:=C_2/<\sigma _2>`$. The curve $`B_1`$ has genus $`1`$ and $`B_2`$ has genus $`2`$. We let $`_2`$ act freely on the product $`C_1\times C_2`$ via the involution $`\sigma _1\times \sigma _2`$. The quotient surface $`X:=(C_1\times C_2)/_2`$ is a surface with $`K_X^2=8`$ satisfying Assumption 2.1. The projections of $`C_1\times C_2`$ onto $`C_1`$ and $`C_2`$ induce fibrations $`p_i:XB_i`$, $`i=1,2`$. The singular fibres of $`p_1`$ are two double fibres with smooth support, occurring at the branch points of $`C_1B_1`$, while the fibres of $`p_2`$ are all smooth. The Albanese variety of $`X`$ is isogenous to the product of the Jacobians of $`B_1`$ and $`B_2`$.

Our aim is to prove the following:

###### Theorem 2.2.

The possibilities for a smooth minimal surface $`X`$ with $`p_g(X)=q(X)=3`$ are the following:

* $`K_X^2=6`$ and $`X`$ is the surface of Example 1;
* $`K_X^2=8`$ and $`X`$ is the surface of Example 2.

Before proving Theorem 2.2 we deduce some consequences from it.

###### Corollary 2.3.

The bicanonical map of a minimal surface of general type $`X`$ with $`p_g(X)=q(X)=3`$ has degree $`2`$.

###### Proof.

By Theorem 2.2 $`X`$ is either the surface of Example 1 or the surface of Example 2. In the former case the bicanonical map has degree 2 by Proposition 3.17 of \[CCM\]. In the latter case, the degree is 2 by Theorem 5.6 of \[Xi\]. ∎

###### Corollary 2.4.

The moduli space $``$ of surfaces of general type with $`p_g=q=3`$ has two irreducible connected components of dimensions respectively $`6`$ and $`5`$.

###### Proof.

By Theorem 2.2, $``$ is a disjoint union $`_6_8`$, where $`_\alpha :=\{[X]|K_X^2=\alpha \}`$. The sets $`_\alpha `$ are open since $`K^2`$ is a topological invariant, thus we only have to show that $`_6`$ and $`_8`$ are irreducible of dimension $`6`$ and $`5`$ respectively. The points of $`_6`$ are in one-to-one correspondence with the isomorphism classes of curves of genus 3, thus the result is well known in this case.

If $`[X]_8`$, then $`p_2:XB_2`$ is the only irrational pencil of genus 2 of $`X`$. This can be seen in several ways, for instance by observing that a base-point free pencil is determined uniquely by the span of its class in $`H^2(X,)`$ and that $`H^2(X,)`$, being of dimension 2, has only two isotropic lines, spanned by the classes of the general fibre of $`p_1`$ and $`p_2`$. It follows that the double cover $`C_1\times C_2X`$ is also determined uniquely, since it is the étale cover of $`X`$ that kills the monodromy of the pencil $`p_2:XB_2`$. So $`[X]`$ is determined by the choice, up to isomorphism, of a curve $`C_1`$ of genus $`2`$ with an elliptic involution $`\sigma _1`$ and of a curve $`C_2`$ of genus $`3`$ with a free involution $`\sigma _2`$. The pair $`(C_1,\sigma _1)`$ is determined by the quotient curve $`E_1:=C_1/\sigma _1`$, by the line bundle $`L`$ of degree 1 on $`E_1`$ such that $`\psi _{}𝒪_{C_1}=𝒪_{E_1}L^1`$, where $`\psi :C_1E_1`$ is the quotient map, and by the branch divisor $`D2L`$ of $`\psi `$. So, taking into account the action of the automorphism group of $`E_1`$, we see that $`(C_1,\sigma _1)`$ depends on 2 parametres. In addition, it is not difficult to write down an irreducible global family containing all the isomorphism classes of double covers of genus 3 of elliptic curves. Thus the isomorphism classes of the pairs $`(C_1,\sigma _1)`$ form an irreducible family of dimension 2. Analogously, the isomorphism class of $`(C_2,\sigma _2)`$ is determined by the genus 2 curve $`B_2:=C_2/\sigma _2`$ and by the choice of a $`2`$torsion line bundle $`L`$ of $`B_2`$. The pairs $`(B_2,L)`$ form a $`3`$dimensional irreducible family (cf. for instance \[LB\], Chapter 8, §3). ∎

We now turn to the proof of Theorem 2.2. Surfaces satisfying Assumption 2.1 are studied in section $`3`$ of \[CCM\], where it is proven that if $`K_X^2=6`$ then $`X`$ is the surface of Example 1. We recall some general facts from \[CCM\].

###### Proposition 2.5.

Let $`X`$ be a surface as in Assumption 2.1. Then:

* $`6K_X^29`$;
* the Albanese image of $`X`$ is a surface;
* if $`X`$ has an irrational pencil of genus $`g>1`$, then $`X`$ is the surface of Example 2.

###### Proof.

Statement i) follows from Miyaoka–Yau inequality $`K_X^29\chi `$ and from the inequality $`K_X^22p_g`$ of \[De\]. Statements ii) and iii) correspond to Proposition 3.1, i) and Theorem 3.23 of \[CCM\], respectively. ∎

The proof of Theorem 2.2 is based on the study of the set $`V^1(X):=\{P\text{Pic}^0(X)|h^1(P)>0\}`$. The sets $`V^i(Y):=\{P\text{Pic}^0(Y)|h^i(P)>0\}`$, for $`Y`$ a variety of any dimension, have been studied by Green and Lazarsfeld (\[GL1\], \[GL2\]), by Simpson (\[Si\]), and in the case of surfaces by Beauville (\[Be1\]). We recall here only those properties of $`V^1(X)`$ that we are going to use:

###### Theorem 2.6.

Let $`X`$ be a complex surface of maximal Albanese dimension. Then:

* $`V^1(X)`$ is a proper subvariety of $`\text{Pic}^0(X)`$;
* the irreducible components of $`V^1(X)`$ are translates of abelian subvarieties of $`\text{Pic}^0(X)`$ by torsion points;
* $`V^1(X)`$ has a component of dimension $`>1`$ iff $`X`$ has an irrational pencil of genus $`>1`$:
* Let $`PV^1(X)`$ be a point, let $`vH^1(X,𝒪_X)`$ be a nonzero vector and let $`\sigma H^0(X,\mathrm{\Omega }_X^1)`$ be the conjugate of $`v`$. If $`v`$ is in the tangent cone to $`V^1(X)`$ at $`P`$, then the map $`H^0(X,\mathrm{\Omega }_X^1(P))\stackrel{\sigma }{}H^0(X,\omega _X(P))`$ is not injective;
* Let $`PV^1(X)`$. Then $`\{P\}`$ is a component of $`V^1(X)`$ iff the map $`H^0(X,\mathrm{\Omega }_X^1(P))\stackrel{\sigma }{}H^0(X,\omega _X(P))`$ is injective for all nonzero $`\sigma H^0(X,\mathrm{\Omega }_X^1)`$.

###### Proof.

Statement i) is Theorem 1 of \[GL1\]. The fact that the components of $`V^1(X)`$ are translates of abelian subvarieties follows from Theorem 0.1 of \[GL2\] and the fact that the translation is by a torsion point follows from Theorem 4.2 of \[Si\]. Statement iii) follows from \[Be1\], Corollary 2.3. Statement iv) follows by combining Theorem 1.6, Lemma 2.3 and Lemma 2.6 of \[GL1\]. Statement v) is a consequence of Theorem 1.2, (1.2.3) of \[EL\]. ∎

If $`X`$ is the surface of Example 2, then the set $`V^1(X)`$ has a component of dimension 2 by Theorem 2.6, iii). On the other hand, using adjunction on $`A:=\text{Pic}^2(C)`$, it is easy to show that for the surface of Example 1 one has $`V^1(X)=\{𝒪_X\}`$. The results that follow show that the structure of $`V^1(X)`$ characterizes $`X`$.

###### Proposition 2.7.

If $`X`$ does not have an irrational pencil of genus $`>1`$, then the dimension of $`V^1(X)`$ is $`0`$.

###### Proof.

We remark first of all that, in view of the assumption, we have $`dimV^1(X)1`$ by Theorem 2.6, iii).

Assume now that there is a $`1`$dimensional component $`T`$ of $`V^1(X)`$. By Theorem 2.6, ii), $`T=T_0+Q`$, where $`T_0`$ is an abelian subvariety of $`\text{Pic}^0(X)`$ and $`Q`$ is a torsion point. Notice that $`QT_0`$, since by Proposition 4.1 of \[GL1\] $`𝒪_X`$ is an isolated point of $`V^1(X)`$. Fix a torsion point $`PT`$, denote by $`n`$ its order and assume that $`n`$ is minimal. This is the same as saying that if $`kPT_0`$ then $`kP=0`$. Let $`vH^1(𝒪_X)`$ be a nonzero vector tangent to $`T`$ and let $`\sigma H^0(\mathrm{\Omega }_X^1)`$ be the conjugate of $`v`$. The vector $`v`$ lies in the tangent cone to $`V^1(X)`$ at $`P`$ and therefore the map $`H^0(\mathrm{\Omega }_X^1(P))\stackrel{\sigma }{}H^0(\omega _X(P))`$ is not injective by Theorem 2.6, iv). Denote by $`\tau `$ a nonzero element in the kernel of this map. Let $`\pi :YX`$ be the connected étale cyclic cover associated to the finite subgroup $`<P>\text{Pic}^0(X)`$. The group $`<P>`$ can be naturally identified with the dual group of the Galois group $`G_n`$ of $`\pi `$, and $`\pi ^{}H^0(\mathrm{\Omega }_X^1(P))`$ is the eigenspace of $`H^0(\mathrm{\Omega }_Y^1)`$ on which $`G`$ acts via the character corresponding to $`P`$. Since $`\pi ^{}\sigma \pi ^{}\tau =0`$, by the Castelnuovo–de Franchis Theorem there exists a fibration $`q:YB`$ onto a curve of genus at least $`2`$, such that $`\pi ^{}\sigma `$ and $`\pi ^{}\tau `$ are pull-backs from $`B`$. The fibres of $`q`$ are integral curves of $`\pi ^{}\sigma `$. Since $`\pi ^{}\sigma `$ is $`G`$invariant, it follows that $`G`$ permutes the fibres of $`q`$ and thus induces a pencil $`p:XE:=B/G`$. More precisely, we have a commutative diagram:

$$\begin{array}{ccc}Y& \stackrel{\pi }{}& X\\ q& & p& & \\ B& \stackrel{\overline{\pi }}{}& E\end{array}$$

Let $`\overline{\sigma }`$ be the $`1`$form on $`B`$ such that $`\pi ^{}\sigma =q^{}\overline{\sigma }`$. By commutativity of the diagram, $`\overline{\sigma }`$ is $`G`$invariant and thus it is a pull-back from $`E`$. This shows that $`E`$ is not rational. In view of the assumptions, we conclude that $`E`$ has genus $`1`$. Since $`\sigma `$ is a pull-back from $`E`$, comparing the tangent spaces at the origin one sees that $`T_0=p^{}\text{Pic}^0(E)`$.

Now let $`\overline{\tau }`$ be the $`1`$form on $`B`$ such that $`\pi ^{}\tau =q^{}\overline{\tau }`$. By commutativity of the diagram, $`\overline{\tau }`$ is an eigenvector for $`G`$ with character corresponding to $`P`$. Since this character generates the dual group $`G^{}`$, the action of $`G`$ on $`B`$ is effective, i.e. $`\overline{\pi }:BE`$ is a $`G`$cover.

We claim that $`\overline{\pi }`$ is totally ramified, namely it does not factor through an étale cover of $`E`$. Assume otherwise, and denote by $`HG`$ the subgroup generated by the elements that do not act freely on $`B`$. Set $`Y^{}:=Y/H`$, $`B^{}:=B/H`$. Then we have a commutative diagram:

$$\begin{array}{ccc}Y^{}& \stackrel{\pi ^{}}{}& X\\ q^{}& & p& & \\ B^{}& \stackrel{\overline{\pi }^{}}{}& E\end{array}$$

where the maps are the obvious ones. In particular, $`\overline{\pi }^{}`$ is étale by construction. If we denote by $`d<n`$ the order of $`H`$, then the cover $`\pi ^{}`$ corresponds to the subgroup of $`\text{Pic}^0(X)`$ generated by $`dP`$. On the other hand, $`\pi ^{}`$ is obtained from $`\overline{\pi }^{}`$ by taking base change with $`p`$, so the subgroup of $`\text{Pic}^0(X)`$ corresponding to $`\pi ^{}`$ is actually a subgroup of $`p^{}\text{Pic}^0(E)`$, i.e. $`dPp^{}\text{Pic}^0(E)=T_0`$. This contradicts the minimality assumption on $`n`$, and we conclude that $`\overline{\pi }`$ is totally ramified. The $`G`$action on $`B`$ gives a decomposition $`\overline{\pi }_{}𝒪_B=𝒪_E_{\chi G^{}\{1\}}L_\chi ^1`$, where the $`L_\chi `$ are line bundles and $`L_\chi ^1`$ is the eigenspace of $`\overline{\pi }_{}𝒪_B`$ on which $`G`$ acts via the character $`\chi G^{}`$. Saying that $`\overline{\pi }`$ is totally ramified is the same as saying that $`\mathrm{deg}L_\chi >0`$ for every $`\chi G^{}\{1\}`$. The standard formulas for abelian covers (cf. \[Pa\], Proposition 4.1), give $`g(B)=g(E)+_{\chi G^{}\{1\}}h^0(\omega _EL_\chi )=1+_{\chi G^{}\{1\}}\mathrm{deg}L_\chi n`$. Denote by $`f`$ the genus of the general fibre of $`q`$. The Corollary on page 344 of \[Be2\] gives: $`\chi (Y)=n\chi (X)=n(f1)(g(B)1)(f1)(n1)`$. Thus we either have $`f=2`$ or $`n=2`$, $`f=3`$. Recall that $`f`$ is also the genus of the general fibre of $`p`$. Then $`f=2`$ is impossible: indeed by the Lemma on page 345 of \[Be2\] the equality $`3=q(X)=g(E)+f`$ would imply that $`X`$ is the product of $`E`$ with a curve of genus $`2`$, contradicting the fact that $`X`$ is of general type. So we are left with the case $`n=2`$, $`f=3`$. Notice that in this case we also have $`g(B)=2`$, so that $`2=\chi (Y)=(g(B)1)(f1)`$. So, again by the Corollary of page 344 of \[Be2\], the fibration $`q`$ is isotrivial with smooth fibres, and the only singular fibres of $`p`$ are two double fibres with smooth support, occurring at the two branch points of $`\overline{\pi }:BE`$. Hence by \[Se\], Theorem 2.1 and Remark 2.3, there exist a curve $`C_1`$ of genus $`3`$, a curve $`C_2`$ of genus $`g_2`$, and a finite group $`G`$ acting faithfully both on $`C_1`$ and on $`C_2`$ such that:

i) $`C_2/G`$ is isomorphic to $`E`$;

ii) the diagonal action on $`C_1\times C_2`$ defined by $`(x,y)\stackrel{g}{}(gx,gy)`$ is free;

iii) $`X`$ is isomorphic to the quotient $`(C_1\times C_2)/G`$, and the fibration $`p`$ corresponds to the map $`(C_1\times C_2)/GC_2/G=E`$ induced by the second projection $`C_1\times C_2C_2`$.

In addition, the following hold:

a) $`C_1/G`$ has genus $`2`$ (since $`q(X)=g(C_2/G)+g(C_1/G)=1+g(C_1/G)`$ by Proposition 2.2 of \[Se\]);

b) $`2(g_21)=|G|`$ (since $`2(g_21)=\chi (C_1\times C_2)=|G|\chi (X)=|G|`$).

Applying the Hurwitz formula to the quotient map $`C_1C_1/G`$ we see that $`G`$ has order $`2`$. Condition b) now implies $`g_2=2`$, hence $`X`$ is the surface of Example 2 and $`p`$ is the pencil $`p_1`$. Thus $`X`$ has also an irrational pencil of genus $`2`$, contrary to the assumptions. ∎

###### Proposition 2.8.

If $`X`$ does not have an irrational pencil of genus $`>1`$, then $`V^1(X)=\{𝒪_X\}`$.

###### Proof.

Let $`𝒪_XPV^1(X)`$. By Proposition 2.7, $`\{P\}`$ is a component of $`V^1(X)`$. It follows from Theorem 2.6, v) that for all $`0\sigma H^0(X,\mathrm{\Omega }_X^1)`$ the map $`H^0(X,\mathrm{\Omega }_X^1(P))\stackrel{\sigma }{}H^0(X,\omega _X(P))`$ is injective. Using Hodge theory with twisted coefficients it follows that the map induced by cup product

$$H^1(P)H^1(X,𝒪_X)H^2(P)$$

is non zero on (non zero) simple tensors. Therefore, by a result of H. Hopf (see \[ACGH\] pg. 108) $`h^2(P)h^1(P)+h^1(𝒪_X)1`$. Hence

$$1=\chi (𝒪_X)=\chi (P)=h^2(P)h^1(P)2.$$

This is the required contradiction. ∎

The last ingredient of the proof of Theorem 2.2 is the following result from \[Hac\]:

###### Theorem 2.9.

Let $`Z`$ be a smooth complex projective variety of dimension $`n`$, let $`A`$ be an abelian variety and let $`f:ZA`$ be a generically finite morphism such that $`f(Z)`$ is a divisor. Assume that:

i) $`h^0(Z,\mathrm{\Omega }_Z^i)=`$ $`\left(\genfrac{}{}{0pt}{}{n+1}{i}\right)`$ for $`0in`$;

ii) $`h^i(Z,\omega _Z(f^{}P))=0`$ for all $`𝒪_AP\text{Pic}^0(A)`$ and all $`i>0`$.

Then $`A`$ is principally polarized and $`f(Z)`$ is a theta divisor.

###### Proof.

Cf. \[Hac\], Corollary 3.4. ∎

###### Proof of Theorem 2.2.

By Proposition 2.5, iii), $`X`$ has an irrational pencil of genus $`>1`$ iff $`X`$ is the surface of Example 1.

If $`X`$ has no irrational pencil of genus $`>1`$, then $`V^1(X)=\{𝒪_X\}`$ by Proposition 2.8. Thus we can apply Theorem 2.9 to the Albanese map $`a:XA`$. It follows that $`A`$ is pricipally polarized and $`Y:=a(X)`$ is a theta divisor. It is well known (cf. \[LB\], Ch. 11, Corollary 8.2,b)) that an abelian threefold with an irreducible principal polarization is the Jacobian of a curve $`C`$ of genus $`3`$. As already explained in Example 1, the theta divisor is the canonical model of the symmetric product of $`C`$. Thus $`K_Y`$ is an ample Cartier divisor with $`K_Y^2=6`$. To finish the proof, it suffices to show that the map $`a:XY`$ is birational. If we denote by $`R`$ the divisorial part of the ramification locus of $`a`$, the adjunction formula gives $`K_X=a^{}K_Y+R`$. If we denote by $`d`$ the degree of $`a`$, then we have:

$$K_X^2=a^{}K_YK_X+RK_Xa^{}K_YK_X(a^{}K_Y)^2=6d$$

where the first inequality follows from the fact that $`K_X`$ is nef and the second one from the fact that $`a^{}K_Y`$ is nef. Since $`K_X^29`$ by Proposition 2.5, i), it follows that $`d=1`$ and $`X`$ and $`Y`$ are isomorphic. ∎

Christopher D. Hacon

Department of Mathematics

Sproul Hall 2208

University of California

Riverside, CA 92521-013 USA

hacon@math.ucr.edu

Rita Pardini

Dipartimento di Matematica

Università di Pisa

Via Buonarroti, 2

56127 Pisa, ITALY

pardini@dm.unipi.it


text:
# A Transient Instability in Thin Films of 𝑛CB Liquid Crystals

## Abstract

A transient surface instability is reported in thin nematic films of 5CB and 8CB, occurring near the nematic–isotropic phase transition. Although this instability leads to patterns reminiscent of spinodal dewetting, we show that it is actually based on a nucleation mechanism. Its characteristic wavelength does not depend markedly on film thickness, but strongly on the heating rate.

Following several studies on the spreading behavior of liquid crystals (LC) from the $`n`$CB homologous series , undulative instabilities have been observed in thin films of the LC 5AB4 , and 5CB  near the nematic–isotropic (N–I) phase transition. In the case of 5CB, these results have led to some discussion whether a spinodal dewetting mechanism driven by van der Waals forces is at work, as proposed by Vandenbrouck et al. , or wether the instability is driven by a pseudo–Casimir force based on the restricted spectrum of director fluctuations in thin nematic films . In the present paper, we show that neither is true for $`n`$CB thin films. Instead, the instability is caused by textures in the nematic film which largely determine the characteristic wavelength of the emerging pattern. This is not the case, however, in 5AB4.

5CB and 8CB were obtained from Merck KGaA (Darmstadt, Germany) and Frinton Laboratories Inc. (Vineland, NJ) respectively. They were used without further purification. Silicon wafers (100–oriented, p–(Boron–) doped) with a native oxide layer of 2 nm provided by Wacker Chemitronics (Burghausen, Germany) were used as solid substrates. The wafers were cut to samples approximately 1 cm2 in size and cleaned with a SnowjetTM, which uses a cold CO2 gas stream mixed with small particles of dry ice to remove particulate and organic contamination, followed by ultrasonication in ethanol, acetone, and hexane, subsequently.

Immediately after this cleaning process, LC films were spincast onto the samples from hexane solutions. Variation of concentration and spinning rate allows to deposit films of variable thickness. The preparation procedure was performed in a class 100 clean room environment at room temperature. Therefore, the films were initially in the nematic (5CB) or smectic A (8CB) state, respectively. Film thicknesses were recorded with an ellipsometer (Optrel GbR, Berlin, Germany). The samples were placed on a Linkam THMSG 600 heat stage (temperature control better than 0.1 C) and observed in-situ with a Zeiss Axiophot microscope equipped with a digital camera. Unless otherwise noted, no polarizers were used in the microscope setup.

Observations at room temperature showed films of 5CB and 8CB to be stable for hours at thicknesses ranging from 50 nm to 200 nm. Close to the nematic–isotropic transition temperature a surface undulation with a characteristic wavelength can be observed in both types of samples (see figure 1).

The observed undulation does not lead to a complete dewetting of the LC film but rather disappears once the phase transition is complete. The film becomes homogeneous again in the isotropic phase. Upon cooling, a similar transient instability occurs. Complete dewetting of the samples will occur only by heating a few degrees above the N–I transition, resulting in an array of isotropic droplets. Heating/ cooling of the sample between the nematic and isotropic phase can be repeated as indicated in fig. 2, every time resulting in nearly identical undulation patterns. The instability will develop only if the samples are heated or cooled. Keeping them at a fixed temperature close to the N–I phase transition will result in the nucleation of only a few holes in the film. These observations have been made for 5CB and for 8CB, at all film thicknesses investigated. The pattern was found to vanish faster for thicker films after completion of the phase transition.

Polarization microscopy confirmed the coincidence of the instability with the N–I phase transition.

Careful examination of the contrast profile of the images revealed the formation of nematic domains in 8CB films when heated above the smectic A–nematic transition temperature for the first time after preparation (cf. fig. 3). This domain pattern is preserved during the subsequent heating and cooling of the samples which was limited to a few degrees around the N–I transition temperature. On the left hand side of the figure, contrast is enhanced in order to clearly show the domain boundaries, while on the right hand side, the undulative instability occurring near the phase transition is superimposed on the domain boundary pattern. It is clearly seen from the overlay that the undulative pattern is strongly correlated with the domain boundary pattern.

Since films of 5CB are nematic at room temperature, the domain pattern observed immediately after preparation is less pronounced, but nevertheles present. As in the case of 8CB films, this pattern is not influenced during repeated temperature changes of the sample.

Since we have found that the undulations appear only when the sample temperature is swept through the phase transition, it is of interest to investigate the impact of the heating rate. We have thus varied the heating rate form 0.01 K/min to 10 K/min. As shown in fig. 4, the heating rate is indeed a major defining parameter for the wavelength of the undulation: The faster the samples are heated to the isotropic phase, the smaller is the undulation wavelength.

To explain the instability as such we propose the following scenario: After preparation (for 5CB) or after heating to the nematic phase for the first time (for 8CB), a pattern of nematic domains exists in the films that is preserved during the course of the experiment, since close to the substrate nematic or even smectic order exists even at temperatures substantially above the clearing point (see e.g. ). The domain boundaries act as nucleation sites for the isotropic phase upon further heating. Since the surface tension of the liquid crystalline compounds in question is several percent higher in the isotropic than in the nematic phase (see e.g. ) , a Marangoni flow drives the instability. Once the phase transition is completed, the gradient in surface tension vanishes, resulting in a flat isotropic film. It is possible to explain the pronounced effect of the heating upon the wavelength of the undulation with a few assumptions on the nucleation sites. This is beyond the scope of this note, and will be published in a forthcoming paper. It should be noted that apparently similar observations in 5AB4  do not belong to this class of nucleated undulation phenomena, since in that study the temperature was kept constant, and the undulation was not transient, but remained once it was formed.

It is interesting to note that there is no systematic dependence of the patterns observed with $`n`$CB on the film thickness. Samples of different thickness (3 thicknesses each for 5CB and 8CB) show no pronounced dependence of the undulation wavelength on film thickness, as shown in fig. 4. In particular, no indication of a quadratic dependence of the wavelength on film thickness could be detected, which would be expected of a spindoal dewetting scenario, which might be assumed to be present on the basis of the appearance of the patterns.


text:
# Temperature Dependence of the Flux Line Lattice Transition into Square Symmetry in Superconducting LuNi2B2C

\[

## Abstract

We have investigated the temperature dependence of the $`𝑯𝒄`$ flux line lattice structural phase transition from square to hexagonal symmetry, in the tetragonal superconductor LuNi2B2C ($`T_\text{c}=16.6`$ K). At temperatures below 10 K the transition onset field, $`H_2(T)`$, is only weakly temperature dependent. Above 10 K, $`H_2(T)`$ rises sharply, bending away from the upper critical field. This contradicts theoretical predictions of $`H_2(T)`$ merging with the upper critical field, and suggests that just below the $`H_{\text{c2}}(T)`$-curve the flux line lattice might be hexagonal.

\]

Studies of the topology of the magnetic flux line lattice (FLL) in type-II superconductors have a long history. Early neutron scattering experiments on low-$`\kappa `$ superconductors such as niobium revealed a multitude of different FLL symmetries and orientations, mainly determined by the symmetry of the atomic crystal structure in the plane perpendicular to the applied field . This is not surprising since deviations from the hexagonal FLL characteristic of an isotropic superconductor, and the locking to the crystalline lattice are driven by the symmetry of the screening current plane and by nonlocal flux line interactions within a range determined by the coherence length $`\xi _0`$, and the electronic mean free path $`\mathrm{}`$. Later, similar effects were also observed in the strong type-II superconductor V3Si with $`\kappa 17`$ , demonstrating that nonlocal effects can be equally important in high-$`\kappa `$ materials.

Over the last couple of years, effects of nonlocality have been clearly observed in the borocarbide superconductors. The borocarbides are quaternary intermetallics with stochiometry RNi2B2C (R = Y, Gd–Lu) and a tetragonal unit cell (I4/mmm) . These materials have attracted attention due to the coexistence of superconductivity (R = Y, Dy–Tm, Lu) and antiferromagnetic ordering (R = Gd–Tm). The borocarbides are strong type-II superconductors with Ginzburg-Landau (GL) parameter, $`\kappa =`$ 6–15. The discovery of a square FLL in most of the $`𝑯𝒄`$ phase diagram , which undergoes a smooth transformation into hexagonal symmetry at fields below 1 kOe , was the first observation of a purely field driven FLL symmetry transition.

Using nonlocal corrections to the London model and incorporating the symmetry of the screening current plane obtained from band structure calculations, one is able to calculate the FLL free energy, and thereby to determine the stable FLL configuration in different fields in the borocarbides . The model succesfully describes the nature of the FLL square to hexagonal symmetry evolution in the borocarbides with $`𝑯𝒄`$ as the applied field is reduced. Qualitatively, this can be understood as driven by the four fold basal plane anisotropy which makes the vortex current paths “squarish” close to the core. At high densities this leads to a square FLL, whereas at low fields the system appears isotropic resulting in a hexagonal FLL . The onset of the transition occurs as the field decreases, commensing at a critical field $`H_2`$, determined by the range of the nonlocal interactions . Later studies of the FLL in a set of samples doped with various amounts of impurities to systematically change the nonlocality range, showed a quantitative agreement between the predicted and measured onset of the transition . The model also predicted a reorientation transition of the rhombic FLL at a field $`H_1H_2`$, which has been subsequently observed .

Whereas there is a growing experimental and theoretical understanding of the FLL geometry and transitions for fields well into the mixed state, there has been little attempt to understand what happens at fields just below the upper critical field. In this letter we report on detailed measurements of the temperature dependence of the structural transition, $`H_2(T)`$, in LuNi2B2C with the applied field parallel to the crystalline $`c`$-axis, over a broad range of temperatures and applied fields. Below 10 K, $`H_2(T)`$ is essentially constant. Above 10 K, $`H_2(T)`$ rises sharply, eventually bending away from the $`H_{\text{c2}}(T)`$ curve, suggesting the existence of a hexagonal FLL in the region just below the upper critical field.

The FLL in LuNi2B2C ($`T_\text{c}=16.6`$ K) was studied using the small angle neutron scattering spectrometer on the cold neutron beam line at the Risø National Laboratory DR3 research reactor. The sample used was a 1 gram single crystal, grown from a high temperature flux  using isotopically enriched 11B to enhance the neutron transmission. Incident neutrons with wavelengths in the range $`\lambda _\text{n}=615.6`$ Å and a bandwidth $`\mathrm{\Delta }\lambda _\text{n}/\lambda _\text{n}=24`$% were used, and the FLL diffraction pattern was collected by a position sensitive detector at the end of a 6 m evacuated tank. Magnetic fields in the range $`1.5`$ to 10 kOe were applied parallel to the crystalline $`c`$-axis and to the incoming neutrons. In order to keep the resolution of the spectrometer unchanged, the neutron wavelength was varied in concert with the applied field to keep the scattering angle, $`2\theta =q_{10}\lambda _\text{n}/2\pi `$, constant. Here $`q_{10}`$ is the FLL scattering vector shown in figure 1. The measurements were performed at temperatures between $`2`$ and $`20`$ K, following a constant field cooling procedure. A background signal obtained above $`T_\text{c}`$ was subtracted from the data.

In figure 1 we show three different FLL diffraction patterns obtained in LuNi2B2C. In quasi-2D structures such as that of the FLL, the real space flux line configuration and the reciprocal space diffraction pattern are related by a simple $`90^{}`$ rotation and relabeling of the axes. The diffraction pattern therefore directly shows the FLL symmetry and orientation, with the caveat that scattering from differently oriented domains is superposed. For the square FLL there is no orientational degeneracy with respect to the atomic lattice, due to the tetragonal crystal structure of the borocarbides, as reflected in the top panel of figure 1. Here both the FLL (1,0)- and (1,1)-reflections are clearly visible, and resolution limited both in the radial and the azimuthal direction. The square FLL is aligned with the scattering vector $`q_{10}`$ along the $`[110]`$ crystal direction.

However, as soon as the FLL is distorted away from a square symmetry there is a two fold degeneracy, since orientations with the long rhombic unit cell diagonal along either the $`a`$\- or the $`b`$-axis have the same energy. Experimentally this will first manifest itself as an azimuthal broadening and, when the distortion increases as a splitting of the (1,0)-reflections, with the two peaks each belonging to a different domain orientation . The magnitude of the splitting will eventually reach $`30^{}`$ if the FLL is transformed to a perfect hexagonal symmetry. The azimuthal broadening is evident in the middle panel of figure 1, and in the bottom panel the (1,0)-reflections are clearly split. The effect of the transition is also reflected in the square FLL (1,1)-reflections. Ideally a radial splitting should be observed, with one peak moving towards shorter $`q`$ and gaining intensity and the other moving to longer $`q`$ and fading, to become respectively hexagonal (1,0)- and (1,1)-reflections belonging to different domain orientations. However, due to the very rapid decrease in the scattered intensity with increasing $`q`$, one only observes a radial broadening and a relative increase in the intensity.

In general, the azimuthal splitting was only directly observable when above $`10^{}`$, comparable to experimental resolution. To determine the transition onset field $`H_2(T)`$, we analyzed the azimuthal intensity distribution in each diffraction pattern at a scattering vector $`q=q_{10}`$, where $`q_{10}=\alpha \times 2\pi (B/\varphi _0)^{1/2}`$, $`\varphi _0=hc/2e`$ is the flux quantum and $`\alpha `$ is a constant which depends on the FLL symmetry: With a FLL apex angle $`\beta `$ as shown in figure 3, $`\alpha =(\mathrm{sin}\beta )^{1/2}`$, and hence $`\alpha =1`$ for the square case ($`\beta =90^{}`$) and $`(2/\sqrt{3})^{1/2}=1.075`$ for the hexagonal FLL ($`\beta =60^{}`$ or $`120^{}`$). In the top panel of figure 2 we show the temperature dependence of the azimuthal width for $`H=3`$ kOe, obtained by fitting to a single Gaussian. A clear broadening is seen for $`T>10`$ K. The low-$`T`$ width of $`13.8^{}\pm 0.2^{}`$ is a direct measure of the azimuthal resolution, which was kept constant througout the experiment. To determine the azimuthal splitting, the intensity distribution at each temperature and field was then fitted to two Gaussians with a width fixed of $`13.8^{}`$, as demonstrated in the top panel inset. In the bottom panel of figure 2 the azimuthal splitting is plotted versus temperature for a number of fields between $`1.5`$ and 6 kOe. At low temperatures the splitting goes to $`0^{}\pm 2^{}`$ as the field is increased. As $`T`$ is raised the splitting increases smoothly for $`H2`$ kOe, and abruptly above a certain threshold for $`H3`$ kOe. The threshold is determined by $`H_2(T)`$. In addition, one notes a crossing of the curves for $`4.5`$ and 6 kOe, which means that $`H_2(T)`$ is a multivalued function of $`T`$.

Figure 3 is a contour plot of the azimuthal splitting in a $`(H,T)`$-phase diagram. Here we have used the $`3^{}`$ contour, well above the zero-splitting error of $`2^{}`$, as the criterion for the transition onset field. Below 10 K, $`H_2(T)`$ is nearly constant, equal to $`2.25`$ kOe. This is somewhat higher than the litterature values , but as shown by Gammel et al. , $`H_2`$ depends strongly on the sample purity as this affects the range of the nonlocal flux line interactions. Above 10 K, $`H_2(T)`$ increases sharply, bending away from $`H_{\text{c2}}(T)`$ and thereby avoiding to cross the upper critical field. From this it is clear that the square FLL is not stable at $`H_{\text{c2}}`$(T). The strong temperature dependence contradicts predictions based on extended GL theory , where $`H_2(T)`$ intercepts $`H_{\text{c2}}(T)`$ at a finite field. An extrapolation of our measurements suggest that in the vicinity of $`H_{\text{c2}}(T)`$, the FLL may become hexagonal.

Theoretically the nonlocal contribution to the vortex-vortex interaction weakens when the temperature rises, and $`H_2(T)`$ should somewhat increase. This relatively weak increase is essentially captured in the London approach, where the order parameter $`|\mathrm{}|`$ is taken as a constant in space . Moreover, $`|\mathrm{}|`$ is assumed equal to the zero-field uniform value $`\mathrm{}_0(T)`$ which determines the condensation energy $`F_\text{N}F_\text{S}`$ of uniform superconductors ($`\mathrm{}_0^2`$ at low temperatures and $`\mathrm{}_0^4`$ near $`T_\text{c}`$). Being constant in space and field independent, the condensation energy so defined is commonly disregarded in calculations of the equilibrium FLL. Within this scheme, $`|\mathrm{}|`$ affects only the value of the penetration depth, $`\lambda 1/|\mathrm{}|`$. The model is good for flux line spacings large relative to the core size $`\xi (T)`$, i.e. in small fields, and for temperatures well below $`T_\text{c}`$.

However, with increasing density of vortices at a fixed $`T`$, the spatial average $`|\mathrm{}|`$ decreases thus causing an overall increase of the system energy . The $`|\mathrm{}|`$ suppression depends on the ratio $`a/\xi (T)`$, with $`a`$ being the intervortex spacing. Therefore, at a given flux line density, $`B/\varphi _0`$, the system energy can be reduced if the intervortex distance is maximized. This can be interpreted as an extra (to the London interaction) repulsion of vortices. This repulsion is isotropic for cubic materials or for tetragonal crystals with $`𝑯𝒄`$, and will lead to a deviation from square symmetry and eventually to a hexagonal FLL (or triangular with the structure determined only by the ratio $`\xi _\text{a}/\xi _\text{b}`$ for $`𝑯𝒄`$). We speculate that this effect should become dominant on approaching $`H_{\text{c2}}(T)`$ where $`|\mathrm{}|`$ is strongly suppressed, in accord with the data presented in this letter.

In addition, we have earlier reported that in TmNi2B2C at low temperatures the FLL is hexagonal near $`H_{\text{c2}}(T)`$. With decreasing field, the FLL transforms first to a rhombic structure followed by the square . As $`H`$ is further reduced, the FLL should go through the same evolution in inverse order, confirmed by low field decoration data . This material is antiferromagnetic below $`1.5`$ K, and it is possible that the magnetic ordering has a detrimental effect on the nonlocality range in fields near $`H_{\text{c2}}(T)`$. If so, both the antiferromagnetism and the order parameter suppression would have similar effects on the FLL, which may explain why the domain of “reverse evolution” is so broad in TmNi2B2C. Finally, also in agreement with our hypothesis are data on the FLL in V3Si that show how a distorted triangular lattice which is seen at $`T<5`$ K and $`H=10`$ kOe evolves toward hexagonal when $`T`$ approaches $`T_\text{c}(H)`$ .

Within the microscopic theory applied to the mixed state, there is no artificial separation of the electromagnetic (London) intervortex forces and those due to the varying order parameter. This problem, however, has never been addressed for the FLL . The GL approach does provide such a complete description, but it is valid only near the zero-field $`T_{\text{c0}}`$. The accuracy of results obtained within GL for $`T<T_{\text{c0}}`$ is difficult to control. Moreover, the very existence of the GL expansion in powers of the order parameter gradients away from $`T_{\text{c0}}`$ is questionable. The coherence length $`\xi (T)`$ does not diverge as $`TT_\text{c}(H)`$; as a consequence the gradients of $`\mathrm{}`$ are not necessarily small, and the convergence of the GL series is difficult (if not impossible) to monitor. In this respect, calculations based upon keeping certain quartic terms in the GL expansion while discarding others  can only be justified by a microscopic theory, which is still to be done.

In conclusion, we have in this letter reported measurement of the temperature dependence of the FLL square to hexagonal symmetry transition in LuNi2B2C. Our data show that the transition field $`H_2(T)`$, bends away from the upper critical field line, $`H_{\text{c2}}(T)`$. This suggests that while approaching the $`H_{\text{c2}}(T)`$ curve, the FLL is driven towards hexagonal symmetry. We propose a possible qualitative argument for why this might be the case. This poses new questions and challenges concerning the phase diagram of the flux line solid.

This project has recieved support from the Danish Technical Research Council and the Danish Energy Agency. M.R.E. has received support from the Christian and Anny Wendelbo Foundation. A.B.A. is supported by the Danish Research Academy. V.G.K. and P.C.C. are supported by the Director of Energy Research, Office of Basic Energy Science under contract W-7405-Eng.-82.


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# Multiwalled Carbon Nanotubes as Building Blocks in Nanoelectronics

## 1 INTRODUCTION

The large number of organic compounds and living organisms is based on the unique chemical properties of elemental carbon. Carbon forms a variety of compounds and, in pure form, exists in diamond as well as in graphite structures. Despite these well known properties of carbon, the discovery of fullerenes and nanotubes took the science community by surprise. The carbon nanotubes were discovered by Iijima in 1991 in Japan . It was soon realized that both semiconducting and metallic nanotubes should exist . The mass production of nanotubes succeeded in 1992  and the first electrical transport measurements in 1996 . Various possible applications of nanotubes have quickly emerged, for example in molecular electronics. The Coulomb blockade was detected in transport measurements in 1997, demonstrating that the nanotubes are suitable building blocks of single electron transistors (SETs).

The single electron transistor (SET) has, as an ordinary transistor, three terminals: the source, the drain and the gate. In addition, the SET contains a nearly isolated island between the source and the drain contacts. The principle of the SET is based on the repulsive interaction between electrons which becomes important when the island is smaller than about one micron and its contacts to source and drain are weak (resistance larger than the quantum of resistance $`R_Q=h/e^2`$ 26 k$`\mathrm{\Omega }`$). The first successful SET was made by Fulton and Dolan at AT&T Bell Laboratories in 1987 using aluminum thin film technology and electron beam lithography. Since the early success with the Aluminum-SET, SETs have also been manufactured out of two-dimensional electron gas of SiMOSFETs, with metal nanoparticles and lately with carbon nanotubes. In case of carbon nanotubes, the nanotube forms the central island and the relatively poor contact resistance between the leads and the nanotube ensures the required isolation.

In this paper we present work on basic electronic devices made of MWNTs. As a building block of a nanoscale electronic device, the carbon nanotube may fill many functions. Here we introduce different cases, based on our own measurements, where a multiwalled carbon nanotube is used either as the island of a SET, as an Ohmic resistor, or as a transmission line. Furthermore, we compare devices made of nanotubes that were synthesized using different methods.

## 2 BASICS OF NANOTUBES

### 2.1 Electronic properties

Graphite is made out of fairly loosely connected two dimensional carbon layers, each layer having hexagonal lattice structure. Carbon nanotubes are formed from such graphitic layers. A single walled nanotube (SWNT) is formed when a piece of graphite sheet is wrapped into a cylindrical form, the edges are seamlessly joined together and the ends of the cylinder are closed. A multiwalled nanotube (MWNT) is made out of several concentric graphite cylinders. The SWNTs are about 1-2 nm in diameter. The MWNTs, in contrast, can be as large as 20 - 30 nm in diameter and are more convenient for experiments. In constructing a SWNT one has several possibilities to cut the original graphite sheet: The width and the length of the sheet can be varied as well as the angle between the symmetry axis of the hexagonal sheet and the main axis of the final cylinder. The electrical properties of the nanotube are sensitive to the orientation of the hexagonal lattice because it determines the density of electron states at the Fermi level.

The band structure of graphite was calculated already in 1947 by Wallace using the tight binding approximation. A graphite sheet is a semimetal, whose two-dimensional band structure near the Fermi surface consists of six conical energy surfaces in the first Brillouin zone. Fermi surface of the undoped graphite consists of six points, the vertices of the six cones. When the two dimensional graphite sheet is wrapped into cylindrical form, the transverse electron motion around the cylinder surface becomes quantized. The corresponding transverse energy levels of SWNTs are separated by about 1 eV and only the lowest band is occupied at room temperature and below it. The electrons on the lowest band move along the cylinder axis and behave truly one-dimensionally. One can make nanotubes which are several microns long. The longitudinal quantization of the electron motion leads to the fine structure of the energy bands on the energy scale of 1 meV. This fine structure is, however, washed away by the broadening of the levels due to impurity scattering.

Calculations show that undoped SWNTs are either semiconductors or metals, approximately one third of the tubes having the ”metallic” orientation between the underlying hexagonal structure and the tube axis. In the semiconducting nanotubes there are no electron states at the Fermi level and the band gap is several hundreds of meVs. These tubes are good insulators at small bias voltages. In the metallic nanotubes one-dimensional energy bands cross the Fermi level. They are constructed out of the six energy cones of the graphite. Because three of the cones are equivalent, the six energy cones of graphite collapse into two independent one-dimensional conduction channels. Taking into account the spin degeneracy of the electrons, the metallic SWNTs have altogether four independent conduction channels. The number of conduction channels is important because it determines the electrical conductivity of the nanotube. The conductivity of a ballistic one-dimensional system is given by $`e^2M/h`$, where $`e`$ is the charge of electron, $`h`$ Planck’s constant and $`M`$ the number of independent conduction channels. Thus the resistance of a ballistic nanotube is expected to be 6.45 k$`\mathrm{\Omega }`$ ($`M=4`$).

The concentric layers of a MWNT are estimated to be in poor electrical contact to each other. Some experimental results have been interpreted with the assumption that only the outermost layer participates in the electron conduction. Therefore, one expects the electrical properties of the MWNTs and SWNTs to be similar. However, the metallic inner layers can contribute to the electrical properties of the MWNT at high frequencies. In fact, the analysis of tunneling experiments in MWNTs has recently turned out to be more difficult than expected.

### 2.2 Synthesis of multiwalled carbon nanotubes and their properties

Carbon nanotubes are synthesized with various methods that differ from each other in crucial ways with regard to the growth conditions, resulting in nanotubes of different quality. In MWNTs in particular, various defects can appear that distort the structure of the ideal MWNT. In the arc-discharge (AD) and related methods nanotubes are produced in an inert-gas atmosphere from graphite at such a high local temperature that the carbon evaporates and subsequently forms the nanotubes. Later, catalytical synthesis of nanotubes was started using chemical vapor deposition (CVD) methods . In the CVD technique the nanotubes grow from a catalyst over which a carbon-containing gas is led. The upper temperature is limited by the requirement that the gas is not decomposed by itself. Therefore the growth temperature with the CVD technique is lower than with the other techniques. The lower growth temperature of CVD tubes is considered as the main cause for their more defective structure.

AD tubes are generally straight, as shown in Fig. 1a, and exhibit a rather flawless structure in TEM images. Indeed, these are rather good approximations of the ideal nanotubes whose basic electronic properties were discussed above. Multiwalled CVD tubes, on the other hand, often exhibit a significant amount of disorder in TEM analysis, although images of well ordered sections of individual CVD tubes have also been reported . It is likely that CVD material exhibits large variations in quality. This variation is evident in our experiments on CVD tubes treated with reactive ion etching (RIE). In a short etching time most tubes were uniformly thinned by a factor of 2, while some tubes had vanished almost completely. The defects in a low-quality tube are much more susceptible to an etchant than the regular graphitic walls. As a result of the defective structure, CVD tubes are generally curved when observed either as freestanding in a TEM or as deposited on substrates, as shown in the AFM image of Fig. 1b. This curvature is rigid and often extends into three dimensions. The nanotube (diameter 20 nm) in Fig. 1b has a tail to the left which extends more than 100 nm above the substrate, despite the significant van der Waals forces that exist between the substrate and the nanotube. Note that the tail appears broadened due to the interaction between the AFM tip and the upwards pointing tail section. The most impressive of the three dimensionally extended tubes are the regularly coiled 3D spirals of multiwalled CVD-grown tubes , as shown in Fig. 1c. Salvetat et al. presented work comparing the elastic moduli of AD and CVD multiwalled tubes, concluding that the former are significantly stiffer than the latter. Thus, although AD tubes have generally better electronic performance from the point of view of device physics, CVD tubes have their own interesting and useful properties.

## 3 CONSTRUCTION OF NANOTUBE CIRCUITS

For electronic transport measurements individual nanotubes have to be connected to external leads. This is not a trivial task because the nanotubes are quite small, difficult to image and hard to move around. In making simple nanotube circuits one starts from a solution (actually a dispersion). A droplet of this solution is placed on the substrate at a desired location, and the solvent is evaporated away. This leaves behind a number of randomly placed nanotubes on the surface of the substrate. There are two possibilities to connect the nanotubes to the leads. In the first method the leads are evaporated on top of the nanotubes. This method requires accurate imaging of the nanotubes and sophisticated alignment techniques when making the evaporation mask. In the second method one moves the nanotubes on top of prefabricated gold electrodes (or makes a large array of electrodes in the hope of finding one nanotube already extending over at least two electrodes). Both of these methods are hampered by poor electrical contacts between the nanotubes and electrodes. This is a problem especially in the case, where nanotubes are deposited on top of the electrodes. The contact resistances range from a few tens of k$`\mathrm{\Omega }`$ to gigaohms and are not well understood. There are some methods to improve the contacts. Bachtold et al.  successfully used electron bombardment in SEM, while Jeong-O Lee et al. used quick heating at high temperature. We have also used this method in some cases. Contact resistances decrease considerably by a 30 second annealing of the sample in vacuum at 700C. We also have verified the mechanical change in a contact caused by heating: to move the tube after heating required considerably larger applied force.

Usually an atomic force microscope (AFM) is used for imaging surface topography with a tip that has a radius of curvature down to 10 nm. However, it can also be used to move small objects along the substrates. We have developed an AFM based manipulation method where both moving and imaging are done in the non-contact mode. In this mode one probes the attractive van der Waals force between the vibrating AFM tip and the surface. Using our method, the location of the object can be seen during the movement by monitoring the cantilever oscillation amplitude. This is how we can build electrical circuits containing several nanotubes, or move nanotubes on top of gold electrodes.

The differences between the arc-discharge and CVD tubes become clearly visible in our AFM manipulations of these tubes. When an AD tube is pushed with an AFM tip, it usually either moves as a whole, without bending, or bends sharply at a certain point, with the rest of the tube staying on its place. These conclusions are similar to those of Falvo et al. , who studied manipulation of AD tubes more extensively. We have found that manipulation of those CVD tubes that have significant 3D bending out of the surface is very difficult due to the sticking of the tubes to the AFM tip. Also the van der Waals forces that hold the nanotube in place and stabilize strained configurations are reduced. The manipulation of the CVD tubes is also different in the sense that the bending is continuous, without any pivot points, as shown in the manipulation sequence of a CVD tube in Fig. 2. This is of course expected due to the smaller stiffness of CVD tubes. Thus, only manipulation of AD tubes is convenient, when the required distance is several micrometers.

Bending of a nanotube will cause major local changes in the electronic structure, and consequently in intratube transport, as has been shown in calculational work. These references, however, deal basically with single shell nanotubes. On the experimental side, a large increase in resistance has been observed for SWNTs upon bending . For MWNTs, the effect of bending is quite small compared to the total conductance of the tube, as found by Paulson et al.

To observe the effect of bending to the resistance of a nanotube, resistance measurements can be done in-situ under the AFM. We have, for example, studied one sample, where a MWNT (of length 1.7 $`\mu `$m) is below the electrodes (Fig. 3). The tube is CVD synthesized, as can be seen from its shape. During a long sequence of small movements, we observed no dramatic changes: the resistance varied between 340 and 380 k$`\mathrm{\Omega }`$, the initial value. Both increase and decrease of resistance, typically a few k$`\mathrm{\Omega }`$, was observed between adjacent configurations. Based on our experience on CVD tubes, we expect that a sizable share of the resistance is in the tube itself. Thus we conclude that modest bending of a CVD grown MWNT has only a small effect on the intratube resistance. The result becomes more general when we note that similar conclusions were obtained for AD grown MWNTs. It is not surprising that it is more difficult to bend a multiwalled than a single walled tube so sharply that a tunnel junction would emerge at the site of bending.

## 4 EXAMPLES OF SETs MADE OF MWNT

We have fabricated MWNT-SETs both from CVD and AD tubes, some of which are shown in Figure 4. Main characteristics of the samples are given in Table 1. The nanotubes had typical diameters of 20 nm for the CVD tubes and 15 nm for the AD tubes. The length of the tube between the electrodes was 0.3-5 $`\mu `$m for the CVD and 0.3-1.7 $`\mu `$m for the AD tubes. Two of the CVD tubes were etched in a RIE process for 15 seconds which reduced their diameter uniformly from 20 nm to 10 nm. The electrodes were either fabricated on top of the tubes (CVD1-CVD3 and AD1) or the tubes were placed on top of prefabricated electrodes (CVD4, AD2 and AD3). The electrodes were always made of gold with a chromium sticking layer.

The quality of results obtained on our devices varied over a broad range. The results on CVD tubes were, in general, more irregular than those on AD tubes. Some of the AD tubes turned out to be excellent islands for SETs. As we will show below, the geometrical structure and the construction method have a clear influence on the results.

### 4.1 Standard CVD-tube device

Figure 4(a) shows an AFM image of device CVD1. It is made of a 6.8 $`\mu `$m long tube which has 25 nm thick gold electrodes evaporated on top of it. At room temperature, the resistance of the tube was 200 k$`\mathrm{\Omega }`$. Below 4 K a zero-bias gap due to Coulomb blockade became clearly visible.

A few gate modulation curves of this MWNT, measured at $`T=0.8`$ K, are shown in Fig. 5. Instead of the expected Coulomb blockade period of 1V (estimated for the employed side-gate placed a few $`\mu `$m away), only non-regular gate-modulation traces were found. This irregular behavior points to the formation of a series of intra-tube quantum dots, caused by disorder. Disorder-induced splitting of a tube into several separate islands has been suggested by McEuen et al. to explain similar experimental results in SWNTs. From the data set of Fig. 5 and other sets like it, we conclude that CVD tubes, at least with the present amount of disorder, are not very suitable for central islands of SET electrometers.

### 4.2 Arc-discharge tubes: Tube-gated device

In contrast to CVD-tube devices, SETs based on AD tubes display regular $`IV`$-curve modulation with respect to the gate voltage. Such regularity is particularly nicely illustrated by the results on the device of Fig. 4b (AD1). This sample is in fact composed of two crossing MWNTs: the lower tube, which acts as the central island of the SET, is $`2.3`$ $`\mu `$m long, and the crossing upper tube has been pushed into its position with AFM manipulation. The two-point (zero-bias) resistance over the crossing was $``$ 10 M$`\mathrm{\Omega }`$, which increased to $`1`$ G$`\mathrm{\Omega }`$ below 4 K. Thus, we could utilize the upper tube for gating the current in the lower tube in this construction. The device has a room temperature resistance of 71 k$`\mathrm{\Omega }`$. A Coulomb blockade develops fully only at subkelvin temperatures, with a gap of about 1 mV at 150 mK. Figure 6 shows the source-drain current $`I`$ as a function of the source-drain bias voltage $`V_b`$ and the gate voltage $`V_g`$, applied to a separate side gate.

In general, Fourier analysis of the gate modulation curves revealed only one period, indicating the existence of only one island. In contrast to CVD tubes, we conclude that this tube is not broken into sections, neither by defects nor by the other MWNT placed on top of it.

The gate modulation period with the upper tube as a gate was measured as $`\mathrm{\Delta }V_g`$ = 4 mV (using side gate $`\mathrm{\Delta }V_g`$ = 440 mV). The tube had a maximum modulation of 8 nA/$`e`$. We calculate the gate capacitance to the upper tube as $`C_g=e/\mathrm{\Delta }V_g`$ = 40 aF (for side gate $`C_g`$ = 0.4 aF). The present configuration with a crossing nanotube as a large-capacitance gate electrode might be useful in certain SET applications for reducing cross-talk between the gate and the other electrodes. Furthermore, since the voltage gain of a current-biased SET is $`C_g/C_\mathrm{\Sigma }`$ such a construction allows for devices with high voltage gain . Here $`C_\mathrm{\Sigma }`$ refers to the total island capacitance including the tunnel junctions.

### 4.3 AD tubes: 4.2-Kelvin device

Short pieces of nanotubes, equipped with small contact areas, provide a straightforward way to reach SETs with large Coulomb energies. Figure 4c shows one of the shortest nanotube devices (AD3) that we have made from AD tubes. In our short structures, the tubes have been manipulated on top of gold electrodes (AD2 and AD3). The length of the tube between the electrodes is 0.3 $`\mu `$m for both AD2 and AD3. Furthermore, the latter is not touching the substrate between the electrodes. It is separated from the underlying SiO2 by 17 nm.

The room temperature resistance of AD2 was rather high, 5 M$`\mathrm{\Omega }`$, due to weak gold-nanotube contacts, and increased to $``$ 200 M$`\mathrm{\Omega }`$ at 4.2 K. Coulomb blockade effects became clearly observable below a few Kelvin. Figure 7 shows gate modulation of the source-drain current at 4.2 K. The modulation period is 200 mV, giving a gate capacitance of 0.8 aF. From measurements of the constant current curves we obtain the junction capacitances and for the charging energy $`E_c=e^2/2C_\mathrm{\Sigma }`$ = 2.1 meV. Thus this device is a rather simple implementation of a SET working at the relatively high temperature of 4.2 K. Moreover, scaling down the dimensions should be straightforward in order to minimize the island size and, consequently, to raise the operating temperature even further. The low temperature behavior of sample AD2 has been described by Roschier et al .

### 4.4 AD tubes: Low-noise device

Nanotubes are quite susceptible to noise caused by charge trapping to surface states. Multiwalled tubes, fortunately, are not as sensitive in this respect as single walled tubes even though some of our MWNT samples do show quite high noise levels. We obtained the lowest charge noise in device AD3 which had extraordinary properties in several respects when compared with our other samples. Especially, the transport in this tube was close to ballistic, which may be the reason behind its good noise properties.

Sample AD3 had a room temperature resistance of 28 k$`\mathrm{\Omega }`$. At subkelvin temperatures, we measured a total resistance of $``$ 40 k$`\mathrm{\Omega }`$ outside the Coulomb blockade regime. The junction resistance of the nanotube-Au contacts are thus less than the quantum of resistance $`R_Q`$ $``$ 26 k$`\mathrm{\Omega }`$, which means that the Coulomb blockade cannot fully develop. Consequently, the Coulomb oscillations that we measure are smoothened.

As opposed to the usual Coulomb blockade, nanotube AD3 exhibited increased conductance around zero bias, which we attribute to resonant tunneling. Only two weakly quantized steps are seen, and therefore this tube cannot be said to be fully ballistic. The ballisticity of freestanding samples is likely to be enhanced most by the decreased capacitive coupling between impurity states of the substrate and the MWNT.

Current noise $`i_n`$ of AD3, measured at a small voltage bias of 70 $`\mu `$V, is displayed in Fig. 8. Frequency dependence of the noise power ($`i_n^2`$) has a $`1/f^2`$ character over the range $`5<f<50`$ Hz. The input equivalent charge noise $`q_n`$ is obtained from the measured current noise according to the formula $`q_n=C_gi_n/(I/V_g)`$. In the Coulomb blockade regime a modulation of the noise was seen as expected for a SET. At a frequency of 45 Hz, we obtain the charge noise $`q_n=610^6`$ $`e/\sqrt{\text{Hz}}`$, which is comparable to the best metallic SET devices reported to date . Theoretically the minimum noise level for a SET is $`q_n^{min}=\sqrt{\mathrm{}C_\mathrm{\Sigma }\mathrm{\Delta }fR_Q/R_T}`$, where $`\mathrm{\Delta }f`$ denotes the frequency range and $`R_T`$ is the tunneling resistance . Taking $`R_Q/R_T`$ $``$ 1 and assuming no cotunneling, we obtain the minimum noise as $`110^6e/\sqrt{\text{Hz}}`$. This implies that white noise would dominate over $`1/f`$ noise above 3 kHz. In fact, the shot noise limited region has been reached in our most recent experiments.

## 5  MWNTs AS RESISTORS

According to simple Drude-type arguments, disordered MWNTs are good candidates for lumped resistive elements. As was already mentioned above, we have tried to pursue this idea by selecting a couple of CVD tubes for RIE-etching in order to enhance the amount of disorder in them. The etching halved uniformly the diameter from 20 nm to 10 nm. Gold electrodes were placed on top of these tubes. The distance between them is 0.3 $`\mu `$m. Figure 9 shows the IV characteristics of one of these tubes (CVD2) at low temperatures, compared with an untreated CVD-tube (CVD4) that has roughly the same electrode spacing. At room temperature we measure a 2-point resistance of 23 k$`\mathrm{\Omega }`$ in the RIE-etched tube. At $`T=100`$ mK we observe only a weak Coulomb blockade-type nonlinearity in the IV characteristics and no discernible Coulomb oscillations, in contrast with CVD4. We therefore assume a relatively small contact resistance and consequently that the measured 2-point resistance indicates the intrinsic resistivity of the RIE-etched MWNT to be rather large, on the order of 100 k$`\mathrm{\Omega }`$/$`\mu `$m.

These results were confirmed in our second RIE-etched sample (CVD3), measured in a 4-point configuration. With this sample we observed, in addition, that the resistance measured between different electrode pairs scales roughly with the distance, in accord with Ohmic behavior. Presently we can not tell exactly what role the RIE treatment had for the electronic properties of these tubes. Their intrinsic resistance seems to be higher than that of the untreated CVD tubes by a factor $`3`$.

The high intrinsic resistance together with Ohmic addition rule for the nanotube resistance makes the RIE-etched CVD tubes simple nanoscale Ohmic resistors. These resistors perform rather well compared with the standard technology utilizing thin chromium films . Typical thin Cr-wires can be employed as linear resistances up to values 10 k$`\mathrm{\Omega }/\mu `$m while RIE-etched tubes yield 100 k$`\mathrm{\Omega }/\mu `$m if their small nonlinearity in the zero-bias region can be accepted. With better metal-tube contacts, this non-linearity can presumably be made even smaller.

## 6 MWNTs AS TRANSMISSION LINES

In the previous sections (Sects. 4 and 5) we treated MWNTs as lumped elements of simple electronic circuits. Howewer, their high aspect ratio allows for nanotube lengths up to macroscopic dimensions. Thus any longer section of a MWNT and nearby metallic structures form a transmission line, where the nanotube acts as an inner conductor. Because the electrons move nearly ballistically in a metallic defect-free tube, one naively expects MWNTs to be excellent transmission lines for high frequency electromagnetic waves. However, rather the opposite turns out to be true, since MWNTs form special, high impedance transmission lines with a low propagation velocity .

In an ordinary coaxial cable the electromagnetic wave propagates between the metallic outer and inner conductors. The propagation velocity and the impedance of the wave are determined by the electromagnetic inductance and capacitance, with $`v_0=1/\sqrt{lc}`$ and $`Z=\sqrt{l/c}`$. They are close to the propagation velocity and impedance of electromagnetic waves in free space. In an ordinary coaxial cable, the main part of the inductive energy is stored in the magnetic field induced by the moving electrons. In contrast, in nanotubes the kinetic energy of electrons exceeds their magnetic energy and the inertia of the electrons slows down the electromagnetic waves. The large kinetic inductance $`l_{kin}`$ is a consequence of the low electron density of the nanotubes.

The electromagnetic waves traveling along nanotubes are actually electron density waves propagating in one dimension, that is, 1D plasmons. If the MWNT is regarded as a transmission line, then its impedance will determine the current-voltage characteristics for electron tunneling into the tube over a mesoscopic tunnel junction, as described by the environmental quantum fluctuations theory. At low voltages, $`IV^{\alpha +1}`$, where $`\alpha =2Re(Z)/R_Q`$. At high voltages, the tunnel junction capacitance $`C_T`$ starts to shunt the environmental impedance $`Z`$, and the power law turns gradually into an Ohm’s law with a characteristic asymptotic region described by a $`1/V`$-type of tail.

Figure 10 illustrates the asymptotic approach of the $`IV`$-curve of sample AD1 towards Ohm’s law. We plot in Fig. 10 the deficit current $`I_d=V/R_TI`$ which is the deviation of the measured current $`I`$ from the Ohmic value given by $`V/R_T`$. The solid line illustrates the fitting of the theoretical $`1/V`$-tail: $`I_d=\frac{R_Q}{Z}\left(\frac{e}{2\pi C_T}\right)^2\frac{1}{V}`$, which yields for this tube a typical value of $`Z=2.7`$ k$`\mathrm{\Omega }`$. Assuming $`C=70`$ aF/$`\mu `$m, in fact deduced from the Coulomb blockade offset of the same fits, we obtain $`l0.5`$ nH/$`\mu `$m. This inductance value is much higher than expected for magnetic inductance ($`l0.1`$ pH/$`\mu `$m) but quite well in agreement with our estimate for the kinetic inductance: $`l_{kin}10`$ nH/$`\mu `$m for $`M=4`$. We thus conclude that, due to the large kinetic inductance, the propagation velocity in MWNTs is about 1000 km/s and the impedance is on the order of a few k$`\mathrm{\Omega }`$.

## 7 SUMMARY AND PROSPECTS

Carbon nanotubes vary considerably in size and properties. Restricting this variation to normal-sized AD and CVD multiwalled nanotubes, we presented in the preceding sections our work on different device configurations that can be realized from MWNTs. The difference in structural quality between AD and CVD tubes was discussed, concluding that AD tubes were preferable from the point of view of device physics. We have demonstrated the use of multiwalled carbon nanotubes as nanoelectronics building blocks such as SETs, resistors and transmission lines. Our SET made of two MWNTs demonstrated the feasibility of more complex circuits. Under proper conditions, such as separating the tube from the substrate, it is possible to minimize the noise level and, in other aspects as well, to approach the theoretical limits of performance. On the other hand, our present understanding of MWNTs as transmission lines implies that their kinetic inductance severely limits the propagation speed in them. Nevertheless, the great variety of device structures that can be made from carbon nanotubes suggest that they are among the most promising materials for future molecular electronics.

## ACKNOWLEDGMENTS

We acknowledge F. Hekking, E. Sonin, and A. Zaikin for interesting discussions. This work was supported by the Academy of Finland and by the Large Scale Installation Program ULTI-III of the European Union (HPRI-1999-CT-00050).