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Entries categorized as ‘Carbon Nanotubes’

Nanoscale Superconductivity

April 15, 2007 · 1 Comment

I spent some time several weeks ago (over spring break) reading up on nanoscale superconductivity, Andreev reflection, all that fun stuff, and we talked about a few of the relevant papers at journal club recently. Here are some of my notes, summarized.

The 20th century saw two huge milestones in the study of electronic properties of materials in the discovery of superconductivity, and the recently burgeoning field of nanotechnology. Ever since its discovery in 1911, superconductivity has been the subject of an enormous amount of research in physics, the results of which have often been surprising, new, and very important, to say the least. While few applications of superconducting phenomena may exist (partly because of the temperature scales involved - see this or this for a review of the history of high-Tc superconductivity and where it’s potentially headed), Josephson junctions are a famous example of a phenomenon of superconductivity that has found many applications (for example, SQUIDs or physical realizations of qubits). On the other hand, fueled by a lot of promising work in low-dimensional electron gases, carbon nanotubes, and nanowires, nanotechnology has undoubtedly emerged as one of today’s hottest fields. True, the field is rife with hype, but the physics is pretty interesting too, and attempting to engineer and understand nanoscale electronic devices (like nanoscale FETs) is an exciting prospect.

One is led to ask: what happens to superconductivity at the nanoscale? After all, while nanoscale FETs could potentially push Moore’s Law much further and enable incredibly powerful computers (or so they say), superconducting nanoscale electronic devices would potentially revolutionize electronics in further unimaginable ways. Could the unique phenomena associated with superconductors be coupled with those of nanostructures? For example, transistors are important in digital circuits because they utilize the electronic properties of semiconductors and can thus be used as switches. Nanoscale FETs attempt to scale this down by contacting a nanostructure (the ‘channel’) with metal electrodes and modulating the carrier density in the channel via a gate voltage. Could it be possible to somehow retain this switching behavior of nanoscale FETs, while making the currents which flow in them dissipationless? A number of papers - three from the Delft group, one from Cambridge - dealing with this question came out at the end of last year, demonstrating significant progress towards integrating semiconducting nanostructures (in particular, carbon nanotubes, n-type InAs nanowires, Ge/Si core/shell nanowires heterostructures, and graphene) with superconducting materials.

In particular, the sample geometry is such that the nanostructure acts as a ‘weak link’ (as in a Josephson junction), and thus a supercurrent – that is, a current characterized by zero resistance – is found to flow through it. The geometry is similar to conventional FET geometries: the nanostructure bridges two conductive electrodes (a superconducting metal such as Al) which act as a source and a drain when a suitable voltage is applied across them; the electrodes are typically deposited using optical or electron-beam lithography and microfabrication/etching techniques coupled with metal evaporation techniques. The nanostructure then acts as a conduction channel that can be tuned via the electric field effect of a highly doped Si back gate separated using several hundred nm of SiO2 dielectric (or, in the case of the Ge/Si NW paper, using a top-gate separated using a high k HfO2 dielectric) - that is, a quantum dot.

Prof. Dr. Christian Schönenberger has recently written a very nice review of charge and spin transport in carbon nanotubes that is available here. A number of ideas from the paper are relevant to this post, and are nicely encapsulated in its figure 4. A key property of quantum dots is that their energy levels are discretized. If the separation between these is \delta\textit{E}, the charging energy is \textit{U} and the dot-electrode coupling (say it’s the same for both electrodes) is \Gamma, and if \delta\textit{E}\gg\textit{U}, then one can consider three regimes of dot-electrode coupling: \Gamma\ll\textit{U} (weak coupling), \Gamma\sim\textit{U} (intermediate coupling), and \Gamma\gg\textit{U} (strong coupling). As they say, it’s all about contacts, and ultimately, these three kinds of contacts give rise to different physics. For example, transport can be dominated by Coulomb effects, giving rise to ballistic transport in which the maximum conductance is given by \textit{G}_0=2e^2/h (or, more precisely, \textit{G}_0=2e^2/h\cdot(T/R) where \textit{T} and \textit{R} are the transmission and reflection coefficients of the contacts (for carbon nanotubes, this is doubled due to the two-fold degeneracy of the graphene bandstructure). On the other hand, for different dot-electrode coupling, other effects may come into play (such as Kondo / Fabry-Perot / Fano resonance effects). I wrote about the physics of Fabry-Perot interferometers in a previous post; in this case, the nanostructure is the interferometer, with the contacts playing the part of the mirrors. This is nicely illustrated in figure 1b of the Jarillo-Herrero et al. nanotube paper (for T>T_{c}\sim1.2K i.e. ‘normal’ electrodes). The key point of all this is that the electrode-nanostructure coupling is important in devices with superconducting electrodes, as well. In particular, having transparent contacts is key for the measurements done below T_{c}.

What happens in this regime? Among other things, the Bardeen-Cooper-Schrieffer (BCS) theory of superconductivity utilizes the concept of Cooper pairs to develop a quantum mechanical model for superconductivity; here’s an elementary view. Cooper pairs are correlated pairs of conduction electrons of opposite spin. The coupling between the electrons is due to phonons in the crystal lattice, or as one may say, the exchange of ‘virtual’ phonons (since they only exist during the exchange). Simplistically, one can think of a single conduction-band electron attracting nearby positively-charged lattice ion cores, thus creating lattice distortions (phonons) and regions of net positive charge to which another electron will be attracted. Cooper showed in 1956 that the effective interaction between pairs of electrons just outside the Fermi surface (k = kF) is such that this bound state forms, particularly when they have equal and opposite momenta. This was a very surprising result.

Since the net spin of a Cooper pair is zero, it acts as a boson (with a lower energy than the two individual electrons), and when a superconductor is cooled below Tc, the Cooper pairs ‘condense’ (similar to Bose-Einstein Condensation) into a correlated electron state characterized by a macroscopic quantum mechanical phase. A finite amount of energy (equal to the Cooper pair binding energy 2\Delta) is needed to disrupt this condensate and an energy gap \Delta is produced in the spectrum of free electron allowed energy states (a ‘gap to excitations’, so to speak).

Anyway, the distance over which the two electrons are coupled (the coherence length \xi of the Cooper pair) may be many orders of magnitude larger than the lattice spacing itself i.e. several hundred nanometers (in which case, repulsive Coulomb interactions between the two are quite small). In a superconductor-normal conductor-superconductor geometry, if this coherence length is longer than the length of the conduction channel, these Cooper pairs can phase-coherently tunnel through the normal material, leading to a Josephson supercurrent. For example, in the absence of any potential difference between the superconducting electrodes, this is given by I(t)=I_{c}sin(\Phi) through the device, where \Phi is the phase difference of the wavefunctions in the electrodes (see chapter 6 of M. Tinkham’s book on superconductivity for details). I_{c} is known as the critical current, and although the Josephson supercurrent picks up an oscillatory component when a dc voltage is applied across the device, Ambegaokar and Baratoff showed that I_{c}R_n=\pi\Delta/e, where R_n is the normal-state resistance of the device. That is to say, this product is a constant, independent of sample geometry.

At the end of the day, the key question is whether these phenomena carry over to these superconductor-quantum dot-superconductor systems, in which the length of the nanostructure is made to be smaller than \xi. Can a Josephson supercurrent flow in the nanostructure (the weak link)? How does the discretized nature of the electronic states affect this? It turns out that a dissipationless Josephson supercurrent does flow, due to the ‘proximity effect’ that occurs when the superconducting leads are so transparent so as to allow leakage of Cooper pairs from the superconductor into the nanostructure. Surprisingly, given a low enough temperature, this current can flow in the normal conductor over an arbitrarily long length (see this paper, available for free here), and these experiments are able to study the effects of the discrete quantum dot energy levels on the Ambegaokar-Baratoff relation that governs this supercurrent in a ‘conventional’ Josephson device. They tie in their results with theoretical predictions (such as those of Beenakker and van Houten published here and here), and a key point is that I_c is tunable (via the gate voltage) in a controllable manner, which is exciting - see, for example, figure 4a of the Xiang et al. Ge/Si nanowire paper.

mar1.jpg

When considered in the framework of Blonder-Tinkham-Klapwijk (BTK) theory, the existence of this supercurrent is intimately related to the notion of Andreev reflection (AR) or multiple Andreev reflections (MAR). A schematic of this is above, adapted from W. Belzig, Nature Nanotech. 1, 168 (2006). Since electrons with energy within the BCS energy gap can’t exist in the superconducting electrodes (as I discussed a bit earlier) when the contacts are sufficiently transparent, electrons in the nanostructure weak link can’t simply enter the superconducting electrodes (and vice versa). The only way for electrons of a given to enter the superconducting electrodes is by forming Cooper pairs. Charge/momentum conservation decree that a hole (or electron) of energy eV - the energy picked up by the electron as it travels from one lead to the other (V is the bias voltage across the nanostructure weak link) - must also be formed, with an equal and opposite momentum. This is what’s known as Andreev reflection, and this process continues (hence the term multiple Andreev reflections) until the particle bouncing back and forth has more than 2\Delta in energy. It can then enter the superconductor as a ‘normal’ electron in the first excited state. This leads to an important relation: if a charged particle is reflected (that is, it traverses the junction) n times, features will appear in the I-V characteristic curve (for a given gate voltage ) when neV=2\Delta i.e. V=2\Delta/ne. And indeed, this is what is seen in these experiments, although the reason why MAR is observed for certain values of n and isn’t for others seems to be unclear at this point.

And there’s way more to talk about. For starters, there are a large number of previous experiments upon which these build, such as this 1999 paper from Stanford on the gate-controlled proximity effect in nanotubes or the initial experiments on proximity-induced superconductivity in nanoscale systems by this French group (in single-walled nanotubes as well as nanotube ropes, DNA, Gd metallofullerenes, altering the effect in nanotubes using organic polymer coatings, and most recently, observing proximity effects in few layer graphene). It isn’t clear to me what the status of some of these papers are or to what extent this kind of stuff has been reproduced, but it seems interesting. And of course, there’s more data in these experiments that I haven’t talked about (for example, further electronic structure can be probed using an external microwave field, giving rise to ‘Shapiro steps’ as outlined in section 6.3.4 of Tinkham’s book; or for example, the observation of a bipolar supercurrent in graphene). There are also other recent papers that I haven’t mentioned, such as this one or this one on tunable \pi junctions made using InAs nanowire or carbon nanotube Josephson junctions. All in all, this seems to be a very exciting field right now, and it’ll be interesting to see how it continues to develop.

Categories: Carbon Nanotubes · Condensed Matter Physics · Nanoscale Science · Papers · Physics · Quantum Mechanics · Science · Superconductivity

Tonks-Girardeau Gas

March 14, 2007 · No Comments

I had the chance to kick back and read a few papers over spring break, including a number of experimental biophysics and atomic/molecule/optical (AMO) physics papers for well-roundedness. Some dealt with the Tonks-Girardeau gas, something I first encountered in my liquid crystals class last semester (I’m taking a few of the equations below from my notes from that class). Among other things, this system is interesting because it was one of the first exactly-solvable systems in statistical mechanics, of which there still remain very few (the Ising model in 1D/2D being another). From a soft condensed-matter physics point of view, the Tonks gas serves as a good starting point for exploring the notion of excluded volume, a surprisingly important concept (for example, leading to ideas like the depletion attraction and entropic attraction/organization - see this book for a nice introduction.)

Working at the research laboratory of the General Electric company, John Bradshaw Taylor and Irvin Langmuir spent a good deal of time in the early 30’s developing very precise means of determining the number of caesium atoms adsorbed on tungsten and using these to study the properties of such monoatomic films. Motivated by this, Lewi Tonks derived the equation of state not just for a two-dimensional gas, but for a one-dimensional and three-dimensional gas as well, ignoring the nature of the forces between them and treating the simplest case of hard elastic spheres. (Twenty-four years later, Marvin Girardeau established a rigorous one-to-one correspondence between this system and a 1D system of spinless fermions. This ‘fermionization’ helps explain why such a system of bosons doesn’t undergo condensation.)

For example, one can calculate the equation of state for a dilute gas of strongly-interacting impenetrable bosons confined to the one dimensional space 0 < x < L quite simply - since we’re treating the particles as hard spheres of radius R, the associated potential is given by U(x)=\infty for x<2R and U(x)=0 for x>2R. Then the N-sphere partition function is just:

Z_{N} \sim \displaystyle\int_{(N-1)2R}^{L} dx_{N} \displaystyle\int_{(N-2)2R}^{x_{N}-2R} dx_{N-1}\textit{...}  \displaystyle\int_{2R}^{x_{3}-2R} dx_{2}   \displaystyle\int_{0}^{x_{2}-2R} dx_{1}

(There’s a constant prefactor involving N! and what Kittel & Kroemer call the quantum concentration, but it’s not important here since we’ll be taking derivatives.) A slick way of solving this is by changing variables to y_{N} = x_{N} - (N-1)2R :

Z_{N} \sim \displaystyle\int_{0}^{L - (N-1)2R} dy_{N} \displaystyle\int_{0}^{y_{N}} dy_{N-1}\textit{...} \displaystyle\int_{0}^{y_{3}} dy_{2} \displaystyle\int_{0}^{y_{2}} dy_{1} = [L - (N-1)2R]^N

and since F = -k_{B}T\ln Z_{N} and P = -\frac{\partial F}{\partial V} , where in this case the ‘volume’ V = L , one finds that

P = \frac{\partial}{\partial L} \left\{ k_{B}TN\ln [L - (N-1)2R] \right\} \simeq \frac{Nk_{B}T}{L-2NR}

It is interesting to note that including a simplistic two-body attractive interaction regains the van der Waals equation of state exactly (see for example section 4.9 of Mattis’ somewhat misleadingly-titled book on statistical mechanics). This can also be extended to three dimensions by expanding the expression for P and considering the virial expansion, and a lot of interesting concepts, like the depletion interaction, fall out very nicely (see the first chapter of the soft condensed-matter physics book I mentioned above).

Another soft-matter application of the Tonks gas that I came across a while back is this paper by Tom Chou at UCLA. He’s developed an exact one-dimensional theory of histone adsorption and wrapping on DNA by considering each histone as a Tonks gas particle, which I think is pretty neat; after all, histones are pretty much hard spheres confined to a line of sorts - as wikipedia puts it, they “act as spools around which DNA winds”.

(This model can be theoretically extended in other ways, too. For example, Takahashi added in the effect of an arbitrary bounded interaction potential between going from the zero potential to the infinite hard-core potential; see another book by Mattis for more on this.)

But the Tonks gas is important in other areas of physics, as well - in particular, in the study of atomic gases at low temperature and particle density. During the summer of 2004, two groups published papers detailing their experiments using ultracold rubidium-87 atoms trapped using optical lattices in which they observed a transition to the strongly-correlated 1D Tonks gas regime (although they verified this in different ways: the Penn State group studied the energy and size of their system while the European group looked at the momentum distribution, both comparing their results to relevant theoretical predictions). And the research has been continuing ever since: for example, the Penn State group has extended these measurements to the study of a quantum Newton’s cradle, and other groups have studied 1D Bose gases as both Mott insulators and Luttinger liquids (the latter being a particularly nice connection to carbon nanotubes).

Categories: Carbon Nanotubes · Condensed Matter Physics · Models · Papers · Physics · Quantum Mechanics · Science

Funny Journal Content

January 29, 2007 · 1 Comment

1. A candidate for the funniest journal title/paper graphic…
Here’s a cute paper: rolling a single molecular at the atomic scale. The authors look at C44H24, a molecule possessing two triptyene ‘wheels’ (with three ‘paddles’, each) and thus two intramolecular degrees of freedom when adsorbed on a metal surface (the independent rotation of each wheel), and push it along with an STM tip. Interestingly, the STM current is a good indicater of what kind of motion the molecule is undergoing (’rolling’ versus ‘hopping’). What I find most amusing is that the molecule was previously used to construct a ‘molecular wheelbarrow’, a result which was published in Tetrahedron Letters - probably the funniest journal title I’ve come across - and includes the following priceless graphic:

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2. Can a biologist fix a radio? Or, what one scientist learned while studying apoptosis
Speaking of funny papers, this paper by Yuri Lazebnick (via Structure+Strangeness) is great. Here’s an excerpt, dealing with the question of how would a biologist fix a radio, knowing only that it is a box meant to play music?

How would we begin? First, we would secure funds to obtain a large supply of identical functioning radios in order to dissect and compare them to the one that is broken. We would eventually find how to open the radios and will find objects of various shape, color, and size. We would describe and classify them into families according to their appearance. We would describe a family of square metal objects, a family of round brightly colored objects with two legs, round-shaped objects with three legs and so on. Because the objects would vary in color, we will investigate whether changing the colors affects the radio’s performance. Although changing the colors would have only attenuating effects (the music is still playing but a trained ear of some people can discern some distortion), this approach will produce many publications and result in a lively debate.

3. Formation of a nematic fluid at high fields in Sr3Ru2O7:
I had quite a lengthy post on electronic liquid crystals in 2-dimensional electron gases (e.g. GaAs/AlGaAs heterostructures) a while back, and briefly noted that:

Scientists in Europe have measured a large magnetoresistive anisotropy in the correlated electron oxide strontium ruthenate (Sr3Ru2O7) near the ‘metamagnetic quantum critical point’, indicating the formation of a new quantum nematic phase. This is strikingly similar to the tranport anisotropy in 2DEGs I’ve been talking about… in particular, both show strong sensitivity to disorder - and the authors claim that the formation of this phase is tuned by the divergence in the quasiparticle effective mass near this critical point. One can only wonder what other kinds of systems could yield such behavior as well.

This European work is now one of the feature papers for the online Journal Club for Condensed Matter Physics, with a far more in-depth (yet very readable) commentary by Catherine Kallin of McMaster University in Canada.

(Click for more…)

Categories: Academia · Biophysics · Carbon Nanotubes · Condensed Matter Physics · Electronic Liquid Crystals · Interdisciplinary · Nanoscale Science · Nanotechnology · Papers · Physics · Quantum Mechanics · STM · Science · Statistics · Technology · Websites

This Week’s Science Roundup

January 20, 2007 · 2 Comments

This week, there have been some interesting papers dealing with new magnetic materials; using thin-films in new and interesting ways (such as in transistor memory devices and gate dielectrics in carbon nanotube transistors); nanoscale photonics using nanowires and nanotubes; exploring the possibility of creating quantum dots in graphene using electrostatic potential barriers; using scanning tunneling microscopy to look at the Kondo effect in molecules and carrier dynamics in p-n junctions while they’re being operated; figuring out what part of the brain is responsible for our wandering minds; and two interesting applications of quantum mechanics in biology - theoretically considering phonon-assisted tunneling of electrons in elucidating how we smell, and using computational quantum mechanical calculations to study protein splicing. Whew.

Nanoscale/Condensed Matter-Related:
- Hybrid metal-organic materials that are magnetic at room temperature
- Thin-film ferromagnetic devices whose magnetization is modulated via an applied electric field
- A new organic (pentacene) thin-film field-effect transistor (FET) as a possible non-volatile memory device
- Using self-assembled monolayers (SAMs) as the gate dielectric in carbon nanotube FETs
- Nanoscale photonics: nanowire LEDs and nanotube coaxial cables
- Creating quantum dots electrostatically in graphene
- Manipulating the Kondo effect in molecular systems using STM
- Using STM to study carrier dynamics in a p-n junction

Bio-related:
- Why your brain wanders when you’re bored
- Could Humans Recognize Odor by Phonon Assisted Tunneling?
- Studying Protein Cleavage Using Quantum Mechanical Calculations

Read on…

Categories: Biophysics · Carbon Nanotubes · Condensed Matter Physics · Interdisciplinary · Magnetism · Nanoscale Science · Nanotechnology · Papers · Photonics · Physics · Quantum Mechanics · STM · Science · Spintronics