Category Archives: Research

Electron-Hole Droplets

While some condensed matter physicists have moved on from studying semiconductors and consider them “boring”, there are consistently surprises from the semiconductor community that suggest the opposite. Most notably, the integral and fractional quantum Hall effect were not only unexpected, but (especially the FQHE) have changed the way we think about matter. The development of semiconductor quantum wells and superlattices have played a large role furthering the physics of semiconductors and have been central to the efforts in observing Bloch oscillations, the quantum spin Hall effect and exciton condensation in quantum hall bilayers among many other discoveries.

However, there was one development that apparently did not need much of a technological advancement in semiconductor processing — it was simply just overlooked. This was the discovery of electron-hole droplets in the late 60s and early 70s in crystalline germanium and silicon. A lot of work on this topic was done in the Soviet Union on both the theoretical and experiment fronts, but because of this, finding the relevant papers online are quite difficult! An excellent review on the topic was written by L. Keldysh, who also did a lot of theoretical work on electron-hole droplets and was probably the first to recognize them for what they were.

Before continuing, let me just emphasize, that when I say electron-hole droplet, I literally mean something quite akin to water droplets in a fog, for instance. In a semiconductor, the exciton gas condenses into a mist-like substance with electron-hole droplets surrounded by a gas of free excitons. This is possible in a semiconductor because the time it takes for the electron-hole recombination is orders of magnitude longer than the time it takes to undergo the transition to the electron-hole droplet phase. Therefore, the droplet can be treated as if it is in thermal equilibrium, although it is clearly a non-equilibrium state of matter. Recombination takes longer in an indirect gap semiconductor, which is why silicon and germanium were used for these experiments.

A bit of history: The field got started in 1968 when Asnin, Rogachev and Ryvkin in the Soviet Union observed a jump in the photoconductivity in germanium at low temperature when excited above a certain threshold radiation (i.e. when the density of excitons exceeded \sim 10^{16}  \textrm{cm}^{-3}). The interpretation of this observation as an electron-hole droplet was put on firm footing when a broad luminescence peak was observed by Pokrovski and Svistunova below the exciton line (~714 meV) at ~709 meV. The intensity in this peak increased dramatically upon lowering the temperature, with a substantial increase within just a tenth of a degree, an observation suggestive of a phase transition. I reproduce the luminescence spectrum from this paper by T.K. Lo showing the free exciton and the electron-hole droplet peaks, because as mentioned, the Soviet papers are difficult to find online.

EHD-Lo.JPG

From my description so far, the most pressing questions remaining are: (1) why is there an increase in the photoconductivity due to the presence of droplets? and (2) is there better evidence for the droplet than just the luminescence peak? Because free excitons are also known to form biexcitons (i.e. excitonic molecules), the peak may easily interpreted as evidence of biexcitons instead of an electron-hole droplet, and this was a point of much contention in the early days of studying the electron-hole droplet (see the Aside below).

Let me answer the second question first, since the answer is a little simpler. The most conclusive evidence (besides the excellent agreement between theory and experiment) was literally pictures of the droplet! Because the electrons and holes within the droplet recombine, they emit the characteristic radiation shown in the luminescence spectrum above centered at ~709 meV. This is in the infrared region and J.P. Wolfe and collaborators were actually able to take pictures of the droplets in germanium (~ 4 microns in diameter) with an infrared-sensitive camera. Below is a picture of the droplet cloud — notice how the droplet cloud is actually anisotropic, which is due to the crystal symmetry and the fact that phonons can propel the electron-hole liquid!

Pic_EHD.JPG

The first question is a little tougher to answer, but it can be accomplished with a qualitative description. When the excitons condense into the liquid, the density of “excitons” is much higher in this region. In fact, the inter-exciton distance is smaller than the distance between the electron and hole in the exciton gas. Therefore, it is not appropriate to refer to a specific electron as bound to a hole at all in the droplet. The electrons and holes are free to move independently. Naively, one can rationalize this because at such high densities, the exchange interaction becomes strong so that electrons and holes can easily switch partners with other electrons and holes respectively. Hence, the electron-hole liquid is actually a multi-component degenerate plasma, similar to a Fermi liquid, and it even has a Fermi energy which is on the order of 6 meV. Hence, the electron-hole droplet is metallic!

So why do the excitons form droplets at all? This is a question of kinetics and has to do with a delicate balance between evaporation, surface tension, electron-hole recombination and the probability of an exciton in the surrounding gas being absorbed by the droplet. Keldysh’s article, linked above, and the references therein are excellent for the details on this point.

In light of the recent discovery that bismuth (also a compensated electron-hole liquid!) was recently found to be superconducting at ~530 microKelvin, one may ask whether it is possible that electron-hole droplets can also become superconducting at similar or lower temperatures. From my brief searches online it doesn’t seem like this question has been seriously asked in the theoretical literature, and it would be an interesting route towards non-equilibrium superconductivity.

Just a couple years ago, a group also reported the existence of small droplet quanta in GaAs, demonstrating that research on this topic is still alive. To my knowledge, electron-hole drops have thus far not been observed in single-layer transition metal dichalcogenide semiconductors, which may present an interesting route to studying dimensional effects on the electron-hole droplet. However, this may be challenging since most of these materials are direct-gap semiconductors.

Aside: Sadly, it seems like evidence for the electron-hole droplet was actually discovered at Bell Labs by J.R. Haynes in 1966 in this paper before the 1968 Soviet paper, unbeknownst to the author. Haynes attributed his observation to the excitonic molecule (or biexciton), which he, it turns out, didn’t have the statistics to observe. Later experiments confirmed that it indeed was the electron-hole droplet that he had observed. Strangely, Haynes’ paper is still cited in the present time relatively frequently in the context of biexcitons, since he provided quite a nice analysis of his results! Also, it so happened that Haynes died after his paper was submitted and never found out that he had actually discovered the electron-hole droplet.

Disorganized Reflections

Recently, this blog has been concentrating on topics that have lacked a personal touch. A couple months ago, I started a postdoc position and it has gotten me thinking about a few questions related to my situation and some that are more general. I thought it would be a good time to share some of my thoughts and experiences. Here is just a list of some miscellaneous questions and introspections.

  1. In a new role, doing new work, people often make mistakes while getting accustomed to their new surroundings. Since starting at my new position, I’ve been lucky enough to have patient colleagues who have forgiven my rather embarrassing blunders and guided me through uncharted territory. It’s sometimes deflating admitting your (usually) daft errors, but it’s a part of the learning process (at least it is for me).
  2. There are a lot of reasons why people are drawn to doing science. One of them is perpetually doing something new, scary and challenging. I hope that, at least for me, science never gets monotonous and there is consistently some “fear” of the unknown at work.
  3. In general, I am wary of working too much. It is important to take time to exercise and take care of one’s mental and emotional health. One of the things I have noticed is that sometimes the most driven and most intelligent graduate students suffered from burnout due to their intense work schedules at the beginning of graduate school.
  4. Along with the previous point, I am also wary of spending too much time in the lab because it is important to have  time to reflect. It is necessary to think about what you’ve done, what can be done tomorrow and conjure up experiments that one can possibly try, even if they may be lofty. It’s not a bad idea to set aside a little time each day or week to think about these kinds of things.
  5. It is necessary to be resilient, not take things personally and know your limits. I know that I am not going to be the greatest physicist of my generation or anything like that, but what keeps me going is the hope that I can make a small contribution to the literature that some physicists and other scientists will appreciate. Maybe they might even say “Huh, that’s pretty cool” with some raised eyebrows.
  6. Is physics my “passion”? I would say that I really like it, but I could have just as easily studied a host of other topics (such as literature, philosophy, economics, etc.), and I’m sure I would have enjoyed them just as much. I’ve always been more of a generalist in contrast to being focused on physics since I was a kid or teenager. There are too many interesting things out there in the world to feel satiated just studying condensed matter physics. This is sometimes a drawback and sometimes an asset (i.e. I am sometimes less technically competent than my lab-mates, but I can probably write with less trouble).
  7. For me, reading widely is valuable, but I need to be careful that it does not impede or become a substitute for active thought.
  8. Overall, science can be intimidating and it can feel unrewarding. This can be particularly true if you measure your success using a publication rate or some so-called “objective” measure. I would venture to say that a much better measure of success is whether you have grown during graduate school or during a postdoc by being able to think more independently, by picking up some valuable skills (both hard and soft) and have brought a  multi-year project into fruition.

Please feel free to share thoughts from your own experiences! I am always eager to learn about people whose experiences and attitudes differ from mine.

A few nuggets on the internet this week:

  1. For football/soccer fans:
    http://www.espnfc.us/blog/the-toe-poke/65/post/3036987/bayern-munichs-thomas-muller-has-ingenious-way-of-dodging-journalists

  2. Barack Obama’s piece in Science Magazine:
    http://tinyurl.com/jmeoyz5

  3. An interesting read on the history of physics education reform (Thanks to Rodrigo Soto-Garrido for sharing this with me):
    http://aapt.scitation.org/doi/full/10.1119/1.4967888

  4. I wonder if an experimentalist can get this to work:
    http://www.bbc.com/news/uk-england-bristol-38573364

Strontium Titanate – A Historical Tour

Like most ugly haircuts, materials tend to go in and out of style over time. Strontium titanate (SrTiO3), commonly referred to as STO, has, since its discovery, been somewhat timeless. And this is not just because it is often used as a substitute for diamonds. What I mean is that studying STO rarely seems to go out of style and the material always appears to have some surprises in store.

STO was first synthesized in the 1950s, before it was discovered naturally in Siberia. It didn’t take long for research on this material to take off. One of the first surprising results that STO had in store was that it became superconducting when reduced (electron-doped). This is not remarkable in and of itself, but this study and other follow-up ones showed that superconductivity can occur with a carrier density of only ~5\times 10^{17} cm^{-3}.

This is surprising in light of BCS theory, where the Fermi energy is assumed to be much greater than the Debye frequency — which is clearly not the case here. There have been claims in the literature suggesting that the superconductivity may be plasmon-induced, since the plasma frequency is in the phonon energy regime. L. Gorkov recently put a paper up on the arXiv discussing the mechanism problem in STO.

Soon after the initial work on superconductivity in doped STO, Shirane, Yamada and others began studying pure STO in light of the predicted “soft mode” theory of structural phase transitions put forth by W. Cochran and others. Because of an anti-ferroelectric structural phase transition at ~110K (depicted below), they we able to observe a corresponding soft phonon associated with this transition at the Brillouin zone boundary (shown below, taken from this paper). These results had vast implications for how we understand structural phase transitions today, when it is almost always assumed that a phonon softens at the transition temperature through a continuous structural phase transition.

Many materials similar to STO, such as BaTiO3 and PbTiO3, which also have a perovskite crystal structure motif, undergo a phase transition to a ferroelectric state at low (or not so low) temperatures. The transition to the ferroelectric state is accompanied by a diverging dielectric constant (and dielectric susceptibility) much in the way that the magnetic susceptibility diverges in the transition from a paramagnetic to a ferromagnetic state. In 1978, Muller (of Bednorz and Muller fame) and Burkard reported that at low temperature, the dielectric constant begins its ascent towards divergence, but then saturates at around 4K (the data is shown in the top panel below). Ferroelectricity is associated with a zone-center softening of a transverse phonon, and in the case of STO, this process begins, but doesn’t quite get there, as shown schematically in the image below (and you can see this in the data by Shirane and Yamada above as well).

quantumparaelectricity_signatures

Taken from Wikipedia

The saturation of the large dielectric constant and the not-quite-softening of the zone center phonon has led authors to refer to STO as a quantum paraelectric (i.e. because of the zero-point motion of the transverse optical zone-center phonon, the material doesn’t gain enough energy to undergo the ferroelectric transition). As recently as 2004, however, it was reported that one can induce ferroelectricity in STO films at room temperature by straining the film.

In recent times, STO has found itself as a common substrate material due to processes that can make it atomically flat. While this may not sound so exciting, this has had vast implications for the physics of thin films and interfaces. Firstly, this property has enabled researchers to grow high-quality thin films of cuprate superconductors using molecular beam epitaxy, which was a big challenge in the 1990’s. And even more recently, this has led to the discovery of a two-dimensional electron gas, superconductivity and ferromagnetism at the LAO/STO interface, a startling finding due to the fact that both materials are electrically insulating. Also alarmingly, when FeSe (a superconductor at around 7K) is grown as a monolayer film on STO, its transition temperature is boosted to around 100K (though the precise transition temperature in subsequent experiments is disputed but still high!). This has led to the idea that the FeSe somehow “borrows the pairing glue” from the underlying substrate.

STO is a gem of a material in many ways. I doubt that we are done with its surprises.

Wannier-Stark Ladder, Wavefunction Localization and Bloch Oscillations

Most people who study solid state physics are told at some point that in a totally pure sample where there is no scattering, one should observe an AC response to a DC electric field, with oscillations at the Bloch frequency (\omega_B). These are the so-called Bloch oscillations, which were predicted by C. Zener in this paper.

However, the actual observation of Bloch oscillations is not as simple as the textbooks would make it seem. There is an excellent Physics Today article by E. Mendez and G. Bastard that outline some of the challenges associated with observing Bloch oscillations (which was written while this paper was being published!). Since the textbook treatments often use semi-classical equations of motion to demonstrate the existence of Bloch oscillations in a periodic potential, they implicitly assume transport of an electron wave-packet. To generate this wave-packet is non-trivial in a solid.

In fact, if one undertakes a full quantum mechanical treatment of electrons in a periodic potential under the influence of an electric field, one arrives at the Wannier-Stark ladder, which shows that an electric field can localize electrons! It is this ladder and the corresponding localization which is key to observing Bloch oscillations.

Let me use the two-well potential to give you a picture of how this localization might occur. Imagine symmetric potential wells, where the lowest energy eigenstates look like so (where S and A label the symmetric and anti-symmetric states):

Now, imagine that I start to make the wells a little asymmetric. What happens in this case? Well, it turns out that that the electrons start to localize in the following way (for the formerly symmetric and anti-symmetric states):

G. Wannier was able to solve the Schrodinger equation with an applied electric field in a periodic potential in full and showed that the eigenstates of the problem form a Stark ladder. This means that the eigenstates are of identical functional form from quantum well to quantum well (unlike in the double-well shown above) and the energies of the eigenstates are spaced apart by \Delta E=\hbar \omega_B! The potential is shown schematically below. It is also shown that as the potential wells slant more and more (i.e. with larger electric fields), the wavefunctions become more localized (the image is taken from here (pdf!)):

screenshot-from-2016-12-01-222719

A nice numerical solution from the same document shows the wavefunctions for a periodic potential well profile with a strong electric field, exhibiting a strong wavefunction localization. Notice that the wavefunctions are of identical form from well to well.

StarkLadder.png

What can be seen in this solution is that the stationary states are split by \hbar \omega_B, but much like the quantum harmonic oscillator (where the levels are split by \hbar \omega), nothing is actually oscillating until one has a wavepacket (or a linear superposition of eigenstates). Therefore, the Bloch oscillations cannot be observed in the ground state (which includes the the applied electric field) — one must first generate a wavepacket in the solid.

In the landmark paper that finally announced the existence of Bloch oscillations, Waschke et. al. generated a wavepacket in a GaAs-GaAlAs superlattice using a laser pulse. The pulse was incident on a sample with an applied electric field along the superlattice direction, and they were able to observe radiation emitted from the sample due to the Bloch oscillations. I should mention that superlattices must be used to observe the Wannier-Stark ladder and Bloch oscillations because \omega_B, which scales with the width of the quantum well, needs to be fast enough that the electrons don’t scatter from impurities and phonons. Here is the famous plot from the aforementioned paper showing that the frequency of the emitted radiation from the Bloch oscillations can be tuned using an electric field:

PRLBlochOscillations.png

This is a pretty remarkable experiment, one of those which took 60 years from its first proposal to finally be observed.

Kapitza-Dirac Effect

We are all familiar with the fact that light can diffract from two (or multiple) slits in a Young-type experiment. After the advent of quantum mechanics and de Broglie’s wave description of matter, it was shown by Davisson and Germer that electrons could be diffracted by a crystal. In 1927, P. Kapitza and P. Dirac proposed that it should in principle be possible for electrons to be diffracted by standing waves of light, in effect using light as a diffraction grating.

In this scheme, the electrons would interact with light through the ponderomotive potential. If you’re not familiar with the ponderomotive potential, you wouldn’t be the only one — this is something I was totally ignorant of until reading about the Kapitza-Dirac effect. In 1995, Anton Zeilinger and co-workers were able to demonstrate the Kapitza-Dirac effect with atoms, obtaining a beautiful diffraction pattern in the process which you can take a look at in this paper. It probably took so long for this effect to be observed because it required the use of high-powered lasers.

Later, in 2001, this experiment was pushed a little further and an electron-beam was used to demonstrate the effect (as opposed to atoms), as Dirac and Kapitza originally proposed. Indeed, again a diffraction pattern was observed. The article is linked here and I reproduce the main result below:

dirac-kaptiza

(Top) The interference pattern observed in the presence of a standing light wave. (Bottom) The profile of the electron beam in the absence of the light wave.

Even though this experiment is conceptually quite simple, these basic quantum phenomena still manage to elicit awe (at least from me!).

Diversity in and of Physics

When someone refers to a physicist from the early twentieth century, what kind of person do you imagine? Most people will think of an Einstein-like figure, but most likely, one will think of a white male from western Europe or the US.

Today, however, things have changed considerably; physics, both as a discipline and in the people that represent it, has become more diverse. This correlation is probably not an accident. In my mind, the increased diversity is an excellent development, but as with everything, it can be further improved. There are a couple excellent podcasts I listened to recently that have championed diversity in different contexts.

The first podcast was an episode of Reply All entitled Raising the Bar (which you should really start listening to at 11:52 after the rather cringe-worthy Yes-Yes-No segment!). The episode focuses on the lack of diversity in many companies in Silicon Valley. In doing so, they interview an African-American man named Leslie Miley who was a security guard at Apple and went on to work as a software developer and manager at Twitter, Apple, and Google among other companies (i.e. he possessed a completely unorthodox background by Silicon Valley standards). He makes an interesting statement about companies in general (while referring specifically to Twitter) saying:

If you don’t have people of diverse backgrounds building your product, you’re going to get a very narrowly focused product.

He also goes onto say that including people from different backgrounds is not just appropriate from a moral standpoint, but also that:

Diverse teams have better outcomes.

There is plenty of research to support this viewpoint. In particular, Scott Page from the Santa Fe institute and University of Michigan – Ann Arbor is interviewed in the episode and suggests that when teams of people are selected and asked to perform a task, teams of “good people” from diverse backgrounds generally outperform many “excellent people”/experts from similar backgrounds (i.e. the same Ivy League schools, socio-economic status, age etc.).

There is a caveat that is presented in this episode, however. They suggest that it may take longer for a diverse team to gel and to communicate and understand each other. But again, the outcomes in the long-term are generally better.

There is an excellent episode of Hidden Brain that also covers similar topics, but focuses on building a better workplace. The host of the podcast, Shankar Vendantam, interviews the (then) head of human resources at Google, Laszlo Bock, to gain some insight into how Google has been able to build their talent pool. Of specific interest to physicists was how much Google borrows from places like Bell Labs to build a creative workplace environment. Again, Bock stresses the importance of diversity among the employees at Google in order for the company to be successful.

In physics departments across the country, I think it is necessary to take a similar approach. Departments should strive to be diverse and hire people from different backgrounds, schools, genders, and countries. Not only that, graduate students with unorthodox backgrounds should also be welcomed. This again, is not just important for the health of the department, but for the health of the discipline in general.

I strongly suspect that Michael Faraday was one of the greatest experimental physicists in the past few hundred years not in spite of his lack of mathematical acuity, but probably because of it. His mathematical ability famously did not extend much beyond basic algebra and not even as far as trigonometry.

An Interesting Research Avenue, an Update, and a Joke

An Interesting Research Avenue: A couple months ago, Stephane Mangin of the Insitut Jean Lamour gave a talk on all-optical helicity-dependent magnetic switching (what a mouthful!) at Argonne, which was fascinating. I was reminded of the talk yesterday when a review article on the topic appeared on the arXiv. The basic phenomenon is that in certain materials, one is able to send in a femtosecond laser pulse onto a magnetic material and switch the direction of magnetization using circularly polarized light. This effect is reversible (in the sense that circularly polarized light in the opposite direction will result in a magnetization in the opposite direction) and is reproducible. During the talk, Mangin was able to show us some remarkable videos of the phenomenon, which unfortunately, I wasn’t able to find online.

The initial study that sparked a lot of this work was this paper by Beaurepaire et al., which showed ultrafast demagnetization in nickel films in 1996, a whole 20 years ago! The more recent study that triggered most of the current work was this paper by Stanciu et al. in which it was shown that the magnetization direction could be switched with a circularly polarized 40-femtosecond laser pulse on ferromagnetic film alloys of GdFeCo. For a while, it was thought that this effect was specific to the GdFeCo material class, but it has since been shown that all-optical helicity-dependent magnetic switching is actually a more general phenomenon and has been observed now in many materials (see this paper by Mangin and co-workers for example). It will be interesting to see how this research plays out with respect to the magnetic storage industry. The ability to read and write on the femtosecond to picosecond timescale is definitely something to watch out for.

Update: After my post on the Gibbs paradox last week, a few readers pointed out that there exists some controversy over the textbook explanation that I presented. I am grateful that they provided links to some articles discussing the subtleties involved in the paradox. Although one commenter suggested Appendix D of E. Atlee Jackson’s textbook, I was not able to get a hold of this. It looks like a promising textbook, so I may end up just buying it, however!

The links that I found helpful about the Gibbs paradox were Jaynes’ article (pdf!) and this article by R. Swendsen. In particular, I found Jaynes’ discussion of Whifnium and Whoofnium interesting in the role that ignorance and knowledge plays our ability to extract work from a partitioned gases. Swendsen’s tries to redefine entropy classically (what he calls Boltzmann’s definition of entropy), which I have to think about a little more. But at the moment, I don’t think I buy his argument that this resolves the Gibbs paradox completely.

A Joke: 

Q: What did Mrs. Cow say to Mr. Cow?

A: Hubby, could you please mooo the lawn?

Q: What did Mr. Cow say back to Mrs. Cow?

A: But, sweetheart, then what am I going to eat?