Biblioteca Digital

Combined small and wide angle synchrotron x-ray scattering (SAXS and WAXS) techniques have been developed for in situ high pressure samples, enabling exploration of the atomic structure and nanoscale superstructure phase relations. These studies can then be used to find connections between nanoparticle surfaces and internal atomic arrangements. We developed a four-axis control system for the detector, which we then employed for the study of two supercrystals assembled from 5 nm Fe3O4 and 10 nm Au nanoparticles. We optimized the x-ray energy and the sample-to-detector distance to facilitate simultaneous collection of both SAXS and WAXS. We further performedin situ high pressure SAXS and WAXS on a cubic supercrystal assembled from 4 nm wurtzite-structure CdSe nanoparticles. While wurtzite-structure CdSe nanoparticles transform into a rocksalt structure at 6.2 GPa, the cubic superstructure develops into a lamellarlike mesostructure at 9.6 GPa. Nanoparticle coupling and interaction could be enhanced, thus reducing the compressibility of the interparticle spacing above ∼3 GPa. At ∼6.2 GPa, the wurtzite-to-rocksalt phase transformation results in a noticeable drop of interparticle spacing. Above 6.2 GPa, a combined effect from denser CdSe nanoparticle causes the interparticle spacing to expand. These findings could be related to a series of changes including the surface structure...

We report nanoscale patterning of graphene using a helium ion microscope configured for lithography. Helium ion lithography is a direct-write lithography process, comparable to conventional focused ion beam patterning, with no resist or other material contacting the sample surface. In the present application, graphene samples on (Si/SiO_2) substrates are cut using helium ions, with computer controlled alignment, patterning, and exposure. Once suitable beam doses are determined, sharp edge profiles and clean etching are obtained, with little evident damage or doping to the sample. This technique provides fast lithography compatible with graphene, with ~15 nm feature sizes.; Engineering and Applied Sciences; Physics; Other Research Unit

Many condensed matter experiments explore the finite temperature dynamics of systems near quantum critical points. Often, there are no well-defined quasiparticle excitations, and so quantum kinetic equations do not describe the transport properties completely. The theory shows that the transport coefficients are not proportional to a mean free scattering time (as is the case in the Boltzmann theory of quasiparticles), but are completely determined by the absolute temperature and by equilibrium thermodynamic observables. Recently, explicit solutions of this quantum critical dynamics have become possible via the anti-de Sitter/conformal field theory duality discovered in string theory. This shows that the quantum critical theory provides a holographic description of the quantum theory of black holes in a negatively curved anti-de Sitter space, and relates its transport coefficients to properties of the Hawking radiation from the black hole. We review how insights from this connection have led to new results for experimental systems: (i) the vicinity of the superfluid–insulator transition in the presence of an applied magnetic field, and its possible application to measurements of the Nernst effect in the cuprates, (ii) the magnetohydrodynamics of the plasma of Dirac electrons in graphene and the prediction of a hydrodynamic cyclotron resonance.; Physics

Over the past twenty-five years, condensed matter physics has been developing materials with novel electronic characteristics for a wide range of future applications. Two research directions have shown particular promise: topological insulators, and high temperature copper based superconductors (cuprates). Topological insulators are a newly discovered class of materials that can be manipulated for spintronic or quantum computing devices. However there is a poor spectroscopic understanding of the current topological insulators and emerging topological insulator candidates. In cuprate superconductors, the challenge lies in raising the superconducting transition temperature to temperatures accessible in non-laboratory settings. This effort has been hampered by a poor understanding of the superconducting mechanism and its relationship with a mysterious pseudogap phase. In this thesis, I will describe experiments conducted on topological insulators and cuprate superconductors using scanning tunneling microscopy and spectroscopy, which provide nanoscale spectroscopic information in these materials.; Physics

The scientific interface between atomic, molecular and optical (AMO) physics, condensed matter, and quantum information science has recently led to the development of new insights and tools that bridge the gap between macroscopic quantum behavior and detailed microscopic intuition. While the dialogue between these fields has sharpened our understanding of quantum theory, it has also raised a bevy of new questions regarding the out-of-equilibrium dynamics and control of many-body systems. This thesis is motivated by experimental advances that make it possible to produce and probe isolated, strongly interacting ensembles of disordered particles, as found in systems ranging from trapped ions and Rydberg atoms to ultracold polar molecules and spin defects in the solid state. The presence of strong interactions in these systems underlies their potential for exploring correlated many-body physics and this thesis presents recent results on realizing fractionalization and localization. From a complementary perspective, the controlled manipulation of individual quanta can also enable the bottom-up construction of quantum devices. To this end, this thesis also describes blueprints for a room-temperature quantum computer, quantum credit cards and nanoscale quantum thermometry.; Physics

In this thesis properties of various condensed matter systems are studied, whose dependency on electronic behavior is incorporated through coarse-grained interactions. Three specific systems are considered. In the first system of study, high momentum, plane wave states of the electronic wave function are coarse-grained, while the low momentum states are fully resolved. Moreover, the coarse-graining procedure incorporates the response of the high momentum states to environmental changes and its couplings to changes in the low momentum states. Within density functional theory this allows the representation of the electronic wave function, when using a plane wave basis, to be computationally feasible without having to make the pseudopotential approximation. This coarse-graining procedure is beneficial for the study of high pressure systems, where the response of the core region is important. With this method we study a number of solid phases of boron and reveal a number of important structural and electronic properties on its high pressure and superconducting phase. The second system of study focuses on a slightly coarser scale, where a theory for the elasticity of nanometer sized objects is developed. This theory provides a powerful way of understanding nanoscale elasticity in terms of local group contributions and acts as a bridge between the atomic and the continuum regimes. This theory properly describes elastic fluctuations on length scales on the order of the decay length of the force constant matrix; allowing for straightforward development of new relations between the bending and stretching properties of nanomechanical resonators...

Spatial phase inhomogeneity at the nano- to microscale is widely observed in strongly-correlated electron materials. The underlying mechanism and possibility of artificially controlling the phase inhomogeneity are still open questions of critical importance for both the phase transition physics and device applications. Lattice strain has been shown to cause the coexistence of metallic and insulating phases in the Mott insulator VO2. By continuously tuning strain over a wide range in single-crystal VO2 micro- and nanobeams, here we demonstrate the nucleation and manipulation of one-dimensionally ordered metal-insulator domain arrays along the beams. Mott transition is achieved in these beams at room temperature by active control of strain. The ability to engineer phase inhomogeneity with strain lends insight into correlated electron materials in general, and opens opportunities for designing and controlling the phase inhomogeneity of correlated electron materials for micro- and nanoscale device applications.; Comment: 14 pages, 4 figures, with supplementary information

Granular and nanoscale materials containing a relatively small number of constituents have been studied to discover how their properties differ from their macroscopic counterparts. These studies are designed to test how far the known macroscopic approaches such as thermodynamics may be applicable in these cases. A brief review of the recent literature on these topics is given as a motivation to introduce a generic approach called nanothermodynamics. An important feature that must be incorporated into the theory is the non-additive property because of the importance of surface contributions to the physics of these systems. This is achieved by incorporating fluctuations into the theory right from the start. There are currently two approaches to incorporate this property. Hill (and further elaborated more recently with Chamberlin) initiated an approach by modifying the thermodynamic relations by taking into account the surface effects. We generalize Boltzmann-Gibbs statistical mechanics by relaxing the additivity properties of thermodynamic quantities to include nonextensive features of such systems. An outline of this generalization of the macroscopic thermodynamics to nano-systems will be given here.; Comment: 8 pages

The carriers in the high-Tc cuprates are found to be polaron-like "stripons" carrying charge and located in stripe-like inhomogeneities, "quasi-electrons" carrying charge and spin, and "svivons" carrying spin and some lattice distortion. The anomalous spectroscopic and transport properties of the cuprates are understood. The stripe-like inhomogeneities result from the Bose condensation of the svivon field, and the speed of their dynamics is determined by the width of the double-svivon neutron-resonance peak. The connection of this peak to the peak-dip-hump gap structure observed below Tc emerges naturally. Pairing results from transitions between pair states of stripons and quasi-electrons through the exchange of svivons. The pairing symmetry is of the d_{x^2-y^2} type; however, sign reversal through the charged stripes results in features not characteristic of this symmetry. The phase diagram is determined by pairing and coherence lines within the regime of a Mott transition. Coherence without pairing results in a Fermi-liquid state, and incoherent pairing results in the pseudogap state where localized electron and electron pair states exist within the Hubbard gap. A metal-insulator-transition quantum critical point occurs between these two states at T=0 when the superconducting state is suppressed. An intrinsic heterogeneity is expected of superconducting and pseudogap nanoscale regions.; Comment: 26 pages...

Long term aging is studied on several families of chalcogenide glasses including the Ge-Se, As-Se, Ge-P-Se and Ge-As-Se systems. Special attention is given to the As-Se binary, a system that displays a rich variety of aging behavior intimately tied to sample synthesis conditions and the ambient environment in which samples are aged. Calorimetric (Modulated DSC) and Raman scattering experiments are undertaken. Our results show all samples display a sub-Tg endotherm below Tg in glassy networks possessing a mean coordination number r in the 2.25 < r < 2.45 range. Two sets of AsxSe1-x samples aged for 8 years were compared, set A consisted of slow cooled samples aged in the dark, and set B consisted of melt quenched samples aged at laboratory environment. Samples of set B in the As concentration range, 35% < x < 60%, display a pre-Tg exotherm, but the feature is not observed in samples of set A. The aging behavior of set A presumably represents intrinsic aging in these glasses, while that of set B is extrinsic due to presence of light. The reversibility window persists in both sets of samples but is less well defined in set B. These findings contrast with a recent study by Golovchak et al., which finds the onset of the reversibility window moved up to the stoichiometric composition (x = 40%). Here we show that the upshifted window is better understood as resulting due to demixing of As4Se4 and As4Se3 molecules from the backbone...

In this work, fundamental results for carrier statistics in graphene 2-dimensional sheets and nanoscale ribbons are derived. Though the behavior of intrinsic carrier densities in 2d graphene sheets is found to differ drastically from traditional semiconductors, very narrow (sub-10 nm) ribbons are found to be similar to traditional narrow-gap semiconductors. The quantum capacitance, an important parameter in the electrostatic design of devices, is derived for both 2d graphene sheets and nanoribbons.; Comment: 3 pages, 3 figures, submitted to Applied Physics Letters

We present recent results on two attempts at understanding and utilizing large-scale simulations of magnetic materials. In the first study we consider massively parallel implementations on a Cray T3E of the n-fold way algorithm for magnetization switching in kinetic Ising models. We find an intricate relationship between the average time increment and the size of the spin blocks on each processor. This narrows the regime of efficient implementation. The second study concerns incorporating noise into micromagnetic calculations using Langevin methods. This allows measurement of quantities such as the probability that the system has not switched within a given time. Preliminary results are reported for arrays of single-domain nanoscale pillars.; Comment: To appear in Computer Simulation Studies in Condensed Matter Physics XI (Eds. D.P. Landau and H.-B. Schuttler), Springer-Verlag (1998). Plain Tex, 6 pages, 3 ps figures

With the increasing use of ultrashort laser pulses and nanoscale-materials, one is regularly confronted to situations in which the properties of the media supporting propagation are not varying slowly with time (or space). Hence, the usual WKB-type approximations fail, and one has to resort to numerical treatments of the problems, with a considerable loss in our insight into the physics of laser-matter interaction. We will present a new approach which allows a fully analytical solution of such problems, based on a transformation of the propagation equations into a new space where phase accumulation is linear with either time or space, which greatly simplifies their treatment. Though this method is restricted to some special models of the time or space varying dielectric constant, those are however general enough to encompass practically all experimental situations. It allows to introduce the concept of "non-stationarity induced" (or "inhomogeneity induced") dispersion. We will analyse the problem of reflection and propagation in two types of media whose dielectric constant vary rapidly at either the laser period or the laser wavelength scale. Extension of such techniques to the case of arbitrarily high non linearities will be considered too.

For a group of charged particles obeying quantum mechanics interacting with an electromagnetic field, the charge and current density in a pure state of the system are expressed with the many-body wave function of the state. Using these as sources, the microscopic Maxwell equations can be written down for any given pure state of a many-body system. By employing semi-classical radiation theory with these sources, the microscopic Maxwell equations can be used to compute the strong radiation fields produced by interacting charged quantal particles. For a charged quantal particle, three radiation fields involve only the vector potential $\mathbf{A}$. This is another example demonstrating the observability of vector potential. Five radiation fields are perpendicular to the canonical momentum of a single charged particle. For a group of charged particles, a new type of radiation field is predicted to be perpendicular to $\mathbf{A}(\mathbf{x}_{j},t)\times \lbrack\nabla\times(\nabla_{j}\Psi^{\prime})]$, where $\Psi^{'}$ is the many-body wave function. This kind of radiation does not exist for a single charged particle. The macroscopic Maxwell equations are derived from the corresponding microscopic equations for a pure state by the Russakoff-Robinson procedure which requires only a spatial coarse graining. Because the sources of fields are also the responses of a system to an external field...

We study the decoherence and thermalization dynamics of a nanoscale system coupled nonperturbatively to a fully quantum-mechanical bath. The system is prepared out of equilibrium in a pure state of the complete system. We propose a random matrix model and show analytically that there are two robust temporal regimes in the approach of the system to equilibrium --- an initial Gaussian decay followed by an exponential tail, consistent with numerical results on small interacting lattices [S. Genway, A.F. Ho and D.K.K. Lee, Phys. Rev. Lett. 105, 260402 (2010)]. Furthermore, the system decays towards a Gibbs ensemble in accordance with the eigenstate thermalization hypothesis.; Comment: 7 pages, 1 figure

This is an informal paper that contains a list of ``things we know'' and ``things we do not know'' in manganites. It is adapted from the conclusions chapter of a recent book by the author, {\it Nanoscale Phase Separation and Colossal Magnetoresistance. The Physics of Manganites and Related Compounds}, Springer-Verlag, Berlin, November 2002. The main new result of recent manganite investigations is the discovery of tendencies toward inhomogeneous states, both in experiments and in simulations of models. The colossal magnetoresistance effect appears to be closely linked to these mixed-phase tendencies, although considerably more work is needed to fully confirm these ideas. The paper also includes information on cuprates, diluted magnetic semiconductors, relaxor ferroelectrics, cobaltites, and organic and heavy fermion superconductors. These materials potentially share some common phenomenology with the manganites, such as a temperature scale $T^*$ above the ordering temperature where anomalous behavior starts. Many of these materials also present low-temperature phase competition. The possibility of colossal-like effects in compounds that do not involve ferromagnets is briefly discussed. Overall, it is concluded that inhomogeneous ``clustered'' states should be considered a new paradigm in condensed matter physics...

Ultrafast laser material processing has received significant attention due to a growing need for the fabrication of miniaturized devices at micro- and nanoscales. The traditional phenomenological laws, such as Fourier's law of heat conduction, are challenged in the microscale regime and a hyperbolic or dual phase lag model should be employed. During ultrafast laser interaction with metal, the electrons and lattices are not in equilibrium. Various two-temperature models that can be used to describe the nonequilibrium heat transfer are presented. A semi-classical two-step heating model to investigate thermal transport in metals caused by ultrashort laser heating is also presented. The main difference between the semiclassical and the phenomenological two-temperature models is that the former includes the effects of electron drifting, which could result in significantly different electron and lattice temperature response from the latter for higher-intensity and shorter-pulse laser heating. Under higher laser fluence and/or short pulse, the lattice temperature can exceed the melting point and melting takes place. The liquid phase will be resolidified when the lattice is cooled by conducting heat away. Ultrafast melting and resolidification of the thin gold film and microparticles were investigated. At even shorter pulse width...

A Raman profiling method is used to monitor growth of GexSe100-x melts and reveals a two step process of homogenization. Resulting homogeneous glasses show the non-reversing enthalpy at Tg, {\Delta}Hnr(x), to show a square-well like variation with x, with a rigidity transition near xc(1) = 19.5(5)% and stress transition near xc(2) = 26.0(5)%) representing the boundaries of the rigid but stress-free Intermediate Phase (IP). The square-well like variation of {\Delta}Hnr(x) develops sloping walls, a triangular shape and eventually disappears in glasses having an increasing heterogeneity. The {\Delta}Hnr term ages over weeks outside the IP but not inside the IP. An optical analogue of the reversibility window is observed with Raman spectra of as-quenched melts and Tg cycled glasses being the same for glass compositions in the IP but different for compositions outside the IP. Variations of Molar volumes, display three regimes of behavior with a global minimum in the IP and a pronounced increase outside that phase. The intrinsic physical behavior of dry and homogeneous chalcogenides glasses can vary sharply with composition near elastic and chemical phase transitions, showing that the physics of network glasses requires homogeneous samples...

Mirroring their role in electrical and optical physics, two-dimensional crystals are emerging as novel platforms for fluid separations and water desalination, which are hydrodynamic processes that occur in nanoscale environments. For numerical simulation to play a predictive and descriptive role, one must have theoretically sound methods that span orders of magnitude in physical scales, from the atomistic motions of particles inside the channels to the large-scale hydrodynamic gradients that drive transport. Here, we use constraint dynamics to derive a nonequilibrium molecular dynamics method for simulating steady-state mass flow of a fluid moving through the nanoscopic spaces of a porous solid. After validating our method on a model system, we use it to study the hydrophobic effect of water moving through pores of electrically-doped single-layer graphene. The trend in permeability we calculate does not follow the hydrophobicity of the membrane, but is instead governed by a crossover between two competing molecular transport mechanisms.

We study the time evolution and driven motion of thin liquid films lying on top of chemical patterns on a substrate. Lattice-Boltzmann and molecular dynamics methods are used for simulations of the flow of microscopic and nanoscopic films, respectively. Minimization of fluid surface area is used to examine the corresponding equilibrium free energy landscapes. The focus is on motion across patterns containing diverging and converging flow junctions, with an eye towards applications to lab-on-a-chip devices. Both open liquid-vapor systems driven by body forces and confined liquid-liquid systems driven by boundary motion are considered. As in earlier studies of flow on a linear chemical channel, we observe continuous motion of a connected liquid film across repeated copies of the pattern, despite the appearance of pearling instabilities of the interface. Provided that the strength of the driving force and the volume of liquid are not too large, the liquid is confined to the chemical channels and its motion can be directed by small variations in the geometry of the pattern.; Comment: 38 pages, 14 figures