Mildred S. Dresselhaus

Bio: Mildred S. Dresselhaus is an academic researcher from Massachusetts Institute of Technology. The author has contributed to research in topics: Carbon nanotube & Raman spectroscopy. The author has an hindex of 136, co-authored 762 publications receiving 112525 citations. Previous affiliations of Mildred S. Dresselhaus include University of California, Los Angeles & Universidade Federal de Minas Gerais.

Importance of open, heteroatom-decorated edges in chemically doped-graphene for supercapacitor applications

Abstract: Chemically doped graphene has been actively investigated as an electrode material for achieving high-performance electrochemical systems. However, the stability of pure-carbon-rich edges and/or heteroatom-decorated edges, and their effect on the electrochemical performance remain largely unexplored. We found that in a high temperature thermal doping process, the functionalized graphene edges were structurally stable at 1200 °C, whereas the edges at 1500 °C were unstable and coalesced into loops through covalent bond formation between adjacent graphene edges. Interestingly, boron and nitrogen co-doped graphene prepared at 1200 °C showed the largest capacitance in both acidic and alkaline media due to the presence of the BNO moieties along the edge sites. The doped material also showed the best rate capability due to the largely enhanced electrical conductivity originating from the substitutionally doped boron and nitrogen atoms. Our findings regarding the stability of heteroatom-decorated edges without loop formation can now be utilized as a guideline for maximizing the electrochemical activity of graphene in various electrochemical systems.

The Reinforcing Effect of Combined Carbon Nanotubes and Acetylene Blacks on the Positive Electrode of Lithium‐Ion Batteries

Abstract: Here, we demonstrate the preparation of high-performance positive electrodes for lithium-ion batteries by adding small amounts of both carbon nanotubes and acetylene blacks to LiCoO2-based active materials. The merits of using carbon nanotubes together with acetylene blacks as cathode fillers include not only the enhancement of the electrical and the thermal properties of the electrode but also the enhancement of the density of the electrode and the shortening of the electrolyte absorption time. We envisage that the use of carbon nanotubes as multifunctional fillers will increase in both cathode and anode materials for lithium-ion secondary batteries. Since the development of lithium-ion batteries in 1990, they have had an enormous influence on our lives. 2] At present, portable electronic devices and hybrid vehicles have evergrowing requirements for safe and high-performance lithiumion batteries. Therefore, new types of the nanostructure electrode materials or fillers including carbon nanotubes have been examined to improve the electrochemical performance of lithium-ion batteries (e.g. , large capacity, high rate capability and long life cycle), as well as for developing new end-use products (e.g. , cosmetics). In commercial lithium-ion batteries, up to 100 tons per year of highly pure crystalline carbon nanotubes are incorporated as effective fillers in anode materials, in which the resilience and the electrical properties of carbon nanotubes are believed to play an important role in extending the life cycle of the batteries. Similarly, several studies have examined the capability of carbon nanotubes to enhance the electrical conductivity of cathode materials in relation to that of conventionally used carbon blacks as lithium metal oxides, which have low electrical conductivity, experience structural deterioration or capacity degradation during charging and discharging cycles. However, there appears to be a critical question regarding the complete replacement of acetylene blacks by carbon nanotubes in cathodes owing to the capability of acetylene blacks to store a significant amount of electrolyte in their primary structure in addition to enhancing the conductivity. Also, previous studies have emphasized the electrical conductivity of the cathode as the only advantage of the incorporated carbon nanotubes, even though homogeneously distributed carbon nanotubes appear to give rise to additional functions. In this study, we examine the advantages of adding a hybridtype filler, consisting of acetylene blacks and high-purity crystalline thick multiwalled carbon nanotubes, to a LiCoO2-based cathode as compared to a cathode with added acetylene blacks or carbon nanotubes, from the viewpoint of their electrical and thermal properties and electrolyte adsorption capabilities as well as their electrochemical performance. Consequently, we demonstrate that optimally combined carbon nanotubes within a cathode act as electrical, thermal and structure-linking segments and provide suitably created pores, thereby decreasing the electrolyte absorption time. The prepared electrode consisted of three different morphological components: micrometer-sized LiCoO2 particles, long carbon nanotubes and nanometer-sized acetylene blacks. The technical reason for selecting LiCoO2 (Figure 1 c) as an active

Defects in individual semiconducting single wall carbon nanotubes: Raman spectroscopic and in situ Raman spectroelectrochemical study.

Abstract: Raman spectroscopy and in situ Raman spectroelectrochemistry have been used to study the influence of defects on the Raman spectra of semiconducting individual single-walled carbon nanotubes (SWCNTs). The defects were created intentionally on part of an originally defect-free individual semiconducting nanotube, which allowed us to analyze how defects influence this particular nanotube. The formation of defects was followed by Raman spectroscopy that showed D band intensity coming from the defective part and no D band intensity coming from the original part of the same nanotube. It is shown that the presence of defects also reduces the intensity of the symmetry-allowed Raman features. Furthermore, the changes to the Raman resonance window upon the introduction of defects are analyzed. It is demonstrated that defects lead to both a broadening of the Raman resonance profile and a decrease in the maximum intensity of the resonance profile. The in situ Raman spectroelectrochemical data show a doping dependence of the Raman features taken from the defective part of the tested SWCNT.

Anomalies in the magnetoreflection spectrum of bismuth in the low-quantum-number limit

Abstract: We report here anomalies observed at high magnetic fields in the magnetoreflection line shape of bismuth $\stackrel{\ensuremath{\rightarrow}}{H}$ parallel to binary, bisectrix axes) and bismuth-antimony alloys $\stackrel{\ensuremath{\rightarrow}}{H}$ parallel to binary axis) and associated with Landau-level transitions originating from the lowest-quantum-number $j=0$ levels of the valence and conduction bands. Also reported are the corresponding Shubnikov-de Haas measurements made in steady magnetic fields up to 220 kG. To interpret these anomalous magnetoreflection line shapes an accurate model for the dispersion relations of the two coupled $j=0$ magnetic energy levels is developed, including the dependence of the magnetic energy levels on the magnetic field and on the wave-vector component parallel to $\stackrel{\ensuremath{\rightarrow}}{H}$. This model is applied to the interpretation of the Shubnikov-de Haas data and to a magnetoreflection line-shape calculation for the experimental conditions under which these anomalies are observed. The calculated line shapes successfully reproduce the large variety of observed line-shape anomalies as well as their relative intensities, thereby providing strong support for this description of the dispersion relations for the $j=0$ magnetic energy levels.

XPS Study of Copper-Doped Carbon Aerogels

Abstract: Copper-doped carbon aerogels were investigated by X-ray photoelectron spectroscopy to determine the chemical nature and distribution of the copper species in the aerogel framework. The Cu2p spectra of both the organic and carbon aerogels show a fairly uniform distribution of copper species in the aerogel network, with a slight increase in copper content going from the edge to the center of the monolith. The O1s spectra of the copper-doped organic aerogel indicate that both the carboxyl and hydroxyl groups of the aerogel framework are involved in chelation of the copper ions. After carbonization, the content of the copper detected by XPS decreases significantly as the copper ions are reduced into metallic copper nanoparticles. These nanoparticles are difficult to detect by XPS because they are coated by a thin carbon layer and migrate into the carbon matrix. The carbon skeleton of the copper-doped carbon aerogels is mainly composed of a uniform micro-graphite-like crystalline network, and no copper−carbon ...

Electric Field Effect in Atomically Thin Carbon Films

Abstract: We describe monocrystalline graphitic films, which are a few atoms thick but are nonetheless stable under ambient conditions, metallic, and of remarkably high quality. The films are found to be a two-dimensional semimetal with a tiny overlap between valence and conductance bands, and they exhibit a strong ambipolar electric field effect such that electrons and holes in concentrations up to 10 13 per square centimeter and with room-temperature mobilities of ∼10,000 square centimeters per volt-second can be induced by applying gate voltage.

Helical microtubules of graphitic carbon

Abstract: THE synthesis of molecular carbon structures in the form of C60 and other fullerenes1 has stimulated intense interest in the structures accessible to graphitic carbon sheets. Here I report the preparation of a new type of finite carbon structure consisting of needle-like tubes. Produced using an arc-discharge evaporation method similar to that used for fullerene synthesis, the needles grow at the negative end of the electrode used for the arc discharge. Electron microscopy reveals that each needle comprises coaxial tubes of graphitic sheets, ranging in number from 2 up to about 50. On each tube the carbon-atom hexagons are arranged in a helical fashion about the needle axis. The helical pitch varies from needle to needle and from tube to tube within a single needle. It appears that this helical structure may aid the growth process. The formation of these needles, ranging from a few to a few tens of nanometres in diameter, suggests that engineering of carbon structures should be possible on scales considerably greater than those relevant to the fullerenes. On 7 November 1991, Sumio Iijima announced in Nature the preparation of nanometre-size, needle-like tubes of carbon — now familiar as 'nanotubes'. Used in microelectronic circuitry and microscopy, and as a tool to test quantum mechanics and model biological systems, nanotubes seem to have unlimited potential.

The rise of graphene

Abstract: Graphene is a rapidly rising star on the horizon of materials science and condensed-matter physics. This strictly two-dimensional material exhibits exceptionally high crystal and electronic quality, and, despite its short history, has already revealed a cornucopia of new physics and potential applications, which are briefly discussed here. Whereas one can be certain of the realness of applications only when commercial products appear, graphene no longer requires any further proof of its importance in terms of fundamental physics. Owing to its unusual electronic spectrum, graphene has led to the emergence of a new paradigm of 'relativistic' condensed-matter physics, where quantum relativistic phenomena, some of which are unobservable in high-energy physics, can now be mimicked and tested in table-top experiments. More generally, graphene represents a conceptually new class of materials that are only one atom thick, and, on this basis, offers new inroads into low-dimensional physics that has never ceased to surprise and continues to provide a fertile ground for applications.

Fast parallel algorithms for short-range molecular dynamics

Abstract: Three parallel algorithms for classical molecular dynamics are presented. The first assigns each processor a fixed subset of atoms; the second assigns each a fixed subset of inter-atomic forces to compute; the third assigns each a fixed spatial region. The algorithms are suitable for molecular dynamics models which can be difficult to parallelize efficiently—those with short-range forces where the neighbors of each atom change rapidly. They can be implemented on any distributed-memory parallel machine which allows for message-passing of data between independently executing processors. The algorithms are tested on a standard Lennard-Jones benchmark problem for system sizes ranging from 500 to 100,000,000 atoms on several parallel supercomputers--the nCUBE 2, Intel iPSC/860 and Paragon, and Cray T3D. Comparing the results to the fastest reported vectorized Cray Y-MP and C90 algorithm shows that the current generation of parallel machines is competitive with conventional vector supercomputers even for small problems. For large problems, the spatial algorithm achieves parallel efficiencies of 90% and a 1840-node Intel Paragon performs up to 165 faster than a single Cray C9O processor. Trade-offs between the three algorithms and guidelines for adapting them to more complex molecular dynamics simulations are also discussed.

The electronic properties of graphene

Abstract: This article reviews the basic theoretical aspects of graphene, a one-atom-thick allotrope of carbon, with unusual two-dimensional Dirac-like electronic excitations. The Dirac electrons can be controlled by application of external electric and magnetic fields, or by altering sample geometry and/or topology. The Dirac electrons behave in unusual ways in tunneling, confinement, and the integer quantum Hall effect. The electronic properties of graphene stacks are discussed and vary with stacking order and number of layers. Edge (surface) states in graphene depend on the edge termination (zigzag or armchair) and affect the physical properties of nanoribbons. Different types of disorder modify the Dirac equation leading to unusual spectroscopic and transport properties. The effects of electron-electron and electron-phonon interactions in single layer and multilayer graphene are also presented.