Michael L. Steigerwald

Bio: Michael L. Steigerwald is an academic researcher from Columbia University. The author has contributed to research in topics: Conductance & Cluster (physics). The author has an hindex of 66, co-authored 197 publications receiving 17253 citations. Previous affiliations of Michael L. Steigerwald include AT&T & Alcatel-Lucent.

Dependence of single-molecule junction conductance on molecular conformation

Abstract: Since it was first suggested1 that a single molecule might function as an active electronic component, a number of techniques have been developed to measure the charge transport properties of single molecules2,3,4,5,6,7,8,9,10,11,12. Although scanning tunnelling microscopy observations under high vacuum conditions can allow stable measurements of electron transport, most measurements of a single molecule bonded in a metal–molecule–metal junction exhibit relatively large variations in conductance. As a result, even simple predictions about how molecules behave in such junctions have still not been rigorously tested. For instance, it is well known13,14 that the tunnelling current passing through a molecule depends on its conformation; but although some experiments have verified this effect15,16,17,18, a comprehensive mapping of how junction conductance changes with molecular conformation is not yet available. In the simple case of a biphenyl—a molecule with two phenyl rings linked by a single C–C bond—conductance is expected to change with the relative twist angle between the two rings, with the planar conformation having the highest conductance. Here we use amine link groups to form single-molecule junctions with more reproducible current–voltage characteristics19. This allows us to extract average conductance values from thousands of individual measurements on a series of seven biphenyl molecules with different ring substitutions that alter the twist angle of the molecules. We find that the conductance for the series decreases with increasing twist angle, consistent with a cosine-squared relation predicted for transport through π-conjugated biphenyl systems13.

The Quantum Mechanics of Larger Semiconductor Clusters ("Quantum Dots")

Abstract: How can one understand the excited electronic states of a nanometer sized semiconductor crystallite, given that the crystallite structure is simply that of an excised fragment of the bulk lattice? This question is motivated by recent experiments on chemically synthesized "quantum crystallites," sometimes called "quantum dots," in which it is observed that the optical spectra are quite sensitive to size. For example, bulk crystalline CdSe is a semiconductor with an optical band gap at 690 nm, and continuous optical absorption at shorter wavelengths. However, 3540/~ diameter CdSe crystallites containing some 1500 atoms exhibit a series of discrete excited states with a lowest excited state at 530 nm (1-3). With increasing size, these states shift red and merge to form the optical absorption of the bulk crystal. Electron microscopy and Bragg X-ray scattering measurements show that these crystallites have the same structure and unit cell as the bulk semiconductor. Such changes have now been observed in the spectra of many different semiconductors. This phenomenon is a "quantum size effect" related to the development of the band structure with increasing crystallite size (4). Smaller crystallites behave like large molecules (e.g. polycyclic aromatic hydrocarbons) their spectroscopic and photophysical properties. They are true "clusters" that do not exhibit bulk semiconductor electronic properties. In this review

Nucleation and Growth of CdSe on ZnS Quantum Crystallite Seeds and Vice Versa, in Inverse Micelle Media

Abstract: Composite semiconductor crystallites involving CdSe grown on an ZnS seed, and vice versa, have been synthesized and capped with organic ligands in inverse micelle solutions. These composite particles, as well as capped seed crystallites of CdSe and ZnS, are isolated, purified, and characterized for relative atomic composition, structure, and electronic properties. The Debye X-ray scattering equation, when solved for these layered particles, shows that powder X-ray scattering is insensitive to a small foreign inclusion. A simple theoretical model for the LUMO and HOMO of layered crystallites shows that a small (< 15-{angstrom} diameter) interior foreign seed causes only small shifts of the lowest excited state, to either higher or lower energies. The capped CdSe seed and the capped CdSe portion of the layered particle grown on a ZnSe seed undergo low-temperature (169{degree}C) annealing to give near-single-crystal X-ray scattering. However, CdSe annealing is blocked by a surface ZnS layer which is ca. 4 {angstrom} thick. While growth to make composite particles does occur, neither particle shows evidence for epitaxial growth.

Biosynthesis of cadmium sulphide quantum semiconductor crystallites

Abstract: NANOMETRE-SCALE semiconductor quantum crystallites exhibit size-dependent and discrete excited electronic states which occur at energies higher than the band gap of the corresponding bulk solid1–4. These crystallites are too small to have continuous energy bands, even though a bulk crystal structure is present. The onset of such quantum properties sets a fundamental limit to device miniaturization in microelectronics5. Structures with either one, two or all three dimensions on the nanometer scale are of particular interest in solid state physics6. We report here our discovery of the biosynthesis of quantum crystallites in yeasts Candida glabrata and Schizosaccharomyces pombe, cultured in the presence of cad-mium salts. Short chelating peptides of general structure (γ-Glu-Cys)n-Gly control the nucleation and growth of CdS crystallites to peptide-capped intracellular particles of diameter 20 A. These quantum CdS crystallites are more monodisperse than CdS par-ticles synthesized chemically. X-ray data indicate that, at this small size, the CdS structure differs from that of bulk CdS and tends towards a six-coordinate rock-salt structure.

Mechanically controlled binary conductance switching of a single-molecule junction.

Abstract: Molecular-scale components are expected to be central to the realization of nanoscale electronic devices1,2,3. Although molecular-scale switching has been reported in atomic quantum point contacts4,5,6, single-molecule junctions provide the additional flexibility of tuning the on/off conductance states through molecular design. To date, switching in single-molecule junctions has been attributed to changes in the conformation or charge state of the molecule7,8,9,10,11,12. Here, we demonstrate reversible binary switching in a single-molecule junction by mechanical control of the metal–molecule contact geometry. We show that 4,4'-bipyridine–gold single-molecule junctions can be reversibly switched between two conductance states through repeated junction elongation and compression. Using first-principles calculations, we attribute the different measured conductance states to distinct contact geometries at the flexible but stable nitrogen–gold bond: conductance is low when the N–Au bond is perpendicular to the conducting π-system, and high otherwise. This switching mechanism, inherent to the pyridine–gold link, could form the basis of a new class of mechanically activated single-molecule switches. Molecular-scale switches will be central components in nanoscale electronic devices. Switching in single-molecule junctions has so far been achieved through changes in the conformation or charge state of the molecule. Now, reversible binary switching has been demonstrated by mechanical control of the metal–molecule contact geometry—a mechanism which could form the basis for a new class of mechanically activated single-molecule switches.

I and i

Abstract: There is, I think, something ethereal about i —the square root of minus one. I remember first hearing about it at school. It seemed an odd beast at that time—an intruder hovering on the edge of reality. Usually familiarity dulls this sense of the bizarre, but in the case of i it was the reverse: over the years the sense of its surreal nature intensified. It seemed that it was impossible to write mathematics that described the real world in …

疟原虫var基因转换速率变化导致抗原变异[英]／Paul H, Robert P, Christodoulou Z, et al//Proc Natl Acad Sci U S A

Abstract: 抗原变异可使得多种致病微生物易于逃避宿主免疫应答。表达在感染红细胞表面的恶性疟原虫红细胞表面蛋白1（PfPMP1）与感染红细胞、内皮细胞、树突状细胞以及胎盘的单个或多个受体作用，在黏附及免疫逃避中起关键的作用。每个单倍体基因组var基因家族编码约60种成员，通过启动转录不同的var基因变异体为抗原变异提供了分子基础。

Semiconductor Clusters, Nanocrystals, and Quantum Dots

Abstract: Current research into semiconductor clusters is focused on the properties of quantum dots-fragments of semiconductor consisting of hundreds to many thousands of atoms-with the bulk bonding geometry and with surface states eliminated by enclosure in a material that has a larger band gap. Quantum dots exhibit strongly size-dependent optical and electrical properties. The ability to join the dots into complex assemblies creates many opportunities for scientific discovery.

Quantum Dots for Live Cells, in Vivo Imaging, and Diagnostics

Abstract: Research on fluorescent semiconductor nanocrystals (also known as quantum dots or qdots) has evolved over the past two decades from electronic materials science to biological applications. We review current approaches to the synthesis, solubilization, and functionalization of qdots and their applications to cell and animal biology. Recent examples of their experimental use include the observation of diffusion of individual glycine receptors in living neurons and the identification of lymph nodes in live animals by near-infrared emission during surgery. The new generations of qdots have farreaching potential for the study of intracellular processes at the single-molecule level, high-resolution cellular imaging, long-term in vivo observation of cell trafficking, tumor targeting, and diagnostics.