Chemical Bonding and Charge Distribution at Metallic Nanocontacts

We present results of electronic structure calculations for aluminium contacts of atomic size, based on density functional theory and the local density approximation. Addressing the atomic orbitals at the neck of the nanocontact, we find that the local band structure deviates strongly from bulk fcc aluminium. In particular, hybridization between Al 3s and 3p states is fully suppressed due to directed bonds at the contact. Moreover, a charge transfer of 0.6 electrons off the contact aluminium site is found. Both the suppressed hybridization and the violated charge neutrality are characteristic features of metallic nanocontacts. This fact has serious consequences for models aiming at a microscopic description of transport properties.Comment: 6 pages, 3 figures, accepted by Chemical Physics Letter

Spectral diffusion and 14N quadrupole splittings in absorption detected magnetic resonance hole burning spectra of photosynthetic reaction centers

Zero field absorption detected magnetic resonance hole burning measurements were performed on photosynthetic reaction centers of the bacteria Rhodobacter sphaeroides R26 and Rhodopseudomonas viridis. Extrapolation to zero microwave power yielded pseudohomogeneous linewidths of 2.0 MHz for Rhodopseudomonas viridis, 1.0 and 0.9 MHz for the protonated forms of Rhodobacter sphaeroides R26 with and without monomer bacteriochlorophyll exchanged, and 0.25 MHz as an upper limit for fully deuterated reaction centers of Rhodobacter sphaeroides R26. The measured linewidths were interpreted as being due to unresolved hyperfine interaction between the nuclear spins and the triplet electron spin, the line shape being determined by spectral diffusion among the nuclei. The difference in linewidths between Rhodobacter sphaeroides R26 and Rhodopseudomonas viridis is then explained by triplet delocalization on the special pair in the former, and localization on one dimer half on the latter. In the fully deuterated sample, four quadrupole satellites were observed in the hole spectra arising from the eight 14N nitrogens in the special pair. The quadrupole parameters seem to be very similar for all nitrogens and were determined to =1.25±0.1 MHz and =0.9±0.1 MHz. The Journal of Chemical Physics is copyrighted by The American Institute of Physics

Geometry Effects at Atomic-Size Aluminium Contacts

We present electronic structure calculations for aluminium nanocontacts. Addressing the neck of the contact, we compare characteristic geometries to investigate the effects of the local aluminium coordination on the electronic states. We find that the Al 3pz states are very sensitive against modifications of the orbital overlap, which has serious consequences for the transport properties. Stretching of the contact shifts states towards the Fermi energy, leaving the system instable against ferromagnetic ordering. By spacial restriction, hybridization is locally suppressed at nanocontacts and the charge neutrality is violated. We discuss the influence of mechanical stress by means of quantitative results for the charge transfer.Comment: 10 pages, 4 figures, accepted by Chem. Phys. Let

Fractal Conductance Fluctuations in Gold--Nanowires

A detailed analysis of magneto-conductance fluctuations of quasiballistic gold-nanowires of various lengths is presented. We find that the variance $=$ when analyzed for $\Delta B$ much smaller than the correlation field $B_c$ varies according to $<(\Delta G)^2>\propto \Delta B^{\gamma}$ with $\gamma < 2$ indicating that the graph of $G$ vs. $B$ is fractal. We attribute this behavior to the existence of long-lived states arising from chaotic trajectories trapped close to regular classical orbits. We find that $\gamma$ decreases with increasing length of the wires.Comment: 5 pages, Revtex with epsf, 4 Postscript figures, final version accepted as Phys. Rev. Let

Quantum Conductance in Semimetallic Bismuth Nanocontacts

Electronic transport properties of bismuth nanocontacts are analyzed by means of a low temperature scanning tunneling microscope. The subquantum steps observed in the conductance versus elongation curves give evidence of atomic rearrangements in the contact. The underlying quantum nature of the conductance reveals itself through peaks in the conductance histograms. The shape of the conductance curves at 77 K is well described by a simple gliding mechanism for the contact evolution during elongation. The strikingly different behaviour at 4 K suggests a charge carrier transition from light to heavy ones as the contact cross section becomes sufficiently small.Comment: 5 pages including 4 figures. Accepted for publication in Phys. Rev. Let

Subharmonic Shapiro steps and assisted tunneling in superconducting point contacts

We analyze the current in a superconducting point contact of arbitrary transmission in the presence of a microwave radiation. The interplay between the ac Josephson current and the microwave signal gives rise to Shapiro steps at voltages V = (m/n) \hbar \omega_r/2e, where n,m are integer numbers and \omega_r is the radiation frequency. The subharmonic steps (n different from 1) are a consequence of the ocurrence of multiple Andreev reflections (MAR) and provide an unambiguous signature of the peculiar ac Josephson effect at high transmission. Moreover, the dc current exhibits a rich subgap structure due to photon-assisted MARs.Comment: Revtex, 4 pages, 4 figure

Heat dissipation in atomic-scale junctions

Atomic and single-molecule junctions represent the ultimate limit to the miniaturization of electrical circuits. They are also ideal platforms to test quantum transport theories that are required to describe charge and energy transfer in novel functional nanodevices. Recent work has successfully probed electric and thermoelectric phenomena in atomic-scale junctions. However, heat dissipation and transport in atomic-scale devices remain poorly characterized due to experimental challenges. Here, using custom-fabricated scanning probes with integrated nanoscale thermocouples, we show that heat dissipation in the electrodes of molecular junctions, whose transmission characteristics are strongly dependent on energy, is asymmetric, i.e. unequal and dependent on both the bias polarity and the identity of majority charge carriers (electrons vs. holes). In contrast, atomic junctions whose transmission characteristics show weak energy dependence do not exhibit appreciable asymmetry. Our results unambiguously relate the electronic transmission characteristics of atomic-scale junctions to their heat dissipation properties establishing a framework for understanding heat dissipation in a range of mesoscopic systems where transport is elastic. We anticipate that the techniques established here will enable the study of Peltier effects at the atomic scale, a field that has been barely explored experimentally despite interesting theoretical predictions. Furthermore, the experimental advances described here are also expected to enable the study of heat transport in atomic and molecular junctions, which is an important and challenging scientific and technological goal that has remained elusive.Comment: supporting information available in the journal web site or upon reques