An integrated native mass spectrometry and top-down proteomics method that connects sequence to structure and function of macromolecular complexes.

Mass spectrometry (MS) has become a crucial technique for the analysis of protein complexes. Native MS has traditionally examined protein subunit arrangements, while proteomics MS has focused on sequence identification. These two techniques are usually performed separately without taking advantage of the synergies between them. Here we describe the development of an integrated native MS and top-down proteomics method using Fourier-transform ion cyclotron resonance (FTICR) to analyse macromolecular protein complexes in a single experiment. We address previous concerns of employing FTICR MS to measure large macromolecular complexes by demonstrating the detection of complexes up to 1.8 MDa, and we demonstrate the efficacy of this technique for direct acquirement of sequence to higher-order structural information with several large complexes. We then summarize the unique functionalities of different activation/dissociation techniques. The platform expands the ability of MS to integrate proteomics and structural biology to provide insights into protein structure, function and regulation

The change of Fermi surface topology in Bi2Sr2CaCu2O8 with doping

We report the observation of a change in Fermi surface topology of Bi2Sr2CaCu2O8 with doping. By collecting high statistics ARPES data from moderately and highly overdoped samples and dividing the data by the Fermi function, we answer a long standing question about the Fermi surface shape of Bi2Sr2CaCu2O8 close to the (pi,0) point. For moderately overdoped samples (Tc=80K) we find that both the bonding and antibonding sheets of the Fermi surface are hole-like. However for a doping level corresponding to Tc=55K we find that the antibonding sheet becomes electron-like. This change does not directly affect the critical temperature and therefore the superconductivity. However, since similar observations of the change of the topology of the Fermi surface were observed in LSCO and Bi2Sr2Cu2O6, it appears to be a generic feature of hole-doped superconductors. Because of bilayer splitting, though, this doping value is considerably lower than that for the single layer materials, which again argues that it is unrelated to Tc

Self-energy of a nodal fermion in a d-wave superconductor

We re-consider the self-energy of a nodal (Dirac) fermion in a 2D d-wave superconductor. A conventional belief is that Im \Sigma (\omega, T) \sim max (\omega^3, T^3). We show that \Sigma (\omega, k, T) for k along the nodal direction is actually a complex function of \omega, T, and the deviation from the mass shell. In particular, the second-order self-energy diverges at a finite T when either \omega or k-k_F vanish. We show that the full summation of infinite diagrammatic series recovers a finite result for \Sigma, but the full ARPES spectral function is non-monotonic and has a kink whose location compared to the mass shell differs qualitatively for spin-and charge-mediated interactions.Comment: 4pp 3 eps figure

Evolution of the Fermi surface with carrier concentration in Bi_2Sr_2CaCu_2O_{8+\delta}

We show, by use of angle-resolved photoemission spectroscopy, that underdoped Bi_2Sr_2CaCu_2O_{8+\delta} appears to have a large Fermi surface centered at (\pi,\pi), even for samples with a T_c as low as 15 K. No clear evidence of a Fermi surface pocket around (\pi/2,\pi/2) has been found. These conclusions are based on a determination of the minimum gap locus in the pseudogap regime T_c < T < T^*, which is found to coincide with the locus of gapless excitations in momentum space (Fermi surface) determined above T^*. These results suggest that the pseudogap is more likely of precursor pairing rather than magnetic origin.Comment: 4 pages, revtex, 4 postscript color figure

Destroying coherence in high temperature superconductors with current flow

The loss of single-particle coherence going from the superconducting state to the normal state in underdoped cuprates is a dramatic effect that has yet to be understood. Here, we address this issue by performing angle resolved photoemission spectroscopy (ARPES) measurements in the presence of a transport current. We find that the loss of coherence is associated with the development of an onset in the resistance, in that well before the midpoint of the transition is reached, the sharp peaks in the ARPES spectra are completely suppressed. Since the resistance onset is a signature of phase fluctuations, this implies that the loss of single-particle coherence is connected with the loss of long-range phase coherence.Comment: 7 pages, 7 figure

Extending the generalized Chaplygin gas model by using geometrothermodynamics

We use the formalism of geometrothermodynamics (GTD) to derive fundamental thermodynamic equations that are used to construct general relativistic cosmological models. In particular, we show that the simplest possible fundamental equation, which corresponds in GTD to a system with no internal thermodynamic interaction, describes the different fluids of the standard model of cosmology. In addition, a particular fundamental equation with internal thermodynamic interaction is shown to generate a new cosmological model that correctly describes the dark sector of the Universe and contains as a special case the generalized Chaplygin gas model.Comment: 18 pages, 7 figures. Section added: Basics aspects of geometrothermodynamic

The coherent {\it d}-wave superconducting gap in underdoped La2−x_{2-x}Srx_{x}CuO4_4 as studied by angle-resolved photoemission

We present angle-resolved photoemission spectroscopy (ARPES) data on moderately underdoped La$_{1.855}$Sr$_{0.145}$CuO$_4$ at temperatures below and above the superconducting transition temperature. Unlike previous studies of this material, we observe sharp spectral peaks along the entire underlying Fermi surface in the superconducting state. These peaks trace out an energy gap that follows a simple {\it d}-wave form, with a maximum superconducting gap of 14 meV. Our results are consistent with a single gap picture for the cuprates. Furthermore our data on the even more underdoped sample La$_{1.895}$Sr$_{0.105}$CuO$_4$ also show sharp spectral peaks, even at the antinode, with a maximum superconducting gap of 26 meV.Comment: Accepted by Phys. Rev. Let

Hole Pockets in the Doped 2D Hubbard Model

The electronic momentum distribution ${\rm n({\bf k})}$ of the two dimensional Hubbard model is studied for different values of the coupling ${\rm U/t}$, electronic density ${\rm \langle n \rangle}$, and temperature, using quantum Monte Carlo techniques. A detailed analysis of the data on $8\times 8$ clusters shows that features consistent with hole pockets at momenta ${\rm {\bf k}=(\pm {\pi\over{2}},\pm {\pi\over{2}})}$ appear as the system is doped away from half-filling. Our results are consistent with recent experimental data for the cuprates discussed by Aebi et al. (Phys. Rev. Lett. {\bf 72}, 2757 (1994)). In the range of couplings studied, the depth of the pockets is maximum at ${\rm \langle n \rangle \approx 0.9}$, and it increases with decreasing temperature. The apparent absence of hole pockets in previous numerical studies of this model is explained.Comment: 11 pages, 4 postscript figures appended, RevTeX (version 3.0