Tanja Cuk

Anisotropic electron-phonon interaction in the cuprates

We explore manifestations of electron-phonon coupling on the electron spectral function for two phonon modes in the cuprates exhibiting strong renormalizations with temperature and doping. Applying simple symmetry considerations and kinematic constraints, we find that the out-of-plane, out-of-phase O buckling mode (B(1g)) involves small momentum transfers and couples strongly to electronic states near the antinode while the in-plane Cu-O breathing modes involve large momentum transfers and couples strongly to nodal electronic states. Band renormalization effects are found to be strongest in the superconducting state near the antinode, in full agreement with angle-resolved photoemission spectroscopy data.

Using convective flow splitting for the direct printing of fine copper lines

Liquid ribbons of solutions of copper hexanoate in a volatile solvent were drawn on a glass slide using either fine glass capillaries or an ink jet printer. After solvent evaporation, the solute was observed to segregate into multiple pairs of stripes much narrower than the initial ribbon diameter. These stripes were then converted to pure copper by annealing. Surface profiles indicate that the thickness, width, and number of lines formed are strongly dependent on the solution viscosity and volume per unit length deposited. From flow visualization studies and surface profiling, we have found that evaporative cooling produces Benard–Marangoni convection patterns which accrete the solute along two key boundaries of the flow, namely the three phase contact line and the outer edge of a stagnant region about the ribbon apex. These findings suggest that optimization of the deposition and evaporation process can be used to “write” fine metallic lines from a wider liquid precursor.

Coupling of the B1g Phonon to the Antinodal Electronic States ofBi2Sr2Ca0.92Y0.08Cu2O8+delta

Angle-resolved photoemission spectroscopy on optimally doped Bi(2)Sr(2)Ca(0.92)Y(0.08)Cu(2)O(8+delta) uncovers a coupling of the electronic bands to a 40 meV mode in an extended k-space region away from the nodal direction, leading to a new interpretation of the strong renormalization of the electronic structure seen in Bi2212. Phenomenological agreements with neutron and Raman experiments suggest that this mode is the B(1g) oxygen bond-buckling phonon. A theoretical calculation based on this assignment reproduces the electronic renormalization seen in the data.

Multiple bosonic mode coupling in the electron self-energy of (La2-xSrx)CuO4

High resolution angle-resolved photoemission spectroscopy data along the (0, 0)-(pi,pi) nodal direction with significantly improved statistics reveal fine structure in the electron self-energy of the underdoped (La2-xSrx)CuO4 samples in the normal state. Fine structure at energies of (40-46) meV and (58-63) meV, and possible fine structure at energies of ( 23 - 29) meV and ( 75 - 85) meV, have been identified. These observations indicate that, in (La2-xSrx) CuO4, more than one bosonic modes are involved in the coupling with electrons.

Doping dependence of the coupling of electrons to bosonic modes in the single-layer high-temperature Bi2Sr2CuO6 superconductor

A recent highlight in the study of high-T(c) superconductors is the observation of band renormalization or self-energy effects on the quasiparticles. This is seen in the form of kinks in the quasiparticle dispersions as measured by photoemission and interpreted as signatures of collective bosonic modes coupling to the electrons. Here we compare for the first time the self-energies in an optimally doped and strongly overdoped, nonsuperconducting single-layer Bi-cuprate (Bi2Sr2CuO6). In addition to the appearance of a strong overall weakening, we also find that the weight of the self-energy in the overdoped system shifts to higher energies. We present evidence that this is related to a change in the coupling to c-axis phonons due to the rapid change of the c-axis screening in this doping range.

Detecting the oxyl radical of photocatalytic water oxidation at an n-SrTiO3/aqueous interface through its subsurface vibration

Although the water oxidation cycle involves the critical step of O-O bond formation, the transition metal oxide radical thought to be the catalytic intermediate for this step has eluded direct observation. The radical represents the transformation of charge into a nascent catalytic intermediate, which lacks a newly formed bond and is therefore inherently difficult to detect. Here, using theoretical calculations and ultrafast in situ infrared spectroscopy of photocatalysis at an n-SrTiO3/aqueous interface, we reveal a subsurface vibration of the oxygen directly below, and uniquely generated by, the oxyl radical (Ti-O(•)). Intriguingly, this interfacial Ti-O stretch vibration, once decoupled from the lattice, couples to reactant dynamics (water librations). These experiments demonstrate subsurface vibrations and their coupling to solvent and electron dynamics to detect nascent catalytic intermediates at the solid-liquid interface at the molecular level. One can envision using the subsurface vibrations and their coupling across the interface to track and control catalysis dynamically.

How surface potential determines the kinetics of the first hole transfer of photocatalytic water oxidation.

Interfacial hole transfer between n-SrTiO3 and OH(-) was investigated by surface sensitive transient optical spectroscopy of an in situ photoelectrochemical cell during water oxidation. The kinetics reveal a single rate constant with an exponential dependence on the surface hole potential, spanning time scales from 3 ns to 8 ps over a ≈1 V increase. A voltage- and laser illumination-induced process moves the valence band edge at the n-type semiconductor/water interface to continuously change the surface hole potential. This single step of the water oxidation reaction is assigned to the first hole transfer h(+) + OH(-) → OH(•). The kinetics quantify how much a change in the free energy difference driving this first hole transfer reduces the activation barrier. They are also used to extrapolate the kinetic rate due to the activation barrier when that free energy difference is zero, or the Nernstian potential. This is the first time transient spectroscopy has enabled the separation of the first hole transfer from the full four hole transfer cycle and a direct determination of these two quantities. The Nernstian potential for OH(-)/OH(•) is also suggested, in rough agreement with gas-phase studies. The observation of a distinct, much longer time scale upon picosecond hole transfer to OH(-) suggests that a dominant, more stable intermediate of the water oxidation reaction, possibly a surface bound oxo, may result.

High-pressure resistivity technique for quasi-hydrostatic compression experiments

Diamond anvil cell techniques are now well established and powerful methods for measuring materials properties to very high pressure. However, high pressure resistivity measurements are challenging because the electrical contacts attached to the sample have to survive to extreme stress conditions. Until recently, experiments in a diamond anvil cell were mostly limited to non-hydrostatic or quasi-hydrostatic pressure media other than inert gases. We present here a solution to the problem by using focused ion beam ultrathin lithography for a diamond anvil cell loaded with inert gas (Ne) and show typical resistivity data. These ultrathin leads are deposited on the culet of the diamond and are attaching the sample to the anvil mechanically, therefore allowing for measurements in hydrostatic or nearly hydrostatic conditions of pressure using noble gases like Ne or He as pressure transmitting media.

Uncovering a pressure-tuned electronic transition in Bi(1.98)Sr(2.06)Y(0.68)Cu(2)O(8+delta) using Raman scattering and x-ray diffraction.

We report pressure-tuned Raman and x-ray diffraction data of Bi(1.98.)Sr(2.06)Y(0.68)Cu(2)O(8+delta) revealing a critical pressure at 21 GPa with anomalies in electronic Raman background, electron-phonon coupling lambda, spectral weight transfer, density dependent behavior of phonons and magnons, and a compressibility change in the c axis. For the first time in a cuprate, mobile charge carriers, lattice, and magnetism all show anomalies at a distinct critical pressure in the same experimental setting. Furthermore, the spectral changes suggest that the critical pressure at 21 GPa is related to the critical point at optimal doping.

Uncovering a pressure-tuned electronic transition in BiSrYCu2O8 using Raman scattering and x-ray diffraction

We report pressure-tuned Raman and x-ray diffraction data of Bi(1.98.)Sr(2.06)Y(0.68)Cu(2)O(8+delta) revealing a critical pressure at 21 GPa with anomalies in electronic Raman background, electron-phonon coupling lambda, spectral weight transfer, density dependent behavior of phonons and magnons, and a compressibility change in the c axis. For the first time in a cuprate, mobile charge carriers, lattice, and magnetism all show anomalies at a distinct critical pressure in the same experimental setting. Furthermore, the spectral changes suggest that the critical pressure at 21 GPa is related to the critical point at optimal doping.