Single-molecule pump-probe detection resolves ultrafast pathways in individual and coupled quantum systems

We report the first experimental study of individual molecules with femtosecond time resolution using a novel ultrafast single-molecule pump-probe method. A wide range of relaxation times from below 100 up to 400 fs is found, revealing energy redistribution over different vibrational modes and phonon coupling to the nanoenvironment. Addressing quantum-coupled molecules we find longer decay times, pointing towards inhibited intramolecular decay due to delocalized excitation. Interestingly, each individual system shows discrete jumps in femtosecond response, reflecting sudden breakup of the coupled superradiant state.     

Vibrational multilevel quantum coherence due to anharmonic couplings in intermolecular hydrogen bonds

Femtosecond three-pulse photon-echo studies of acetic acid dimers in solution reveal multilevel coherence of O-H stretching excitations caused by the anharmonic coupling between the high-frequency stretching and low-frequency hydrogen-bond motions. We demonstrate for the first time that such multilevel coherence determines the nonexponential decay of the macroscopic O-H stretching polarization, whereas spectral diffusion processes play a minor role. The dephasing time of individual vibrational transitions contributing to the overall polarization is approximately 200 fs.     

State tomography of capacitively shunted phase qubits with high fidelity

We introduce a new design concept for superconducting phase quantum bits (qubits) in which we explicitly separate the capacitive element from the Josephson tunnel junction for improved qubit performance. The number of two-level systems that couple to the qubit is thereby reduced by an order of magnitude and the measurement fidelity improves to 90%. This improved design enables the first demonstration of quantum state tomography with superconducting qubits using single-shot measurements.     

Kinetic roughening of laser deposited polymer films: crossover from single particle character to continuous growth

The crossover in kinetic roughening of thin films from a particle-character-dominated regime to continuous growth behavior has been observed in this work. This has been accomplished by atomic force microscopy investigations of pulsed laser deposited amorphous organic films with thicknesses ranging from several nanometers to more than 4 microm. The early-stage random-deposition-like processes end once a closed layer is formed, which grows without saturation on the characteristic length scales. In addition, the influence of oblique film deposition has been examined and interpreted.     

Convergence of dynamical zeta functions

I study poles and zeros of zeta functions in one-dimensional maps. Numerical and analytical arguments are given to show that the first pole of one such zeta function is given by the first zero ofanother zeta function: this describes convergence of the calculations of the first zero, which is generally the physically interesting quantity. Some remarks on how these results should generalize to zeta functions of dynamical systems with pruned symbolic dynamics and in higher dimensions follow.     

Deconstructing spatiotemporal chaos using local symbolic dynamics

We find that the global symbolic dynamics of a diffusively coupled map lattice is well approximated by a very small local model for weak to moderate coupling strengths. A local symbolic model is a truncation of the full symbolic model to one that considers only a single element and a few neighbors. Using interval analysis, we give rigorous results for a range of coupling strengths and different local model widths. Examples are presented of extracting a local symbolic model from data and of controlling spatiotemporal chaos.     

1/f Flux noise in Josephson phase qubits

We present a new method to measure 1/f noise in Josephson quantum bits (qubits) that yields low-frequency spectra below 1 Hz. A comparison of the noise taken at positive and negative bias of a phase qubit shows the dominant noise source to be flux noise and not junction critical-current noise, with a magnitude similar to that measured previously in other systems. Theoretical calculations show that the level of flux noise is not compatible with the standard model of noise from two-level state defects in the surface oxides of the films.     

Azobenzene-functionalized alkanethiols in self-assembled monolayers on gold

Self-assembled monolayers (SAMs) of 4-trifluoromethyl-azobenzene-4′-methyleneoxy-alkanethiols (CF₃– C₆H₄–N=N–C₆H₄–O–(CH₂) _n –SH on (111)-oriented poly-crystalline gold films on mica were examined by X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS). The spectra are analyzed with the help of density-functional-theory calculations of the isolated molecule. Only one doublet is detected in the sulphur 2p spectra of the investigated SAMs, consistent with a thiolate bond of the molecule to the gold surface. The C 1s XP spectra and the corresponding XAS π ^* resonance exhibit a rich structure which is assigned to the carbon atoms in the different chemical surroundings. Comparing XPS binding energies of the azobenzene moiety and calculated initial-state shifts reveals comparable screening of all C 1s core holes. While the carbon 1s XPS binding energy lies below the π ^*-resonance excitation-energy, the reversed order is found comparing core ionization and neutral core excitation of the nitrogen 1s core-hole of the azo group. This surprising difference in core-hole binding energies is interpreted as site-dependent polarization screening and charge transfer among the densely packed aromatic moieties. We propose that a quenching of the optical excitation within the molecular layer is thus one major reason for the low trans to cis photo-isomerization rate of azobenzene in aromatic-aliphatic SAMs.     

Observation of anomalous phonon softening in bilayer graphene

The interaction of electron-hole pairs with lattice vibrations exhibits a wealth of intriguing physical phenomena such as the renowned Kohn anomaly. Here we report the observation in bilayer graphene of an unusual phonon softening that provides the first experimental proof for another type of phonon anomaly. Similar to the Kohn anomaly, which is a logarithmic singularity in the phonon group velocity [W. Kohn, Phys. Rev. Lett. 2, 393 (1959)], the observed phonon anomaly exhibits a logarithmic singularity in the optical-phonon energy. Arising from a resonant electron-phonon coupling effect, the anomaly was also expected, albeit not observed, in monolayer graphene. We propose an explanation for why it is easier to observe in bilayer samples.