Towards First-principles Electrochemistry

Chemisorbed molecules at a fuel cell electrode are a very sensitive probe of the surrounding electrochemical environment, and one that can be accurately monitored with different spectroscopic techniques. We develop a comprehensive electrochemical model to study molecular chemisorption at either constant charge or fixed applied voltage, and calculate from first principles the voltage dependence of vibrational frequencies -- the vibrational Stark effect -- for CO adsorbed on close-packed platinum electrodes. The predicted vibrational Stark slopes are found to be in very good agreement with experimental electrochemical spectroscopy data, thereby resolving previous controversies in the quantitative interpretation of in-situ experiments and elucidating the relation between canonical and grand-canonicaldescriptions of vibrational surface phenomena.Comment: 10 pages, 2 figure

The Precise Formula in a Sine Function Form of the norm of the Amplitude and the Necessary and Sufficient Phase Condition for Any Quantum Algorithm with Arbitrary Phase Rotations

In this paper we derived the precise formula in a sine function form of the norm of the amplitude in the desired state, and by means of he precise formula we presented the necessary and sufficient phase condition for any quantum algorithm with arbitrary phase rotations. We also showed that the phase condition: identical rotation angles, is a sufficient but not a necessary phase condition.Comment: 16 pages. Modified some English sentences and some proofs. Removed a table. Corrected the formula for kol on page 10. No figure

Optical-fiber source of polarization-entangled photon pairs in the 1550nm telecom band

We present a fiber based source of polarization-entangled photon pairs that is well suited for quantum communication applications in the 1550nm band of standard fiber-optic telecommunications. Polarization entanglement is created by pumping a nonlinear-fiber Sagnac interferometer with two time-delayed orthogonally-polarized pump pulses and subsequently removing the time distinguishability by passing the parametrically scattered signal-idler photon pairs through a piece of birefringent fiber. Coincidence detection of the signal-idler photons yields biphoton interference with visibility greater than 90%, while no interference is observed in direct detection of either the signal or the idler photons. All four Bell states can be prepared with our setup and we demonstrate violations of CHSH form of Bell's inequalities by up to 10 standard deviations of measurement uncertainty.Comment: 12 pages, 4 figures, to be submitted to Phys. Rev. Lett. See also paper QTuB4 in QELS'03 Technical Digest (OSA, Washington, D.C., 2003). This is a more complete versio

Tropical mid-tropospheric CO_2 variability driven by the Madden–Julian oscillation

Carbon dioxide (CO_2) is the most important anthropogenic greenhouse gas in the present-day climate. Most of the community focuses on its long-term (decadal to centennial) behaviors that are relevant to climate change, but there are relatively few discussions of its higher-frequency forms of variability, and none regarding its subseasonal distribution. In this work, we report a large-scale intraseasonal variation in the Atmospheric Infrared Sounder CO_2 data in the global tropical region associated with the Madden–Julian oscillation (MJO). The peak-to-peak amplitude of the composite MJO modulation is ~1 ppmv, with a standard error of the composite mean < 0.1 ppmv. The correlation structure between CO2 and rainfall and vertical velocity indicate positive (negative) anomalies in CO_2 arise due to upward (downward) large-scale vertical motions in the lower troposphere associated with the MJO. These findings can help elucidate how faster processes can organize, transport, and mix CO_2 and provide a robustness test for coupled carbon–climate models

Eulerian and modified Lagrangian approaches to multi-dimensional condensation and collection

Turbulence is argued to play a crucial role in cloud droplet growth. The combined problem of turbulence and cloud droplet growth is numerically challenging. Here, an Eulerian scheme based on the Smoluchowski equation is compared with two Lagrangian superparticle (or su- perdroplet) schemes in the presence of condensation and collection. The growth processes are studied either separately or in combination using either two-dimensional turbulence, a steady flow, or just gravitational acceleration without gas flow. Good agreement between the differ- ent schemes for the time evolution of the size spectra is observed in the presence of gravity or turbulence. Higher moments of the size spectra are found to be a useful tool to characterize the growth of the largest drops through collection. Remarkably, the tails of the size spectra are reasonably well described by a gamma distribution in cases with gravity or turbulence. The Lagrangian schemes are generally found to be superior over the Eulerian one in terms of computational performance. However, it is shown that the use of interpolation schemes such as the cloud-in-cell algorithm is detrimental in connection with superparticle or superdroplet approaches. Furthermore, the use of symmetric over asymmetric collection schemes is shown to reduce the amount of scatter in the results.Comment: 36 pages, 17 figure