Nonlinear spectroscopy of cold atoms in diffuse laser light

The nonlinear spectroscopy of cold atoms in the diffuse laser cooling system is studied in this paper. We present the theoretical models of the recoil-induced resonances (RIR) and the electromagnetically-induced absorption (EIA) of cold atoms in diffuse laser light, and show their signals in an experiment of cooling Rb-87 atomic vapor in an integrating sphere. The theoretical results are in good agreement with the experimental ones when the light intensity distribution in the integrating sphere is considered. The differences between nonlinear spectra of cold atoms in the diffuse laser light and in the optical molasses are also discussed. (c) 2009 Optical Society of America

Quantum Mechanics Studies of Fuel Cell Catalysts and Proton Conducting Ceramics with Validation by Experiment

We carried out quantum mechanics (QM) studies aimed at improving the performance of hydrogen fuel cells. This led to predictions of improved materials, some of which were subsequently validated with experiments by our collaborators.

In part I, the challenge was to find a replacement for the Pt cathode that would lead to improved performance for the Oxygen Reduction Reaction (ORR) while remaining stable under operational conditions and decreasing cost. Our design strategy was to find an alloy with composition Pt3M that would lead to surface segregation such that the top layer would be pure Pt, with the second and subsequent layers richer in M. Under operating conditions we expect the surface to have significant O and/or OH chemisorbed on the surface, and hence we searched for M that would remain segregated under these conditions. Using QM we examined surface segregation for 28 Pt₃M alloys, where M is a transition metal. We found that only Pt₃Os and Pt₃Ir showed significant surface segregation when O and OH are chemisorbed on the catalyst surfaces. This result indicates that Pt₃Os and Pt3Ir favor formation of a Pt-skin surface layer structure that would resist the acidic electrolyte corrosion during fuel cell operation environments. We chose to focus on Os because the phase diagram for Pt-Ir indicated that Pt-Ir could not form a homogeneous alloy at lower temperature. To determine the performance for ORR, we used QM to examine all intermediates, reaction pathways, and reaction barriers involved in the processes for which protons from the anode reactions react with O₂ to form H₂O. These QM calculations used our Poisson-Boltzmann implicit solvation model include the effects of the solvent (water with dielectric constant 78 with pH 7 at 298K). We found that the rate determination step (RDS) was the O_ad hydration reaction (O_ad + H₂O_ad -> OH_ad + OH_ad) in both cases, but that the barrier for pure Pt of 0.50 eV is reduced to 0.48 eV for Pt₃Os, which at 80 degrees C would increase the rate by 218%. We collaborated with the Pu-Wei Wu’s group to carry out experiments, where we found that the dealloying process-treated Pt2Os catalyst showed two-fold higher activity at 25 degrees C than pure Pt and that the alloy had 272% improved stability, validating our theoretical predictions.

We also carried out similar QM studies followed by experimental validation for the Os/Pt core-shell catalyst fabricated by the underpotential deposition (UPD) method. The QM results indicated that the RDS for ORR is a compromise between the OOH formation step (0.37 eV for Pt, 0.23 eV for Pt_2ML/Os core-shell) and H₂O formation steps (0.32 eV for Pt, 0.22 eV for Pt_2ML/Os core-shell). We found that Pt_2ML/Os has the highest activity (compared to pure Pt and to the Pt₃Os alloy) because the 0.37 eV barrier decreases to 0.23 eV. To understand what aspects of the core shell structure lead to this improved performance, we considered the effect on ORR of compressing the alloy slab to the dimensions of pure Pt. However this had little effect, with the same RDS barrier 0.37 eV. This shows that the ligand effect (the electronic structure modification resulting from the Os substrate) plays a more important role than the strain effect, and is responsible for the improved activity of the core- shell catalyst. Experimental materials characterization proves the core-shell feature of our catalyst. The electrochemical experiment for Pt_2ML/Os/C showed 3.5 to 5 times better ORR activity at 0.9V (vs. NHE) in 0.1M HClO₄ solution at 25 degrees C as compared to those of commercially available Pt/C. The excellent correlation between experimental half potential and the OH binding energies and RDS barriers validate the feasibility of predicting catalyst activity using QM calculation and a simple Langmuir–Hinshelwood model.

In part II, we used QM calculations to study methane stream reforming on a Ni-alloy catalyst surfaces for solid oxide fuel cell (SOFC) application. SOFC has wide fuel adaptability but the coking and sulfur poisoning will reduce its stability. Experimental results suggested that the Ni4Fe alloy improves both its activity and stability compared to pure Ni. To understand the atomistic origin of this, we carried out QM calculations on surface segregation and found that the most stable configuration for Ni₄Fe has a Fe atom distribution of (0%, 50%, 25%, 25%, 0%) starting at the bottom layer. We calculated that the binding of C atoms on the Ni4Fe surface is 142.9 Kcal/mol, which is about 10 Kcal/mol weaker compared to the pure Ni surface. This weaker C binding energy is expected to make coke formation less favorable, explaining why Ni₄Fe has better coking resistance. This result confirms the experimental observation. The reaction energy barriers for CHx decomposition and C binding on various alloy surface, Ni₄X (X=Fe, Co, Mn, and Mo), showed Ni₄Fe, Ni₄Co, and Fe₄Mn all have better coking resistance than pure Ni, but that only Ni₄Fe and Fe₄Mn have (slightly) improved activity compared to pure Ni.

In part III, we used QM to examine the proton transport in doped perovskite-ceramics. Here we used a 2x2x2 supercell of perovskite with composition Ba₈X₇M₁(OH)₁O₂₃ where X=Ce or Zr and M=Y, Gd, or Dy. Thus in each case a 4⁺ X is replace by a 3⁺ M plus a proton on one O. Here we predicted the barriers for proton diffusion allowing both includes intra-octahedron and inter-octahedra proton transfer. Without any restriction, we only observed the inter-octahedra proton transfer with similar energy barrier as previous computational work but 0.2 eV higher than experimental result for Y doped zirconate. For one restriction in our calculations is that the O_donor-O_acceptor atoms were kept at fixed distances, we found that the barrier difference between cerates/zirconates with various dopants are only 0.02~0.03 eV. To fully address performance one would need to examine proton transfer at grain boundaries, which will require larger scale ReaxFF reactive dynamics for systems with millions of atoms. The QM calculations used here will be used to train the ReaxFF force field.

Local thermal fixing of a photorefractive LiNbO3 hologram by use of a CO2 laser

A real-time, in situ fixing method by use of heating with a CO2 laser beam is suggested for thermal fixing of a small local hologram in the bulk of a Fe:LiNbO3 photorefractive crystal. For heating up to 100 degrees C-200 degrees C a volume with a shape similar to that of the laser beam a heat-guiding technique is developed. On the basis of the heat-transfer equations, different heating modes with or without metal absorbers for heat guiding-obtained by use of a continuous or pulsed laser beam are analyzed. The optimal mode may be pulsed heating with absorbers. On this basis experiments have been designed and demonstrated. It is seen that the fixing process with CO2 laser beam is short compared with the process by use of an oven, and the fixing efficiency is quite high. (C) 1998 Optical Society of America.

Sinusoidal phase-modulating laser diode interferometer for measuring angular displacement

We propose a sinusoidal phase-modulating laser diode interferometer for measuring small angular displacement. The interferometer is based on a Fabry-Perot plate. It has a simple structure and is insensitive to external disturbance. Sinusoidal phase-modulating interferometry is used for improving the measurement accuracy. A charge-coupled device (CCD) image sensor is used for measuring the distance between the reflected beams from two faces of the Fabry-Perot plate. From the distance, the initial angle of incidence is calculated. Compared with Michelson interferometers and autocollimators, this interferometer has the advantage of compact size and simple structure. The numerical calculation and experimental results verify the usefulness of this novel interferometer. (C) 2004 Society of Photo-Optical Instrumentation Engineers.

Optimization of the multiwavelength erbium-doped fiber laser in a unidirectional cavity without an isolator

A highly uniform multiwavelength erbium-doped fiber ring laser with an intracavity sine phase modulator is demonstrated. The flat output spectrum is achieved by optimizing the cavity structure, modulation amplitude, and frequency of the sine phase modulator. Fifteen lasing lines with wavelength spacing of 0.9 nm appear simultaneously and stably with power differences less than 2 dB and side-mode suppression ratio higher than 32 dB. In addition, the proposed cavity can support unidirectional operation without optical isolators. An output power difference of about 20 dB is realized between the counterclockwise and clockwise directions, which is almost independent of the pump power and lasing wavelengths. (c) 2005 Society of Photo-Optical Instrumentation Engineers.

Distortion of beam shape by a rotating double-prism wide-angle laser beam scanner

We describe the rigorous results of a wide-angle laser beam scanner, obtained with the help of the vector refraction theory. Using the rigorous results, the distortion of the beam shape is discussed. The distortion to the beam varies with the different relative angles of double prisms. The scanner expands the beam in some directions while it contracts the beam in other directions. According to the conservation of energy, the distribution of the laser intensity is changed as well. (c) 2006 Society of Photo-Optical Instrumentation Engineers.

Study of the transmitter antenna gain for intersatellite laser communications

The gain of a transmitter for intersatellite communications is closely related to the performance of all the links. We calculate the transmitter telescope's gain with the help of the rigorous scalar diffraction theory and equivalent optical layout method. Furthermore, a comparison is performed with the conventional imaging method. The results show that the stop inside the telescope can affect the gain of the telescope. Finally, the gain is calculated under the condition of the aberrations. We find that different aberrations cause different effects. (C) 2006 Society of Photo-Optical Instrumentation Engineers.

Lau cavity and phase locking of laser arrays

The Lau cavity is the self-imaging cavity with a phase corrector under the Lau reimaging condition. The author proposes the use of the Lau cavity to utilize both the Talbot and the Lau effects for phase locking one-dimensional and two-dimensional diode-laser arrays into a single-lobe coherent beam. Analyses on the self-reproducing of a coherent lasing field and the reimaging of initial incoherent radiation are given.

The effect of the rotating double-prism wide-angle laser beam scanner on the beam shape

In this paper, we describe a wide-angle laser beam scanner and the rigorous result of the wide-angle laser beam scanner was obtained with the help of the vector refraction theory. Using the rigorous results, the distortion of the beam shape was discussed. The distortion of the beam shape is varying with the different relative angles of the double prisms. According to the conservation of the energy, the distribution of the laser intensity is changed too. (c) 2005 Elsevier GmbH. All rights reserved.

Experimental study of the Talbot effect under femtosecond laser illumination

Experimental results of the Talbot effect of an amplitude grating under femtosecond laser illumination are reported. Compared with Talbot image under continuous wave (CW) illumination, Talbot images under femtosecond laser illumination are different due to the wide spectral bandwidth and the Talbot images are more distorted at longer Talbot distances. The spectrums and the pulsewidths of femtosecond laser pulses are measured with the frequency-resolved optical gating (FROG) apparatus. Experimental results are in good agreement with the theoretical analysis. (c) 2005 Elsevier B.V. All rights reserved.

Splitting of femtosecond laser pulses by using a Dammann grating and compensation gratings

When a Dammann grating is used to split a beam of femtosecond laser pulses into multiple equal-intensity beams, chromatic dispersion will occur in beams of each order of diffraction and with different scale of angular dispersion because the incident ultrashort pulse contains a broad range of spectral bandwidths. We propose a novel method in which the angular dispersion can be compensated by positioning an m-time-density grating to collimate the mth-order beam that has been split, producing an array of beams that are free of angular dispersion. The increased width of the compensated output pulses and the spectral walk-off effect are discussed. We have verified this approach theoretically and validated it through experiments. It should be highly interesting in practical applications of splitting femtosecond laser pulses for pulse-width measurement, pump-probe measurement, and micromachining at multiple points. (c) 2005 Optical Society of America.

Femtosecond laser speckles

The concept of femtosecond laser speckles is put forward. The theory of a speckle pattern in light of finite bandwidth is applied to describe femtosecond laser speckles. Basic representations of the contrast and the spectral correlation of femtosecond laser speckles are presented. The relationship between the speckle contrast and the bandwidth of a femtosecond laser is given. Experimental results are given that indicate an obvious difference between the speckle patterns produced by a continuous-wave laser and those produced by a femtosecond laser. (c) 2005 Optical Society of America

Coherence measurement of a Ti:sapphire femtosecond pulsed laser

The interference patterns produced by Gaussian-shaped broad-bandwidth femtosecond pulsed laser sources are derived. The interference pattern contains both spatial and temporal properties of laser beam. Interference intensity dependent on the bandwidth of femtosecond laser are given. We demonstrate experimentally both the spatial and the temporal coherence properties of a Ti:sapphire femtosecond pulse laser, as well as its power spectrum by using a pinhole pair.

Magnetic field and pressure effects in a saturated gas laser amplifier

Theoretical and experimental studies of a gas laser amplifier are presented, assuming the amplifier is operating with a saturating optical frequency signal. The analysis is primarily concerned with the effects of the gas pressure and the presence of an axial magnetic field on the characteristics of the amplifying medium. Semiclassical radiation theory is used, along with a density matrix description of the atomic medium which relates the motion of single atoms to the macroscopic observables. A two-level description of the atom, using phenomenological source rates and decay rates, forms the basis of our analysis of the gas laser medium. Pressure effects are taken into account to a large extent through suitable choices of decay rate parameters.

Two methods for calculating the induced polarization of the atomic medium are used. The first method utilizes a perturbation expansion which is valid for signal intensities which barely reach saturation strength, and it is quite general in applicability. The second method is valid for arbitrarily strong signals, but it yields tractable solutions only for zero magnetic field or for axial magnetic fields large enough such that the Zeeman splitting is much larger than the power broadened homogeneous linewidth of the laser transition. The effects of pressure broadening of the homogeneous spectral linewidth are included in both the weak-signal and strong-signal theories; however the effects of Zeeman sublevel-mixing collisions are taken into account only in the weak-signal theory.

The behavior of a He-Ne gas laser amplifier in the presence of an axial magnetic field has been studied experimentally by measuring gain and Faraday rotation of linearly polarized resonant laser signals for various values of input signal intensity, and by measuring nonlinearity - induced anisotropy for elliptically polarized resonant laser signals of various input intensities. Two high-gain transitions in the 3.39-μ region were used for study: a J = 1 to J = 2 (3s₂ → 3p₄) transition and a J = 1 to J = 1 (3s₂ → 3p₂) transition. The input signals were tuned to the centers of their respective resonant gain lines.

The experimental results agree quite well with corresponding theoretical expressions which have been developed to include the nonlinear effects of saturation strength signals. The experimental results clearly show saturation of Faraday rotation, and for the J = 1 t o J = 1 transition a Faraday rotation reversal and a traveling wave gain dip are seen for small values of axial magnetic field. The nonlinearity induced anisotropy shows a marked dependence on the gas pressure in the amplifier tube for the J = 1 to J = 2 transition; this dependence agrees with the predictions of the general perturbational or weak signal theory when allowances are made for the effects of Zeeman sublevel-mixing collisions. The results provide a method for measuring the upper (neon 3s₂) level quadrupole moment decay rate, the dipole moment decay rates for the 3s₂ → 3p₄ and 3s₂ → 3p₂ transitions, and the effects of various types of collision processes on these decay rates.