Ion acceleration with mixed solid targets interacting with circularly polarized lasers

The interaction of a circularly polarized laser pulse with a mixed solid target containing two species of ions is studied by particle in cell simulations and analytical model. After the interaction tends to be stable, it is demonstrated that the acceleration is more efficient for the heavier ions than that in plasmas containing a single kind of heavy ion and the acceleration efficiency is higher when its proportion is lower. To obtain monoenergetic heavy-ion beams, a sandwich target with a thin mixed ion layer between two light ion layers and a microstructured target are proposed. The influences of parameters of the laser pulse and target on ion acceleration are discussed in detail. It is found that, when the target is thick enough, a cold target is more appropriate for heavy-ion acceleration than a warm target, and the velocity of the reflected heavy ions is proportional to the laser amplitude.

Theoretical and experimental study on femtosecond laser induced damage in CaF2 crystals

We report on the damage threshold in CaF2 crystals induced by femtosecond laser at wavelengths of 800 nm and 400 nm, respectively. The dependences of ablation depths and ablation volumes on laser fluences are also presented. We investigate theoretically the coupling constants between phonon and conduction band electrons (CBE), and calculate the rates of CBE absorbing laser energy. A theoretical model including CBE production, laser energy deposition, and CBE diffusion is applied to study the damage mechanisms. Our results indicate that energy diffusion greatly influences damage threshold and ablation depth.

Ultraviolet-infrared femtosecond laser-induced damage in fused silica and CaF2 crystals

The damage in fused silica and CaF2 crystals induced by wavelength tunable femtosecond lasers is studied. The threshold fluence is observed to increase rapidly with laser wavelength lambda in the region of 250-800 nm, while it is nearly a constant for 800

Crystal Coulomb energies: I. Organic donor-acceptor complexes--a review. II. Classical Ewald calculations of the Coulomb binding energy of four donor-acceptor crystals and Wurster's blue perchlorate. III. A rapid-convergence quantum-mechanical formalism for crystal electronic energies

Chapter I

Theories for organic donor-acceptor (DA) complexes in solution and in the solid state are reviewed, and compared with the available experimental data. As shown by McConnell et al. (Proc. Natl. Acad. Sci. U.S., 53, 46-50 (1965)), the DA crystals fall into two classes, the holoionic class with a fully or almost fully ionic ground state, and the nonionic class with little or no ionic character. If the total lattice binding energy 2ε₁ (per DA pair) gained in ionizing a DA lattice exceeds the cost 2ε_o of ionizing each DA pair, ε₁ + ε_o less than 0, then the lattice is holoionic. The charge-transfer (CT) band in crystals and in solution can be explained, following Mulliken, by a second-order mixing of states, or by any theory that makes the CT transition strongly allowed, and yet due to a small change in the ground state of the non-interacting components D and A (or D⁺ and A^-). The magnetic properties of the DA crystals are discussed.

Chapter II

A computer program, EWALD, was written to calculate by the Ewald fast-convergence method the crystal Coulomb binding energy E_C due to classical monopole-monopole interactions for crystals of any symmetry. The precision of E_C values obtained is high: the uncertainties, estimated by the effect on E_C of changing the Ewald convergence parameter η, ranged from ± 0.00002 eV to ± 0.01 eV in the worst case. The charge distribution for organic ions was idealized as fractional point charges localized at the crystallographic atomic positions: these charges were chosen from available theoretical and experimental estimates. The uncertainty in E_C due to different charge distribution models is typically ± 0.1 eV (± 3%): thus, even the simple Hückel model can give decent results.

E_C for Wurster's Blue Perchl orate is -4.1 eV/molecule: the crystal is stable under the binding provided by direct Coulomb interactions. E_C for N-Methylphenazinium Tetracyanoquino- dimethanide is 0.1 eV: exchange Coulomb interactions, which cannot be estimated classically, must provide the necessary binding.

EWALD was also used to test the McConnell classification of DA crystals. For the holoionic (1:1)-(N,N,N',N'-Tetramethyl-para- phenylenediamine: 7,7,8,8-Tetracyanoquinodimethan) E_C = -4.0 eV while 2ε_o = 4.6₅ eV: clearly, exchange forces must provide the balance. For the holoionic (1:1)-(N,N,N',N'-Tetramethyl-para- phenylenediamine:para-Chloranil) E_C = -4.4 eV, while 2ε_o = 5.0 eV: again EC falls short of 2ε₁. As a Gedankenexperiment, two nonionic crystals were assumed to be ionized: for (1:1)-(Hexamethyl- benzene:para-Chloranil) E_C = -4.5 eV, 2ε_o = 6.6 eV; for (1:1)- (Napthalene:Tetracyanoethylene) E_C = -4.3 eV, 2ε_o = 6.5 eV. Thus, exchange energies in these nonionic crystals must not exceed 1 eV.

Chapter III

A rapid-convergence quantum-mechanical formalism is derived to calculate the electronic energy of an arbitrary molecular (or molecular-ion) crystal: this provides estimates of crystal binding energies which include the exchange Coulomb inter- actions. Previously obtained LCAO-MO wavefunctions for the isolated molecule(s) ("unit cell spin-orbitals") provide the starting-point. Bloch's theorem is used to construct "crystal spin-orbitals". Overlap between the unit cell orbitals localized in different unit cells is neglected, or is eliminated by Löwdin orthogonalization. Then simple formulas for the total kinetic energy Q^(XT)_λ, nuclear attraction [λ/λ]^XT, direct Coulomb [λλ/λ'λ']^XT and exchange Coulomb [λλ'/λ'λ]^XT integrals are obtained, and direct-space brute-force expansions in atomic wavefunctions are given. Fourier series are obtained for [λ/λ]^XT, [λλ/λ'λ']^XT, and [λλ/λ'λ]^XT with the help of the convolution theorem; the Fourier coefficients require the evaluation of Silverstone's two-center Fourier transform integrals. If the short-range interactions are calculated by brute-force integrations in direct space, and the long-range effects are summed in Fourier space, then rapid convergence is possible for [λ/λ]^XT, [λλ/λ'λ']^XT and [λλ'/λ'λ]^XT. This is achieved, as in the Ewald method, by modifying each atomic wavefunction by a "Gaussian convergence acceleration factor", and evaluating separately in direct and in Fourier space appropriate portions of [λ/λ]^XT, etc., where some of the portions contain the Gaussian factor.

Design of adjustable superresolving filters based on birefringent crystals

A two-mode adjustable superresolving filter based on a birefringent filter is proposed. This kind of filter has superresolution in two modes of adjustment. One is rotation of the binary pupil filter on the optical axis of the system and the other is the tilt of the filter away from the pupil plane on axis parallel or perpendicular to the optical axis of the crystal. The filters act as complex amplitude filters in the former mode, and as pure phase filters in the latter. By analyzing two superresolving parameters, we obtain the optimal design parameters that ensure a large field of view, a large superresolving range, and a high setting accuracy. This kind of filter can provide more flexibility in practical applications. (c) 2006 Optical Society of America.

Study of noncollinear quasi-phase matching optical parametric amplification with group-velocity matching based on periodically poled crystals

The properties of noncollinear optical parametric amplification (NOPA) based on quasi-phase matching of periodically poled crystals are investigated, under the condition that the group velocity matching (GVM) of the signal and idler pulses is satisfied. Our study focuses on the dependence of the gain spectrum upon the noncollinear angle, crystal temperature, and crystal angle with periodically poled KTiOPO4 (PPKTP), periodically poled LiNbO3 (PPLN), and periodically poled LiTaO3 (PPLT), and the NOPA gain properties of the three crystals are compared. Broad gain bandwidth exists above 85 nm at a signal wavelength of 800 nm with a 532 nm pump pulse, with proper noncollinear angle and grating period at a fixed temperature for GVM. Deviation from the group-velocity-matched noncollinear angle can be compensated by accurately tuning the crystal angle or temperature with a fixed grating period for phase matching. Moreover, there is a large capability of crystal angle tuning.

Functionalization of Si(111) surfaces and the formation of mixed monolayers for the covalent attachment of molecular catalysts in photoelectrochemical devices

The functionalization of silicon surfaces with molecular catalysts for proton reduction is an important part of the development of a solar-powered, water-splitting device for solar fuel formation. The covalent attachment of these catalysts to silicon without damaging the underlying electronic properties of silicon that make it a good photocathode has proven difficult. We report the formation of mixed monolayer-functionalized surfaces that incor- porate both methyl and vinylferrocenyl or vinylbipyridyl (vbpy) moieties. The silicon was functionalized using reaction conditions analogous to those of hydrosilylation, but instead of a H-terminated Si surface, a chlorine-terminated Si precursor surface was used to produce the linked vinyl-modified functional group. The functionalized surfaces were characterized by time-resolved photoconductivity decay, X-ray photoelectron spectroscopy (XPS), electro- chemical, and photoelectrochemical measurements. The functionalized Si surfaces were well passivated, exhibited high surface coverage and few remaining reactive Si atop sites, had a very low surface recombination velocity, and displayed little initial surface oxidation. The surfaces were stable toward atmospheric and electrochemical oxidation. The surface coverage of ferrocene or bipyridine was controllably varied from 0 up to 30% of a monolayer without loss of the underlying electronic properties of the silicon. Interfacial charge transfer to the attached ferrocene group was relatively rapid, and a photovoltage of 0.4 V was generated upon illumination of functionalized n-type silicon surfaces in CH₃CN. The immobilized bipyridine ligands bound transition metal ions, and thus enabled the assembly of metal complexes on the silicon surface. XPS studies demonstrated that [Cp∗Rh(vbpy)Cl]Cl, [Cp∗Ir(vbpy)Cl]Cl, and Ru(acac)₂vbpy were assembled on the surface. For the surface prepared with iridium, x-ray absorption spectroscopy at the Ir L_III edge showed an edge energy and post-edge features virtually identical to a powder sample of [Cp∗Ir(bipy)Cl]Cl (bipy is 2,2 ́-bipyridyl). Electrochemical studies on these surfaces confirmed that the assembled complexes were electrochemically active.

Mixed entanglement distillation by means of parity measurements

We present a mixed entanglement distillation protocol by means of the parity measurement of qubits. Without the use of controlled-NOT (CNOT) operations, the efficiency of our protocol can approach that of the CNOT protocol. In comparison, the total successful probability of our protocol can reach a quantity twice as large as that of the linear optics-based protocol.

Effects of gamma-irradiation on Al2O3 crystals grown under reducing atmosphere

Gamma-ray irradiation-induced color centers in Al2O3 crystals grown by temperature gradient techniques (TGT) under a strongly reducing atmosphere were studied. The transition F+ -> F takes place during the irradiation process. Glow discharge mass spectroscopy (GDMS) and annealing treatments show that Fe3+ impurity ions are present in the crystals. A composite (F+-Fe3+) defect was presented to explain the origin of the 255 nm band absorption in the TGT-Al2O3 crystals. (C) 2006 Elsevier B.V. All rights reserved.

Femtosecond laser ablation of crystals SiO2 and YAG

Damage threshold of crystals SiO2 and YAG against 60-900 fs, 800 nm laser pulses are reported. The breakdown mechanisms were discussed based on the double-flux model and Keldysh theory. We found that impact ionization plays the important role in the femtosecond laser-induced damage in crystalline SiO2, while the roles of photoionization and impact ionization in YAG crystals depend on the laser pulse durations. (C) 2007 Elsevier B.V. All rights reserved.

Crystals that count! Physical principles and experimental investigations of DNA tile self-assembly

Algorithmic DNA tiles systems are fascinating. From a theoretical perspective, they can result in simple systems that assemble themselves into beautiful, complex structures through fundamental interactions and logical rules. As an experimental technique, they provide a promising method for programmably assembling complex, precise crystals that can grow to considerable size while retaining nanoscale resolution. In the journey from theoretical abstractions to experimental demonstrations, however, lie numerous challenges and complications.

In this thesis, to examine these challenges, we consider the physical principles behind DNA tile self-assembly. We survey recent progress in experimental algorithmic self-assembly, and explain the simple physical models behind this progress. Using direct observation of individual tile attachments and detachments with an atomic force microscope, we test some of the fundamental assumptions of the widely-used kinetic Tile Assembly Model, obtaining results that fit the model to within error. We then depart from the simplest form of that model, examining the effects of DNA sticky end sequence energetics on tile system behavior. We develop theoretical models, sequence assignment algorithms, and a software package, StickyDesign, for sticky end sequence design.

As a demonstration of a specific tile system, we design a binary counting ribbon that can accurately count from a programmable starting value and stop growing after overflowing, resulting in a single system that can construct ribbons of precise and programmable length. In the process of designing the system, we explain numerous considerations that provide insight into more general tile system design, particularly with regards to tile concentrations, facet nucleation, the construction of finite assemblies, and design beyond the abstract Tile Assembly Model.

Finally, we present our crystals that count: experimental results with our binary counting system that represent a significant improvement in the accuracy of experimental algorithmic self-assembly, including crystals that count perfectly with 5 bits from 0 to 31. We show some preliminary experimental results on the construction of our capping system to stop growth after counters overflow, and offer some speculation on potential future directions of the field.

Gamma-ray induced color centers in Yb : YAG crystals grown by Czochralski method

20 at.% Yb:YAG single crystals have been grown by the CZ method and gamma-ray irradiation induced color centers and valence change of Fe3+ and Yb3+ ions in Yb:YAG have been studied. One significant 255 nm absorption band was observed in as-grown crystals and was attributed to Fe3+ ions. Two additional absorption (AA) bands located at 255 nm and 345 nm, respectively, were produced after gamma irradiation. The changes in the AA spectra after gamma irradiation and air annealing are mainly related to the charge exchange of the Fe3+, Fe2+, oxygen vacancies and F-type color centers. Analysis shows that the broad AA band is associated with Fe2+ ions and F-type color centers. The transition Yb3+ Yb2+ takes place as an effect of recharging of one of the Yb3+ ions from a pair in the process of gamma irradiation. (C) 2006 Elsevier Ltd. All rights reserved.