Controllable group velocity of the probe light in a Lambda-type system with two fold levels

The group velocities of the probe laser field are studied in a A-type system where one lower state has two fold levels coupled by a control field. It is found that the interaction of double dark states leads to controllable group velocity of the probe field in this system. It can be easily realized, due to the interacting double dark resonances, that one of the group velocities at transparency positions is much slower than the other by tuning the control field to be off resonance. In particular, when the control field is on resonance. we can obtain two equal slow group velocities with a broader EIT width, which provides potential applications in quantum storage and retrieval of light. (c) 2005 Elsevier B.V. All rights reserved.

用半导体激光器对 Yb3+:LYSO 晶体的高效率激光特性的研究

本文报导了采用半导体激光器泵浦的高效连续可调谐Yb:LYSO激光器的输出特性。LYSO晶体同时具有LSO晶体良好的激光性能和YSO晶体易于生长且成本低廉的优点，实验中我们采用5at%掺杂的Yb:LYSO晶体进行研究，获得了最大输出功率2.84W、输出波长1085nm、光-光转换效率54.5%的高效输出。并且得到了1030-1111nm，一共81nm的波长调谐范围，这是目前我们所知道的从Yb:LYSO激光器获得的最宽的调谐输出。

Comparison of laser performances of 5at.% Yb : Gd2xY2(1-x)SiO5 crystals between different cutting directions

We investigate the laser actions of 5at.% Yb:Gd2xY2(1-x)SiO5 (Yb:GYSO; x = 0.1) crystals with different cutting directions, parallel and vertical to the growth axis. Our results show that the cutting direction of the sample plays an astonished role in the laser operation. The sample cut vertically to the growth axis possesses the favourable lasing characteristics. Its output power reaches 3.13W at 1060nm with a slope efficiency of 44.68% when the absorbed pump power is 8.9 W. In contrast, the sample cut parallel reaches only 1.65 W at 1044 nm with a slope elLiciency of 33.76% with absorbed pump power of 7.99 W. The absorption and emission spectra of the two samples are examined and the merit factor M is calculated. Our analysis is in agreement well with the experimental results. The wavelength tuning range of the superior sample covers from 1013.68 nm to 1084.82 nm.

Laser intensity dependence of high-order harmonic generation from aligned CO2 molecules

We investigate experimentally the high-order harmonic generation from aligned CO2 molecules and demonstrate that the modulation inversion of the harmonic yield with respect to molecular alignment can be altered dramatically by fine-tuning the intensity of the driving laser pulse for harmonic generation. The results can be modeled by employing the strong field approximation including a ground state depletion factor. The laser intensity is thus proved to be a parameter that can control the high-harmonic emission from aligned molecules.

Widely tunable quasi-phase-matched optical parametric amplification in infrared region using periodically poled lithium niobate

Widely tunable optical parametric amplification (OPA) in the IR region through quasi-phase-matching technology is demonstrated theoretically in periodically-poled lithium niobate (PPLN). For a 532nm pump wavelength and a broadband signal wavelength near 1300 nm, we can obtain the optimum grating period from phase-matching curves for different grating periods to achieve continuously tunable OPA by tuning the angle in a small range. Tunable OPA range of 200nm near 1300 mn can be obtained with a tuning incidence signal angle of 2.2 degrees.

Optimization of optical parametric chirped pulse amplification with different pump wavelengths

Optical parametric chirped pulse amplification with different pump wavelengths was investigated using LBO crystal, at signal central wavelength of 800 nm. According to our theoretical simulation, when pump wavelength is 492.5 nm, there is a maximal gain bandwidth of 190 nm. centered at 805 nm in optimal noncollinear angle using LBO. Presently, pump wavelength of 492.5 nm can be obtained from second harmonic generation of a Yb:Sr-5(PO4)(3)F laser. The broad gain bandwidth can completely support similar to 6 fs with a spectral centre of seed pulse at 800 nm. The deviation from optimal noncollinear angle can be compensated by accurately tuning crystal angle for phase matching. The gain spectrum with pump wavelength of 492.5 nm is much better than those with pump wavelengths of 400, 526.5 and 532 nm, at signal centre of 800 nm. (c) 2005 Elsevier B.V. All rights reserved.

Phase conjugation via four-wave mixing in a resonant medium

This thesis describes the theoretical solution and experimental verification of phase conjugation via nondegenerate four-wave mixing in resonant media. The theoretical work models the resonant medium as a two-level atomic system with the lower state of the system being the ground state of the atom. Working initially with an ensemble of stationary atoms, the density matrix equations are solved by third-order perturbation theory in the presence of the four applied electro-magnetic fields which are assumed to be nearly resonant with the atomic transition. Two of the applied fields are assumed to be non-depleted counterpropagating pump waves while the third wave is an incident signal wave. The fourth wave is the phase conjugate wave which is generated by the interaction of the three previous waves with the nonlinear medium. The solution of the density matrix equations gives the local polarization of the atom. The polarization is used in Maxwell's equations as a source term to solve for the propagation and generation of the signal wave and phase conjugate wave through the nonlinear medium. Studying the dependence of the phase conjugate signal on the various parameters such as frequency, we show how an ultrahigh-Q isotropically sensitive optical filter can be constructed using the phase conjugation process.

In many cases the pump waves may saturate the resonant medium so we also present another solution to the density matrix equations which is correct to all orders in the amplitude of the pump waves since the third-order solution is correct only to first-order in each of the field amplitudes. In the saturated regime, we predict several new phenomena associated with degenerate four-wave mixing and also describe the ac Stark effect and how it modifies the frequency response of the filtering process. We also show how a narrow bandwidth optical filter with an efficiency greater than unity can be constructed.

In many atomic systems the atoms are moving at significant velocities such that the Doppler linewidth of the system is larger than the homogeneous linewidth. The latter linewidth dominates the response of the ensemble of stationary atoms. To better understand this case the density matrix equations are solved to third-order by perturbation theory for an atom of velocity v. The solution for the polarization is then integrated over the velocity distribution of the macroscopic system which is assumed to be a gaussian distribution of velocities since that is an excellent model of many real systems. Using the Doppler broadened system, we explain how a tunable optical filter can be constructed whose bandwidth is limited by the homogeneous linewidth of the atom while the tuning range of the filter extends over the entire Doppler profile.

Since it is a resonant system, sodium vapor is used as the nonlinear medium in our experiments. The relevant properties of sodium are discussed in great detail. In particular, the wavefunctions of the 3S and 3P states are analyzed and a discussion of how the 3S-3P transition models a two-level system is given.

Using sodium as the nonlinear medium we demonstrate an ultrahigh-Q optical filter using phase conjugation via nondegenerate four-wave mixing as the filtering process. The filter has a FWHM bandwidth of 41 MHz and a maximum efficiency of 4 x 10^-3. However, our theoretical work and other experimental work with sodium suggest that an efficient filter with both gain and a narrower bandwidth should be quite feasible.

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.

Investigation of near-collinear degenerated quasi-phase matching optical parametric amplification using PPKTP crystal

The gain properties of near-collinear degenerated phase-matched optical parametric amplification (OPA) using PPKTP crystal are investigated theoretically. The results indicate that the type-0 phase matching of PPKTP has larger accepted angle and better gain spectrum by tuning crystal temperature or rotating crystal angle.

Investigation of noncollinear QPM optical parametric amplification based on periodically poled KTP

The properties of noncollinear optical parametric amplification based on quasi-phase matching of periodically poled KTP are investigated theoretically. Our numerical simulation focuses on the gain spectrum of dependence upon noncollinear angle, crystal temperature and crystal angle. At the optimal noncollinear angle and grating period with fixed temperature, there exists a broadest gain bandwidth about 130 nm at signal wavelength of 800 nm. The deviation from optimal noncollinear angle can be compensated by accurately tuning the crystal angle or temperature with a fixed grating period for phase matching. (c) 2004 Elsevier B.V. All rights reserved.

Enhancement of Kerr nonlinearity with vanishing absorption in a tripod scheme

The giant enhancement of Kerr nonlinearity in a four-level tripod type system is investigated theoretically. By tuning the value of the Rabi frequency of the coherent control field, owing to the double dark resonances, the giant-enhanced Kerr nonlinearity can be achieved within the right transparency window. The in fluence of Doppler broadening is also discussed.

Biological electron transfer in copper proteins

Nature has used a variety of protein systems to mediate electron transfer. In this thesis I examine aspects of the control of biological electron transfer by two copper proteins that act as natural electron carriers.

In the first study, I have made a mutation to one of the ligand residues in the azurin blue copper center, methionine 121 changed to a glutamic acid. Studies of intramolecular electron transfer rates from that mutated center to covalently attached ruthenium complexes indicate that the weak axial methionine ligand is important not only for tuning the reduction potential of the blue copper site but also for maintaining the low reorganization energy that is important for fast electron transfer at long distances.

In the second study, I begin to examine the reorganization energy of the purple copper center in the CuA domain of subunit II of cytochrome c oxidase. In this copper center, the unpaired electron is delocalized over the entire binuclear site. Because long-range electron transfer into and out of this center occurs over long distances with very small driving forces, the reorganization energy of the CuA center has been predicted to be extremely low. I describe a strategy for measuring this reorganization energy starting with the construction of a series of mutations introducing surface histidines. These histidines can then be labeled with a series of ruthenium compounds that differ primarily in their reduction potentials. The electron transfer rates to these ruthenium compounds can then be used to determine the reorganization energy of the CuA site.

Low-noise THz Niobium SIS Mixers

This thesis describes the development of low-noise heterodyne receivers at THz frequencies for submillimeter astronomy using Nb-based superconductor-insulator-superconductor (SIS) tunneling junctions. The mixers utilize a quasi-optical configuration which consists of a planar twin-slot antenna and antisymmetrically-fed two-junctions on an antireflection-coated silicon hyperhemispherical lens. On-chip integrated tuning circuits, in the form of microstrip lines, are used to obtain maximum coupling efficiency in the designed frequency band. To reduce the rf losses in the integrated tuning circuits above the superconducting Nb gap frequency (~ 700 GHz), normal-metal Al is used to replace Nb as the tuning circuits.

To account the rf losses in the micros trip lines, we calculated the surface impedance of the AI films using the nonlocal anomalous skin effect for finite thickness films. Nb films were calculated using the Mattis-Bardeen theory in the extreme anomalous limit. Our calculations show that the losses of the Al and Nb microstrip lines are about equal at 830 GHz. For Al-wiring and Nb-wiring mixers both optimized at 1050 GHz, the RF coupling efficiency of Al-wiring mixer is higher than that of Nb-wiring one by almost 50%. We have designed both Nb-wiring and Al-wiring mixers below and above the gap frequency.

A Fourier transform spectrometer (FTS) has been constructed especially for the study of the frequency response of SIS receivers. This FTS features large aperture size (10 inch) and high frequency resolution (114 MHz). The FTS spectra, obtained using the SIS receivers as direct detectors on the FTS, agree quite well with our theoretical simulations. We have also, for the first time, measured the FTS heterodyne response of an SIS mixer at sufficiently high resolution to resolve the LO and the sidebands. Heterodyne measurements of our SIS receivers with Nb-wiring or Al-wiring have yielded results which arc among the best reported to date for broadband heterodyne receivers. The Nb-wiring mixers, covering 400 - 850 GHz band with four separate fixed-tuned mixers, have uncorrected DSB receiver noise temperature around 5hv/k_b to 700 GHz, and better than 540 K at 808 GHz. An Al-wiring mixer designed for 1050 GHz band has an uncorrected DSB receiver noise temperature 840 K at 1042 GHz and 2.5 K bath temperature. Mixer performance analysis shows that Nb junctions can work well up to twice the gap frequency and the major cause of loss above the gap frequency is the rf losses in the microstrip tuning structures. Further advances in THz SIS mixers may be possible using circuits fabricated with higher-gap superconductors such as NbN. However, this will require high-quality films with low RF surface resistance at THz frequencies.

Nonlinear Effects in Granular Crystals with Broken Periodicity

When studying physical systems, it is common to make approximations: the contact interaction is linear, the crystal is periodic, the variations occurs slowly, the mass of a particle is constant with velocity, or the position of a particle is exactly known are just a few examples. These approximations help us simplify complex systems to make them more comprehensible while still demonstrating interesting physics. But what happens when these assumptions break down? This question becomes particularly interesting in the materials science community in designing new materials structures with exotic properties In this thesis, we study the mechanical response and dynamics in granular crystals, in which the approximation of linearity and infinite size break down. The system is inherently finite, and contact interaction can be tuned to access different nonlinear regimes. When the assumptions of linearity and perfect periodicity are no longer valid, a host of interesting physical phenomena presents itself. The advantage of using a granular crystal is in its experimental feasibility and its similarity to many other materials systems. This allows us to both leverage past experience in the condensed matter physics and materials science communities while also presenting results with implications beyond the narrower granular physics community. In addition, we bring tools from the nonlinear systems community to study the dynamics in finite lattices, where there are inherently more degrees of freedom. This approach leads to the major contributions of this thesis in broken periodic systems. We demonstrate the first defect mode whose spatial profile can be tuned from highly localized to completely delocalized by simply tuning an external parameter. Using the sensitive dynamics near bifurcation points, we present a completely new approach to modifying the incremental stiffness of a lattice to arbitrary values. We show how using nonlinear defect modes, the incremental stiffness can be tuned to anywhere in the force-displacement relation. Other contributions include demonstrating nonlinear breakdown of mechanical filters as a result of finite size, and the presents of frequency attenuation bands in essentially nonlinear materials. We finish by presenting two new energy harvesting systems based on our experience with instabilities in weakly nonlinear systems.

First principles based multiparadigm modeling of electronic structures and dynamics

Electronic structures and dynamics are the key to linking the material composition and structure to functionality and performance.

An essential issue in developing semiconductor devices for photovoltaics is to design materials with optimal band gaps and relative positioning of band levels. Approximate DFT methods have been justified to predict band gaps from KS/GKS eigenvalues, but the accuracy is decisively dependent on the choice of XC functionals. We show here for CuInSe₂ and CuGaSe₂, the parent compounds of the promising CIGS solar cells, conventional LDA and GGA obtain gaps of 0.0-0.01 and 0.02-0.24 eV (versus experimental values of 1.04 and 1.67 eV), while the historically first global hybrid functional, B3PW91, is surprisingly the best, with band gaps of 1.07 and 1.58 eV. Furthermore, we show that for 27 related binary and ternary semiconductors, B3PW91 predicts gaps with a MAD of only 0.09 eV, which is substantially better than all modern hybrid functionals, including B3LYP (MAD of 0.19 eV) and screened hybrid functional HSE06 (MAD of 0.18 eV).

The laboratory performance of CIGS solar cells (> 20% efficiency) makes them promising candidate photovoltaic devices. However, there remains little understanding of how defects at the CIGS/CdS interface affect the band offsets and interfacial energies, and hence the performance of manufactured devices. To determine these relationships, we use the B3PW91 hybrid functional of DFT with the AEP method that we validate to provide very accurate descriptions of both band gaps and band offsets. This confirms the weak dependence of band offsets on surface orientation observed experimentally. We predict that the CBO of perfect CuInSe₂/CdS interface is large, 0.79 eV, which would dramatically degrade performance. Moreover we show that band gap widening induced by Ga adjusts only the VBO, and we find that Cd impurities do not significantly affect the CBO. Thus we show that Cu vacancies at the interface play the key role in enabling the tunability of CBO. We predict that Na further improves the CBO through electrostatically elevating the valence levels to decrease the CBO, explaining the observed essential role of Na for high performance. Moreover we find that K leads to a dramatic decrease in the CBO to 0.05 eV, much better than Na. We suggest that the efficiency of CIGS devices might be improved substantially by tuning the ratio of Na to K, with the improved phase stability of Na balancing phase instability from K. All these defects reduce interfacial stability slightly, but not significantly.

A number of exotic structures have been formed through high pressure chemistry, but applications have been hindered by difficulties in recovering the high pressure phase to ambient conditions (i.e., one atmosphere and room temperature). Here we use dispersion-corrected DFT (PBE-ulg flavor) to predict that above 60 GPa the most stable form of N₂O (the laughing gas in its molecular form) is a 1D polymer with an all-nitrogen backbone analogous to cis-polyacetylene in which alternate N are bonded (ionic covalent) to O. The analogous trans-polymer is only 0.03-0.10 eV/molecular unit less stable. Upon relaxation to ambient conditions both polymers relax below 14 GPa to the same stable non-planar trans-polymer, accompanied by possible electronic structure transitions. The predicted phonon spectrum and dissociation kinetics validate the stability of this trans-poly-NNO at ambient conditions, which has potential applications as a new type of conducting polymer with all-nitrogen chains and as a high-energy oxidizer for rocket propulsion. This work illustrates in silico materials discovery particularly in the realm of extreme conditions.

Modeling non-adiabatic electron dynamics has been a long-standing challenge for computational chemistry and materials science, and the eFF method presents a cost-efficient alternative. However, due to the deficiency of FSG representation, eFF is limited to low-Z elements with electrons of predominant s-character. To overcome this, we introduce a formal set of ECP extensions that enable accurate description of p-block elements. The extensions consist of a model representing the core electrons with the nucleus as a single pseudo particle represented by FSG, interacting with valence electrons through ECPs. We demonstrate and validate the ECP extensions for complex bonding structures, geometries, and energetics of systems with p-block character (C, O, Al, Si) and apply them to study materials under extreme mechanical loading conditions.

Despite its success, the eFF framework has some limitations, originated from both the design of Pauli potentials and the FSG representation. To overcome these, we develop a new framework of two-level hierarchy that is a more rigorous and accurate successor to the eFF method. The fundamental level, GHA-QM, is based on a new set of Pauli potentials that renders exact QM level of accuracy for any FSG represented electron systems. To achieve this, we start with using exactly derived energy expressions for the same spin electron pair, and fitting a simple functional form, inspired by DFT, against open singlet electron pair curves (H₂ systems). Symmetric and asymmetric scaling factors are then introduced at this level to recover the QM total energies of multiple electron pair systems from the sum of local interactions. To complement the imperfect FSG representation, the AMPERE extension is implemented, and aims at embedding the interactions associated with both the cusp condition and explicit nodal structures. The whole GHA-QM+AMPERE framework is tested on H element, and the preliminary results are promising.