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Thomas F. George

Publications and source records attributed to Thomas F. George.

31 records · Page 2Linked to original sources

Theoretical analysis of nanoparticle-induced homeotropic alignment in nematic liquid crystals

A theoretical analysis of homeotropic alignment induced by nanoparticles (NPs) in a nematic liquid crystal (NLC) sample cell is presented. It is found that such alignment on the surface of a NP causes a change in the orientation of the molecular director near the surface, which in turn induces variations in the elastic constants and free energy. The induced NLC properties allow coupling between nearby NPs, mediated by the NLC molecules. The rotation of the coupled NPs close to the substrate tends to induce a long-range orientation of the NLC molecular director, leading to modification in the alignment at the interface of NLC and substrate which induces the orientation from homogeneous (planar) to homeotropic (vertical) in the bulk material.

physics.optics↗

Magnetic spin moment reduction in photoexcited ferromagnets through exchange interaction quenching: Beyond the rigid band approximation

The exchange interaction among electrons is one of the most fundamental quantum mechanical interactions in nature and underlies any magnetic phenomena from ferromagnetic ordering to magnetic storage. The current technology is built upon a thermal or magnetic field, but a frontier is emerging to directly control magnetism using ultrashort laser pulses. However, little is known about the fate of the exchange interaction. Here we report unambiguously that photoexcitation is capable of quenching the exchange interaction in all three $3d$ ferromagnetic metals. The entire process starts with a small number of photoexcited electrons which build up a new and self-destructive potential that collapses the system into a new state with a reduced exchange splitting. The spin moment reduction follows a Bloch-like law as $M_z(ΔE)=M_z(0)(1-{ΔE}/{ΔE_0})^{\frac{1}β}$, where $ΔE$ is the absorbed photon energy and $β$ is a scaling exponent. A good agreement is found between the experimental and our theoretical results. Our findings may have a broader implication for dynamic electron correlation effects in laser-excited iron-based superconductors, iron borate, rare-earth orthoferrites, hematites and rare-earth transition metal alloys.

cond-mat.mtrl-sci↗

Imaging superatomic molecular orbitals in a ${\bf C_{60}}$ molecule through four 800-nm photons

Superatomic molecular orbitals (SAMO) in C60 are ideal building blocks for functional nanostructures. However, imaging them spatially in the gas phase has been unsuccessful. It is found experimentally that if C60 is excited by an 800-nm laser, the photoelectron casts an anisotropic velocity image, but the image becomes isotropic if excited at a 400-nm wavelength. This diffuse image difference has been attributed to electron thermal ionization, but more recent experiments (800 nm) reveal a clear non-diffuse image superimposed on the diffuse image, whose origin remains a mystery. Here we show that the non-diffuse anisotropic image is the precursor of the $f$ SAMO. We predict that four 800-nm photons can directly access the $1f$ SAMO, and with one more photon, can image the orbital, with the photoelectron angular distribution having two maxima at 0$^\circ$ and 180$^\circ$ and two humps separated by 56.5$^\circ$. Since two 400-nm photons only resonantly excite the spherical $1s$ SAMO and four 800-nm photon excite the anisotropic $1f$ SAMO, our finding gives a natural explanation of the non-diffuse image difference, complementing the thermal scenario.

cond-mat.mtrl-sci↗

On adiabatic evolution for a general time-dependent quantum system

The unitary operator corresponding to the classical canonical transformation that connects a general closed system to an open system under adiabatic conditions is found. The quantum invariant operator of the adiabatic open system is derived from the unitary transformation of the quantum Hamiltonian of the closed system. On the basis of these results, we investigate the evolution of the general quantum adiabatic system and construct a revised adiabatic theorem. The adiabatic theorem developed here exactly reduces to the well-known Berry adiabatic theorem when the control parameter

quant-ph↗

Manipulative resonant nonlinear optics: nonlinear interference effects and quantum control of nonlinearity, dispersion, transparency and inversionless amplification in an extended strongly-absorbing inhomogeneously-broadened medium

Specific features of nonlinear interference processes at quantum transitions in near- and fully-resonant optically-dense Doppler-broadened medium are studied. The feasibility of overcoming of the fundamental limitation on a velocity-interval of resonantly coupled molecules imposed by the Doppler effect is shown based on quantum coherence. This increases the efficiency of nonlinear-optical processes in atomic and molecular gases that possess the most narrow and strongest resonances. The possibility of all-optical switching of the medium to opaque or, alternatively, to absolutely transparent, or even to strongly-amplifying states is explored, which is controlled by a small variation of two driving radiations. The required intensities of the control fields are shown to be typical for cw lasers. These effects are associated with four-wave mixing accompanied by Stokes gain and by their interference in fully- and near-resonant optically-dense far-from-degenerate double-Lambda medium. Optimum conditions for inversionless amplification of short-wavelength radiation above the oscillation threshold at the expense of the longer-wavelength control fields, as well as for Raman gain of the generated idle infrared radiation, are investigated. The outcomes are illustrated with numerical simulations applied to sodium dimer vapor. Similar schemes can be realized in doped solids and in fiber optics.

quant-ph↗

Adiabatic passage and dissociation controlled by interference of two laser-induced continuum structures

We have developed a theory of three-pulse coherent control of photochemical processes. It is based on adiabatic passage and quantum coherence and interference attributed to the lower-lying dissociation continuum and excited upper discrete states, which are otherwise not connected to the ground state by one-photon transitions. Novel opportunities offered by the proposed scheme are demonstrated through extensive numerical simulations with the aid of a model relevant to typical experiments. The opportunities for manipulating the distribution of the population among discrete and continuous states with any necessary ratio by the end of the pulses are demonstrated.

quant-ph↗

Theory of four-wave mixing and accompanying dissociation and population transfer controlled with laser-induced continuum structures

A theory is developed and applied to the study of opportunities and specific features of coherent control of four-wave mixing as well as of the accompanying processes in the continuous-wave regime, which involve transitions between bound and free quantum states. Such opportunities become feasible through constructive and destructive interference of quantum pathways. Two coupling schemes of practical importance are investigated. In the first, a ladder energy level scheme, fully-resonant sum-frequency nonlinear-optical generation of short-wavelength radiation driven by several strong fields is investigated. The relaxation processes as well as absorption of the fundamental and generated radiations, which play an important role, are taken into consideration. It is shown that the generation output can be considerably increased through the appropriate adjustment of several laser-induced continuum structures. In the second, a folded scheme, a possible control of two-photon dissociation (Lambda-scheme) using auxiliary laser radiation applied to the adjacent bound-free transition (V-configuration) is investigated. Besides dissociation, the proposed method enables one to control population transfer between two upper discreet levels via the lower-energy dissociation continuum, while direct transition between these states is not allowed. The opportunities of manipulating these processes as well as of four-wave-mixing-based spectroscopy are explored both analytically and through a numerical simulation for Na_2 dimers.

quant-ph↗

Optics of Nanostructured Fractal Silver Colloids

Based on the theory of the optical properties of fractal clusters, which is an operator-based modification of the coupled-dipole method, an alternate solution is proposed for the problem of adequately describing the evolution of optical spectra of any polydisperse silver colloid with particles falling within the range of most characteristic sizes (5 - 30 nm). This is the range over which the results of the application of the well-known methods of classical electrodynamics, including the Mie theory, disagree with experimental data. The effect of variation of the parameters of such media on optical spectra is studied by a numerical simulation, which accounts for particle electrodynamic dipole-dipole interactions. Indeed, such interactions are shown to be a key factor in determining the broadening of the sol absorption spectra during the course of fractal aggregation. A quantitative explanation is given for the reasons for the appearance of individual specific features in the contours of the spectral absorption of different types of silver colloids.

physics.optics↗

Theory of deep ultraviolet generation at maximum coherence assisted by Stark-chirped two-photon resonance

A scheme is analyzed for effcient generation of vacuum ultraviolet radiation through four-wave mixing processes assisted by the technique of Stark-chirped rapid adiabatic passage. These opportunities are associated with pulse excitation of laddertype short-wavelength two-photon atomic or molecular transitions so that relaxation processes can be neglected. In this three-laser technique, a delayed-pulse of strong oR-resonant infrared radiation sweeps the laser-induced Stark-shift of a two-photon transition in a such way that facilitates robust maximum two-photon coherence induced by the first ultraviolet laser. A judiciously delayed third pulse scatters at this coherence and generates short-wavelength radiation. A theoretical analysis of these problems based on the density matrix is performed. A numerical model is developed to carry out simulations of a typical experiment. The results illustrate a behavior of populations, coherence and generated radiation along the medium as well as opportunities of effcient generation of deep (vacuum) ultraviolet radiation.

quant-ph↗

Ienversionless gain in an optically-dense resonant Doppler-broadened medium

Resonant nonlinear-optical interference processes in four-level Doppler-broadened media are studied. Specific features of amplification and optical switching of short-wavelength radiation in a strongly-absorbing resonant gas under coherent quantum control with two longer wavelength radiations, are investigated. The major outcomes are illustrated with virtual experiments aimed at inversionless short-wavelength amplification, which also address deficiencies in this regard in recent experiments. With numerical simulations related to the proposed experiment in optically-dense sodium dimer vapor, we show optimal condition for optical switching and the expected gain of the probe radiation, which is above the oscillation threshold.

physics.optics↗

Four-wave mixing at maximum coherence and eliminated Doppler broadening controlled with the driving fields

New feasibity of coherent quantum control of four-wave mixing processes in a resonant Doppler-broadened medium are studied. We propose a technique which enables one to enhance the quantum efficiency of nonlinear optical conversion. At the same time, it allows one to decrease the required intensities of the fundamental beams compared to those necessary in the approach based on coherent population trapping. The major outcomes of the analysis are illustrated with numerical simulation addressed within a practical medium.

physics.optics↗

Coherence-controlled transparency and far-from-degenerate parametric gain in a strongly-absorbing Doppler-broadened medium

An inversionless gain of anti-Stokes radiation above the oscillation threshold in an optically-dense far-from-degenerate double-Lambda Doppler-broadened medium accompanied by Stokes gain is predicted. The outcomes are illustrated with numerical simulations applied to sodium dimer vapor. Optical switching from absorption to gain via transparency controlled by a small variation of the medium and of the driving radiation parameters which are at a level less than one photon per molecule is shown. Related video/audio clips see in: A.K. Popov, S.A. Myslivets, and T.F. George, Optics Express Vol. 7, No 3, 148 (2000)(http://epubs.osa.org/oearchive/source/22947.htm) or download: http://kirensky.krasn.ru/popov/opa/opa.htm

quant-ph↗