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Springer eBooks

Theory of Spectroscopy and Dynamics in Laser-Irradiated Adspecies-Surface Systems

Thomas F. George, Daniel A. Jelski, Xi-Yi Huang, A. C. Beri

Published Jan 1, 1987• 0 citations
Publisher
DOI
10.1007/978-94-017-1915-5_10

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A quantum model of a heterogeneous system consisting of a mixture of isotopes adsorbed on a solid surface and subjected to laser radiation is presented. The model system is described by a total Hamiltonian including direct and indirect (surface-phonon-mediated) couplings. The equations of motion are derived in the Heisenberg–Markovian picture in which the many-body effects of the surface phonon modes and the adspecies are reduced to an overall broadening (damping factor) given by the sum of the energy (T1) and phase (T 2) relaxations. The effects of the dephasing and anharmonicity on the average excitation are investigated. The ‘‘bistability’’ feature with a red-shifted optimal detuning is discussed in terms of the solution of a cubic equation. A diagonalization procedure is presented in a new basis which reveals the effects of the coupling strength, the frequency difference, and the level width of the isotopes on the total steady-state excitation, which in turn reflects the surface spectrum of the model system. Finally, the isotope selectivity given by the numerical results of the time-integrated excitation is discussed. It is shown that the optimal detuning for a weak coupling strength is further red-shifted for a strong isotopic coupling strength. Finally, energy feedback effects of the bath modes on the excitations of the active modes are investigated by combining a quantum excitation equation and a classical heat diffusion equation.
Shallow, negatively-charged Nitrogen-Vacancy centers (NV-) in diamond have been proposed for high-sensitivity magnetometry and spin-polarization transfer applications. However, surface effects tend to favor and stabilize the less useful neutral form, the NV0 centers. Here, we report the effects of green laser irradiation on ensembles of nanometer-shallow NV centers in flat and nanostructured diamond surfaces as a function of laser power in a range not previously explored (up to 150 mW/μm2). Raman spectroscopy, optically-detected-magnetic-resonance (ODMR) and charge-photoconversion fluorescence detection are applied to characterize the properties and dynamics of NV- and NV0 centers. We demonstrate that high laser power strongly promotes photoconversion of NV0 to NV- centers. Surprisingly, the excess NV- population is stable over a time scale of one hundred milliseconds after switching off the laser, resulting in long-lived enrichment of shallow NV-. The beneficial effect of photoconversion is less marked in nanostructured samples. Our results are important to inform the design of samples and experimental procedures for applications relying on ensembles of shallow NV- centers in diamond.
We report on the effects of dense optical systems on the static and dynamic properties of laser light. The measurements of the angular irradiance distribution as a function of the optical density and the size of the scattering centers confirm previous measurements performed by Woodward. Our study of the scattered irradiance correlation function indicates that, in the presence of multiple scattering, the relaxation time may be significantly smaller than that predicted on the basis of the single-particle Brownian model. Furthermore, the angular dependence of the irradiance relaxation time deviates from the usual proportionality to the inverse square of the momentum transfer. We discuss a number of tests that have been performed to minimize the possibility that some of our conclusions could be affected in part by particle aggregation, surface charges, and depolarization of the scattered light.