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Journal of Microscopy

State‐selective optical near‐field resonant ionization spectroscopy of atoms near a dielectric surface

Yasuo Ohdaira, K. Kijima, K. Terasawa, Masato Kawai, Hirokazu Hori, Kazuo Kitahara

Published Apr 1, 2001• 8 citations
Publisher

Abstract

Spin-sensitive optical near-field microscopy and spectroscopy are proposed based on the study on the conserved quantities in optical near-field interactions of atoms with dielectric surfaces. A two-step photoionization spectra of Cs atoms resolving hyperfine structures are demonstrated near a planar dielectric surface by using evanescent waves. These techniques of state/spin-selective excitation and highly sensitive detection, combined with the techniques of optical pumping, will open up possibilities of space- and polarization-sensitive detection of optical near-fields using atomic probes. This novel method provides us with a useful technique for the observation of polarization nature of the optical near-field and controlling the spin states of mesoscopic electronic systems.

DOI
10.1046/j.1365-2818.2001.00799.x

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Spin-sensitive optical near-field microscopy and spectroscopy are proposed based on the study on the conserved quantities in optical near-field interactions of atoms with dielectric surfaces. A two-step photoionization spectra of Cs atoms resolving hyperfine structures are demonstrated near a planar dielectric surface by using evanescent waves. These techniques of state/spin-selective excitation and highly sensitive detection, combined with the techniques of optical pumping, will open up possibilities of space- and polarization-sensitive detection of optical near-fields using atomic probes. This novel method provides us with a useful technique for the observation of polarization nature of the optical near-field and controlling the spin states of mesoscopic electronic systems.
Abstract A practical method to measure the spin polarization of optically pumped alkali atoms is demonstrated. In order to realize transverse measurement, the transverse spin component of spin-polarized alkali atoms is created by a rotating exciting magnetic field, and detected using the optical rotation of a near-resonant probe beam for realizing a high detection sensitivity. The dependency of the optical rotation on the spin polarization of 133 Cs atoms is derived theoretically and verified experimentally. By changing the direction of the rotating magnetic field, we realize the transverse measurement of the spin polarization of 133 Cs atoms in either ground-state hyperfine level.
On the basis of the procedure for controlling the spins of atoms using circularly polarized evanescent light proposed by Hori et al.[(1996) Abstracts of the 1st Asia-Pacific Workshop on Near-field Optics] we discuss the influence of boundary conditions on the probability of spontaneous emission and thus on the spin polarization efficiency, which was not considered in the Hori et al. study. Using the Carniglia-Mandel mode expansion of electromagnetic fields, we derive the spontaneous emission and spin polarization probabilities of atoms near a dielectric surface, and show the atom-surface distance dependence and refractive index dependence. Numerical evaluation for the 6P1/2-6S1/2 transition of a Cs atom indicates an increase in the efficiency of spin polarization by 30%.
The penetration depth and pseudomomentum (wave vector) of evanescent electromagnetic waves are measured at a planar dielectric surface by means of laser spectroscopy using the Cs D2{\mathrm{D}}_{2}D2​ line with a wavelength of 852.1 nm. The same experimental setup is employed in all the experiments. The first result shows a sharp, asymmetric absorption profile, which is explained in terms of the thin penetration depth, and the second shows an actual transfer of the pseudomomentum of the surface electromagnetic mode to atoms via a resonance interaction. The measured penetration depth and pseudomomentum agree with the natural interpretation of the complex wave number characterizing evanescent waves at a planar dielectric-vapor interface. Direct excitation of evanescent waves by excited Cs atoms has also been observed as atomic fluorescence emitted into the dielectric material at the angle of total internal reflection. The results are in good agreement with the theoretical predictions and exhibit the characteristics of excitation transfer or tunneling from Cs atoms into the surface mode.
We compare the interactions of spin-polarized Na with glass surfaces that are either bare or silicone coated. For this purpose, we reflect a laser beam that is resonant with the Na atoms from the interface, using an angle of incidence close to the critical angle of total internal reflection. Polarization-selective detection of the reflected light provides information about the ground-state orientation of the atoms, which is created by optical pumping with a second laser beam. Our theoretical description treats the atomic vapor as a homogeneous anisotropic medium characterized by a macroscopic magnetization. Comparative experimental studies performed with silicone-coated and bare glass surfaces provide evidence that wall relaxation can be observed by reflection spectroscopy.
Coherent spin resonance techniques, such as nuclear and electron spin resonance spectroscopy, have revolutionized non-invasive imaging by providing spectrally resolved information about spin dynamics. Motivated by the recent emergence of electron microscopy methods capable of sensing microwave-excitations, we establish a theoretical framework for Spin Resonance Spectroscopy (SRS) in transmission electron microscopy (TEM). This technique combines microwave pump fields with focused electron probe beams to enable state-selective spin imaging at the atomic scale. Using scattering theory, we model the interaction between free-space electrons and electron spin systems, capturing both elastic and inelastic processes. The strongest effect of the spin system on the free electron is a magnetic phase shift. Our simulations demonstrate that phase shifts from individual electron spins are detectable in both image mode and diffraction mode. In principle, differential measurements under microwave control allow the extraction of local resonance frequencies that are influenced by the surrounding spin environment. By evaluating the Classical Fisher Information (CFI), we identify imaging conditions that maximize the signal-to-noise ratio (SNR), showing how defocus and beam width affect the measurement sensitivity. These findings establish a foundation for integrating SRS with high-resolution TEM, bridging spin spectroscopy and atomic-scale imaging, and enabling new capabilities in quantum spin research and nanoscale materials characterization.
Non-intrusive laser-spectroscopical methods for the diagnostics of the gas-surface interaction in the near-field of a dielectric surface have been developed both experimentally and theoretically. The techniques base on either two-photon evanescent wave excitation or combined evanescent-volume wave excitation. Spectra obtained for sodium atoms at a glass-vacuum interface are quantitatively reproduced by a rigorous theoretical approach. In the case of pure evanescent wave excitation the excitation conditions can be chosen such that either the velocity distribution of desorbing atoms is determined or that atom-surface interaction parameters (polarizability of the adsorbed atoms, desorption rate, sticking coefficient) are obtained from the Autler- Townes splitting of the two-photon lines. By the use of combined evanescent-volume wave excitation one is able to distinguish optically between different groups of atoms interacting with the surface and one can extract their two- dimensional velocity distributions. In addition, information is obtained about superelastic scattering of the atoms interacting with the dielectric substrate.