Optical nanofibers and spectroscopy

We review our recent progress in the production and characterization of tapered optical fibers with a sub-wavelength diameter waist. Such fibers exhibit a pronounced evanescent field and are therefore a useful tool for highly sensitive evanescent wave spectroscopy of adsorbates on the fiber waist or of the medium surrounding. We use a carefully designed flame pulling process that allows us to realize preset fiber diameter profiles. In order to determine the waist diameter and to verify the fiber profile, we employ scanning electron microscope measurements and a novel accurate in situ optical method based on harmonic generation. We use our fibers for linear and non-linear absorption and fluorescence spectroscopy of surface-adsorbed organic molecules and investigate their agglomeration dynamics. Furthermore, we apply our spectroscopic method to quantum dots on the surface of the fiber waist and to caesium vapor surrounding the fiber. Finally, towards dispersive measurements, we present our first results on building and testing a single-fiber bi-modal interferometer.Comment: 13 pages, 18 figures. Accepted for publication in Applied Physics B. Changes according to referee suggestions: changed title, clarification of some points in the text, added references, replacement of Figure 13

Optical imaging spectroscopy

During the recent solar maximum the combination of imaging and spectroscopy in the visible part of the spectrum became a powerful tool for observational study of flares primarily because of the development of two-dimensional charge-coupled-device (CCD) arrays. In combination with appropriate new operational methods, this has led to the ability to observe, for the first time, the preflare and impulsive-phase physical processes associated with spatially resolved features of flare loops. As a result of concurrent theoretical developments, modeling progressed from an empirical to a physical level. This made it possible to interpret imaging spectra in terms of coronal pressure and heat flux, particle beam heating, chromospheric evaporation, and explosive chromospheric dynamics at the footpoints of flare loops. There is clear potential for further advances in the near future, taking advantage of improvements in digital recording speed (approx. 10-fold), number of photosensitive elements per array (approx. 10-fold), real-time data pre-reduction (potentially 10- to 100-fold), and using multiple CCD arrays. By the time of the next solar maximum imaging spectroscopy is expected to achieve spatial resolution or approx. arc 1 arc s, temporal resolution or approx. 5 s, and simultaneous critically-sampled spectroscopy of several lines and continua. As a result, continued increase in our understanding of the physical processes and configurations of solar flares in the chromosphere, temperature minimum region, and photosphere can be anticipated. Even greater progress toward a more global understanding of flares will obviously come about when simultaneous optical, X-ray, and gamma-ray imaging spectroscopy are possible

Direct Kerr-frequency-comb atomic spectroscopy

Microresonator-based soliton frequency combs - microcombs - have recently emerged to offer low-noise, photonic-chip sources for optical measurements. Owing to nonlinear-optical physics, microcombs can be built with various materials and tuned or stabilized with a consistent framework. Some applications require phase stabilization, including optical-frequency synthesis and measurements, optical-frequency division, and optical clocks. Partially stabilized microcombs can also benefit applications, such as oscillators, ranging, dual-comb spectroscopy, wavelength calibration, and optical communications. Broad optical bandwidth, brightness, coherence, and frequency stability have made frequency-comb sources important for studying comb-matter interactions with atoms and molecules. Here, we explore direct microcomb atomic spectroscopy, utilizing a cascaded, two-photon 1529-nm atomic transition of rubidium. Both the microcomb and the atomic vapor are implemented with planar fabrication techniques to support integration. By fine and simultaneous control of the repetition rate and carrier-envelope-offset frequency of the soliton microcomb, we obtain direct sub-Doppler and hyperfine spectroscopy of the $4^2D_{5/2}$ manifold. Moreover, the entire set of microcomb modes are stabilized to this atomic transition, yielding absolute optical-frequency fluctuations of the microcomb at the kilohertz-level over a few seconds and < 1 MHz day-to-day accuracy. Our work demonstrates atomic spectroscopy with microcombs and provides a rubidium-stabilized microcomb laser source, operating across the 1550 nm band for sensing, dimensional metrology, and communication.Comment: 5 pages, 3 figure

Simulation of optical response functions in molecular junctions

We discuss theoretical approaches to nonlinear optical spectroscopy of molecular junctions. Optical response functions are derived in the form convenient for implementation of Green function techniques, and their expressions in terms of pseudoparticle nonequilibrium Green functions are proposed. The formulation allows to account for both intra-molecular interactions and hybridization of molecular states due to coupling to contacts. Two-dimensional optical spectroscopy in junctions is considered as an example.Comment: 11 pages, 7 figure

Optical spectroscopy of molecular junctions: Nonequilibrium Green's functions perspective

We consider optical spectroscopy of molecular junctions from the quantum transport perspective when radiation field is quantized and optical response of the system is simulated as photon flux. Using exact expressions for photon and electronic fluxes derived within the nonequilibrium Green function (NEGF) methodology and utilizing fourth order diagrammatic perturbation theory in molecular coupling to radiation field we perform simulations employing realistic parameters. Results of the simulations are compared to the bare perturbation theory (PT) usually employed in studies on nonlinear optical spectroscopy to classify optical processes. We show that the bare PT violates conservation laws, while flux conserving NEGF formulation mixes optical processes.Comment: 10 pages, 6 figure

Self-normalizing phase measurement in multimode terahertz spectroscopy based on photomixing of three lasers

Photomixing of two near-infrared lasers is well established for continuous-wave terahertz spectroscopy. Photomixing of three lasers allows us to measure at three terahertz frequencies simultaneously. Similar to Fourier spectroscopy, the spectral information is contained in an nterferogram, which is equivalent to the waveform in time-domain spectroscopy. We use one fixed terahertz frequency \nu_ref to monitor temporal drifts of the setup, i.e., of the optical path-length difference. The other two frequencies are scanned for broadband high-resolution spectroscopy. The frequency dependence of the phase is obtained with high accuracy by normalizing it to the data obtained at \nu_ref, which eliminates drifts of the optical path-length difference. We achieve an accuracy of about 1-2 microns or 10^{-8} of the optical path length. This method is particularly suitable for applications in nonideal environmental conditions outside of an air-conditioned laboratory.Comment: 5 pages, 5 figure

Noise spectroscopy of optical microcavity

The intensity noise spectrum of the light passed through an optical microcavity is calculated with allowance for thermal fluctuations of its thickness. The spectrum thus obtained reveals a peak at the frequency of acoustic mode localized inside the microcavity and depends on the size of the illuminated area. The estimates of the noise magnitude show that it can be detected using the up-to-date noise spectroscopy technique.Comment: 10 pages, 1 figur