Mid-infrared frequency comb for broadband high precision and sensitivity molecular spectroscopy.

We report on the experimental demonstration of the metrological and spectroscopic performances of a mid-infrared comb generated by a nonlinear downconversion process from a Ti:sapphire-based near-infrared comb. A quantum cascade laser at 4330 nm was phase-locked to a single tooth of this mid-infrared comb and its frequency-noise power spectral density was measured. The mid-infrared comb itself was also used as a multifrequency highly coherent source to perform ambient air direct comb spectroscopy with the Vernier technique, by demultiplexing it with a high-finesse Fabry-Perot cavity.

Direct observation of coherent interorbital spin-exchange dynamics.

We report on the first direct observation of fast spin-exchange coherent oscillations between different long-lived electronic orbitals of ultracold 173Yb fermions. We measure, in a model-independent way, the strength of the exchange interaction driving this coherent process. This observation allows us to retrieve important information on the interorbital collisional properties of 173Yb atoms and paves the way to novel quantum simulations of paradigmatic models of two-orbital quantum magnetism.

High-coherence mid-infrared frequency comb.

We report on the generation of a frequency comb around 4330 nm with an unprecedented coherence of the single teeth. Generating the comb within a Ti:sapphire laser cavity by a difference-frequency process and using a phase-lock scheme based on direct digital synthesis, we achieve a tooth linewidth of 2.0 kHz in a 1-s timescale (750 Hz in 20 ms). The generated per-tooth power of 1 µW ranks this comb among the best ever realized in the mid-infrared in terms of power spectral density.

Subkilohertz linewidth room-temperature mid-infrared quantum cascade laser using a molecular sub-Doppler reference.

We report on the narrowing of a room-temperature mid-IR quantum cascade laser by frequency locking it to a CO2 sub-Doppler transition obtained by polarization spectroscopy. A locking bandwidth of 250 kHz has been achieved. The laser linewidth is narrowed by more than two orders of magnitude below 1 kHz, and its absolute frequency is stabilized at the same level.

Direct link of a mid-infrared QCL to a frequency comb by optical injection.

A narrow-linewidth comb-linked nonlinear source is used as master radiation to injection lock a room-temperature mid-infrared quantum cascade laser (QCL). This process leads to a direct lock of the QCL to the optical frequency comb, providing the unique features of narrow linewidth, absolute frequency, higher output power, and wide mode-hop-free tunability. The QCL reproduces the injected radiation within more than 94%, with a reduction of the frequency-noise spectral density by 3 to 4 orders of magnitude up to about 100 kHz, and a linewidth narrowing from a few MHz to 20 kHz.

Optical frequency comb assisted laser system for multiplex precision spectroscopy.

A laser system composed of two lasers phase-locked onto an Optical Frequency Comb Synthesizer (OFCS), operating around 1083 nm, was developed. An absolute frequency precision of 6x10(-13) at 1s, limited by the OFCS, was measured with a residual rms phase-noise of 71 mrad and 87 mrad for the two phase-locks, respectively. Multiplex spectroscopy on 1083 nm Helium transitions with this set-up is demonstrated. Generalization of this system to a larger number of OFCS assisted laser sources for wider frequency separations, even in other spectral regions, is discussed.

Molecular gas sensing below parts per trillion: radiocarbon-dioxide optical detection.

Radiocarbon ((14)C) concentrations at a 43 parts-per-quadrillion level are measured by using saturated-absorption cavity ringdown spectroscopy by exciting radiocarbon-dioxide ((14)C(16)O(2)) molecules at the 4.5 µm wavelength. The ultimate sensitivity limits of molecular trace gas sensing are pushed down to attobar pressures using a comb-assisted absorption spectroscopy setup. Such a result represents the lowest pressure ever detected for a gas of simple molecules. The unique sensitivity, the wide dynamic range, the compactness, and the relatively low cost of this table-top setup open new perspectives for ^{14}C-tracing applications, such as radiocarbon dating, biomedicine, or environmental and earth sciences. The detection of other very rare molecules can be pursued as well thanks to the wide and continuous mid-IR spectral coverage of the described setup.

Ti:sapphire laser intracavity difference-frequency generation of 30 mW cw radiation around 4.5 µm.

A cw mid-IR coherent source based on difference-frequency generation is designed and characterized. For mid-IR generation, a periodically poled MgO:LiNbO(3) crystal is placed inside a compact Ti:sapphire laser cavity. This provides high-power pump radiation for the nonlinear process. Optical injection by an external-cavity diode laser ensures single-frequency operation of the Ti:sapphire laser, while signal radiation is provided by a fiber-amplified Nd:YAG laser. Mid-IR radiation can be generated with 3850-4540 nm tuning range, narrow linewidth, Cs-standard traceability, and TEM(00) spatial mode. 30 mW power is obtained at 4510 nm.

Saturated-absorption cavity ring-down spectroscopy.

We report on a novel approach to cavity ring-down spectroscopy with the sample gas in saturated-absorption regime. This technique allows us to decouple and simultaneously retrieve the empty-cavity background and absorption signal, by means of a theoretical model that we developed and tested. The high sensitivity and frequency precision for spectroscopic applications are exploited to measure, for the first time, the hyperfine structure of an excited vibrational state of 17O12C16O in natural abundance with an accuracy of a few parts in 10{-11}.

Observing the intrinsic linewidth of a quantum-cascade laser: beyond the Schawlow-Townes limit.

A comprehensive investigation of the frequency-noise spectral density of a free-running midinfrared quantum-cascade laser is presented for the first time. It provides direct evidence of the leveling of this noise down to a white-noise plateau, corresponding to an intrinsic linewidth of a few hundred hertz. The experiment is in agreement with the most recent theory on the fundamental mechanism of line broadening in quantum-cascade lasers, which provides a new insight into the Schawlow-Townes formula and predicts a narrowing beyond the limit set by the radiative lifetime of the upper level.

Ultra-stable, widely tunable and absolutely linked mid-IR coherent source.

We report on a new coherent source that, using a phase-lock scheme to an optical frequency-comb synthesizer, achieves a 10-Hz intrinsic linewidth, is tunable from 4 to 4.5 microm with a presettable absolute frequency and, when coupled to a high-finesse cavity, can provide a short-term absorption sensitivity of 1.3 x 10(-11) cm(-1)Hz,(-1/2). These unique spectral features make this source a precise tool for molecular physics.

Lamb-dip-locked quantum cascade laser for comb-referenced IR absolute frequency measurements.

The frequency of a DFB quantum cascade laser (QCL) emitting at 4.3 microm has been long-term stabilized to the Lamb-dip center of a CO2 ro-vibrational transition by means of first-derivative locking to the saturated absorption signal. Thanks to the non-linear sum-frequency generation (SFG) process with a fiber-amplified Nd:YAG laser, the QCL mid-infrared (IR) radiation has been linked to an optical frequency-comb synthesizer (OFCS) and its absolute frequency counted with a kHz-level precision and an overall uncertainty of 75 kHz.

Phase-locking to a free-space terahertz comb for metrological-grade terahertz lasers.

Optical frequency comb synthesizers have represented a revolutionary approach to frequency metrology, providing a grid of frequency references for any laser emitting within their spectral coverage. Extending the metrological features of optical frequency comb synthesizers to the terahertz domain would be a major breakthrough, due to the widespread range of accessible strategic applications and the availability of stable, high-power and widely tunable sources such as quantum cascade lasers. Here we demonstrate phase-locking of a 2.5 THz quantum cascade laser to a free-space comb, generated in a LiNbO(3) waveguide and covering the 0.1-6 THz frequency range. We show that even a small fraction (<100 nW) of the radiation emitted from the quantum cascade laser is sufficient to generate a beat note suitable for phase-locking to the comb, paving the way to novel metrological-grade terahertz applications, including high-resolution spectroscopy, manipulation of cold molecules, astronomy and telecommunications.

Frequency-comb-referenced quantum-cascade laser at 4.4 microm.

We report what we believe to be the first absolute frequency measurement performed using a quantum-cascade laser (QCL) referenced to an optical frequency comb synthesizer (OFCS). A QCL at 4.43 microm has been used for producing near-infrared radiation at 858 nm by means of sum-frequency generation with a Nd:YAG source in a periodically poled lithium niobate nonlinear crystal. The absolute frequency of the QCL source has been measured by detecting the beat note between the sum frequency and a diode laser at the same wavelength, while both the Nd:YAG and the diode laser were referenced to the OFCS. Doppler-broadened line profiles of (13)CO(2) molecular transitions have been recorded with such an absolute frequency reference.

Frequency-comb-based absolute frequency measurements in the mid-infrared with a difference-frequency spectrometer.

We demonstrate the possibility of extending the well-established metrological performance of optical frequency-comb synthesizers to the mid-IR region by phase locking the pump and signal lasers of a difference-frequency source to two near-IR teeth of an optical comb. An uncertainty of 800 Hz (1.1 x 10(-11)) in the absolute frequencies of CO2 transitions near 4.2 microm has been measured by cavity-enhanced saturated-absorption spectroscopy. Prospects for the creation of a new dense set of high-quality molecular frequency standards in the IR are discussed.

Spatial mode control of radiation generated by frequency difference in periodically poled crystals.

We demonstrate the possibility to control the spatial mode of a narrow-linewidth, continuous-wave, infrared radiation beam generated by difference frequency in a periodically poled crystal. This can be achieved by acting directly on a few experimental parameters. We show that hollow beams can be generated. A numerical routine has been developed and results agree with experimental observations, without requiring any free parameters. The relevance of these results for high-resolution spectroscopy and atom manipulation is discussed.

Search for exchange-antisymmetric states for spin-0 particles at the 10(-11) level.

We set a new upper limit of 1.7x10(-11) to the probability that two spin-0 16O nuclei are in forbidden exchange-antisymmetric states, testing the validity of fundamental principles of quantum mechanics. A newly designed difference-frequency spectrometer is used to look for the existence of these states. The experimental test was performed by tuning the spectrometer across a molecular transition of 12C 16O (2) belonging to the rovibrational band at 4.25 microm, connecting the forbidden states (00(0)0,J = 25) and (00(0)1,J = 26).

Precision frequency measurement of visible intercombination lines of strontium.

We report the direct frequency measurement of the visible 5s(2) 1S0-5s5p 3P1 intercombination line of strontium that is considered a possible candidate for a future optical-frequency standard. The frequency of a cavity-stabilized laser is locked to the saturated fluorescence in a thermal Sr atomic beam and is measured with an optical-frequency comb generator referenced to the SI second through a global positioning system signal. The 88Sr transition is measured to be at 434 829 121 311 (10) kHz. We measure also the 88Sr-86Sr isotope shift to be 163 817.4 (0.2) kHz.

The Stimulated Raman Spectrum of Symmetric 13C Cyanogen, 13C2N2.

The Raman spectrum of cyanogen 13C214N2 has been investigated at nearly Doppler resolution by means of a stimulated Raman technique. The regions around the bandheads of the nu1 (2260 cm-1) and nu2 (835 cm-1) vibrations have been recorded. Besides the fundamentals, hot bands arising from v5 = 1-3 and v4 = 1 have been observed. A number of strong perturbations have been detected. The spectra have been analyzed and rotational constants for the excited states have been obtained. Computer simulations of the Raman contours have been carried out as a test of the assignments. A few weak DeltaJ = -2 lines have also been observed in the nu1 region.

Osteonecrosis in HIV: a case-control study.

BACKGROUND: Osteonecrosis (avascular necrosis) has been infrequently reported in HIV-infected patients. It is not known whether HIV itself is an independent risk factor for osteonecrosis. METHODS: We identified 25 patients with osteonecrosis from 1984 to 1999 from a large county teaching hospital and two large practices in Dallas County that specialize in HIV-disease related therapy. A retrospective chart review was performed to evaluate potential risk factors for osteonecrosis. Each case was matched with two controls for HIV positive status and date of osteonecrosis diagnosis. RESULTS: In the study, 22 of 25 (88%) case patients had at least one osteonecrosis risk factor compared with 24 of 50 (48%) controls, p =.003. The most common osteonecrosis risk factors were hyperlipidemia (32%), alcoholism (28%), pancreatitis (16%), corticosteroids (12%), and hypercoaguability (12%). Of the cases, 12% were idiopathic. Multiple joints were involved in 72% of cases. Four of the case patients compared with none of the controls received megesterol acetate before the diagnosis of osteonecrosis, p =.01. No significant differences were found between cases and controls with respect to liver function tests, testosterone levels, triglyceride levels, cholesterol levels, or CD4 cell counts. Saquinavir was independently associated with osteonecrosis, p <.05. However, no differences in overall use of protease inhibitors among cases and controls were noted: 79% versus 76%, respectively. CONCLUSIONS: The increased incidence of osteonecrosis in HIV/AIDS may be due to an increased frequency of risk factors previously associated with osteonecrosis such as hyperlipidemia, corticosteroid use, alcohol abuse, and hypercoaguability. Use of protease inhibitors was not independently associated with osteonecrosis.