Optical-optical double-resonance dual-comb spectroscopy with pump-intensity modulation.

We apply an intensity-modulation technique to dual-comb spectroscopy to improve its detection sensitivity. The scheme is demonstrated via Doppler-free optical-optical double-resonance spectroscopy of Rb by modulating the intensity of a pump laser with frequencies set at rates 3 times lower and 50,000 times higher than the difference in the repetition rates of the two frequency combs. The signal-to-noise ratios are enhanced by 3 and 6 times for slow and fast modulations, respectively, compared to those of conventional dual-comb spectroscopy without any intensity modulation. The technique is widely applicable to pump-probe spectroscopy with dual-comb spectroscopy and provides high detection sensitivity.

Direct-comb molecular spectroscopy by heterodyne detection with continuous-wave laser for high sensitivity.

We have demonstrated direct-comb molecular spectroscopy in which an individual-comb mode is resolved by heterodyne detection with a continuous-wave (cw) laser. This simple, fast, and sensitive technique was demonstrated for atomic spectroscopy in [ Appl. Phys. Lett.101, 051105 ( 2012)], but is more suitable for molecular spectroscopy. Four rotation-vibration transitions of methane have simultaneously been recorded in a Doppler-limited resolution using a spectrally broadened comb based on an Er-doped fiber laser and a cw 1651-nm distributed-feedback laser diode. Even though the power level of the comb modes and the sample absorption are weaker than those of the previous studies, in this work the cw laser frequency is stabilized to one of the comb modes, and the data are thereby averaged for extended periods of time, resulting an improvement in sensitivity.

Doppler-free dual-comb spectroscopy of Rb using optical-optical double resonance technique.

We present a Doppler-free high-resolution dual-comb spectroscopy technique in which a dual-comb system is employed to perform optical-optical double-resonance (OODR) spectroscopy. In our experimental study, Doppler-free high-resolution and high-frequency-accuracy broadband measurements were realized using the proposed OODR dual-comb spectroscopic technique, which does not require high-power-per-mode frequency combs. We observed fully resolved hyperfine spectra of 5P3/2 - 4D5/2, 4D3/2 transitions of Rb at 1530 nm and precisely determined the absolute frequencies of the transitions, with an uncertainty of less than 1 MHz. The variations of the OODR spectral line shapes due to power broadening and alignment and the effects of polarization on the dual-comb OODR spectra were also analyzed. This study provides a widely applicable technique for Doppler-free dual-comb spectroscopy of various gaseous species.

Generation of a frequency comb spanning more than 3.6 octaves from ultraviolet to mid infrared.

We have observed an ultra-broadband frequency comb with a wavelength range of at least 0.35 to 4.4 µm in a ridge-waveguide-type periodically poled lithium niobate device. The PPLN waveguide is pumped by a 1.0-2.4 µm wide frequency comb with an average power of 120 mW generated using an erbium-based mode-locked fiber laser and a following highly nonlinear fiber. The coherence of the extended comb is confirmed in both the visible (around 633 nm) and the mid-infrared regions.

Ortho-Para-Dependent Pressure Effects Observed in the Near Infrared Band of Acetylene by Dual-Comb Spectroscopy.

We demonstrate that dual-comb spectroscopy, which allows one to record broadband spectra with high frequency accuracy in a relatively short time, provides a real advantage for the observation of pressure-broadening and pressure-shift effects. We illustrate this with the ν_{1}+ν_{3} vibration band of ^{12}C_{2}H_{2}. We observe transitions from P(26) to R(29), which extend over a 3.8 THz frequency range, at six pressures ranging up to 2654 Pa. Each observed absorption line profile is fitted to a Voigt function yielding pressure-broadening and pressure-shift coefficients for each rotation-vibration transition. The effectiveness of this technique is such that we are able to discern a clear dependence of the pressure-broadening coefficients on the nuclear spin state, i.e., on the ortho or para modification. This information, combined with the pressure-shift coefficients, can facilitate a detailed understanding of the mechanism of molecular collisions.

Dual wavelength 3.2-µm source for isotope ratio measurements of (13)CH(4)/(12)CH(4).

Difference frequency generation using one 1.58-µm and two 1.06-µm distributed feedback Bragg-grating laser diodes and a ridge-type PPLN alternately provide two 3.2-µm coaxial waves resonant with individual isotopic transitions separated by 13 cm(-1). The ν(3) band R(6) A(2) allowed transition of (13)CH(4) and the ν(3) band R(6) A(2) weakly allowed transition of (12)CH(4) are an ideal pair for isotope ratio measurements. The (13)CH(4)/(12)CH(4) isotope ratio is determined for three sample gases with a relative uncertainty of 0.7 ‰, and it is confirmed that the temperature dependence is smaller than the uncertainty.

Sub-Doppler resolution mid-infrared spectroscopy using a difference-frequency-generation source spectrally narrowed by laser linewidth transfer.

The spectral linewidth of a 3.28 µm difference-frequency-generation source has been reduced to 3.5 kHz using a laser linewidth transfer technique [Opt. Express21, 7891 (2013)]. We use an optical frequency comb with a broad servo bandwidth to transfer a narrow linewidth of a pump laser, a 1.06 µm Nd:YAG laser, to a signal laser, a 1.57 µm external-cavity laser diode. This source enables us to record the Lamb dip of the ν3 band R(2) E transition of methane with a molecular spectral linewidth of 21 kHz while the frequency axis is absolutely calibrated.

Design of cavity-enhanced absorption cell for reducing transit-time broadening.

To reduce the linewidth of Lamb dips, we introduce a cavity-enhanced absorption cell (CEAC) coupled with a Gaussian beam with a 1.9-mm 1/e(2) radius at the beam waist for the reduction of transit-time broadening. We state that transit-time broadening depends only on the beam radius at the beam waist. This fact is useful for the design of the CEAC, and a pair of concave and convex mirrors is thereby employed. We have carried out sub-Doppler resolution spectroscopy of the ν(3) band of CH(4) and the ν(1) band of CH(3)D using a difference-frequency-generation source and the CEAC, and the recorded Lamb dips narrow to 80 kHz (HWHM).

A novel frequency control scheme for comb-referenced sensitive difference-frequency-generation spectroscopy.

We present a novel scheme of frequency scan and wavelength modulation of a difference-frequency-generation source for comb-referenced sensitive spectroscopy. While the pump and signal frequencies are phase-locked to an optical frequency comb (OFC), the offset frequency between the signal wave and the nearest comb tooth is modulated to apply a wavelength-modulation technique, and the idler wave frequency is repeatedly swept for signal accumulation by changing the repetition frequency of the OFC. The spectrometer is applied to absolute frequency measurement of weak hyperfine-resolved rovibration transitions of the ν(1) band of CH(3)I, and the uncertainty in frequency determination is reduced by one order of magnitude in compared with that of the previous work published in Optics Express 20, 9178-9186 (2012).

Absolute frequency list of the ν3-band transitions of methane at a relative uncertainty level of 10(-11).

We determine the absolute frequencies of 56 rotation-vibration transitions of the ν(3) band of CH(4) from 88.2 to 90.5 THz with a typical uncertainty of 2 kHz corresponding to a relative uncertainty of 2.2 × 10(-11) over an average time of a few hundred seconds. Saturated absorption lines are observed using a difference-frequency-generation source and a cavity-enhanced absorption cell, and the transition frequencies are measured with a fiber-laser-based optical frequency comb referenced to a rubidium atomic clock linked to the international atomic time. The determined value of the P(7) F(2)((2)) line is consistent with the International Committee for Weights and Measures recommendation within the uncertainty.

An efficient and compact difference-frequency-generation spectrometer and its application to (12)CH(3)D/(12)CH(4) isotope ratio measurements.

We have developed an efficient and compact 3.4 µm difference-frequency-generation spectrometer using a 1.55 µm distributed feedback (DFB) laser diode, a 1.06 µm DFB laser diode, and a ridge-waveguide periodically poled lithium niobate. It is continuously tunable in the 30 cm(-1) span and is applied to (12)CH(3)D/(12)CH(4) isotope ratio measurements. The suitable pair of (12)CH(3)D ν(4) (p)P(7,6) and (12)CH(4) ν(2)+ν(4) R(6) F(1)((1)) lines enabled us to determine their isotope ratio with a precision repeatability of 0.8‰ using a sample and a working standard of pure methane with an effective signal averaging time of 100 ms.

Huge transverse deformation in nonspecular reflection of a light beam possessing orbital angular momentum near critical incidence.

We derive a general expression for the field distribution of Hermite- and Laguerre-Gaussian (LG) beams reflected at a dielectric interface. The intensity distributions of the reflected LG light beam at the beam waist are also observed experimentally in the vicinity of the critical incidence. They are greatly deformed because of the nonspecular transverse shift induced by the orbital angular momentum of the LG beam. The observed and calculated intensity distributions agree well and indicate that a large fraction of the electromagnetic energy flows as much as the transverse beam size.

Spectroscopic isotope ratio measurement of doubly-substituted methane.

We have determined the isotope ratios of (13)CH(3)D /(12)CH(3)D as well as (13)CH(3)D /(12)CH(4) with an uncertainty of ~20‰ using a sensitive difference-frequency-generation spectrometer in the 3.4 µm region. Cooling the absorption cell drastically reduces overlap of the (13)CH(3)D lines with the other abundant isotopic lines, and the extensive tunability of the spectrometer enables us to access transition pairs appropriate for isotope ratio measurements. We measure the intensity of the (13)CH(3)D ν(4)(R)P (7, 0) line, the (12)CH(3)D 2ν(5)(R)Q (9, 0) line, and the (12)CH(4)ν(2)+ν(4) R(10) F(2) line at 2953 cm(-1) as well as the (13)CH(3)D ν(4)(P)P (6, 3) line and the (12)CH(4)ν(3) P (6) E line at 2955 cm(-1) because they have similar transition frequencies, absorption strengths, and low state energies.

Sub-Doppler resolution 3.4 microm spectrometer with an efficient difference-frequency-generation source.

We have developed a 3.4 mum spectrometer for sub-Doppler resolution molecular absorption spectroscopy. The source is based on the difference frequency generation using a 1.06 microm Nd:YAG laser, a 1.55 microm distributed-feedback laser diode, and a ridge waveguide periodically poled lithium niobate with a conversion efficiency of 9%/W. The generated radiation has a power level of about 300 microW, a linewidth of less than 100 kHz, and a continuous tuning range over 10 cm(-1). The spectrometer allows us to observe six saturated absorption lines of C12H(4) with 0.3-0.4 MHz width and 1.3%-1.7% depth relative to the corresponding linear absorption lines.

Significant deformations and propagation variations of Laguerre-Gaussian beams reflected and transmitted at a dielectric interface.

We observe TM and TE Laguerre-Gaussian (LG) light beams reflected and transmitted at a dielectric interface near critical incidence. The intensity distribution of the reflected beam is transversely deformed near the beam waist, and that of the transmitted beam is similar to that of a diagonal Hermite-Gaussian beam. The former rotates around the optical axis by approximately pi/2 with propagation, and the latter returns to that of the incident LG beam. These observations agree well with numerical calculations based on an angular spectral analysis and are attributable to the helical wavefront of the LG beams, the sharp incidence-angle dependence of the Fresnel reflection and transmission coefficients, and the Gouy phase.

Versatile generation of optical vortices based on paraxial mode expansion.

We demonstrate a simple and versatile method for generating various configurations of optical vortices from a Gaussian light beam by using glass plates and an astigmatic mode converter (AMC). The glass plates are inserted into the Gaussian beam to imprint nodal lines along the edges, and the AMC then transforms the beam with the nodes into a vortex beam. The procedures are discussed in terms of a transverse-mode expansion of the paraxial light beam, in which each Hermite-Gaussian mode is converted into the corresponding Laguerre-Gaussian mode by the AMC. We generated several vortex configurations, and the results show good agreement with the theoretical predictions.