Mid-infrared trace gas detection using continuous-wave difference frequency generation in periodically poled RbTiOAsO4

A tunable mid-infrared continuous-wave (cw) spectroscopic source in the 3.4–4.5 μm region is reported, based on difference frequency generation (DFG) in a quasi-phase-matched periodically poled RbTiOAsO₄ (PPRTA) crystal, DFG power levels of 10 μW were generated at approximately 4 μm in a 20-mm long PPRTA crystal by mixing two cw single-frequency Ti:Al₂O₃ lasers operating near 713 nm and 871 nm, respectively, using a laser pump power of 300 mW. A quasi-phase-matched infrared wavelength-tuning bandwidth (FWHM) of ∼12 cm^-1 and a temperature tuning rate of 1.02 cm^-1/°C were achieved. Experimental details regarding the feasibility of trace gas detection based on absorption spectroscopy of CO₂ in ambient air using this DFG radiation source are also described. Received: 23 October 2000 / Revised version: 22 January 2001 / Published online: 27 April 2001     

Frequency stabilization of a frequency-doubled 197.2 THz distributed feedback diode laser on rubidium 5S1/2→7S1/2 two-photon transitions

A 197.2 THz (1520.2 nm) ITU-T grid distributed feedback (DFB) diode laser is frequency stabilized at 197.198 THz by 1ocking its second harmonic (SH) signal on the rubidium 5S_1/2→7S_1/2 two-photon transition at 394.396 THz (760.1 nm). With 100 mW from the DFB diode laser and amplifying by an erbium-doped fiber amplifier, we obtain an SH power of 15 mW using a periodically poled lithium niobate (PPLN) waveguide frequency doubler. The stability was 2×10⁻¹¹ (10 s), corresponding to a frequency variation of 4 kHz at 1520.2 nm. Our scheme provides a compact and high performance frequency reference in the communication band.     

Melting behaviours of nickel nanorods

We report the synthesis and measurement of an ultra-precise and extremely stable optical frequency in the telecommunications window around 1543 nm. Using a fibre-based femtosecond frequency comb we have phase-stabilised a fibre laser at 194 THz to an optical frequency standard at 344 THz, thus transferring the properties of the optical frequency standard to another spectral region. Relative to the optical frequency standard, the synthesised frequency at 194 THz is determined to within 1 mHz and its fractional frequency instability is measured to be less than 2×10^-15 at 1 s, reaching 5× 10^-18 after 8000 s. We also measured the synthesised frequency against a caesium fountain clock: here the frequency comparison itself contributes less than 4 mHz (2×10^-17) to the uncertainty. Our results confirm the suitability of fibre based frequency comb technology for precision measurements and frequency synthesis, and enable long-distance comparison of optical clocks by using optical fibres to transmit the frequency information.     

Continuous-wave and passively Q-switched Nd:LYSO lasers

Continuous-wave (CW) and passively Q-switched performance of a Nd-doped oyorthosilicate mixing crystal, (Nd_0.005Lu_0.4975Y_0.4975)₂SiO₅ (Nd:LYSO), were reported. As a result, new dual-wavelength all-solid-state lasers at 1075 and 1079 nm were achieved. When the absorbed pump power was 3.87 W, the CW laser produced 1.1 W output, corresponding to an optical conversion efficiency of 28.4% and a slope efficiency of 32.4%. By using a Cr⁴⁺:YAG wafer as the saturable absorber, we achieved Q-switching operation of Nd:LYSO crystal. The maximal average output power, shortest pulse width, largest pulse energy and highest peak power were measured to be 294 mW, 27.5 ns, 34.3 μJ and 1.18 kW, respectively. By difference frequency, these dual-wavelength lasers have potential applications for the generation of a broadband coherent radiation from 0.7–1.3 THz.     

Large third-order nonlinear optical susceptibility of Au-Al2O3 composite films near the resonant frequency

2 O₃ composite films with high Au concentrations (30%–60% in volume fraction) were prepared by reactive co-sputtering and post rapidly thermal annealing. The structure of the films and the size distributions of the Au nanoclusters were examined by TEM, and the third-order nonlinear optical susceptibility χ⁽³⁾ was measured by degenerated four-wave mixing using a 70-ps pulse laser at 532 nm. The maximum value of the χ⁽³⁾ was about 1.2×10^-6 esu in the annealed films and occurred at around 45% Au concentration. The figure of merit, χ⁽³⁾/α (α is the absorption coefficient), has a value of 7×10^-12 esu cm over a wide range of Au concentrations. Received: 23 July 1997     

Off-axis continuous-wave cavity-enhanced absorption spectroscopy of narrow-band and broadband absorbers using red diode lasers

We present an application of continuous-wave (cw) cavity-enhanced absorption spectroscopy (CEAS) with off-axis alignment geometry of the cavity and with time integration of the cavity output intensity for detection of narrow-band and broadband absorbers using single-mode red diode lasers at λ=687.1 nm and λ=662 nm, respectively. Off-axis cw CEAS was applied to kinetic studies of the nitrate radical using a broadband absorption line at λ=662 nm. A rate constant for the reaction between the nitrate radical and E-but-2-eneof (3.78±0.17)×10^-13 cm³ molecule^-1 s^-1 was measured using a discharge-flow system. A nitrate-radical noise-equivalent (1σ≡ root-mean-square variation of the signal) detection sensitivity of 5.5×10⁹ molecule cm^-3 was achieved in a flow tube with a diameter of 4 cm and for a mirror reflectivity of ∼99.9% and a lock-in amplifier time constant of 3 s. In this case, a noise-equivalent fractional absorption per one optical pass of 1.6×10^-6 was demonstrated at a detection bandwidth of 1 Hz. A wavelength-modulation technique (modulation frequency of 10 kHz) in conjunction with off-axis cw CEAS has also been used for recording 1f- and 2f-harmonic spectra of the ^RR(15) absorption of the b¹Σ_g ⁺-X³Σ_g ^- (1,0) band of molecular oxygen at =14553.947 cm^-1. Noise-equivalent fractional absorptions per one optical pass of 1.35×10^-5, 6.9×10^-7 and 1.9×10^-6 were obtained for direct detection of the time-integrated cavity output intensity, 1f- and 2f-harmonic detection, respectively, with a mirror reflectivity of ∼99.8%, a cavity length of 0.22 m and a detection bandwidth of 1 Hz. Received: 24 June 2002 / Revised version: 12 August 2002 / Published online: 15 November 2002 RID="*" ID="*"Corresponding author. Fax: +44-1865/275410, E-mail: vlk@physchem.ox.ac.uk     

Absolute frequency measurement of a CO2/OsO4 stabilized laser at 28.8 THz

A cw carbon dioxide laser operating on the 10 μm R(0)_I transition (28.832 THz) was frequency stabilized by a servo lock to the saturated absorption dip of the Q(15) transition of ¹⁸⁸OsO₄. The laser frequency was measured with a cesium-clock-based frequency chain. In addition, the absorption line frequencies Q(14) of ¹⁸⁸OsO₄ and sQ(4,3) of ¹⁵NH₃, were measured relative to the frequency of Q(15). Received: 21 August 2000 / Revised version: 15 January 2001 / Published online: 30 March 2001     

Leakage current and capacitance characteristics of Si/SiO2/Si single-barrier varactor

We investigate, both experimentally and theoretically, current and capacitance (I–V/C–V) characteristics and the device performance of Si/SiO₂/Si single-barrier varactor diodes (SBVs). Two diodes were fabricated with different SiO₂ layer thicknesses using the state-of-the-art wafer bonding technique. The devices have very low leakage currents (about 5×10^-2 and 1.8×10^-2 mA/mm²) and intrinsic capacitance levels of typically 1.5 and 50 nF/mm² for diodes with 5-nm and 20-nm oxide layers, respectively. With the present device physical parameters (25-mm² device area, 760-μm modulation layer thickness and ≈10¹⁵-cm^-3 doping level), the estimated cut-off frequency is about 5×10⁷ Hz. With the physical parameters of the present existing III–V triplers, the cut-off frequency of our Si-based SBV can be as high as 0.5 THz. Received: 9 February 2001 / Accepted: 9 February 2001 / Published online: 23 March 2001     

Multiple-wavelength lasing by multiform self-frequency conversion in Nd<Superscript>3+</Superscript>-doped La<Subscript>2</Subscript>CaB<Subscript>10</Subscript>O<Subscript>19</Subscript> crystals

The self-sum-frequency process was firstly demonstrated in Nd³⁺-doped La₂CaB₁₀O₁₉ (LCB) crystal. In addition, simultaneous participation of the fundamental laser in multi-self-frequency conversion including the self-frequency doubling was reported. Emissions at five different wavelengths (525, 529, 533.6, 1050 and 1069 nm) were simultaneously obtained. The output power of the three green visible lasers (525, 529 and 533.6 nm) generated by multi-self-frequency-conversion of the fundamental laser is up to 26.64 mW, and the light-light conversion efficiency is up to 4.85%. The lasers at 525 and 529 nm are very close to the green primary color G (526.3 nm) defined by the 1964CIERGB system, which has potential applications in laser-based high brightness display. The large frequency differences of 4–6 THz between 525 and 529 nm, 529 and 533.6 nm, as well as 1050 and 1069 nm, are also potential useful in generating THz waves by difference frequency generation (DFG) technique in a nonlinear optical (NLO) crystal.     

V:YAG – a new passive Q-switch for diode-pumped solid-state lasers

gsa =3.0×10^-18 cm² and σ_esa=1.4×10^-19 cm² at 1064 nm, and σ_gsa=7.2×10^-18 cm² and σ_esa=7.4×10^-19 cm² at 1342 nm. Q-switched operation was demonstrated at 1064 nm and 1342 nm from a Nd:YVO₄ microchip laser, producing pulses as short as 9.3 ns at 1342 nm with peak powers of 350 W. Received: 17 March 1998/Revised version: 8 June 1998     

Efficient diode-pumped Nd:GGG laser operation at 933.6 and 937.3 nm

CW laser emission on the quasi 3-level (⁴F_3/2→⁴I_9/2) transition in Nd:GGG is reported for different pump focusing and resonator dimensions. A nearly hemispherical plano-concave resonator led at 937.3 nm to a maximum output power of 4.1 W for an incident pump power of 21.7 W, thus corresponding to a slope efficiency of about 23.5%. Laser operation was also obtained for the first time around 933.6 nm by using a glass etalon for frequency selection with a maximum output power of 2.3 W and a slope efficiency of 16% with respect to the incident pump power. Dual-wavelength operation (around 933.6 and 937.3 nm), which offers a potential source to generate THz radiation, is also reported.     

Phase-coherent comparison of two optical frequency standards over 146 km using a telecommunication fiber link

We have explored the performance of two “dark fibers” of a commercial telecommunication fiber link for a remote comparison of optical clocks. The two fibers, linking the Leibniz University of Hanover (LUH) with the Physikalisch-Technische Bundesanstalt (PTB) in Braunschweig, are connected in Hanover to form a total fiber length of 146 km. At PTB the performance of an optical frequency standard operating at 456 THz was imprinted to a cw transfer laser at 194 THz, and its frequency was transmitted over the fiber. In order to detect and compensate phase noise related to the optical fiber link we have built a low-noise optical fiber interferometer and investigated noise sources that affect the overall performance of the optical link. The frequency stability at the remote end has been measured using the clock laser of PTB’s Yb⁺ frequency standard operating at 344 THz. We show that the frequency of a frequency-stabilized fiber laser can be transmitted over a total fiber length of 146 km with a relative frequency uncertainty below 1×10⁻¹⁹, and short term frequency instability given by the fractional Allan deviation of σ _y (τ)=3.3×10⁻¹⁵/(τ/s).     

Four-wave mixing spectroscopy of aqueous suspensions of single-wall carbon nanotubes in the ranges of 0.1–10 and 100–250 cm<Superscript>−1</Superscript>

Distinctive optical properties of single-wall carbon nanotubes (SWNT) are highly sensitive to variations in the environment. Here, we have studied SWNT in aqueous suspensions at a low (less than 0.1 μg ml⁻¹) concentration by four-wave mixing (FWM) spectroscopy in the spectral bands of 0.1 to 10 cm⁻¹ (≈300 GHz) and 100 to 250 cm⁻¹ (3 to 7.5 THz). We directly investigated the hydration layers around SWNT. A comparison of the FWM spectra of an SWNT aqueous suspension and Milli-Q water shows a considerable increase in the intensity of low-frequency Raman modes, which are attributed to the rotational transitions of H₂O₂ and H₂O molecules. We explain the observed phenomenon by the hydrogen peroxide production and formation of a low-density depletion layer at the water-nanotube interface. We have observed several SWNT radial breathing modes ω _RBM =118.5, 164.7, and 233.5 cm⁻¹ in an SWNT aqueous suspension and estimated the corresponding SWNT diameters as ≈2.0, 1.5, and 1 nm.     

Beat frequency intercomparisons of127I2 stabilized ion lasers at 514.5 nm

International comparisons of I₂ stabilized ion lasers operated at 514.5 nm have shown a laser frequency reproducibility of 2·10⁻¹⁰ v to 5·10⁻¹² v. These results encouraged the international acceptance of the wavelength value λ_vac=514.673467 for thea ₃ hyperfine component of the¹²⁷I₂ line 43-0P(13).     

Precise frequency measurements of lines in the near infrared by Rb reference lines

Frequency measurements of 16 lines of I₂ in the near infrared have been performed using different Rb frequency references: diode lasers stabilised to the Rb D1 line at 377 THz, to the Rb D2 line at 384 THz and to the 5 s -5 d two photon transition at 385 THz. The relative uncertainties of the measurements of are limited by the frequency stability of the laser source locked to I₂ in the case of the Rb D2 and two photon transition or by the accuracy of the Rb D1 line. The internal consistency of calibrations of iodine lines is shown to be better than by measurements of the difference frequencies of calibrated iodine lines using four-wave mixing in laser diodes. Received 12 July 1999 and Received in final form 12 December 1999     

Synthesis of optical standard frequencies in the S, C and L telecommunication bands by use of four-wave mixing in semiconductor optical amplifiers

The generation of standard reference frequencies close to the ITU channels is essential for the calibration and maintenance of DWDM systems. This work describes a method to synthesize frequency references in the range from 187.1 to 205.1 THz (1462-1602 nm). The method is based on the generation of four equispaced frequencies (by the process of four-wave mixing in a semiconductor amplifier) of which two are locked to absorption lines of the acetylene ¹²C₂H₂ (1511-1542 nm).     

Absolute frequency measurements and comparisons in iodine at 735 nm and 772 nm

We report frequency measurements at the rovibronic transition P(42)1-14 (772 nm) and R(114)2-11 (735 nm) from the electronic transition of the iodine molecule ¹²⁷I₂ with the help of a frequency comb as a reference. By using Doppler-free saturation spectroscopy a frequency precision in the 7 × 10⁻¹⁰ region is reached and two iodine cells both operated at 550-600 °C are compared. To relate our results to other measurements, the absolute transition frequency of the hyperfine structure line P(148)1-14 a₁ at 780 nm with an already known transition frequency was also determined.     

Efficient cascaded difference frequency conversion in periodically poled Ti:LiNbO3 waveguides using pulsed and cw pumping

Using an FM-mode-locked Ti:Er:LiNbO₃ waveguide laser as the fundamental source, wavelength conversion by cascaded χ⁽²⁾:χ⁽²⁾-difference frequency generation with a conversion efficiency of up to +3(-4.6) dB was demonstrated at a pulse repetition rate of about 2 (10) GHz. In addition, multi-channel conversion was demonstrated with a fully packaged wavelength converter using a continuous fundamental source. Received: 29 May 2001 / Revised version: 10 August 2001 / Published online: 2 November 2001     

Nonlinear optical properties of a new two-photon-absorption organic dye: HEASPS

Trans-4-[p-(N-hydroxyethyl-N-ethylamino)styryl]-N-methylpyridinium p-toluene sulfonate (abbreviated as HEASPS) is a two-photon-absorption (TPA) dye newly synthesized by our research group. It possesses a much larger TPA cross-section and much stronger upconversion fluorescence emission than those of common organic dyes (such as rhodamine) when excited with near-infrared (IR) radiation. TPA spectrum and upconversion efficiency spectrum of HEASPS solution at different wavelengths have been measured. The largest molecular TPA cross-section σ₂ ^′ is measured to be 2.06×10^-47 cm⁴ s/photon at 930 nm. At 1064 nm, σ₂ ^′ is 2.71×10^-48 cm⁴ s/photon, which is only one-ninth of that at 930 nm. The upconverted lasing efficiency spectrum has been measured at different wavelengths. The highest efficiency is 5.1% at 1020 nm, whereas it is 3.5% at 1064 nm. Its optical-power-limiting properties at 930 nm have also been illustrated. Received: 30 November 2000 / Published online: 27 April 2001     

Nonlinear optical studies in tetraphenyl-porphyrin-doped boric acid glass using picosecond pulses

We report the results of our studies on the nonlinear optical response of thin films of tetraphenyl porphyrin doped in boric acid glass for picosecond-duration pulses. The fluence-dependent transmission measurements show that the sample exhibits reverse saturation behavior at 532 nm and saturable absorber action at 683 nm. By fitting the nonlinear transmission data at these wavelengths to a rate equation model, values for σ^S _e and σ_L the excited singlet and ground state cross sections were obtained. The large value (≈8) for σ^S _e/σ_L makes it a potential material for optical limiting at 532 nm, whereas at 683 nm the ratio σ_L/σ^S _e≈4.3. Intensity dependence of degenerate forward four-wave mixing at 683 nm was also investigated to establish the order and magnitude of the nonlinearity. The forward four-wave mixing signal at 683 nm showed a cubic dependence on the input intensity, establishing the third-order nonlinearity. A value of 4×10^-12 esu for the third-order susceptibility |χ⁽³⁾| was estimated from the measured efficiency. The time response of the nonlinearity was measured by the pump-probe transmission experiment, resulting in a decay constant of about 1.8 ns for the repopulation of the ground singlet state at 683 nm. Received: 13 April 2000 / Published online: 20 September 2000