Optical parametric oscillator based off-axis integrated cavity output spectroscopy for rapid chemical sensing

An optical parametric oscillator (OPO), pumped by a fiber-amplified diode laser, is combined with off-axis integrated cavity output spectroscopy (OA-ICOS). The cw OPO (power 1.2 W, tunability 3-4 μm, 5 cm(-1) mode-hop-free tuning) has a tuning speed of 100 THz/s, which is ideal for rapid and sensitive trace gas detection. Combined with OA-ICOS, a detection limit of 50 parts per trillion by volume (1×10(12)) of ethane (C(2)H(6)) in nitrogen was obtained in 0.25s at 2997 cm(-1), corresponding to a noise equivalent absorption sensitivity of 4.8×10(-11) cm(-1) Hz(-1/2). The system demonstrates real-time measurements of methane and water in exhaled human breath.     

Real-time monitoring of ethane in human breath using mid-infrared cavity leak-out spectroscopy

We report on spectroscopic real-time analysis of ethane traces in exhaled human breath. Ethane is considered the most important volatile marker of free-radical induced lipid peroxidation and cell damage in the human body. Our measurements were carried out by means of mid-infrared cavity leak-out spectroscopy in the 3 μm region, a cw variant of cavity ring-down spectroscopy. The spectrometer is based on a CO overtone laser with tunable microwave sidebands. The resulting system proved to be an unique tool with high sensitivity and selectivity for rapid and precise breath testing. With a 5 s integration time, we achieved a detection limit on the order of 100 parts per trillion ethane in human breath. Thus, sample preconcentration is unnecessary. Time-resolved monitoring of the decaying ethane fraction in breath after smoking a cigarette is demonstrated. Received: 13 March 2001 / Published online: 9 May 2001     

Mid-infrared cavity leak-out spectroscopy for ultrasensitive detection of carbonyl sulfide

We present a ringdown absorption spectrometer based on a continuous-wave CO laser in the mid-infrared spectral region near lambda = 5 microm. Using a linear ringdown cavity (length, 0.5 m) with R > = 99.99% mirrors, we observed a noise-equivalent absorption coefficient of 7 x 10(-11) cm(-1) Hz(-1/2). This is 2 orders of magnitude improved compared with previous values. With this setup we studied the spectroscopic detection of carbonyl sulfide (here abbreviated OCS) traces in ambient air and in exhaled breath. We achieved a detection limit of 7 parts in 10(12) (parts per trillion) OCS in ambient air, which is unprecedented and shows great promise for environmental and biomedical applications.     

Ultra-sensitive mid-infrared cavity leak-out spectroscopy using a cw optical parametric oscillator

We report a portable, all-solid-state, mid-infrared spectrometer for trace-gas analysis. The light source is a continuous-wave optical parametric oscillator based on PPLN and pumped by a Nd:YAG laser at 1064 nm. The generated single-frequency idler output covers the wavelength region between 2.35 and 3.75 μm. With its narrow line width, this light source is suitable for precise trace-gas analysis with very high sensitivity. Using cavity leak-out spectroscopy we achieved a minimum detectable absorption coefficient of 1.2×10^-9 /cm (integration time: 16 s), corresponding, for example, to a detection limit of 300 parts per trillion ethane. This sensitivity and the compact design make this trace-gas analyzer a promising tool for various in situ environmental and medical applications. Received: 19 September 2002 / Published online: 15 November 2002 RID="*" ID="*"Corresponding author. Fax: +49-228/733-474, E-mail: frank.kuehnemann@iap.uni-bonn.de     

Time resolved simultaneous detection of 14NO and 15NO via mid-infrared cavity leak-out spectroscopy

We present a ring-down absorption spectrometer based on a continuous-wave CO laser in the mid-infrared spectral region near lambda = 5 microm. Using a linear ring-down cavity (length: 0.5 m) with high reflective mirrors (R = 99.988 %), we observed a noise-equivalent absorption coefficient of 3 x 10(-10) cm(-1)Hz(-1/2). This corresponds to a noise-equivalent concentration of 800 parts per trillion (ppt) for (14)NO and 40 ppt for (15)NO in 1 s averaging time. We achieve a time resolution of 1 s which allows time resolved simultaneous detection of the two N isotopes. The delta(15)N value was obtained with a precision of +/-1.2 per thousand in a sample with a NO fraction of 11 ppm. The simultaneous detection enables the use of (15)NO as a tracer molecule for endogenous biomedical processes.     

Thermal-noise limit in the frequency stabilization of lasers with rigid cavities

We evaluate thermal noise (Brownian motion) in a rigid reference cavity used for frequency stabilization of lasers, based on the mechanical loss of cavity materials and the numerical analysis of the mirror-spacer mechanics with the direct application of the fluctuation dissipation theorem. This noise sets a fundamental limit for the frequency stability achieved with a rigid frequency-reference cavity of order 1 Hz/ square root Hz (0.01 Hz/ square root Hz) at 10 mHz (100 Hz) at room temperature. This level coincides with the world-highest level stabilization results.     

Achieving geodetic motion for LISA test masses: ground testing results

The low-frequency resolution of space-based gravitational wave observatories such as LISA (Laser Interferometry Space Antenna) hinges on the orbital purity of a free-falling reference test mass inside a satellite shield. We present here a torsion pendulum study of the forces that will disturb an orbiting test mass inside a LISA capacitive position sensor. The pendulum, with a measured torque noise floor below 10 fN m/square root of Hz from 0.6 to 10 mHz, has allowed placement of an upper limit on sensor force noise contributions, measurement of the sensor electrostatic stiffness at the 5% level, and detection and compensation of stray dc electrostatic biases at the millivolt level.     

Intrinsic noise properties of atomic point contact displacement detectors

We measure the noise added by an atomic point contact operated as a displacement detector. With a microwave technique, we increase the measurement speed of atomic point contacts by a factor of 500. The measurement is then fast enough to detect the resonant motion of a nanomechanical beam at frequencies up to 60 MHz and sensitive enough to observe the random thermal motion of the beam at 250 mK. We demonstrate a shot-noise limited imprecision of 2.3 fm/square root[Hz] and observe a 78 aN/square root[Hz] backaction force, yielding a total uncertainty in the beam's displacement that is 42 times the standard-quantum limit.     

Infrared laser-spectroscopic analysis of <Superscript>14</Superscript>NO and <Superscript>15</Superscript>NO in human breath

We report on monitoring of nitric oxide (NO) traces in human breath via infrared cavity leak-out spectroscopy. Using a CO sideband laser near 5 μm wavelength and an optical cavity with two high-reflectivity mirrors (R=99.98%), the minimum detectable absorption is 2×10⁻¹⁰ cm⁻¹ Hz^1/2. This allows for spectroscopic analysis of rare NO isotopologues with unprecedented sensitivity. Application to simultaneous online detection of ¹⁴NO and ¹⁵NO in breath samples collected in the nasal cavity is described for the first time. We achieved a noise-equivalent detection limit of 7 parts per trillion for nasal ¹⁵NO (integration time: 70 s).     

Continuous wave,distributed feedback diode laser based sensor for trace-gas detection of ethane

The development of a continuous wave (CW), thermoelectrically cooled (TEC), distributed feedback (DFB) laser diode based spectroscopic trace-gas sensor for ultra-sensitive and selective ethane (C₂H₆) concentration measurements is reported. The sensor platform used tunable diode laser absorption spectroscopy (TDLAS) based on a 2f wavelength modulation (WM) detection technique. TDLAS was performed with a 100 m optical path length astigmatic Herriott cell. For an interference free C₂H₆ absorption line located at 2976.8 cm⁻¹ a 1σ minimum detection limit of 240 pptv (part per trillion by volume) with a 1 second lock-in amplifier time constant was achieved. In addition, reliable and long-term sensor performance was obtained when operating the sensor in an absorption line locked mode.     

Online monitoring of ethane traces in exhaled breath with a difference frequency generation spectrometer

We report a transportable mid-infrared laser cavity leak-out spectrometer for online detection of trace gases. The laser spectrometer is based on continuous-wave difference-frequency generation in the wavelength region around 3 μm. Sensitive spectroscopic trace gas monitoring was achieved using a high-finesse ring-down cavity. For difference-frequency generation, we use a periodically poled lithium niobate (PPLN) crystal, pumped by a Nd:YAG laser (signal wave) and a diode laser (pump wave) with a tapered amplifier. A maximum power of 280 μW near λ=3.3 μm is achieved using a pump power of 180 mW at 807 nm, a signal power of 890 mW at 1064.46 nm, and a 50-mm-long PPLN crystal. The resulting system proved to be a unique tool with high sensitivity and specificity for rapid and precise breath testing. We demonstrate spectroscopic online monitoring of ethane traces in exhaled human breath with a precision of 270 parts per trillion (1σ) and a time resolution of 1 s. PACS 42.62.Be; 42.60.-v; 07.57.Ty     

Experimental demonstration of a laterally deformable optical nanoelectromechanical system grating transducer

We experimentally demonstrate operation of a laterally deformable optical nanoelectromechanical system grating transducer. The device is fabricated in amorphous diamond with standard lithographic techniques. For small changes in the spacing of the subwavelength grating elements, lossy propagating resonant modes in the plane of the grating cause a large change in the optical reflection amplitude. An in-plane motion detection sensitivity of 160 fm/square root(Hz) was measured, exceeding that of any other optical microelectromechanical system transducer to our knowledge. Calculations predict that this sensitivity could be improved to better than 40 fm/square root(Hz) in future designs. In addition to having applications in the field of inertial sensors, this device could also be used as an optical modulator.     

Toward a more accurate Q value measurement of tritium: status of THe-Trap

The goal of the THe-Trap experiment is to measure the tritium/helium-3 mass ratio in order to deduce the Q value of the tritium β-decay. A relative uncertainty of 10 parts per trillion in the mass ratio would allow determining the Q value with a precision of 30 meV. This value is of relevance for the Karlsruhe Tritium Neutrino (KATRIN) collaboration, which is building a spectrometer to measure the mass of the electron antineutrino. In this contribution, we present the progress made in the past 2 years. We can, e.g., store, manipulate and detect single ions. To demonstrate the current accuracy, we measured the carbon-12 to oxygen-16 mass ratio with a relative uncertainty of 120 parts per trillion in early 2013. The improvements, current status and future perspectives will be presented.     

Cavity ringdown spectroscopy using mid-infrared quantum-cascade lasers

Cavity ringdown spectra of ammonia at 10 parts in 10(9) by volume (ppbv) and higher concentrations were recorded by use of a 16-mW continuous-wave quantum-casacde distributed-feedback laser at 8.5 mum whose wavelength was continuously temperature tuned over 15 nm. A sensitivity (noise-equivalent absorbance) of 3.4x10(-9) cm(-1) Hz(-1/2) was achieved for ammonia in nitrogen at standard temperature and pressure, which corresponds to a detection limit of 0.25 ppbv.     

Time-resolved Fourier transform intracavity spectroscopy with a Cr2+:ZnSe laser

Intracavity laser absorption spectroscopy (ICLAS) with an evacuated Cr2+:ZnSe laser is performed with a high-resolution time-resolved Fourier transform interferometer with a minimum detectable absorption coefficient equal to 4 x 10(-9) cm(-1) Hz(-1/2) in the 2.5 microm region. This represents the extreme limit currently reached in the infrared by ICLAS with Doppler-limited resolution. The broad gain band of the crystal allows a spectral coverage at most equal to 125 nm, wide enough to see entire vibration bands. Weak CO2 bands observed up to now only in the Venusian atmosphere are recorded for the first time, to our knowledge, in a laboratory. An H2O detection limit down to 0.9 parts per billion by volume is also demonstrated.     

Effects of frequency and duration on psychometric functions for detection of increments and decrements in sinusoids in noise

Psychometric functions for detecting increments or decrements in level of sinusoidal pedestals were measured for increment and decrement durations of 5, 10, 20, 50, 100, and 200 ms and for frequencies of 250, 1000, and 4000 Hz. The sinusoids were presented in background noise intended to mask spectral splatter. A three-interval, three-alternative procedure was used. The results indicated that, for increments, the detectability index d' was approximately proportional to delta I/I. For decrements, d' was approximately proportional to delta L. The slopes of the psychometric functions increased (indicating better performance) with increasing frequency for both increments and decrements. For increments, the slopes increased with increasing increment duration up to 200 ms at 250 and 1000 Hz, but at 4000 Hz they increased only up to 50 ms. For decrements, the slopes increased for durations up to 50 ms, and then remained roughly constant, for all frequencies. For a center frequency of 250 Hz, the slopes of the psychometric functions for increment detection increased with duration more rapidly than predicted by a "multiple-looks" hypothesis, i.e., more rapidly than the square root of duration, for durations up to 50 ms. For center frequencies of 1000 and 4000 Hz, the slopes increased less rapidly than predicted by a multiple-looks hypothesis, for durations greater than about 20 ms. The slopes of the psychometric functions for decrement detection increased with decrement duration at a rate slightly greater than the square root of duration, for durations up to 50 ms, at all three frequencies. For greater durations, the increase in slope was less than proportional to the square root of duration. The results were analyzed using a model incorporating a simulated auditory filter, a compressive nonlinearity, a sliding temporal integrator, and a decision device based on a template mechanism. The model took into account the effects of both the external noise and an assumed internal noise. The model was able to account for the major features of the data for both increment and decrement detection.     

Trace measurement of BrO at the ppt level by a transportable mode-locked frequency-doubled cavity-enhanced spectrometer

Pptv levels of BrO radical have been detected around 338.5-nm wavelength probing a rotationally structured A←X (7,0) electronic transition using mode-locked cavity-enhanced spectroscopy (ML-CEAS). The spectrometer is composed by a widely tunable, broadband frequency-doubled Ti:Sa mode-locked frequency comb laser injected into a high-finesse optical cavity and a high-resolution spectrometer based on a high-order diffraction grating and a high-sensitivity back-thinned CCD camera. A typical minimum detectable absorption coefficient of 1×10⁻⁹ cm⁻¹ in 30 s of acquisition has been achieved, leading to a detection limit of 1.7 parts per trillion of BrO at atmospheric pressure. The compact and robust ultrasensitive broadband UV spectrometer is intended to be employed for in situ long-term direct measurements of BrO and other halogenated radicals, thus responding to the lack of analytical techniques to monitor the concentrations of such highly chemically reactive species.     

基于中红外分布反馈量子级联激光器的光声光谱技术用于痕量甲烷气体检测

由于工业监控和环境检测的需要,甲烷气体检测日益得到人们的关注。研究了基于中红外分布反馈量子级联激光器(DFB-QCL)的光声光谱技术,并应用于痕量甲烷的检测。自主研发的DFB-QCL室温工作时的激射波长在7.6μm附近,覆盖了甲烷的特征吸收谱线1 316.83cm-1。待测甲烷气体充入亥姆霍兹光声谐振腔中,DFB-QCL的工作频率为234Hz、室温脉冲工作时峰值功率为80mW。中红外光经过甲烷吸收后,产生的声波信号经麦克风检测,由锁相放大器对信号进行采集并输入计算机进行处理。按信噪比为1计算,得到甲烷的探测极限为189nmol.mol-1。     

Inductive single-electron transistor

We demonstrate a sensitive method of charge detection based on radio-frequency readout of the Josephson inductance of a superconducting single-electron transistor. Charge sensitivity 1.4 x 10(-4) e/square root Hz, limited by a preamplifier, is achieved in an operation mode which takes advantage of the nonlinearity of the Josephson potential. Owing to reactive readout, our setup has more than 2 orders of magnitude lower dissipation than the existing method of radio-frequency electrometry. With an optimized sample, we expect uncoupled energy sensitivity below variant Planck's over h in the same experimental scheme.     

Time resolved simultaneous detection of 14NO and 15NO via mid-infrared cavity leak-out spectroscopy

We present a ring-down absorption spectrometer based on a continuous-wave CO laser in the mid-infrared spectral region near λ?=?5 μm. Using a linear ring-down cavity (length: 0.5 m) with high reflective mirrors (R?=?99.988 %), we observed a noise-equivalent absorption coefficient of 3?×?10^?10 cm^?1Hz^?1/2. This corresponds to a noise-equivalent concentration of 800 parts per trillion (ppt) for ¹⁴NO and 40 ppt for ¹⁵NO in 1 s averaging time. We achieve a time resolution of 1 s which allows time resolved simultaneous detection of the two N isotopes. The δ¹⁵N value was obtained with a precision of ±1.2‰ in a sample with a NO fraction of 11 ppm. The simultaneous detection enables the use of ¹⁵NO as a tracer molecule for endogenous biomedical processes.