arXiv subjects

Christophe Daussy

Publications and source records attributed to Christophe Daussy.

At least 19 recordsLinked to original sources

arXiv2015

Accurate determination of the Boltzmann constant by Doppler spectroscopy: Towards a new definition of the kelvin

Accurate molecular spectroscopy in the mid-infrared region allows precision measurements of fundamental constants. For instance, measuring the linewidth of an isolated Doppler-broadened absorption line of ammonia around 10 $μ$m enables a determination of the Boltzmann constant k B. We report on our latest measurements. By fitting this lineshape to several models which include Dicke narrowing or speed-dependent collisional effects, we find that a determination of k B with an uncertainty of a few ppm is reachable. This is comparable to the best current uncertainty obtained using acoustic methods and would make a significant contribution to any new value of k B determined by the CODATA. Furthermore, having multiple independent measurements at these accuracies opens the possibility of defining the kelvin by fixing k B, an exciting prospect considering the upcoming redefinition of the International System of Units.

physics.atom-ph↗

arXiv2014

Quantum cascade laser frequency stabilisation at the sub-Hz level

Quantum Cascade Lasers (QCL) are increasingly being used to probe the mid-infrared "molecular fingerprint" region. This prompted efforts towards improving their spectral performance, in order to reach ever-higher resolution and precision. Here, we report the stabilisation of a QCL onto an optical frequency comb. We demonstrate a relative stability and accuracy of 2x10-15 and 10-14, respectively. The comb is stabilised to a remote near-infrared ultra-stable laser referenced to frequency primary standards, whose signal is transferred via an optical fibre link. The stability and frequency traceability of our QCL exceed those demonstrated so far by two orders of magnitude. As a demonstration of its capability, we then use it to perform high-resolution molecular spectroscopy. We measure absorption frequencies with an 8x10-13 relative uncertainty. This confirms the potential of this setup for ultra-high precision measurements with molecules, such as our ongoing effort towards testing the parity symmetry by probing chiral species.

physics.optics↗

arXiv2014

Absorption line shape recovery beyond the detection bandwidth limit: application to the precision spectroscopic measurement of the Boltzmann constant

A theoretical model of the influence of detection bandwidth properties on observed line shapes in laser absorption spectroscopy is described. The model predicts artificial frequency shifts, extra broadenings and line asymmetries which must be taken into account in order to obtain accurate central frequencies and other spectroscopic parameters. This reveals sources of systematic effects most probably underestimated so far potentially affecting spectroscopic measurements. This may impact many fields of research, from atmospheric and interstellar physics to precision spectroscopic measurements devoted to metrological applications, tests of quantum electrodynamics or other fundamental laws of nature. Our theoretical model is validated by linear absorption experiments performed on H2O and NH3 molecular lines recorded by precision laser spectroscopy in two distinct spectral regions, near- and mid-infrared. Possible means of recovering original line shape parameters or experimental conditions under which the detection bandwidth has a negligible impact, given a targeted accuracy, are proposed. Particular emphasis is put on the detection bandwidth adjustments required to use such high-quality molecular spectra for a spectroscopic determination of the Boltzmann constant at the 1 ppm level of accuracy.

quant-ph↗

arXiv2014

A widely tunable 10-$μ$m quantum cascade laser phase-locked to a state-of-the-art mid-infrared reference for precision molecular spectroscopy

We report the coherent phase-locking of a quantum cascade laser (QCL) at 10-$μ$m to the secondary frequency standard of this spectral region, a CO2 laser stabilized on a saturated absorption line of OsO4. The stability and accuracy of the standard are transferred to the QCL resulting in a line width of the order of 10 Hz, and leading to our knowledge to the narrowest QCL to date. The locked QCL is then used to perform absorption spectroscopy spanning 6 GHz of NH3 and methyltrioxorhenium, two species of interest for applications in precision measurements.

physics.optics↗

arXiv2013

Probing weak force induced parity violation by high resolution mid-infrared molecular spectroscopy

To date no experiment has reached the level of sensitivity required to observe weak nuclear force induced parity violation (PV) energy differences in chiral molecules. In this paper, we present the approach, adopted at Laboratoire de Physique des Lasers (LPL), to measure frequency differences in the vibrational spectrum of enantiomers. We review different spectroscopic methods developed at LPL leading to the highest resolutions, as well as 20 years of CO2 laser stabilization work enabling such precise measurements. After a first attempt to observe PV vibrational frequency shifts using sub-Doppler saturated absorption spectroscopy in a cell, we are currently aiming at an experiment based on Doppler-free two-photon Ramsey interferometry on a supersonic beam. We report on our latest progress towards observing PV with chiral organo-metallic complexes containing a heavy rhenium atom.

physics.atom-ph↗

arXiv2013

A revised uncertainty budget for measuring the Boltzmann constant using the Doppler Broadening Technique on ammonia

We report on our on-going effort to measure the Boltzmann constant, kB, using the Doppler Broadening Technique. The main systematic effects affecting the measurement are discussed. A revised error budget is presented in which the global uncertainty on systematic effects is reduced to 2.3 ppm. This corresponds to a reduction of more than one order of magnitude compared to our previous Boltzmann constant measurement. Means to reach a determination of kB at the part per million accuracy level are outlined.

quant-ph↗

arXiv2012

Progress towards an accurate determination of the Boltzmann constant by Doppler spectroscopy

In this paper, we present significant progress performed on an experiment dedicated to the determination of the Boltzmann constant, k, by accurately measuring the Doppler absorption profile of a line in a gas of ammonia at thermal equilibrium. This optical method based on the first principles of statistical mechanics is an alternative to the acoustical method which has led to the unique determination of k published by the CODATA with a relative accuracy of 1.7 ppm. We report on the first measurement of the Boltzmann constant by laser spectroscopy with a statistical uncertainty below 10 ppm, more specifically 6.4 ppm. This progress results from improvements in the detection method and in the statistical treatment of the data. In addition, we have recorded the hyperfine structure of the probed saQ(6,3) rovibrational line of ammonia by saturation spectroscopy and thus determine very precisely the induced 4.36 (2) ppm broadening of the absorption linewidth. We also show that, in our well chosen experimental conditions, saturation effects have a negligible impact on the linewidth. Finally, we draw the route to future developments for an absolute determination of with an accuracy of a few ppm.

quant-ph↗

arXiv2012

Evidence for speed-dependent effects in NH3 self-broadened spectra: towards a new determination of the Boltzmann constant

In this paper we present an accurate analysis of the shape of an isolated rovibrational ammonia line from the strong nu2 band around 10 $μ$m, recorded by laser absorption spectroscopy. Experimental spectra obtained under controlled temperature and pressure, are confronted to various models that take into account Dicke narrowing or speed-dependent effects. Our results show clear evidence for speed-dependent broadening and shifting, which had never been demonstrated so far in NH3. Accurate lineshape parameters of the nu2 saQ(6,3) line are obtained. Our current project aiming at measuring the Boltzmann constant, kB, by laser spectroscopy will straight away benefit from such knowledge. We anticipate that a first optical determination of kB with a competitive uncertainty of a few ppm is now reachable.

physics.atom-ph↗

arXiv2010

High resolution spectroscopy of methyltrioxorhenium: towards the observation of parity violation in chiral molecules

Originating from the weak interaction, parity violation in chiral molecules has been considered as a possible origin of the biohomochirality. It was predicted in 1974 but has never been observed so far. Parity violation should lead to a very tiny frequency difference in the rovibrational spectra of the enantiomers of a chiral molecule. We have proposed to observe this predicted frequency difference using the two photon Ramsey fringes technique on a supersonic beam. Promising candidates for this experiment are chiral oxorhenium complexes, which present a large effect, can be synthesized in large quantity and enantiopure form, and can be seeded in a molecular beam. As a first step towards our objective, a detailed spectroscopic study of methyltrioxorhenium (MTO) has been undertaken. It is an ideal test molecule as the achiral parent molecule of chiral candidates for the parity violation experiment. For the 187Re MTO isotopologue, a combined analysis of Fourier transform microwave and infrared spectra as well as ultra-high resolution CO2 laser absorption spectra enabled the assignment of 28 rotational lines and 71 rovibrational lines, some of them with a resolved hyperfine structure. A set of spectroscopic parameters in the ground and first excited state, including hyperfine structure constants, was obtained for the antisymmetric Re=O stretching mode of this molecule. This result validates the experimental approach to be followed once a chiral derivative of MTO will be synthesized, and shows the benefit of the combination of several spectroscopic techniques in different spectral regions, with different set-ups and resolutions. First high resolution spectra of jet-cooled MTO, obtained on the set-up being developed for the observation of molecular parity violation, are shown, which constitutes a major step towards the targeted objective.

physics.atom-ph↗

arXiv2010

Progress toward a first observation of parity violation in chiral molecules by high-resolution laser spectroscopy

Parity violation (PV) effects in chiral molecules have so far never been experimentally observed. To take this challenge up, a consortium of physicists, chemists, theoreticians and spectroscopists has been established and aims at measuring PV energy differences between two enantiomers by using high-resolution laser spectroscopy. In this article, we present our common strategy to reach this goal, the progress accomplished in the diverse areas, and point out directions for future PV observations. The work of André Collet on bromochlorofluoromethane enantiomers, their synthesis and their chiral recognition by cryptophanes made feasible the first generation of experiments presented in this paper.

physics.atom-ph↗

arXiv2009

Determination of the Boltzmann constant by laser spectroscopy as a basis for future measurements of the thermodynamic temperature

In this paper, we present the latest results on the measurement of the Boltzmann constant kB, by laser spectroscopy of ammonia at 10 ?m. The Doppler absorption profile of a ro-vibrational line of an NH3 gas sample at thermal and pressure equilibrium is measured as accurately as possible. The absorption cell is placed inside a large 1m3 thermostat filled with an ice-water mixture, which sets the temperature very close to 273.15 K. Analysing this profile, which is related to the Maxwell-Boltzmann molecular speed distribution, leads to a determination of the Boltzmann constant via a measurement of the Doppler width (proportional tosqrt(kBT)). A spectroscopic determination of the Boltzmann constant with an uncertainty as low as 37 ppm is obtained. Recent improvements with a new passive thermostat lead to a temperature accuracy, stability and homogeneity of the absorption cell better than 1 ppm over a day.

physics.atom-ph↗

arXiv2009

Measurement of the Boltzmann constant by the Doppler broadening technique at a 3,8x10-5 accuracy level

In this paper, we describe an experiment performed at the Laboratoire de Physique des Lasers and dedicated to an optical measurement of the Boltzmann constant. With the proposed innovative technique, determining comes down to an ordinary frequency measurement. The method consists in measuring as accurately as possible the Doppler absorption profile of a rovibrational line of ammonia in thermal equilibrium. This profile is related to the Maxwell-Boltzmann molecular velocity distribution along the laser beam. A fit of the absorption line shape leads to a determination of the Doppler width proportional to sqrt(kT) and thus to a determination of the Boltzmann constant. The laser source is an ultra-stable CO2 laser with a wavelength . The absorption cell is placed in a thermostat keeping the temperature at 273.15 K within 1.4 mK. We were able to measure with a relative uncertainty as small as 3.8x10-5, which represents an improvement of an order of magnitude for an integration time comparable to our previous measurement published in 2007 [1]

physics.atom-ph↗

arXiv2008

86-km optical link with a resolution of 2.10-18 for RF frequency transfer

RF frequency transfer over an urban 86 km fibre has been demonstrated with a resolution of 2.10-18 at one day measuring time using an optical compensator. This result is obtained with a reference carrier frequency of 1 GHz, and a rapid scrambling of the polarisation state of the input light in order to reduce the sensitivity to the polarisation mode dispersion in the fibre. The limitation due to the fibre chromatic dispersion associated with the laser frequency fluctuations is highlighted and analyzed. A preliminary test of an extended compensated link over 186 km using optical amplifiers gives a resolution below 10-17 at 1 day.

quant-ph↗

arXiv2007

HCOOH high resolution spectroscopy in the 9.18$μ$m region

We report on higly accurate absolute frequency measurement against a femtosecond frequency comb of 6 saturated absorption lines of formic acid (HCOOH) with an accuracy of 1 kHz. We also report the frequency measurement of 17 other lines with an accuracy of 2 kHz. Those lines are in quasi coincidence with the 9R(36) to 9R(42) CO$_2$ laser emission lines and are probed either by a CO$_2$ or a widely tunable quantum cascade laser phase locked to a master CO$_2$ laser. The relative stability of two HCOOH stabilized lasers is characterized by a relative Allan deviation of 4.5 10$^{-12}$ $τ^{-1/2}$. They give suitable frequency references for H$_2^+$ Doppler free two-photon spectroscopy.

physics.atom-ph↗

arXiv2007

First direct determination of the Boltzmann constant by an optical method

We have recorded the Doppler profile of a well-isolated rovibrational line in the \nu2 band of 14NH3. Ammonia gas was placed in an absorption cell thermalized by a water-ice bath. By extrapolating to zero pressure, we have deduced the Doppler width which gives a first measurement of the Boltzmann constant, kB, by laser spectroscopy. A relative uncertainty of 2x10-4 has been obtained. The present determination should be significantly improved in the near future and contribute to a new definition of the kelvin.

quant-ph↗

arXiv2006

High Resolution Frequency Standard Dissemination via Optical Fibre Metropolitan Network

We present in this paper results on a new dissemination system of ultra-stable reference signal at 100 MHz on a standard fibre network. The 100 MHz signal is simply transferred by amplitude modulation of an optical carrier. Two different approaches for compensating the noise introduced by the link have been implemented. The limits of the two systems are analyzed and several solution suggested in order to improve the frequency stability and to further extend the distribution distance. Nevertheless, our system is a good tool for the best cold atom fountains comparison between laboratories, up to 100 km, with a relative frequency resolution of 10-14 at one second integration time and 10-17 for one day of measurement. The distribution system may be upgraded to fulfill the stringent distribution requirements for the future optical clocks.

physics.optics↗

arXiv2005

Absolute frequency measurement of an SF6 two-photon line using a femtosecond optical comb and sum-frequency generation

We demonstrate a new simple technique to measure IR frequencies near 30 THz using a femtosecond (fs) laser optical comb and sum-frequency generation. The optical frequency is directly compared to the distance between two modes of the fs laser, and the resulting beat note is used to control this distance which depends only on the repetition rate fr of the fs laser. The absolute frequency of a CO2 laser stabilized onto an SF6 two-photon line has been measured for the first time. This line is an attractive alternative to the usual saturated absorption OsO4 resonances used for the stabilization of CO2 lasers. First results demonstrate a fractional Allan deviation of 3.10-14 at 1 s.

quant-ph↗

arXiv2005

Long-distance frequency dissemination with a resolution of 10-17

We use a new technique to disseminate microwave reference signals along ordinary optical fiber. The fractional frequency resolution of a link of 86 km in length is 10-17 for a one day integration time, a resolution higher than the stability of the best microwave or optical clocks. We use the link to compare the microwave reference and a CO2/OsO4 frequency standard that stabilizes a femtosecond laser frequency comb. This demonstrates a resolution of 3.10-14 at 1 s. An upper value of the instability introduced by the femtosecond laser-based synthesizer is estimated as 1.10-14 at 1 s.

quant-ph↗