Highly sensitive detection of trace gases using the time-resolved frequency downchirp from pulsed quantum-cascade lasers

A spectrometer using a pulsed, 10.25-μm-wavelength, thermoelectrically cooled quantum-cascade distributed-feedback laser has been developed for sensitive high-resolution infrared absorption spectroscopy. This spectrometer is based upon the use of the almost linear frequency downchirp of up to 75 GHz produced by a square current drive pulse. The behavior of this downchirp has been investigated in detail using high-resolution Fourier-transform spectrometers. The downchirp spectrometer provides a real-time display of the spectral fingerprint of molecular gases over a wave-number range of up to 2.5 cm-1. Using an astigmatic Herriott cell with a maximum path length of 101 m and a 5-kHz pulse repetition rate with 12-s averaging, absorption lines having an absorbance of less than 0.01 (an absorption of less than 1%) may be measured.

[1]  A. J. Merer,et al.  The high-resolution infrared spectrum of the 201 band of carbonyl fluoride: Determination of the far infrared laser frequencies , 1985 .

[2]  F. Capasso,et al.  Quantum-cascade laser measurements of stratospheric methane and nitrous oxide. , 2001, Applied optics.

[3]  E. Cohen,et al.  Further measurements of the rotational spectrum of COF2: Improved molecular constants for the ground and ν2 states , 1991 .

[4]  Laurence S. Rothman,et al.  Reprint of: The HITRAN molecular spectroscopic database and HAWKS (HITRAN Atmospheric Workstation): 1996 edition , 1998 .

[5]  E. Normand,et al.  Characterisation of the spectral behaviour of pulsed quantum cascade lasers using a high resolution Fourier transform infrared spectrometer , 2001 .

[6]  Geoffrey Duxbury Infrared Vibration-Rotation Spectroscopy: From Free Radicals to the Infrared Sky , 2000 .

[7]  R. May,et al.  Aircraft (ER-2) laser infrared absorption spectrometer (ALIAS) for in-situ stratospheric measurements of HCI, N(2)O, CH(4), NO(2), and HNO(3). , 1994, Applied optics.

[8]  A A Kosterev,et al.  Trace-gas detection in ambient air with a thermoelectrically cooled, pulsed quantum-cascade distributed feedback laser. , 2000, Applied optics.

[9]  Mattias Beck,et al.  Continuous Wave Operation of a Mid-Infrared Semiconductor Laser at Room Temperature , 2001, Science.

[10]  A. G. Maki,et al.  Wavenumber calibration tables from heterodyne frequency measurements , 1991 .

[11]  G Duxbury,et al.  Fast, real-time spectrometer based on a pulsed quantum-cascade laser. , 2003, Optics letters.

[12]  A. Cho,et al.  Sensitive absorption spectroscopy with a room-temperature distributed-feedback quantum-cascade laser. , 1998, Optics letters.

[13]  W. J. Lafferty,et al.  Diode laser heterodyne spectroscopy on the ν4 and ν9 bands of 1,1-difluoroethylene , 1981 .

[14]  R. Bracewell The Fourier Transform and Its Applications , 1966 .

[15]  R. May,et al.  Airborne laser infrared absorption spectrometer (ALIAS-II) for in situ atmospheric measurements of N2O, CH4, CO, HCl, and NO2 from balloon or remotely piloted aircraft platforms. , 1999, Applied optics.

[16]  A. Kosterev,et al.  Chemical sensors based on quantum cascade lasers , 2002 .

[17]  J B McManus,et al.  Astigmatic mirror multipass absorption cells for long-path-length spectroscopy. , 1995, Applied optics.

[18]  Graham R. Fleming,et al.  Chemical applications of ultrafast spectroscopy , 1986 .