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Maximizing performance of quantum cascade laser-pumped molecular lasers

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 Added by Fan Wang
 Publication date 2021
  fields Physics
and research's language is English




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Quantum cascade laser (QCL)-pumped molecular lasers (QPMLs) have recently been introduced as a new source of powerful (>1 mW), tunable (>1 THz), narrow-band (<10 kHz), continuous-wave terahertz radiation. The performance of these lasers depends critically on molecular collision physics, pump saturation, and on the design of the laser cavity. Using a validated three-level model that captures the essential collision and saturation behaviors of the QPML gas nitrous oxide (N2O),we explore how threshold pump power and output terahertz power depend on pump power, gas pressure, as well as on the diameter, length, and output-coupler transmissivity of a cylindrical cavity.The analysis indicates that maximum power occurs as pump saturation is minimized in a manner that depends much more sensitively on pressure than on cell diameter, length, or transmissivity. A near-optimal compact laser cavity can produce more than 10 mW of power tunable over frequencies above 1 THz when pumped by a multi-watt QCL.

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We report the observation of a clear single-mode instability threshold in continuous-wave Fabry-Perot quantum cascade lasers (QCLs). The instability is characterized by the appearance of sidebands separated by tens of free spectral ranges (FSR) from the first lasing mode, at a pump current not much higher than the lasing threshold. As the current is increased, higher-order sidebands appear that preserve the initial spacing, and the spectra are suggestive of harmonically phase-locked waveforms. We present a theory of the instability that applies to all homogeneously broadened standing-wave lasers. The low instability threshold and the large sideband spacing can be explained by the combination of an unclamped, incoherent Lorentzian gain due to the population grating, and a coherent parametric gain caused by temporal population pulsations that changes the spectral gain line shape. The parametric term suppresses the gain of sidebands whose separation is much smaller than the reciprocal gain recovery time, while enhancing the gain of more distant sidebands. The large gain recovery frequency of the QCL compared to the FSR is essential to observe this parametric effect, which is responsible for the multiple-FSR sideband separation. We predict that by tuning the strength of the incoherent gain contribution, for example by engineering the modal overlap factors and the carrier diffusion, both amplitude-modulated (AM) or frequency-modulated emission can be achieved from QCLs. We provide initial evidence of an AM waveform emitted by a QCL with highly asymmetric facet reflectivities, thereby opening a promising route to ultrashort pulse generation in the mid-infrared. Together, the experiments and theory clarify a deep connection between parametric oscillation in optically pumped microresonators and the single-mode instability of lasers, tying together literature from the last 60 years.
Four-wave-mixing-based quantum cascade laser frequency combs (QCL-FC) are a powerful photonic tool, driving a recent revolution in major molecular fingerprint regions, i.e. mid- and far-infrared domains. Their compact and frequency-agile design, together with their high optical power and spectral purity, promise to deliver an all-in-one source for the most challenging spectroscopic applications. Here, we demonstrate a metrological-grade hybrid dual comb spectrometer, combining the advantages of a THz QCL-FC with the accuracy and absolute frequency referencing provided by a free-standing, optically-rectified THz frequency comb. A proof-of-principle application to methanol molecular transitions is presented. The multi-heterodyne molecular spectra retrieved provide state-of-the-art results in line-center determination, achieving the same precision as currently available molecular databases. The devised setup provides a solid platform for a new generation of THz spectrometers, paving the way to more refined and sophisticated systems exploiting full phase control of QCL-FCs, or Doppler-free spectroscopic schemes.
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Soliton microcombs offer the prospect of advanced optical metrology and timing systems in compact form factors. In these applications, pumping of microcombs directly from a semiconductor laser without amplification or triggering components is desirable for reduced power operation and to simplify system design. At the same time, low repetition rate microcombs are required in many comb applications for interface to detectors and electronics, but their increased mode volume makes them challenging to pump at low power. Here, 10 GHz repetition rate soliton microcombs are directly pumped by low-power (< 20 mW) diode lasers. High-Q silica microresonators are used for this low power operation and are packaged into fiber-connectorized modules that feature temperature control for improved long-term frequency stability.
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