We present both an innovative theoretical model and an experimental validation of a molecular gas optically pumped far-infrared (OPFIR) laser at 0.25 THz that exhibits 10× greater efficiency (39% of the Manley-Rowe limit) and 1,000× smaller volume than comparable commercial lasers. Unlike previous OPFIR-laser models involving only a few energy levels that failed even qualitatively to match experiments at high pressures, our ab initio theory matches experiments quantitatively, within experimental uncertainties with no free parameters, by accurately capturing the interplay of millions of degrees of freedom in the laser. We show that previous OPFIR lasers were inefficient simply by being too large and that high powers favor high pressures and small cavities. We believe that these results will revive interest in OPFIR laser as a powerful and compact source of terahertz radiation.
We investigate laser emission from optically-pumped rotationally excited molecular gases confined in a metallic cavity. To this end, we have developed a theoretical framework able to accurately describe, both in the spatial and temporal domains, the molecular collisional and diffusion processes characterizing the operation of this class of lasers. The effect on the main lasing features of the spatial variation of the electric field intensity and the ohmic losses associated to each cavity mode are also included in our analysis. Our simulations show that, for the exemplary case of methyl fluoride gas confined in a cylindrical copper cavity, the region of maximum population inversion is located near the cavity walls. Based on this fact, our calculations show that the lowest lasing threshold intensity corresponds to the cavity mode that, while maximizing the spatial overlap between the corresponding population inversion and electric-field intensity distributions, simultaneously minimizes the absorption losses occurring at the cavity walls. The dependence of the lasing threshold intensity on both the gas pressure and the cavity radius is also analyzed and compared with experiment. We find that as the cavity size is varied, the interplay between the overall gain of the system and the corresponding ohmic losses allows for the existence of an optimal cavity radius which minimizes the intensity threshold for a large range of gas pressures. The theoretical analysis presented in this work expands the current understanding of lasing action in optically-pumped far-infrared lasers and, thus, could contribute to the development of a new class of compact far-infrared and terahertz sources able to operate efficiently at room temperature.
Rotational spectroscopy is introduced as a new in situ method for monitoring gas-phase reactants and products during chemical reactions. Exploiting its unambiguous molecular recognition specificity and extraordinary detection sensitivity, rotational spectroscopy at terahertz frequencies was used to monitor the decomposition of carbonyl sulfide (OCS) over an aluminum nanocrystal (AlNC) plasmonic photocatalyst. The intrinsic surface oxide on AlNCs is discovered to have a large number of strongly basic sites that are effective for mediating OCS decomposition. Spectroscopic monitoring revealed two different photothermal decomposition pathways for OCS, depending on the absence or presence of H2O. The strength of rotational spectroscopy is witnessed through its ability to detect and distinguish isotopologues of the same mass from an unlabeled OCS precursor at concentrations of <1 nanomolar or partial pressures of <10 μTorr. These attributes recommend rotational spectroscopy as a compelling alternative for monitoring gas-phase chemical reactants and products in real time.
A method for highly selective remote sensing of atmospheric trace polar molecular gases is described. Based on infrared-terahertz double-resonance spectroscopic techniques, the molecule-specific coincidence between the lines of a CO 2 laser and rotational-vibrational molecular absorption transitions provide two dimensions of recognition specificity: infrared coincidence frequency and the corresponding terahertz frequency whose absorption strength is modulated by the laser. Atmospheric pressure broadening expands the molecular recognition "specificity matrix" by simultaneously relaxing the infrared coincidence requirement and strengthening the corresponding terahertz signature. Representative double-resonance spectra are calculated for prototypical molecules CH 3 F and CH 3 Cl and their principal isotopomers from which a heuristic model is developed to estimate the specificity matrix and double-resonance signature strength for any polar molecule.
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