Investigations of masers utilizing cross-relaxation
Cross relaxation processes in millimeter wave maser technology for obtaining maser amplification at higher frequencies
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Cross relaxation processes in millimeter wave maser technology for obtaining maser amplification at higher frequencies
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The processes that take place in the excited states of a trivalent Thulium (Tm) ion in an Yttrium Aluminum Garnet (YAG) crystal, being relevant to the use of this system for laser applications, have been the object of several studies. We have reexamined this system focusing our attention on the dynamics of Tm following its excitation in the H-3(sub 4) level. Under these conditions the system relaxes through a cross-relaxation process. H-3(sub 4) yields F-3(sub 4), H-3(sub 6) yields F-3(sub 4), whose rate depends upon both the concentration of the Tm ion and the temperature of the crystal. The excitation spectrum obtained by monitoring the 1.8 micron emission of Tm (due to the F-3(sub 4) yields H-3(sub 6) transition) indicates an increase in the contribution to this emission from the H-3(sub 4) level relative to the H-3(sub 5) level as the Tm concentration increases; this shows the increased role played by the H-3(sub 4) level in pumping the infrared emission. Correspondingly, the duration of the luminescence originating in the H-3(sub 4) level is shortened as the concentration of Tm increases. The concentration quenching of this lifetime can be fit to a model which assumes that the cross-relaxation is due to a dipole-dipole interaction; from this fit, the intrinsic Tm lifetime in the absence of cross relaxation can be derived. We have used this lifetime to calculate the rate of the cross-relaxation process. We have evaluated this rate as a function of the temperature and found it to be fastest at 77 K. We have also calculated the microscopic interaction parameters for the cross-relaxation process by using two independent experimental features: (1) the time evolution of the emission from the H-3(sub 4) level; and (2) the spectral overlap between the H-3(sub 4) yields F-3(sub 4) emission and the H-3(sub 6) yields F-3(sub 4) absorption. We have also considered the migration of excitation among the Tm ions in the F-3(sub 4) level and calculated the relevant microparameter by the use of the relevant spectral overlap. The data are consistent with the model in which the Tm ions, once excited into the H-3(sub 4) level decay by cross-relaxation to the F-3(sub 4), and then transfer rapidly their energy to other Tm ions.
The energy transfer processes in Tm,Ho:YAG lasers were investigated in spectral studies and measurements of the temporal response to pulsed excitation. These processes include the population of the 3H4 pump band of Tm, cross-relaxation in Tm, the transfer of energy from Tm to Ho, and various loss mechanisms. It was found that the Tm cross-relaxation is due to a dipole-dipole interaction between Tm ions and that the rate of this process is a function of temperature and ion concentration.
The paper compares the cross-relaxation, energy transfer and loss processes in Tm- and Ho-doped YAG and YLF as a function of temperature, Tm concentration, and excitation power. Significant differences in the behavior of Tm and Tm,Ho in YAG and YLF crystals were found. The cross-relaxation rates of Tm(6 pct) are faster in YLF (about 5 microsec) than YAG (about 10 microsec). The energy transfer rates between Tm and Ho are faster in YLF than YAG. The time it takes for the maximum intensity of 1.7-micron emission to drop 10 percent is 25 microsec for YLF:Tm(6 pct),Ho(0.6 pct) and 65 microsec YAG:Tm(6 pct),Ho(0.5 pct). The losses occurring with increasing pump power for 2.1-micron emission of the above samples are 30 percent less in YLF than YAG. These qualitative differences point to YLF as a valuable 2-micron laser host material.
Microwave spectroscopy - electric field effects in nuclear magnetic resonance of fluids, expansion of velocity surfaces in spherical harmonics, and electron cross relaxation in dilute ruby
Spin defects in solids offer promising platforms for quantum sensing and memory due to their long coherence times and optical addressability. Here, we integrate a single nitrogen-vacancy (NV) center in diamond with scanning probe microscopy to detect, read out, and spatially map spin-based quantum sensors at the nanoscale. Using the boron vacancy ($V$$^{–}_{B}$) center in hexagonal boron nitride—an emerging two-dimensional spin system—as a model, we detect its electron spin resonance indirectly via changes in the spin relaxation time (T 1 ) of a nearby NV center, eliminating the need for optical excitation or fluorescence detection of the $V$$^{–}_{B}$. Cross-relaxation between NV and $V$$^{–}_{B}$ ensembles significantly reduces NV T1, enabling quantitative nanoscale mapping of defect densities beyond the optical diffraction limit and clear resolution of hyperfine splitting in isotopically enriched h 10 B 15 N. Our method demonstrates interactions between spin sensors in 3D and 2D materials, establishing NV centers as versatile probes for characterizing otherwise inaccessible spin defects.
This work examines molecular dynamics and interactions in ethylene glycol–choline chloride (EG–ChCl) mixtures across 0–33 mol % ChCl, spanning the true eutectic region near 17–20 mol % and the commonly used 1:2 formulation. We combine pulsed-field-gradient (PFG) diffusion, fast-field-cycling (FFC) relaxometry, temperature-dependent 13 C T 1 , and nuclear Overhauser effect spectroscopy (NOESY) to disentangle local from macroscopic dynamics. PFG and FFC show that both translational and average rotational motions largely track the strong increase in viscosity with ChCl content, with ethylene glycol consistently diffusing faster than the choline cation and no global dynamical anomaly at the eutectic composition. More subtle, site-specific composition effects nevertheless emerge. The ratio of the diffusion coefficient of the hydroxyl group of choline to the diffusion coefficient of the methyl group of choline displays a shallow minimum in the 17–25 mol % region, indicating a modest change in how the hydroxyl-bearing end of choline samples the underlying translational motion relative to the methyl groups. 13 C T 1 analysis shows that rotational correlation times at 25 °C generally increase with ChCl, reflecting viscosity-coupled slowing, while the CH 2 –N α site exhibits a small but reproducible deviation from this monotonic trend near the eutectic. NOESY spectra at similar compositions reveal enhanced cross-relaxation between EG and choline protons, consistent with increased headgroup–solvent contact density rather than a wholesale structural rearrangement. Overall, our multitechnique study demonstrates that EG–ChCl dynamics are predominantly viscosity-dominated, with the eutectic region acting as a subtle dynamical crossover where specific choline segments become maximally coupled to the hydrogen-bond network. These insights refine the structure–dynamics picture of choline-chloride DESs and provide practical guidance for tuning composition in electrochemical, separation, and catalytic applications.
In order to compute relaxation 'cross sections' for molecule-molecule collisions, it is convenient to employ a coupled angular-momentum representation which differs from that generally used. An explicit expression for collision-induced spectral pressure broadening in this representation is given, and this is used to examine the difference between para- and ortho-H2 for broadening of HCl.
The infinite order sudden (IOS) approximation is extended to rotational excitation of symmetric tops by collisions with atoms. After development of a formalism for 'primitive' or 'one-ended' tops, proper parity-adapted linear combinations describing real rotors are considered and modifications needed for asymmetric rigid rotors are noted. The generalized spectroscopic relaxation cross sections are discussed. IOS calculations for NH3-He and H2CO-He are performed and compared with more accurate calculations, and the IOS approximation is found to provide a reasonably accurate description.
A striking feature of astrophysical masers is the tendency for either one or the other of the circular polarizations to dominate in the radiation from the strong, widely observed masing transitions of OH at 18 cm. Spectral line profiles are calculated for polarized maser radiation due to the combined effects of a velocity gradient and, as is indicated for these transitions, a Zeeman splitting that is at least comparable with the thermal contributions to the breadths of the spectral lines. The resulting spectral features are similar in appearance, including the presence of large net circular polarization and narrow line breadths, to the commonly observed spectra of OH masers in molecular clouds. The calculations presented here are performed as a function of frequency without making the approximations of a large velocity gradient. Rapid cross relaxation, which has been advocated by others for the OH masers, is assumed.
A systematic analysis of energy transfer processes in crystals of YAG doped with varying concentrations of Cr and Tm is described. Both spectral measurements and measurements of the temporal response to pulsed excitation are used to give independent determinations of the microscopic interaction parameter for Cr to Tm transfer. The different factors in influencing the temperature dependence of the Cr to Tm transfer are discussed. The dependence of the Tm cross-relaxation rate on Tm concentration is determined.
The formation mechanisms and optical properties of polycyclic aromatic hydrocarbons (PAH) isolated in argon and neon matrices were studied in a systematic manner in an attempt to provide spectroscopic data on PAH ions under conditions relevant to astrophysical applications. The results obtained indicate the strong influence of the matrix material on the competing radiative (fluorescence and phosphorescence) and nonradiative (internal conversion and intersystem crossing) relaxation processes of the trapped molecule.
Self-, N2- and Ar-broadening coefficients were measured for the stretch-bend infrared combination bands nu-1 + nu-1/2 (4004/cm) of HCN and nu-1 + nu-1/5 (4091/cm) of C2H2, using a tunable difference-frequency laser. At atmospheric pressures, the Q branches of these bands exhibit significant rotational narrowing or line mixing. The broadening coefficients are fit with empirical rotationally inelastic collision rate laws, which are then used to model the line mixing in the overlapped Q-branch profiles. Simple energy gap fitting laws appear to be suitable for the shorter-range intermolecular quadrupole-quadrupole and induction forces, whereas an energy-corrected-sudden scaling law works better for the longer-range dipole-dipole and dipole-quadrupole collision partners. In all cases, the line-coupling coefficients are substantially reduced from the rotationally inelastic rates fit to the broadening coefficients, indicating that 35-70 percent of the broadening may be due to other collisional mechanisms such as cross-relaxation to the degenerate H state vibrational level.
A detailed study of the spectroscopy and excitation dynamics Tm3+ and Ho3+ in yttrium lithium fluoride, LiYF4 (YLF), has been done. Absorption spectroscopy is utilized in the Judd-Ofelt theory to determine radiative transition rates of spontaneous emission. Luminescence spectroscopy is studied under cw diode laser excitation at 785nm. The effect of dopant ion concentration and excitation power on the observed luminescence are considered in these measurements. An analysis of these measurements have been used to determine channels of energy transfer between Tm3+ and Ho3+ ions. The temporal response of Tm and Ho in singly and co-doped YLF to pulsed laser excitation with a Ti:Al2O3 laser and a CoMgF2 laser turned to various wavelengths have also been studied. The energy transfer mechanisms of cross relaxation, upconversion, and resonant energy transfer between Tm3+ and Ho3+ ions have been modeled, and the model parameters extracted by a fitting procedure to the measured temporal response curves. Rate equation approaches to modeling are presented that result in predictions of rate constants for energy transfer processes, as well as more conventional approaches to modeling such as the Forster-Dexter models, which give the interaction strengths in terms of microscopic interaction parameters.
The compressible extensions of time asymptotic relaxation states of incompressible two-dimensional magnetohydrodynamic turbulence are studied. A polytropic equation of state is used with viscous and resistive dissipation. The incompressible case is known to allow three distinct time asymptotic types of behavior: magnetic energy dominated relaxation, kinetic energy dominated relaxation, and cross helicity dominated relaxation. At low Mach numbers the incompressible scenario is reproducible from the compressible simulations, and compressibility plays only a secondary role. At moderate, but still subsonic, Mach numbers the distinct incompressible processes are still recognizable, but strong compressibility features dominate the high-wave-number regime of several simulations. In particular, the magnetic and kinetic energy dominated simulations display regions of strong acoustic turbulence near the dissipation scale.
Strontium titanates ceramics containing various trivalent rare earth ions, observing dielectric relaxation