The invention described herein was made in the course of, or under, Contract No. W-7405-Eng-48, with the United States Energy Research and Development Administration.

BACKGROUND OF THE INVENTION

This invention is directed to laser systems, particularly to a thermally pumped/optically depumped gas laser systems, and more particularly to a fundamentally different method for obtaining laser action between an upper energy level and a lower energy level of a gaseous lasing medium by optically depumping the lower energy level.

An essential condition for laser action is an inverted population between an upper and a lower energy level in a lasing medium. The traditional method of obtaining such a population inversion is to "pump" the medium into the upper energy level; i.e., by exposing it to some kind of energy source (flash lamps, electron beams, electrical discharge, etc.) which excite the lasing species in the ground state so as to reach the upper energy or laser level.

A generic laser initiated technique for the photoseparation of heavy isotopes requires the selective excitation of a vibrational level of the working molecular gas. The relevant vibrational modes often lie in the mid infrared spectral region beyond ten microns where powerful tunable lasers do not exist. At the present time there is particular interest in developing powerful, and tunable lasers operating between 10 and 30 microns, a region moderately inaccessible by current technology. For example, a need exists for a reasonance (isotopic) laser at long wavelength, such as 16 microns, for UF₆ or SF₆, using CO₂ as the lasing medium. Since conventional "pumping" techniques affect each of the energy levels proportionally, a need exists for more effective methods of creating the desired population inversion in the desired energy level.

SUMMARY OF THE INVENTION

The present invention is fundamentally different than previously known pumping methods for gaseous lasing medium, in that the population inversion is obtained by diminishing the concentration of species in the lower energy level, rather than increasing the upper energy level population. This, of course, presupposes the presence of a useful population in the upper level at the time of depumping the lower level, whereby laser action can be obtained between the upper and lower levels.

Therefore, the present invention comprises a technique for the generation of coherent radiation in the low-lying vibrational-rotational transitions of polyatomic molecules. The carbon dioxide molecule is used herein as a specific model to illustrate the method because sufficient information is known for the CO₂ molecule to permit estimates of laser performance. However, the technique of producing a population inversion among the low-lying vibrational levels of molecules is quite general and other molecules of interest will be suggested hereinafter. The system of this invention is not sensitive to the kinds of means employed to populate the upper level or depopulate the lower one, and this has general application as to conventional lasing medium and means for accomplishing the pumping and depumping. However, a specifically preferred system is one wherein the mediums involved are polar molecular species and the energy levels are the vibrational states close to the ground state. In such systems, these low-lying vibrational states can be populated to a useful degree by simply elevating the temperature of the medium. Thereafter a transient population inversion is produced by rapidly pumping the molecules in the ground state to a higher energy level. Lasing is achieved by carrying out this process in a cavity resonant with respect to the desired laser transition, for example 16 microns. Thus, the invention encompasses a thermally pumped/optically depumped laser and is particularly directed to a 16 micron CO₂ laser, although other mediums and wavelengths can be utilized by this principle.

Therefore, it is an object of this invention to provide a method and apparatus for achieving laser action by optically depumping lower states of the lasing medium.

A further object of the invention is to provide a thermally pumped/optically depumped laser system.

Another object of the invention is to provide a method for obtaining laser action in a gaseous medium by diminishing the concentration of species in the lower energy level of a medium having a useful population in the upper energy level at the time of depumping the lower level.

Another object of the invention is to obtain laser action between an upper energy level and a lower energy level of a gaseous medium by populating to a degree the upper level and thereafter establishing an inverted population by transiently and selectively depumping the lower level.

Another object of the invention is to provide a thermally pumped/optically depumped 16 micron CO₂ laser system.

Other objects of the invention will become readily apparent from the following description and accompanying drawings.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 diagrammatically shows the relevant low-lying vibrational levels of a "typical" polyatomic molecule;

FIG. 2 diagrammatically illustrates the low-lying CO₂ vibrational levels;

FIG. 3 graphically shows the population inversion density as a function of temperature for two cases;

FIG. 4 graphically shows the available energy density and required pump energy density as functions of temperature for the two cases;

FIG. 5 schematically illustrates a flash lamp pumped CO₂ laser system for carrying out the invention; and

FIG. 6 schematically illustrates a parallel nozzle gas dynamic laser system for carrying out the invention.

DESCRIPTION OF THE INVENTION

In its broad aspects, the present invention involves a new method or technique for obtaining laser action between an upper energy level and a lower energy level of a gaseous medium. This method is fundamentally different, in that the population inversion is obtained by diminishing the concentration of species in the lower level, rather than increasing the upper level population as is done in conventional systems. The method is carried out by populating the upper level to some degree (short of achieving a conventional inverted population) by any suitable pumping means, and thereafter establishing an inverted population by transiently and selectively depumping the lower level, such as by exposing the medium to an intense source of radiation, which selectively causes the transformation of said lower level species to some other energy level. This method is not sensitive to the kinds of means employed to populate the upper level or depopulate the lower one. However, a preferred system utilizes a gaseous medium having polar molecular species and the energy levels are the vibrational states close to the ground state. In such systems, these low-lying vibrational states can be populated to a useful degree by simply elevating the temperature of the medium. Thereafter a transient population inversion is produced by rapidly pumping the molecules in the ground state to a higher energy level. Lasing is achieved by carrying out this process in a cavity resonant with respect to the desired laser transition. While not limited to the wavelength or medium the following description is directed to a 16 micron CO₂ laser system. Another example is SF₆ or UF₆ as the gaseous medium wherein the lower level can be depumped with a CO₂ laser.

By employing a thermal source to put population density in an upper energy or laser of a gaseous medium, such as CO₂, SF₆ or UF₆, and an optical (incoherent) source to transiently depump the lower laser (ground) level, an (isotopic) resonance laser at long wavelength, such as 16 microns, can be accomplished. It is also possible using this concept to attain continuous wave (CW) coherent radiation using a flowing working medium.

FIG. 1 shows the relevant low-lying vibrational levels to a "typical" polyatomic molecule with the g-values giving the vibrational degeneracies of the respective level. Level 1 is the vibrationless ground level, level 2 is the lowest-lying vibrational level connected to the ground level by an "allowed" electric dipole transition, and level k is some higher lying vibrational level also connected to the ground level by an electric dipole transition. Level j represents all other vibrational levels of the molecule. The following is set forth to illustrate how to create a transient population inversion between vibrational energy level 2 and the vibrationless ground level 1, providing for net gain at a photon energy E₁ (or wavelength λ_l = hc/E₁). A population inversion, ΔN, between these two levels can be expressed as ##EQU1## where the f-superscript indicates the pumped, nonequilibrium condition.

The generic technique to achieve this condition is as follows. Start with a working gas sample at some equilibrium pressure P⁰ and temperature T⁰ (N_T molecules/cc.). The molecules will be distributed among all of the vibrational and rotational modes (levels) of the molecule according to a Boltzman distribution. As the temperature is raised, level 2 gains population at the expense of level 1, as expressed by ##EQU2##where energy, E, is expressed in cm^{- 1} and T in ^o K and the superscript "o" indicates initial, thermodynamic equilibrium conditions. To achieve the population condition expressed by Eq. (1), we can act on the gas, either by putting more molecules into level 2, or removing molecules from level 1, in a time short compared with the time for the system to return to equilibrium. The following utilizes the latter option. It is proposed to depump the lower (ground) laser level (1) by irradiation of the gas sample at wavelengths corresponding to the transition ν_p shown in FIG. 1. The initial (equilibrium) population of level k is given by ##EQU3##

The equilibrium population density of N_l.sup. o (T) depends on the temperature T and is given by ##EQU4## where the sum -j is over all vibrational levels besides levels 1 and 2. Upon application of a saturating pulse of radiation at frequency ν_p, the populations of levels j and k will be modified to maximum "depumped" values N_l ^f and N_k ^f given by ##EQU5## and ##EQU6##where we have taken g_l = 1 appropriate for vibrationless ground levels. If the depumping pulse of radiation is sufficiently fast (see below) the initial and final values of level 2 populations will be the same

N2 f = N2 o                              (7)

Combining equations (2) - (7), we can write the induced population inversion density ΔN as ##EQU7## From Eq. (8), we observe that a population inversion density ΔN≧0 will exist above some temperature T_min, (when the quantity within the bracket exceeds zero) where T_min is defined by ##EQU8## This transcendental equation cannot be directly solved for T_min, but in the limit when E_k >>T_min, Eq. (9) reduces to ##EQU9## so that ##EQU10## Obviously, a high value for g_k is desirable since it can reduce T_min significantly. Expansion of Eq. (9) for large temperatures also shows that a population inversion can always be induced at some temperature provided E_k and E₂ satisfy the inequality which for the worst case (g_k = 1) requires E_k =2E₂. However, since N₁ ^o (T) → O as T → ∞ , the population inversion density ΔN(T) may not be significantly large for high values of T. The number of pump photon absorbed per unit volume to achieve maximum depumping of the ground level is ##EQU11## and the pump energy absorbed per unit volume is ##EQU12## Similarly, the maximum available stored energy density for this (essentially) two-level laser system is ##EQU13##

As an example of the "thermally-pumped, optically-depumped" laser technique, consider the CO₂ molecule. The low-lying CO₂ vibration levels are shown in FIG. 2. The lowest-lying vibrational level is that of the fundamental bending mode, (01¹ 0) which is coupled to the ground level by a large electric dipole transition centered at a wavelength λ_l = 15.0 microns (ν_l = 667 cm^{- 1}). We consider two specific depumping cases for inverting the (01¹ 0) level with respect to the (00^o 0) ground level. Case I, pumping in the 4.35 μ fundamental band (00^o 0) → (00^o 1) to the singly degenerate (00^o 1) asymmetric stretching mode. Case II, pumping in the 2.7 μ combination bands (00^o 0) → (10^o 1)(02^o 1), with an effective degeneracy of g.sub. k = 2. We assume an operating pressure of 10 torr CO₂ for all temperatures and calculate N₁ ^o (T), ΔN(T), S_p, and E_l for Case I (g.sub. k = 1, E_k = 2349 cm^{- 1}), and Case II (g.sub. k = 2, E_k = 3650 cm^{- 1}). FIG. 3 shows the population inversion density as a function of temperature for the two cases and FIG. 4 shows the available energy density and required pump energy density as functions of temperature for both cases. Note the relatively larger inversion density and available laser energy density occurring at lower temperature in Case II, due primarily to the greater pump level degeneracy (g.sub. k = 2). Taking the calculated inversion densities, the measured electric dipole transition moment for the 00^o 0 → 01¹ 0 transition (R = 0.18 Debye), and the expressions for vibrational-rotational linestrengths given by Rademacker and Reiche, Zeit f. Phys. K, 41,453 (1927) and by Crawford and Dinsmore J. Chem. Phys. 18, 983 (1950), estimates for the small signal gains of the P, Q, and R branch transitions can be made. Detailed calculations will not be presented here; peak P-branch calculated gains are several percent per cm and appear to be adequate for operation of laser devices.

The characteristic time, t_p, required for the pump energy to be delivered to attain population inversion is determined by the vibrational, rotational, and translational kinetics. Upon pump irradiation, all of the excited vibrational energy levels will be out of thermodynamic equilibrium. In the case of CO₂, the 01¹ 0 bending mode may return to equilibrium through collisions of the type:

CO2 (011 0) + CO2 (011 0) → CO2 (02°0) + CO2 (00°0) + 50 cm- 1 (16)

CO2 (011 0) + M → CO2 (00°0) + M + 667 cm- 1                                            (17)

Typical rates for the V-V (Vibration-Vibration) processes (Eq. 16), are 10⁶ sec ^{- 1} torr^{- 1} ; the V-T (Vibration-Translation) deactivation rate for ν₂ of CO₂ at 1000° K is 1.6 × 10³ sec^{- 1} torr^{- 1}. It therefore appears that V-V processes will constrain the pumping pulse width to values less than one μsec for pressures of a torr or greater. The pump source in the example of CO₂ can be HBr laser (Case I) which has been used to pump the (00°0) → (00°1) transition in CO₂ and in N₂ O, see Chang et al, Appl. Phys. Letters 21, 19 (1972); 23, 370 (1973); and 22, 93 (1973). The HF laser with emission wavelengths near 2.7 μ may be useful for pumping CO₂ in Case II. FIG. 5 schematically illustrates an optical resonator for containing the gaseous medium and a flashlamp type pump source therefore operating at frequency .sub.(λ_l = 16μ), as indicated by the arrow. However, the flashlamp can be replaced by another type of an intense spectral source.

It has been assumed here that the pump intensity is sufficient to saturate the pump transition and that the pump does not drive overtone transitions. If this occurs, the maximum inversion densities calculated above may be increased further. Radiation transport and V-V kinetics must be examined for each molecule and pump source to establish attainable population inversion densities, output energies, and optimum laser/pump geometries.

Table I lists a number of simple polyatomic molecules which may be used for infrared lasers based on the thermally-pumped, optically inverted molecular lasers of this invention. The energies and wavelengths given under the heading "Laser Band" correspond to the lower lying, infrared active transitions of the molecules listed in the left hand column. Only mean transition wavelengths are listed in lieu of all possible P, Q, and R vibration-rotational transition wavelengths. Isotopically substituted working species can greatly extend the number of attainable transition wavelengths. Possible pump transitions are listed under the heading "Pump Band" together with an indication of the transition strength, R(νν¹).

                                  TABLE 1__________________________________________________________________________MOLECULE  LASER BAND    PUMP BAND__________________________________________________________________________  E(cm- 1)         λ(μ)              Mode                 E(cm- 1)                        λ(μ)                             Mode R(νν1)__________________________________________________________________________SO2  519    19.3 ν2                 1151.2 8.69 ν1                                  Strong                 1361.  7.35 ν3                                  Strong                 1871.  5.34 ν2 +ν3                                  MediumCO2  667.3  15.0 ν2                 2349.3 4.26 ν3                                  Strong                 3609.  2.77 2ν2 +ν3                                  Medium                 3716.  2.69 ν1 +ν3                                  MediumN2 O  588.8  17.0 ν2                 1285.0 7.78 ν1                                  Strong                 2223.5 4.50 ν3                                  StrongCS2  396.7  25.2 ν2                 1523.  6.57 ν3                                  StrongHCN    712.   14.0 ν2                 1412.  7.08 2ν2                                  Strong                 2800.  3.57 ν1 +ν2                                  Medium                 3312.  3.02 ν3                                  MediumHDS    1090.  9.17 ν2                 2109.  4.75 2ν2                                  Medium                 2684.  3.73 ν3                                  StrongD2 S  934.   10.7 ν2                 1999.  5.00 ν3                                  StrongNO2  648.   15.4 ν2                 1621.  6.17 ν3                                  StrongO3  710.   14.1 ν2                 1043.4 9.58 ν1                                  Strong                 1740.  5.75 ν3                                  WeakC2 H2  729.1  13.7 ν5                 3287.  3.04 ν3                                  Strong                 1328.  7.53 ν4 +ν5                                  MediumC2 D2  539.1  18.5 ν5                 1044.  9.58 ν4 +ν5                                  Weak                 2427.  4.12 ν3                                  StrongC2 HD  518.8  19.3 ν4                 1851.2 5.40 ν2                                  Medium  683.   14.6 ν5                 2584.  3.87 ν3                                  Strong                 3334.8 3.00 ν1                                  StrongC2 N2  226.   44.2 ν5                 732.   13.7 ν4 +ν5                                  Strong                 2149.  4.65 ν3                                  StrongB10 F3  482.0  20.7 ν4                 1497.  6.68 ν3                                  Strong  719.5  13.9 ν2CD4  995.6  10.0 ν4                 2258.2 4.43 ν3                                  StrongCH3 Cl  732.1  13.6 ν3                 1015.  9.58 ν6                                  Medium                 1354.9 7.38 ν2                                  Strong                 1454.6 6.87 ν5                                  Medium                 2966.2 3.37 ν1                                  V. Strong                 3041.8 3.29 ν4                                  MediumCH3 Br  611.   16.4 ν3                 952.   10.5 ν6                                  Medium                 1305.  7.66 ν2                                  Strong                 1445.  6.92 ν5                                  Medium                 2972.0 3.36 ν1                                  V. Strong                 3055.9 3.27 ν4                                  MediumCH2 Cl2  704.   14.2 ν3                 1155.  8.66 ν5                                  Weak(Methylene  737.   13.6 νg                 1266.  7.90 ν8                                  V. StrongChloride)  899.   11.1 ν7                 1429.  7.00 ν2                                  StrongCH3 C ≡ CH  643.   15.6 νg                 926.   10.8 ν5                                  StrongMethyl                1041.  9.6  ν8                                  WeakAcetylene                 2994.  3.34 ν6                                  V. Strong                 3429.  2.92 ν1                                  Strong__________________________________________________________________________

An alternative system is illustrated in FIG. 6 and consists of parallel gas dynamic laser (GDL) nozzles where the stagnation temperature (T) and pressures (P) for each nozzle are adjusted to provide the desired supersonic flow characteristics. Medium CO₂ in one nozzle at T_o, P_p, ν_o is the working laser medium which is irradiated before equilibrium by depumping radiation from the CO₂ medium in the other nozzle at T₁, P₁, ν₁. A reflector M₃ directs depumping radiation downward as indicated by the arrow. The optical resonator, not shown, (composed of mirrors or reflectors similar to M₁ and M₂ in FIG. 5) at λ=16 is placed perpendicular to the plane of the paper in the laser medium.

Each of the illustrated and/or described systems can be numerically evaluated since the 01¹ 0 - 00⁰ 0 equilibration time is known as a function of temperature, and the required optical transition strengths are available for CO₂.

Again, it is pointed out that while the description has been primarily directed to CO₂ as the gaseous lasing medium, use of other mediums such as UF₆ and SF₆ and those set forth in Table I, are within the scope of this invention. For example, with SF₆, where the lower level can be depumped with a CO₂ laser, the second level is thermally populated for laser action at room temperature.

While the invention has been described with respect to 16 .sub.μ frequencies, the advantage of the method is that it provides an ability to achieve laser radiation at many frequencies (10-30 .sub.μ) at which no other lasers are presently available.

It has thus been shown that the present invention provides a fundamentally different method of achieving laser action, that being, by optically depumping lower energy levels rather than increasing the upper energy levels as previously done. Thus, this invention provides a substantial advance in the gas laser art.

While particular parameters and means for carrying out the invention have been illustrated and described, modifications will become apparent to those skilled in the art, and it is intended to cover in the appended claims all such modifications as come within the spirit and scope of the invention.