Non-linear infrared spectroscopy of SF6 at 30 K

Hodgkinson, D.P.; Taylor, Antoinette; Wright, Doug; Robiette, A. G.

doi:10.1016/0009-2614(82)80032-8

Cited by 18 publications

(11 citation statements)

References 10 publications

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“…At 30 K there is encouraging agreement between theoretical and experimental multiphoton absorption spectra [12,16]. At this temperature, all molecules are initially in the vibrational ground state and distributed over about thirty rotational levels.…”

Section: Introductionmentioning

confidence: 69%

“…This is plausible since similar situations occur elsewhere, for example with octahedral splittings in the ~' a ladder [10][11][12] and with cubic potential energy terms which induce transitions to the vav a + (v S + v~) manifold of states [22].…”

Section: Introductionmentioning

confidence: 94%

“…The basic theory describing the excitation of v 3 mode vibration-rotation states by an intense infrared laser is described elsewhere [10][11][12]26]. Consequently, this section concentrates on the differences which arise when the Downloaded by [The University Of Melbourne Libraries] at 03: 36 19 June 2016 excitation starts from a state where one quantum of a triply-degenerate bending mode v~ (n=4, 5 or 6) is excited.…”

Section: Theorymentioning

confidence: 99%

“…Each laser excitation calculation then selects relevant molecular states and diagonalizes the lasermolecule interaction V(t). This procedure allows molecular states which are far from resonance or weakly coupled to the initial state to be excluded from the laser excitation calculations, thus reducing their size and cost [11,12].…”

Section: Theorymentioning

confidence: 99%

“…The major exception to this rule is the excitation of the v 3 mode of SF e by intense infrared radiation from a pulsed CO 2 laser. For this system, molecular parameters derived from high-resolution spectroscopy [4][5][6][7][8][9] have allowed quantitative calculations to be performed [10][11][12][13][14] and compared with experiments using gas-dynamically cooled SF 6 [15][16][17][18]. The refinement of such calculations and experiments, and their intercomparison, offers the best hope for gaining a full quantitative understanding of the initial stages of multiphoton absorption.…”

Section: Introductionmentioning

confidence: 99%

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Hot-band multiphoton absorption in SF₆

Hodgkinson¹,

Taylor²

1984

Molecular Physics

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Calculations have been carried out to investigate the differences between multiphoton absorption in SFe from the ground vibrational state and lowlying bending-mode states, using currently available estimates of the intermode mixing parameters G3n, S'3n and Tan. It is shown that in addition to being anharmonically shifted, the multiphoton absorption spectrum from the v4 state is anharmonically broadened and shows less pronounced structure than the equivalent absorption spectrum from the ground state.

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Section: Introductionmentioning

confidence: 69%

Section: Introductionmentioning

confidence: 94%

Section: Theorymentioning

confidence: 99%

Section: Theorymentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Hot-band multiphoton absorption in SF₆

Hodgkinson¹,

Taylor²

1984

Molecular Physics

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The Role of “Rotational Freezing” in the Polarisation‐Dependent Two‐Photon Excitation of Triply Degenerate Vibrations in Spherical‐Top‐Molecules

Ritze

1986

Annalen der Physik

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A b s t r a c t . Under certain circumstances at low rotational temperatures the multiphoton excitation probabilities of vibrational-rotational levels in high-symmetric molecules do not depend on the rotational quantum numbers J and M of the initially populated levels. Then the rotation of the molecule as a whole is "frozen". This has the consequence that during the absorption process the photon spin is not transferred to the molecular rotation but to the molecular vibration. I n more detail the two-photon A,,(v = 0 ) -+ A,,(v = 2) transition in SF, at 944.5 cm-1 is theoretically studied: If the "average lifetime" in the intermediate (v = 1)-level is small compared with the effective molecular rotation period the considered transition is forbidden for circularly polarised light. Further the excitation process of the E,(v = 2) and F2,(v = 2) vibrational levels is investigated; it is discussed under which conditions i t is not necessary to consider the rotational degrees of freedom for a calculation of transition dipole moments. Die Rolle der ,,Rotationseinfrierung" bei der polarisationsabhangigen Zwei-Photonen-Anregung dreifach entarteter Schwingungn in kugelkreiselartigen Molekiilen I n h a l t s i i b e r s i c h t . Unter gewissen Umstanden hangen bei tiefen Rotationstemperaturen dieMehrphotonen-Anregungswahrscheinlichkeiten von Schwingungs-Rotations-Niveaus hochsymmetrischer Molekule nicht von den Rotationsquantenzahlen J und 41 der anfanglich thermisch besetzten Niveaus ab. Dann ist die R'otation des Molekiils als gmzes ,,eingefroren". Dies hat zur Folge, da13 wahrend des Absorptionsprozesses der Photonenspin nicht auf die Molekiilrotation sondern anf die Molekulschwingung ubertragen wird. Detaillierter wird der Zwei-Photonen-A,,(v = 0) + A,,(v = 2 ) -Ubergang in SF, bei 944,6 cm-1 theoretisch untcrsucht : Wenn die ,,mittlere Verweildauer" im ( t l = 1)-Zwischenniveau klein im Vergleich zur effektiven Molekulrotationsperiode ist, ist der betrachtete Ubergang fur zirkular polarisiertes Licht vorboten. Des weiteren wird der AnregungsprozeB der X,(v = 2)-sowie F2,(v = 2)-Schwingungsniveaus untersucht; es wird diskutiert, unter melchen Bedingungen die Rotationsfreiheitsgrade bei einer Berechnung der ubergangsdipolmomente nicht berucksichtigt zu werden brauchen. (0 = 0,1= 0) -(v = I, 1 = 1) $ ill -+ Jf L+ M + M + l @? -1 w -1 ) ( J -41)

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