Photoacoustic detection of stimulated emission pumping in <i>p</i>-difluorobenzene

Moll, David; Parker, G. R. Jun.; Kuppermann, Aron

doi:10.1063/1.446500

Cited by 9 publications

(4 citation statements)

References 31 publications

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“…Equation 19 provides a general solution for the monochromatic TC-RFWM signal intensity generated when the SEP process of Figure 1 takes place in a medium possessing intrinsic angular momentum anisotropy, as defined by nonvanishing multipole moments, 〈T Q (K) (η g J g ) † 〉, of rank K > 0. 38,42 Consequently, this expression should be applicable to a variety of experimental measurements performed on nonequilibrated ensembles of target molecules that display net orientation and/or alignment, 28,41 including state-resolved probes of the nascent products emerging from chemical reactions and photofragmentation events.…”

Section: Theoretical Backgroundmentioning

confidence: 99%

“…The utility of this approach for studies of structure and dynamics stems from the unparalleled access that it affords to chemically relevant (i.e., vibrationally highly excited) regions of the molecular potential energy surface, with the selection rules imposed upon complementary infrared absorption techniques being supplanted by the less restrictive and, often times, more favorable considerations of Franck-Condon factors. The most common means of SEP detection rely on the competition that ensues between spontaneous and (-induced) stimulated emission processes acting on (-prepared) molecules in the intermediate state; however, several alternatives to this historical fluorescence-dip (FD-SEP) scheme have been proposed, including variants based on transient gain, linear birefringence/dichroism, photoacoustic, ionization-dip, and DFWM , measurements.…”

Section: Introductionmentioning

confidence: 99%

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Dissection of Rovibronic Structure by Polarization-Resolved Two-Color Resonant Four-Wave Mixing Spectroscopy

2009

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A synergistic theoretical and experimental investigation of stimulated emission pumping (SEP) as implemented in the coherent framework of two-color resonant four-wave mixing (TC-RFWM) spectroscopy is presented, with special emphasis directed toward the identification of polarization geometries that can distinguish spectral features according to their attendant changes in rotational quantum numbers. A vector-recoupling formalism built upon a perturbative treatment of matter-field interactions and a state-multipole expansion of the density operator allowed the weak-field signal intensity to be cast in terms of a TC-RFWM response tensor, RQ(K)(epsilon4*epsilon3epsilon2*epsilon1;Jg,Je,Jh,Jf), which separates the transverse characteristics of the incident and generated electromagnetic waves (epsilon4*epsilon3epsilon2*epsilon1) from the angular momentum properties of the PUMP and DUMP resonances (Jg,Je,Jh,Jf). For an isolated SEP process induced in an isotropic medium, the criteria needed to discriminate against subsets of rovibronic structure were encoded in the roots of a single tensor element, R0(0)(epsilon4*epsilon3epsilon2*epsilon1;Jg,Je,Jh,Je). By assuming all optical fields to be polarized linearly and invoking the limit of high quantum numbers, specific angles of polarization for the detected signal field were found to suppress DUMP resonances selectively according to the nature of their rotational branch and the rotational branch of the meshing PUMP line. These predictions were corroborated by performing SEP measurements on the ground electronic potential energy surface of tropolone in two distinct regimes of vibrational excitation, with the near-ultraviolet 1B2-1A1 (pi*<--pi) absorption system affording the requisite PUMP and DUMP transitions.

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Section: Theoretical Backgroundmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Dissection of Rovibronic Structure by Polarization-Resolved Two-Color Resonant Four-Wave Mixing Spectroscopy

2009

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“…Thus there should be no interference from the luminescence. For example, the photoacoustic method has been reported for the TA detection with a high sensitivity. − The thermal lens method is another way for that purpose. , Here I will show two methods of the two-step excitation transient grating (TSETG) detection technique for the detection of TA, compare both methods each other, and characterize the temporal profiles and sensitivities.…”

Section: Introductionmentioning

confidence: 99%

Two Methods of Two-Step Excitation Thermal Grating Technique for Detection of Transient Absorption and Stimulated Emission

Terazima

1997

J. Phys. Chem. A

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Two different methods for detection of the transient absorption (TA) and stimulated emission (SE) by using a two-step excitation thermal grating technique are characterized. The sensitivity and the temporal profile of the signals are analyzed in detail. One of them, prepulse−(delay)−grating pulse sequence, provides a very sensitive TA detection with a zero background. The other one, grating pulses−(delay)−boosting pulse sequence, has also a very high sensitivity for the detection of TA and SE together with an easy probe wavelength scanning. The high sensitivity of these methods comes from the cyclic excitation of the excited state and accumulation of the thermal energy. These methods are used to measure the T1−T n absorption spectrum of benzophenone, and the T1−T n absorption and SE spectra of rhodamine 6G.

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“…The advantages of employing photoacoustic (PA) technique for characterizing various molecular processes have been extensively discussed earlier [1,2]. The method relies essentially on the study of acoustic waves generated in the sample due to nonradiative transitions following the absorption of light energy.…”

Section: Introductionmentioning

confidence: 99%

Pulsed photoacoustic technique to study nonlinear processes in liquids: Results in toluene

et al. 1995

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Abstract. Pulsed photoacoustic measurements have been carried out in toluene at 532 nm wavelength using a Q-switched frequency doubled Nd:YAG laser. The variation of photoacoustic signal amplitude with incident laser power indicates that at lower laser powers one photon absorption takes place at this wavelength while a clear two photon absorption occurs in this liquid at higher laser powers. The studies made here demonstrate that pulsed photoacoustic technique is simple and effective for the investigation of multiphoton processes in liquids.

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Photoacoustic detection of stimulated emission pumping in p-difluorobenzene

Cited by 9 publications

References 31 publications

Dissection of Rovibronic Structure by Polarization-Resolved Two-Color Resonant Four-Wave Mixing Spectroscopy

Dissection of Rovibronic Structure by Polarization-Resolved Two-Color Resonant Four-Wave Mixing Spectroscopy

Two Methods of Two-Step Excitation Thermal Grating Technique for Detection of Transient Absorption and Stimulated Emission

Pulsed photoacoustic technique to study nonlinear processes in liquids: Results in toluene

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