Applications of the time-resolved two-colour two-photon excitation of UV fluorophores using femtosecond laser pulses

Denicke, Stefan; Quentmeier, Stefan; Ehlers, Jan-Eric; Gericke, Karl‐Heinz

doi:10.1088/0031-8949/80/04/048105

Cited by 3 publications

(8 citation statements)

References 28 publications

(42 reference statements)

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“…Experiments on the time-resolved polarized TPEF have been pioneered by Lakowicz et al, [18][19][20] and a number of studies have been performed since that time. 7,8,16,[21][22][23][24][25] In this paper we report experimental and theoretical studies of TPEF in p-terphenyl molecules dissolved in cyclohexane/ paraffin using a 2C2P excitation scheme with femtosecond laser pulses combined with the time-resolved detection of the polarized molecular fluorescence. The 2C2P excitation scheme was earlier used by Lakowicz et al 21,22 in the UV spectral region with picosecond laser pulses.…”

Section: Introductionmentioning

confidence: 99%

“…The 2C2P excitation scheme was earlier used by Lakowicz et al 21,22 in the UV spectral region with picosecond laser pulses. The 2C2P scheme utilizing femtosecond laser pulses has recently been realized by the Braunschweig group 25,26 and possible biological and microscopic applications have been pointed out. 27 p-Terphenyl (PTP) is an important aromatic hydrocarbon that is widely used in the chemical and pharmaceutical industry as an antioxidant.…”

Section: Introductionmentioning

confidence: 99%

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Dynamics of Two-Color Two-Photon Excited Fluorescence of p-Terphenyl: Determination and Analysis of the Molecular Parameters

Denicke

Gericke²,

Smolin³

et al. 2010

J. Phys. Chem. A

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We present the experimental and theoretical study of the two-photon excited polarized fluorescence of p-terphenyl dissolved in cyclohexane/paraffin. The fluorescence was produced within a two-color two-photon (2C2P) excitation scheme utilizing simultaneous absorption of two femtosecond laser pulses at 400 nm and at 800 nm with the total excitation energy of 4.649 eV. The fluorescence was detected by a time correlated single photon counting (TCSPC) system with two detectors. Using different combinations of the absorbed photon polarizations we extracted seven time-dependent molecular parameters from experiment that contain all information on the dynamics of the three-photon process under study. The analysis of the obtained molecular parameter values was based on the ab initio calculations of the vertical excitation energies and transition matrix elements in p-terphenyl and allowed for determination of the whole structure of the two-photon absorption tensor, fluorescence lifetime, and the rotational correlation time. The obtained results imply that the fluorescence in the conditions of our experiment was governed mostly by the d(z) component of the fluorescence transition dipole moment that is parallel to the molecular long axis Z. The tensor was found to be symmetric. The two-photon excitation in p-terphenyl occurs simultaneously via two channels, one of them resulting in the population of the totally symmetric excited state and the other in the population of the nontotally symmetric excited state. Moreover, the energetically allowed pure electron transitions are dipole forbidden and become allowed by vibronic coupling.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Dynamics of Two-Color Two-Photon Excited Fluorescence of p-Terphenyl: Determination and Analysis of the Molecular Parameters

Denicke

Gericke²,

Smolin³

et al. 2010

J. Phys. Chem. A

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“…2,3 While most of the TPEF studies relied on the two-photon excitation with identical photons, the most general TPEF experiments employ a two-color two-photon (2C2P) excitation scheme. [4][5][6][7][8][9] In his seminal paper, 10 McClain has pointed out that for any experimental geometry the fluorescence polarization can be described by a linear combination of a number of molecular parameters which depend only on the intermolecular properties and excited state dynamics. As shown by McClain, 11 if the molecular excited state is not degenerate, the total number of molecular parameters is seven.…”

Section: Introductionmentioning

confidence: 99%

“…The use of femtosecond laser pulses in TPEF experiments makes it possible to track the evolution of the fluorescence from the anisotropic ensembles of excited molecules in the real time domain with high temporal resolution. 8,16 The Braunschweig group 8,9,17,18 has recently used the femtosecond 2C2P excitation scheme for detailed investigation of important UV fluorophores: p-terphenyl (PTP) 17 and 2-methyl-5-t-butylp-quaterphenyl (DMQ). 18 The complete set of molecular parameters has been determined from experiment in those studies which met the conditions of the complete polarization experiment.…”

Section: Introductionmentioning

confidence: 99%

Two-color two-photon excited fluorescence of indole: Determination of wavelength-dependent molecular parameters

Herbrich

Al-Hadhuri

Gericke

et al. 2015

The Journal of Chemical Physics

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We present a detailed study of two-color two-photon excited fluorescence in indole dissolved in propylene glycol. Femtosecond excitation pulses at effective wavelengths from 268 to 293.33 nm were used to populate the two lowest indole excited states (1)La and (1)Lb and polarized fluorescence was then detected. All seven molecular parameters and the two-photon polarization ratio Ω containing information on two-photon absorption dynamics, molecular lifetime τf, and rotation correlation time τrot have been determined from experiment and analyzed as a function of the excitation wavelength. The analysis of the experimental data has shown that (1)Lb-(1)La inversion occurred under the conditions of our experiment. The two-photon absorption predominantly populated the (1)La state at all excitation wavelengths but in the 287-289 nm area which contained an absorption hump of the (1)Lb state 0-0 origin. The components of the two-photon excitation tensor S were analyzed giving important information on the principal tensor axes and absorption symmetry. The results obtained are in a good agreement with the results reported by other groups. The lifetime τf and the rotation correlation time τrot showed no explicit dependence on the effective excitation wavelength. Their calculated weighted average values were found to be τf = 3.83 ± 0.14 ns and τrot = 0.74 ± 0.06 ns.

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“…In the current paper the experimental and theoretical studies of the two-photon excited fluorescence of DMQ dissolved in paraffin/cyclohexane are reported. The two-color two-photon (2C2P) excitation scheme ,,, was applied. Femtosecond laser pulses were used for the molecular excitation, and the temporal dependence of the polarized molecular fluorescence was detected in the real time domain.…”

Section: Introductionmentioning

confidence: 99%

Two-Color Two-Photon Excited Fluorescence of 2-Methyl-5-tert-butyl-p-quaterphenyl (DMQ): Ab Initio Calculations and Experimental Determination of the Molecular Parameters

et al. 2014

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The paper presents experimental and theoretical studies of two-photon excitation dynamics in 2-methyl-5-tert-butyl-p-quaterphenyl (DMQ) dissolved in cyclohexane/paraffin. Experimentally, a two-color two-photon (2C2P) excitation by two femtosecond laser pulses at 800 and 400 nm has been used in combination with the time-resolved detection of polarized molecular fluorescence. The fluorescence decay was found to be two-exponential, resulting in the molecular excited state lifetime of 753 ± 10 ps and the rotational correlation time of 724 ± 45 ps. Control over the excited and fluorescent photons polarization has been used for determination from experiment of seven independent molecular parameters. The experimental data were analyzed on the basis of the recent theoretical approach [Shternin, P. S., Gericke, K.-H., and Vasyutinskii, O. S. Mol. Phys. 2010, 108, 813-825] supported by ab initio computations of the DMQ electronic structure and transition dipole moments. The results obtained imply that the two-photon absorption tensor S is mostly diagonal and that the Szz tensor component onto the molecular long axis gives the major contribution of 93%. However, it was also found that a number of different symmetry two-photon transitions related to the dipole moment components dxdz and dydz are excited in the conditions of our measurements.

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Applications of the time-resolved two-colour two-photon excitation of UV fluorophores using femtosecond laser pulses

Cited by 3 publications

References 28 publications

Dynamics of Two-Color Two-Photon Excited Fluorescence of p-Terphenyl: Determination and Analysis of the Molecular Parameters

Dynamics of Two-Color Two-Photon Excited Fluorescence of p-Terphenyl: Determination and Analysis of the Molecular Parameters

Two-color two-photon excited fluorescence of indole: Determination of wavelength-dependent molecular parameters

Two-Color Two-Photon Excited Fluorescence of 2-Methyl-5-tert-butyl-p-quaterphenyl (DMQ): Ab Initio Calculations and Experimental Determination of the Molecular Parameters

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