Femtosecond stimulated Raman spectroscopy

Frontiera, Renee R.; Mathies, Richard A.

doi:10.1002/lpor.200900048

Cited by 96 publications

(120 citation statements)

References 78 publications

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“…The destruction of the cluster sizes and shapes needed for the SE-CARS process mechanically or due to laser ablation result in a signal decrease. This is also reported in the SE-FSRS experiments by Renee et al [47] Our observations made with SNOM tips as well as with AFM tips, which have nanometer-sized gold spheres attached, confirmed that SE-CARS can be used also for near-field microscopy. A better understanding of the SE effect is however needed.…”

Section: Figure 10supporting

confidence: 87%

“…Christian et al [46] performed SE-CARS on benzenethiol molecules adsorbed onto nano-structured gold surfaces; they observed an enhancement factor of 10 9 . Renee et al [47] used gold nano-antennas to enhance the femtosecond stimulated Raman signal (SE-FSRS), where they could observe an enhancement of 10 4 . In our studies, the largest enhancement factor observed for femtosecond SE-CARS was 10 when using a pump wavelength of 550 nm.…”

Section: Figure 10mentioning

confidence: 99%

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Nonlinear spectroscopy in the near-field: time resolved spectroscopy and subwavelength resolution non-invasive imaging

et al. 2014

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Abstract:The combination of near-field microscopy along with nonlinear optical spectroscopic techniques is presented here. The scanning near-field imaging technique can be integrated with nonlinear spectroscopic techniques to improve spatial and axial resolution of the images. Additionally, ultrafast dynamics can be probed down to nano-scale dimension. The review shows some examples for this combination, which resulted in an exciton map and vibrational contrast images with subwavelength resolution. Results of two-color femtosecond time-resolved pump-probe experiments using scanning near-field optical microscopy (SNOM) on thin films of the organic semiconductor 3,4,9,10 Perylenetetracarboxylic dianhydride (PTCDA) are presented. While nonlinear Raman techniques have been used to obtain highly resolved images in combination with near-field microscopy, the use of femtosecond laser pulses in electronic resonance still constitutes a big challenge. Here, we present our first results on coherent anti-Stokes Raman scattering (fs-CARS) with femtosecond laser pulses detected in the near-field using SNOM. We demonstrate that highly spatially resolved images can be obtained from poly(3-hexylthiophene) (P3HT) nano-structures where the fs-CARS process was in resonance with the P3HT absorption and with characteristic P3HT vibrational modes without destruction of the samples. Sub-diffraction limited lateral resolution is achieved. Especially the height resolution clearly surpasses that obtained with standard microCARS. These results will be the basis for future investigations of mode-selective dynamics in the near-field.

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Section: Figure 10supporting

confidence: 87%

Section: Figure 10mentioning

confidence: 99%

Nonlinear spectroscopy in the near-field: time resolved spectroscopy and subwavelength resolution non-invasive imaging

et al. 2014

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“…[4][5][6][7][8][9][10][11][12][13][14][15][16][17][18] Interestingly, Chen et al reported that for such systems the switching between conducting and non-conducting states appears to be related to the dihedral angles between the chromophores. 19,20 The photophysical properties of 1,4-bis(phenylethynyl) benzene (BPEB) (Fig.…”

Section: Introductionmentioning

confidence: 99%

Mode specific excited state dynamics study of bis(phenylethynyl)benzene from ultrafast Raman loss spectroscopy

Roy

Kayal

Ariese

et al. 2017

The Journal of Chemical Physics

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Femtosecond transient absorption (fs-TA) and Ultrafast Raman Loss Spectroscopy (URLS) have been applied to reveal the excited state dynamics of bis(phenylethynyl)benzene (BPEB), a model system for one-dimensional molecular wires that have numerous applications in opto-electronics. It is known from the literature that in the ground state BPEB has a low torsional barrier, resulting in a mixed population of rotamers in solution at room temperature. For the excited state this torsional barrier had been calculated to be much higher. Our femtosecond TA measurements show a multi-exponential behaviour, related to the complex structural dynamics in the excited electronic state. Time-resolved, excited state URLS studies in different solvents reveal mode-dependent kinetics and picosecond vibrational relaxation dynamics of high frequency vibrations. After excitation, a gradual increase in intensity is observed for all Raman bands, which reflects the structural reorganization of Franck-Condon excited, non-planar rotamers to a planar conformation. It is argued that this excited state planarization is also responsible for its high fluorescence quantum yield. The time dependent peak positions of high frequency vibrations provide additional information: a rapid, sub-picosecond decrease in peak frequency, followed by a slower increase, indicates the extent of conjugation during different phases of excited state relaxation. The CC triple (–C≡C–) bond responds somewhat faster to structural reorganization than the CC double (>C=C<) bonds. This study deepens our understanding of the excited state of BPEB and analogous linear pi-conjugated systems and may thus contribute to the advancement of polymeric “molecular wires.”

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“…However, using the conventional method, it is difficult to obtain the satisfactory frequency resolution for Raman spectroscopy due to the uncertainty principle of quantum mechanics. Femtosecond timeresolved Raman spectroscopy can become feasible using the process of stimulated Raman scattering [42][43][44][45]. Three laser pulses are used in the femtosecond stimulated Raman spectroscopy.…”

Section: Time-resolved Raman Gain and Loss Spectroscopiesmentioning

confidence: 99%

Ultrafast time-resolved vibrational spectroscopies of carotenoids in photosynthesis

Hashimoto

Sugisaki

Yoshizawa

2015

Biochimica et Biophysica Acta (BBA) - Bioenergetics

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This review discusses the application of time-resolved vibrational spectroscopies to the studies of carotenoids in photosynthesis. The focus is on the ultrafast time regime and the study of photophysics and photochemistry of carotenoids by femtosecond time-resolved stimulated Raman and four-wave mixing spectroscopies. This article is part of a Special Issue entitled: Vibrational spectroscopies and bioenergetic systems.

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Femtosecond stimulated Raman spectroscopy

Cited by 96 publications

References 78 publications

Nonlinear spectroscopy in the near-field: time resolved spectroscopy and subwavelength resolution non-invasive imaging

Nonlinear spectroscopy in the near-field: time resolved spectroscopy and subwavelength resolution non-invasive imaging

Mode specific excited state dynamics study of bis(phenylethynyl)benzene from ultrafast Raman loss spectroscopy

Ultrafast time-resolved vibrational spectroscopies of carotenoids in photosynthesis

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