Ultrafast Time-Resolved Spontaneous and Coherent Raman Spectroscopy: The Structure and Dynamics of Photogenerated Transient Species

Hamaguchi, Hiro O.; Gustafson, Terry L.

doi:10.1146/annurev.pc.45.100194.003113

Cited by 122 publications

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“…The timescales and nature of these processes are extremely important in designing these complexes because they are responsible for the partitioning of photon energy between desirable electron-transfer and undesirable energy-dissipation mechanisms through vibrational coupling or nonradiative decay. Time-resolved FSRS spectra of the initial dynamics upon photon absorption by Ru(bpy) 3 2+ are presented in Figure 5b. As the time delay is increased from 0 fs, the growth of vibrational bands at 1208, 1498, and 1548 cm -1 can be observed and is complete in ~300 fs.…”

Section: Ridiculously Fast Time-resolved Fsrsmentioning

confidence: 99%

Femtosecond Stimulated Raman Spectroscopy

Kukura

Yoon²,

Mathies³

2006

Anal. Chem.

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R aman spectroscopy is a powerful analytical technique for revealing vibrational structure. It is widely used in biology, chemistry, and studies of molecular reaction dynamics (1-3). One of the technique's greatest advantages is that a single spectrum contains a wealth of vibrational structural information about the sample. The large number of well-resolved vibrational bands provides unique information analogous to a human fingerprint, and the technique is very sensitive to molecular structure. Changes in bond lengths of as little as 0.01 Å can produce clear differences in the vibrational spectrum. This specificity and sensitivity make Raman an excellent tool for trace analysis and for studies of chemically induced structural changes.Although a wide variety of Raman techniques have been developed over the years and applied to analytical problems, significant room for improvement still exists. FT Raman methods are often used in industrial applications to avoid background fluorescence-via intense laser radiation in the NIR-and to exploit the FT multiplex advantage. Clinical applications of FT Raman range from identification of cancerous tissues to microscopic imaging (4). However, it can suffer from weak resonance enhancement and intense Rayleigh scattering caused by the noise distribution of the FT (5). In surface-enhanced Raman spectroscopy, spectra of molecules adsorbed to roughened metallic surfaces or nanostructures can be taken with extreme sensitivity; however, the technique relies on the not-easily-controlled interaction of the metallic substrates with the analyte (6). Raman imaging has recently been advanced through the use of nonlinear Raman techniques, in particular coherent anti-stokes Raman scattering (CARS), which has been used, for example, to monitor biological processes in real time (7,8). Despite these advances, limitations exist that prevent these methods from exploiting the full potential of Raman scattering. We asked: Can an analytical resonance Raman technique be developed that can produce high-S/N spectra that are immune to background fluorescence, with short data-acquisition times?Time-resolved vibrational spectroscopies are also extensively used in structural studies of dynamics of chemical and biological reactions. The earliest (<50-fs) events in photochemical and photophysical processes are best studied by resonance Raman intensity analysis, an extremely powerful technique that can provide detailed excited-state structural information (9, 10). Spontaneous time-resolved resonance A new approach for obtaining vibrational Raman spectra and for studying chemical reaction dynamics. 9 4 A N A LY T I C A L C H E M I S T R Y / S E P T E M B E R 1 , 2 0 0 6Raman spectroscopy is limited to the picosecond time domain because of the transform limit; this prevents the technique from being applied to chemical reactions that occur on the order of 10 f s-1 ps. This limitation has recently been overcome by the availability of femtosecond pulses in the IR. As a consequence, pump-probe approaches for measu...

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Section: Ridiculously Fast Time-resolved Fsrsmentioning

confidence: 99%

Femtosecond Stimulated Raman Spectroscopy

Kukura

Yoon²,

Mathies³

2006

Anal. Chem.

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“…Furthermore, the structural information obtained from luminescence spectroscopy is rather limited. These difficulties can be well compensated for by time-resolved vibrational (infrared and Raman) spectroscopy which looks directly into the structure of excited states [1,2].…”

Section: Introductionmentioning

confidence: 99%

Recent Developments in Ultrafast Time-Resolved Vibrational Spectroscopy of Electronically Excited States

Hamaguchi

1999

Acta Phys. Pol. A

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Developments of three new time-resolved vibrational spectroscopies and their applications to electronically excited states are reviewed. Transform--limited picosecond time-resolved Raman spectroscopy has been used to study the vibrational dynamics of trans-stilbene in the lowest excited singlet state. Picosecond time-frequency two-dimensional multiplex Coherent Antistokes Raman Scattering spectroscopy has been used to probe the structure of diphenylacetylene in the lowest and the second lowest excited singlet states. Nanosecond time-resolved dispersive infrared spectroscopy has detected the singlet and triplet intramolecular charge transfer states of 4-(dimethylamino)benzonitrile. Strong evidence for a charge transfer structure has been obtained.

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“…Thus, in the presence of very strong fluorescence, shifted excitation techniques on their own are insufficient. In this work we demonstrate the advantages of time-resolved Raman spectroscopy [28,29] using a 532 nm excitation source. This technique offers a means of using a visible light (green) excitation source while at the same time effectively reducing fluorescence interference.…”

Section: Source Wavelength Selectionmentioning

confidence: 99%

Miniaturized time-resolved Raman spectrometer for planetary science based on a fast single photon avalanche diode detector array

et al. 2016

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We present recent developments in time-resolved Raman spectroscopy instrumentation and measurement techniques for in situ planetary surface exploration, leading to improved performance and identification of minerals and organics. The time-resolved Raman spectrometer uses a 532 nm pulsed microchip laser source synchronized with a single photon avalanche diode array to achieve sub-nanosecond time resolution. This instrument can detect Raman spectral signatures from a wide variety of minerals and organics relevant to planetary science while eliminating pervasive background interference caused by fluorescence. We present an overview of the instrument design and operation and demonstrate high signal-to-noise ratio Raman spectra for several relevant samples of sulfates, clays, and polycyclic aromatic hydrocarbons. Finally, we present an instrument design suitable for operation on a rover or lander and discuss future directions that promise great advancement in capability.

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Ultrafast Time-Resolved Spontaneous and Coherent Raman Spectroscopy: The Structure and Dynamics of Photogenerated Transient Species

Cited by 122 publications

References 0 publications

Femtosecond Stimulated Raman Spectroscopy

Femtosecond Stimulated Raman Spectroscopy

Recent Developments in Ultrafast Time-Resolved Vibrational Spectroscopy of Electronically Excited States

Miniaturized time-resolved Raman spectrometer for planetary science based on a fast single photon avalanche diode detector array

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