Applications of infrared free-electron lasers: basic research on the dynamics of molecular systems

Dlott, Dana D.; Fayer, M. D.

doi:10.1109/3.104151

Cited by 36 publications

(11 citation statements)

References 53 publications

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“…For this purpose, we use the CLIO infrared free-electron laser (CLIO is the ''Centre Laser Infrarouge d'Orsay''). More than 15 years ago, Dlott and Fayer [1] pointed out the interest of infrared free-electron laser (FEL) sources for basic research on the vibrational dynamics of molecular systems. Such sources generate continuously tunable picosecond IR pulses suitable for time-resolved experiments based on pump-probe or photon-echo configurations.…”

Section: Introductionmentioning

confidence: 99%

IR spectra and vibrational dephasing of the CO stretching mode in W(CO)6 doped cryogenic matrices

et al. 2007

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Section: Introductionmentioning

confidence: 99%

IR spectra and vibrational dephasing of the CO stretching mode in W(CO)6 doped cryogenic matrices

et al. 2007

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“…Current methods of populating vibrational states include IR absorption using intense far IR laser light [1,3], stimulated Raman processes [1,2], and stimulated emission pumping [4].…”

mentioning

confidence: 99%

Population Pumping of Excited Vibrational States by Spontaneous Surface-Enhanced Raman Scattering

et al. 1996

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We observed significant transfer of ground state population to the first excited vibrational state by spontaneous surface-enhanced Raman scattering (SERS) which can be explained by unexpectedly large SERS cross sections. Evidence for this pumping includes (i) anti-Stokes to Stokes ratios which exceed those expected from a Boltzmann distribution, (ii) a quadratic dependence of the anti-Stokes signal on the excitation intensity, whereas the Stokes signal remains linearly dependent, and (iii) a component of n 1 to n 2 Raman transitions in the SERS Stokes signals. PACS numbers: 33.20.Fb, 42.62.Hk, 82.65.Pa New methods of exciting coherent and incoherent molecular vibrations are of growing interest as a prerequisite for studying phase and energy vibrational relaxation processes [1], as well as for creating chemical pathways which may not occur under normal excitation conditions [2]. Current methods of populating vibrational states include IR absorption using intense far IR laser light [1,3], stimulated Raman processes [1,2], and stimulated emission pumping [4].The extremely small cross sections of spontaneous Raman scattering preclude its use for pumping vibrational states. However, this situation is dramatically altered for surface-enhanced Raman scattering (SERS). Surfaceenhancement factors on the order of 10 10 or larger [5,6] increase the effective Raman cross sections from a range of 10 -31 -10 -29 to about 10 -20 cm 2 , suggesting that SERS can be a valuable tool for pumping vibrational states and performing vibrational pump-probe experiments on adsorbed molecules [7].In this Letter we show that SERS can significantly populate the first excited vibrational states of molecules adsorbed on the surface of colloidal metal particles, even under cw conditions at relatively low excitation intensities. We studied near infrared excited surfaceenhanced Stokes and anti-Stokes Raman scattering of crystal violet (CV) and rhodamine 6G (R6G) adsorbed on colloidal silver in aqueous solution. Samples were prepared in the same way as described previously [8,9] to achieve optimal conditions for SERS at near IR excitation.SERS spectra were measured from a 100 ml droplet of the colloidal sample solution placed on a glass microscope slide. A microscope attachment was used for excitation and for collecting the scattered light. The water immersion microscope objective was brought into direct contact with the droplet. Raman spectra were excited by means of an argon-ion laser pumped cw Ti:sapphire laser operating at 830 nm with a power of 10 to 150 mW at the sample. The scattered light was dispersed using a Chromex spectrograph with a deep depletion charge coupled device detector, This experimental geometry provides efficient signal acquisition, due to both a large collection angle and total overlap of excitation and collection volumes, as well as relatively high excitation intensities, between 4 3 10 23 and 5 3 10 24 photons͞cm 2 s. Figures 1(a) and 1(b) show Stokes and anti-Stokes SERS spectra of CV and R6G measured at 150 mW excita...

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“…There is currently considerable interest in compact, tunable radiation sources capable 3 of operating in the vibrational infrared (IR) (3-30pm) [12]. Conventional RF linac freeelectron lasers (FELs) with magnetostatic wigglers can operate in this region, but their use is constrained by size, cost, and shielding requirements.…”

Section: Introductionmentioning

confidence: 99%

New results and applications for the quasioptical gyrotron*

Fliflet

Fischer

Manheimer

1993

Physics of Fluids B: Plasma Physics

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Applications of infrared free-electron lasers: basic research on the dynamics of molecular systems

Cited by 36 publications

References 53 publications

IR spectra and vibrational dephasing of the CO stretching mode in W(CO)6 doped cryogenic matrices

IR spectra and vibrational dephasing of the CO stretching mode in W(CO)6 doped cryogenic matrices

Population Pumping of Excited Vibrational States by Spontaneous Surface-Enhanced Raman Scattering

New results and applications for the quasioptical gyrotron*

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