Generation, shaping, and characterization of intense femtosecond pulses tunable from 3 to 20 μm

Kaindl, Robert A.; Wurm, Matthias; Reimann, K.; Hamm, Peter; Weiner, Andrew M.; Woerner, M.

doi:10.1364/josab.17.002086

Cited by 300 publications

(171 citation statements)

References 40 publications

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“…[47] Tunable mid-infrared probe pulses of 100-150 fs duration were generated by difference frequency mixing of signal and idler pulses from a near-infrared optical parametric amplifier. [48] After spectral dispersion with a polychromator the probe pulses were detected by a multichannel detector for the mid-IR. The whole pump-probe setup was purged with nitrogen gas to avoid spectral and temporal reshaping of the mid-IR pulse by the absorption of water vapour in the air.…”

Section: Methodsmentioning

confidence: 99%

Solvent‐Dependent Photoacidity State of Pyranine Monitored by Transient Mid‐Infrared Spectroscopy

et al. 2005

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We investigate with femtosecond mid‐infrared spectroscopy the vibrational‐mode characteristics of the electronic states involved in the excited‐state dynamics of pyranine (HPTS) that ultimately lead to efficient proton (deuteron) transfer in H2O (D2O). We also study the methoxy derivative of pyranine (MPTS), which is similar in electronic structure but does not have the photoacidity property. We compare the observed vibrational band patterns of MPTS and HPTS after electronic excitation in the solvents: deuterated dimethylsulfoxide, deuterated methanol and H2O/D2O, from which we conclude that for MPTS and HPTS photoacids the first excited singlet state appears to have charge‐transfer (CT) properties in water within our time resolution (150 fs), whereas in aprotic dimethylsulfoxide the photoacid appears to be in a nonpolar electronic excited state, and in methanol (less polar and less acidic than water) the behaviour is intermediate between these two extremes. For the fingerprint vibrations we do not observe dynamics on a time scale of a few picoseconds, and with our results obtained on the OH stretching vibration we argue that the dynamic behaviour observed in previous UV/Vis pump–probe studies is likely to be related to solvation dynamics.

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Section: Methodsmentioning

confidence: 99%

Solvent‐Dependent Photoacidity State of Pyranine Monitored by Transient Mid‐Infrared Spectroscopy

et al. 2005

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“…6,26 Briefly, tunable mid-IR pulses with a center frequency between 1000 and 1300 cm −1 , a spectral bandwidth of 200 cm −1 , and a duration of 100 fs are generated by nonlinear parametric frequency conversion. 48 2D spectra are acquired with a noncollinear 3-pulse photon echo experiment.…”

Section: A Experimentalmentioning

confidence: 99%

Ultrafast phosphate hydration dynamics in bulk H2O

Costard

Tyborski

Fingerhut

et al. 2015

The Journal of Chemical Physics

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Phosphate vibrations serve as local probes of hydrogen bonding and structural fluctuations of hydration shells around ions. Interactions of H2PO4− ions and their aqueous environment are studied combining femtosecond 2D infrared spectroscopy, ab-initio calculations, and hybrid quantum-classical molecular dynamics (MD) simulations. Two-dimensional infrared spectra of the symmetric (νS(PO2−)) and asymmetric (νAS(PO2−)) PO2− stretching vibrations display nearly homogeneous lineshapes and pronounced anharmonic couplings between the two modes and with the δ(P-(OH)2) bending modes. The frequency-time correlation function derived from the 2D spectra consists of a predominant 50 fs decay and a weak constant component accounting for a residual inhomogeneous broadening. MD simulations show that the fluctuating electric field of the aqueous environment induces strong fluctuations of the νS(PO2−) and νAS(PO2−) transition frequencies with larger frequency excursions for νAS(PO2−). The calculated frequency-time correlation function is in good agreement with the experiment. The ν(PO2−) frequencies are mainly determined by polarization contributions induced by electrostatic phosphate-water interactions. H2PO4−/H2O cluster calculations reveal substantial frequency shifts and mode mixing with increasing hydration. Predicted phosphate-water hydrogen bond (HB) lifetimes have values on the order of 10 ps, substantially longer than water-water HB lifetimes. The ultrafast phosphate-water interactions observed here are in marked contrast to hydration dynamics of phospholipids where a quasi-static inhomogeneous broadening of phosphate vibrations suggests minor structural fluctuations of interfacial water.

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“…The OPA with a β-barium borate (BBO) crystal pumped by the fundamental of a Ti:sapphire amplifier generates a signal and an idler wave in the wavelength range between 1 and 2.5 µm, and the difference frequency generation between the signal and the idler in a AgGaS 2 crystal produces an MIR pulse [6,7]. Such a system has already been commercially available (TOPAS, light conversion).…”

Section: Introductionmentioning

confidence: 99%

Generation of Phase-Stable Sub-Cycle Mid-Infrared Pulses from Filamentation in Nitrogen

Fuji

Nomura

2013

Applied Sciences

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Sub-single-cycle pulses in the mid-infrared (MIR) region were generated through a laser-induced filament. The fundamental (ω 1 ) and second harmonic (ω 2 ) output of a 30-fs Ti:sapphire amplifier were focused into nitrogen gas and produce phase-stable broadband MIR pulses (ω 0 ) by using a four-wave mixing process (ω 1 + ω 1 − ω 2 → ω 0 ) through filamentation. The spectrum spread from 400 cm −1 to 5500 cm −1 , which completely covered the MIR region. The low frequency components were detected by using an electro-optic sampling technique with a gaseous medium. The efficiency of the MIR pulse generation was very sensitive to the delay between the fundamental and second harmonic pulses. It was revealed that the delay dependence of the efficiency came from the interference between two opposite parametric processes, ω 1 + ω 1 − ω 2 → ω 0 and ω 2 − ω 1 − ω 1 → ω 0 . The pulse duration was measured as 6.9 fs with cross-correlation frequency-resolved optical gating by using four-wave mixing in nitrogen. The carrier-envelope phase of the MIR pulse was passively stabilized. The instability was estimated as 154 mrad rms in 2.5 h.

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Generation, shaping, and characterization of intense femtosecond pulses tunable from 3 to 20 μm

Cited by 300 publications

References 40 publications

Solvent‐Dependent Photoacidity State of Pyranine Monitored by Transient Mid‐Infrared Spectroscopy

Solvent‐Dependent Photoacidity State of Pyranine Monitored by Transient Mid‐Infrared Spectroscopy

Ultrafast phosphate hydration dynamics in bulk H2O

Generation of Phase-Stable Sub-Cycle Mid-Infrared Pulses from Filamentation in Nitrogen

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