Femtosecond Pump Pulses Research Articles

Generation of Second-Harmonics Near Ultraviolet Wavelengths From Femtosecond Pump Pulses

Second-harmonic generation (SHG) near ultraviolet wavelengths is experimentally demonstrated by coupling femtosecond pump pulses into the normal dispersion region far away from the zero-dispersion wavelength of the fundamental mode in a silica photonic crystal fiber (PCF) fabricated in our laboratory. When the pump pulses with average input power $P_{\mathrm {av}}$ of 500 mW and center wavelength $\lambda _{\mathrm {p}}$ of 820 nm are used, the maximum conversion efficiency $\eta _{\mathrm {SH}} ^{^{^{}}}$ of the second harmonics centered at 410 nm can be up to $1.6\times 10^{-6}$ , corresponding to the output power $P_{\mathrm {SH}}$ of 520 nW. By measuring $P_{\mathrm {SH}}$ at different PCF lengths and studying the temporal dependence of $P_{\mathrm {SH}}$ , it is confirmed that the physical mechanism of SHG is dominated by surface nonlinearity polarization, which is resulted from the local inhomogeneities in the silica core region and at the core-air-silica cladding interface of PCF. Finally, a theoretical model is established to analyze the nonlinear optical process.

Mid-infrared supercontinuum generation in silica photonic crystal fibers.

A mid-infrared supercontinuum (SC) light source, which has important applications in many fields, has been extensively investigated in soft glass fibers. However, the poor instinct properties of soft glass fibers and the development of ultrashort pulse lasers left an opportunity for mid-infrared SC generation in silica fiber. Until now, silica fiber has been the commonly used medium for SC generation due to its outstanding properties. In this paper, mid-infrared SC generation in short silica photonic crystal fibers (PCFs) is investigated theoretically and systematically. In the case of a 1550�nm pump, the soliton self-frequency shift effect is utilized to extend the long wavelength edge of SC. Adopting a fiber that has a zero dispersion wavelength away from the pump pulse is a benefit for the suppression of blue spectral component and energy distribution in the long wavelength band. In the case of a 1950�nm pump, the generation of a red-shifted dispersive wave is an efficient way to extend the long wavelength edge of SC. Additionally, the coherence for femtosecond pulse pumping is discussed in this paper. Finally, the long wavelength edge of SC is beyond 3000�nm when a 1950�nm femtosecond pump pulse propagates in a PCF with negative dispersive slope around the pump pulse.

High-energy multicolor femtosecond pulses in the deep-ultraviolet generated through four-wave mixing induced by three-color pulses

Multicolor deep-ultraviolet femtosecond pulses are generated in a spectral range of 220–300 nm with pulse energies exceeding 1 μJ. Pulses with shorter wavelengths are also generated with the shortest wavelength of 185 nm. These pulses are generated through cascaded four-wave mixing induced in hydrogen gas by use of three-color femtosecond pump pulses at 1200, 800, and 267 nm. The third pulse dramatically enhances the intensities of the multicolor deep-ultraviolet pulses. The cross-phase modulation induced by the two intense near-infrared pulses broadens the spectral width of each multicolor emission, resulting in a spectral width supporting a transform-limited duration shorter than 10 fs.

Communication: XUV transient absorption spectroscopy of iodomethane and iodobenzene photodissociation.

Time-resolved extreme ultraviolet (XUV) transient absorption spectroscopy of iodomethane and iodobenzene photodissociation at the iodine pre-N4,5 edge is presented, using femtosecond UV pump pulses and XUV probe pulses from high harmonic generation. For both molecules the molecular core-to-valence absorption lines fade immediately, within the pump-probe time-resolution. Absorption lines converging to the atomic iodine product emerge promptly in CH3I but are time-delayed in C6H5I. We attribute this delay to the initial π → σ(*) excitation in iodobenzene, which is distant from the iodine reporter atom. We measure a continuous shift in energy of the emerging atomic absorption lines in CH3I, attributed to relaxation of the excited valence shell. An independent particle model is used to rationalize the observed experimental findings.

Controlling nanoscale acoustic strains in silicon using chirped femtosecond laser pulses

The influence of femtosecond laser pulse chirp on laser-generated longitudinal acoustic strains in Si (100) monocrystal substrates is studied. Degenerate femtosecond pump-probe transient reflectivity measurements are performed using a layered structure of thin Ti transducer film on an Si substrate. Experimental results show that acoustic strains, manifested as strong Brillouin oscillations, are more effectively induced when negatively chirped femtosecond laser pulses pump the transducer. These results are theoretically supported by a modified thermo-mechanical model based on the combination of a revised two-temperature model and elasticity theory that takes into account the instantaneous frequency of the chirped femtosecond laser pump pulses.

Spectrally-isolated violet to blue wavelength generation by cascaded degenerate four-wave mixing in a photonic crystal fiber.

Generation of spectrally-isolated wavelengths in the violet to blue region based on cascaded degenerate four-wave mixing (FWM) is experimentally demonstrated for the first time in a tailor-made photonic crystal fiber, which has two adjacent zero dispersion wavelengths (ZDWs) at 696 and 852 nm in the fundamental mode. The influences of the wavelength λp and the input average power Pav of the femtosecond pump pulses on the phase-matched frequency conversion process are studied. When femtosecond pump pulses at λp of 880, 870, and 860 nm and Pav of 500 mW are coupled into the normal dispersion region close to the second ZDW, the first anti-Stokes waves generated near the first ZDW act as a secondary pump for the next FWM process. The conversion efficiency ηas2 of the second anti-Stokes waves, which are generated at the violet to blue wavelengths of 430, 456, and 472 nm, are 4.8, 6.48, and 9.66%, for λp equalling 880, 870, and 860 nm, respectively.

Ultrafast transient absorption revisited: Phase-flips, spectral fingers, and other dynamical features.

We rebuild the theory of ultrafast transient-absorption/transmission spectroscopy starting from the optical response of an individual molecule to incident femtosecond pump and probe pulses. The resulting description makes use of pulse propagators and free molecular evolution operators to arrive at compact expressions for the several contributions to a transient-absorption signal. In this alternative description, which is physically equivalent to the conventional response-function formalism, these signal contributions are conveniently expressed as quantum mechanical overlaps between nuclear wave packets that have undergone different sequences of pulse-driven optical transitions and time-evolution on different electronic potential-energy surfaces. Using this setup in application to a simple, multimode model of the light-harvesting chromophores of PC577, we develop wave-packet pictures of certain generic features of ultrafast transient-absorption signals related to the probed-frequency dependence of vibrational quantum beats. These include a Stokes-shifting node at the time-evolving peak emission frequency, antiphasing between vibrational oscillations on opposite sides (i.e., to the red or blue) of this node, and spectral fingering due to vibrational overtones and combinations. Our calculations make a vibrationally abrupt approximation for the incident pump and probe pulses, but properly account for temporal pulse overlap and signal turn-on, rather than neglecting pulse overlap or assuming delta-function excitations, as are sometimes done.

A tunable femtosecond stimulated Raman scattering system based on spectrally narrowed second harmonic generation

In this work we present a femtosecond stimulated Raman scattering system. The setup is based on a commercial femtosecond laser system supplemented by a pair of travelling-wave optical parametric amplifiers. One of the parametric amplifiers is used to generate the femtosecond actinic pump pulses, whereas the output of the other (high-power) parametric amplifier undergoes a combination of spectrally narrowed second harmonic generation in a long non-linear crystal and subsequent spectral filtering for the generation of narrowband Raman pump pulses. Chirped white light supercontinuum is used as the Raman probe. The setup offers tunability of the Raman pump pulses in the 400–800 nm range, and spectral and temporal resolutions of ca. 6 cm–1 and ca. 70 fs, respectively. We present the basic technical and optical aspects of the system along with data acquisition and signal retrieval techniques. We characterize the system by exploring the time-resolved vibrational dynamics of the S2(11Bu+) and S1(21Ag–) excited states of β-carotene.

Non-linear increase and saturation of third-harmonic yield from supported silver nanostructures excited by IR femtosecond laser pulses

A second-power yield of resonantly enhanced third harmonic and three-photon luminescence of 744 nm femtosecond laser pump pulses, weakly focused onto a layer of silver nanorolls on a silica substrate, was spectrally detected in the fluence range of 4–20 mJ cm−2, saturating at higher fluences. The third-harmonic yield and its saturation were explored in terms of ultrafast carrier dynamics, based on direct three-photon or cascade one- and two-photon transitions balanced by Auger recombination (and the final band-filling effect) which limited the radiative recombination output in the form of the third harmonic and three-photon luminescence.

Probing nonadiabatic molecular alignment by spectral modulation.

We investigated molecular alignment wakes of femtosecond laser pulses. Evolution of nonadiabatic molecular alignment in nitrogen gas has been measured via its nonlinear interaction effects with a variably delayed probe pulse. The induced rotational wave packet was mapped as a function of the angular difference between polarization directions of femtosecond pump and probe pulses as well as their relative delay and the plot of the variations of the rotational wave packet, i.e. "quantum carpet", was found to be in good agreement with the calculated angular and temporal dependencies of molecular alignment parameter.

Four-Wave Optical Parametric Amplification in a Raman-Active Gas

Four-wave optical parametric amplification (FWOPA) in a Raman-active medium is experimentally investigated by use of an air-filled hollow fiber. A femtosecond pump pulse shorter than the period of molecular motion excites the coherent molecular motion of the Raman-active molecules during the parametric amplification of a signal pulse. The excited coherent motion modulates the frequency of the signal pulse during the parametric amplification, and shifts it to lower frequencies. The magnitude of the frequency redshift depends on the pump intensity, resulting in intensity-dependent spectral characteristics that are different from those in the FWOPA induced in a noble-gas-filled hollow fiber.

A scenario for magnonic spin-wave traps.

Spatially resolved measurements of the magnetization dynamics on a thin CoFeB film induced by an intense laser pump-pulse reveal that the frequencies of resulting spin-wave modes depend strongly on the distance to the pump center. This can be attributed to a laser generated temperature profile. We determine a shift of 0.5 GHz in the spin-wave frequency due to the spatial thermal profile induced by the femtosecond pump pulse that persists for up to one nanosecond. Similar experiments are presented for a magnonic crystal composed of a CoFeB-film based antidot lattice with a Damon Eshbach mode at the Brillouin zone boundary and its consequences are discussed.

Kerr nonlinear switching in a hybrid silica-silicon microspherical resonator.

A hybrid silicon-core, silica-clad microspherical resonator has been fabricated from the semiconductor core fiber platform. Linear and nonlinear characterization of the resonator properties have shown it to exhibit advantageous properties associated with both materials, with the low loss cladding supporting high quality (Q) factor whispering gallery modes which can be tuned through the nonlinear response of the crystalline core. By exploiting the large wavelength shift associated with the Kerr nonlinearity, we have demonstrated all-optical modulation of a weak probe on the timescale of the femtosecond pump pulse. This novel geometry offers a route to ultra-low loss, high-Q silica-based resonators with enhanced functionality.

Vibrational energy flow in photoactive yellow protein revealed by infrared pump-visible probe spectroscopy.

Vibrational energy flow in the electronic ground state of photoactive yellow protein (PYP) is studied by ultrafast infrared (IR) pump-visible probe spectroscopy. Vibrational modes of the chromophore and the surrounding protein are excited with a femtosecond IR pump pulse, and the subsequent vibrational dynamics in the chromophore are selectively probed with a visible probe pulse through changes in the absorption spectrum of the chromophore. We thus obtain the vibrational energy flow with four characteristic time constants. The vibrational excitation with an IR pulse at 1340, 1420, 1500, or 1670 cm(-1) results in ultrafast intramolecular vibrational redistribution (IVR) with a time constant of 0.2 ps. The vibrational modes excited through the IVR process relax to the initial ground state with a time constant of 6-8 ps in parallel with vibrational cooling with a time constant of 14 ps. In addition, upon excitation with an IR pulse at 1670 cm(-1), we observe the energy flow from the protein backbone to the chromophore that occurs with a time constant of 4.2 ps.

Femtosecond lasing from a fluorescent protein in a one dimensional random cavity.

We present evidence of random lasing from the fluorescent protein DsRed2 embedded in a random one-dimensional cavity. Lasing is achieved when a purified protein solution, placed inside a layered random medium, is optically excited with a femtosecond pump pulse in the direction perpendicular to the plane of random layers. We demonstrate that pumping with ultrashort pulses resulted in a lasing threshold two orders of magnitude lower than that found for nanosecond excitation.

Separating nuclear spin isomers using a pump–dump laser scheme

The concept of nuclear spin isomers was already introduced in the early days of quantum mechanics. Despite its importance, not much work has been done to separate them experimentally by pushing the ratio away from its equilibrium value. We propose to use ultrashort laser pulses in a pump–dump-like experiment to enhance the ratio between different nuclear spin isomers. Exemplary wave packet simulations with optimized femtosecond pump and dump laser pulses are shown on a quinodimethane derivative to illustrate that the ratio between two different groups of nuclear spin isomers is enhanced.

Vacuum space charge effects in sub-picosecond soft X-ray photoemission on a molecular adsorbate layer.

Vacuum space charge induced kinetic energy shifts of O 1s and Ru 3d core levels in femtosecond soft X-ray photoemission spectra (PES) have been studied at a free electron laser (FEL) for an oxygen layer on Ru(0001). We fully reproduced the measurements by simulating the in-vacuum expansion of the photoelectrons and demonstrate the space charge contribution of the high-order harmonics in the FEL beam. Employing the same analysis for 400 nm pump-X-ray probe PES, we can disentangle the delay dependent Ru 3d energy shifts into effects induced by space charge and by lattice heating from the femtosecond pump pulse.

Modelling the effect of nuclear motion on the attosecond time-resolved photoelectron spectra of ethylene

Using time-dependent density functional theory we examine the energy, angular and time-resolved photoelectron spectra (TRPES) of ethylene in a pump–probe setup. To simulate TRPES we expose ethylene to an ultraviolet femtosecond pump pulse, followed by a time delayed extreme ultraviolet probe pulse. Studying the photoemission spectra as a function of this delay provides us direct access to the dynamic evolution of the molecule’s electronic levels. Further, by including the nuclei’s motion, we provide direct chemical insight into the chemical reactivity of ethylene. These results show how angular and energy resolved TRPES could be used to directly probe electron and nucleus dynamics in molecules.

Temporal and spectral correlations in bulk continua and improved use in transient spectroscopy

Newly generated frequencies during bulk continuum generation with femtosecond pump pulses do not fluctuate statistically and show strong correlations in spectrum and time. When a femtosecond continuum is used as probe light for transient spectroscopic measurements, these correlations result in a seemingly low noise level but large-scale pseudo-structures that obscure the interpretation. We investigate the correlations for continua generated in YAG and calcium fluoride plates and incorporate the results into the design of our pump–probe setup. The high degree of correlation to the next pulse is utilized through chopping of the pump and referencing between successive laser shots. To suppress the adverse effect of the high degree of correlation to other wavelengths, we extend the detection by multichannel referencing with a second camera. The combination of both referencing schemes renders a precise spectral calibration unnecessary and increases the sensitivity of our spectrometer by a factor of 5 down to 20 μOD. This is already very close to the shot noise limit. To demonstrate the improvements, we present and discuss measurements on two different molecular solutions.

Formation of coherent rotational wavepackets in small molecule-helium clusters using impulsive alignment.

We show that rotational line spectra of molecular clusters with near zero permanent dipole moments can be observed using impulsive alignment. Aligned rotational wavepackets were generated by non-resonant interaction with intense femtosecond laser pump pulses and then probed using Coulomb explosion by a second, time-delayed femtosecond laser pulse. By means of a Fourier transform a rich spectrum of rotational eigenstates was derived. For the smallest cluster, C(2)H(2)-He, we were able to establish essentially all rotational eigenstates up to the dissociation threshold on the basis of theoretical level predictions. The C(2)H(2)-He complex is found to exhibit distinct features of large amplitude motion and very early onset of free internal rotor energy level structure.