ABSTRACT
We perform a beat-frequency-resolved analysis for two-dimensional electronic spectroscopy using a high-speed and stable 2D electronic spectrometer and few-cycle visible laser pulses to disentangle the vibrational coherences in an artificial fluorescent protein. We develop a highly stable ultrashort light source that generates 5.3-fs visible pulses with a pulse energy of 4.7 µJ at a repetition rate of 10 kHz using multi-plate pulse compression and laser filamentation in a gas cell. The above-5.3-fs laser pulses together with a high-speed multichannel detector enable us to measure a series of 2D electronic spectra, which are resolved in terms of beat frequency related to vibrational coherence. We successfully extract the discrete vibrational peaks behind the inhomogeneous broadening in the absorption spectra and the vibrational quantum beats of the excited electronic state behind the strong incoherent population background in the typical 2D electronic spectra.
ABSTRACT
We demonstrate the broadband operation of a synchronously pumped optical parametric oscillator (SPOPO) with a spatially dispersed beam and a fan-out type MgO-doped periodically poled LiTaO3 (MgO:PPLT). Spatial dispersion was generated using a glass prism placed in the SPOPO cavity. The poling period was designed to match the spatial dispersion and phase matching in MgO:PPLT, and the spectral dispersion in the cavity was compensated for using a fused silica plate, which had a negative dispersion at a signal wavelength of 1500-1600 nm. We succeeded in generating signal pulses with a pulse length of 81 fs, which was approximately 1/5 of the pump pulse length.
ABSTRACT
An intense white light (WL) continuum from 1600 to 2400 nm is generated in a 20-mm-long YAG irradiated by 1-ps, 1030-nm pulses. Long filamentation formed in the YAG is proven to be responsible for the enhancement of the longer-wavelength spectral part of the WL. The WL is compressed down to 24.6 fs ( 3.9 cycles at 1900 nm) after optical parametric chirped-pulse amplification in a lithium niobate crystal near degeneracy, confirming that its spectral phase is well behaved. The pulse compression experiment reveals that the group delay introduced in the WL generation process is dominated by the dispersion of YAG.
ABSTRACT
Time-resolved terahertz (THz) spectroscopy is applied for a microcrystalline film of methylammonium lead bromide perovskite, CH3NH3PbBr3, to observe the carrier dynamics around the band edge. The ultrafast response of the transmitted THz electric field amplitude after carrier generation is modeled with a biexponential curve with â¼5 and 180 ps time constants, which are ascribed to Auger and electron-hole recombination processes, respectively. From the pump photon energy dependence of the time evolution of the THz electric field amplitude, it is shown that the bound exciton states and free interband excited carrier states show a clearly different temporal response. These measurements support the idea that the bound excitons generated in CH3NH3PbBr3 remain as stable excitons even at room temperature (RT). This is in clear contrast to the cases in CH3NH3PbI3 in which the excitons and band-edge free carriers are interchangeable at RT.
ABSTRACT
We demonstrate an optical parametric oscillator pumped at a repetition rate of 100 kHz by a burst-mode Yb-doped fiber laser. Pulse energies of 1.5 µJ were generated with five 4.8-µJ pump pulses. Pulse-to-pulse fluctuations could be suppressed even when only five pump pulses were used. The measured pulse length was 190 fs, which was considerably shorter than the 350-fs pump pulse length. The burst-mode operation is an easy and powerful way to increase the pulse energies of optical parametric oscillators pumped with femtosecond pulses.
ABSTRACT
We demonstrate plasma-mirror frequency-resolved optical gating (PM-FROG) using a liquid-sheet jet of water and characterize a waveform of a high-repetition laser pulse (1 kHz) in the ultraviolet (UV) region. The measured PM-FROG trace is reconstructed by the least-squares generalized projections algorithm. The retrieved UV spectral phase is consistent with that by self-diffraction FROG. The complex reflection coefficient of a plasma mirror is discussed in terms of the free electron density dependence. The PM-FROG technique is applicable to not only the pulse characterization, but also the investigation of ionization dynamics of a liquid.
ABSTRACT
Valence molecular orbitals play a crucial role in chemical reactions. Here, we reveal that an intense laser field deforms an inner valence orbital (10a') in the ethanol molecule. We measure the recoil-frame photoelectron angular distribution (RFPAD), which corresponds to the orientation dependence of the ionization probability of the orbital, using photoelectron-photoion coincidence momentum imaging with a circularly polarized laser pulse. Ab initio simulations show that the orbital deformation depends strongly on the laser field direction and that the measured RFPAD cannot be reproduced without taking the orbital deformation into account. Our findings suggest that the laser-induced orbital deformation occurs before electron emission on a suboptical cycle time scale.
ABSTRACT
We demonstrate that vacuum ultraviolet (VUV) pulses (λâ¼160 nm) with 20-fs duration can be fully characterized by plasma-mirror frequency-resolved optical gating. Plasma is formed as an ultrafast optical switch on a fused silica surface by irradiation of an intense near-infrared (NIR) femtosecond laser pulse. We measure the spectra of the VUV pulses reflected off plasma as a function of the delay with respect to the NIR pulse and reconstruct it to simultaneously extract a nearly Fourier-transform limited VUV pulse shape and a time-dependent reflectivity of plasma using the least-squares generalized projections algorithm. We show that there is almost no spatial dependence of the VUV pulse shape, whereas the plasma mirror reflectivity strongly depends on the spatial region.
ABSTRACT
We propose and experimentally demonstrate a method for characterizing vacuum ultraviolet (VUV) pulses based on time-resolved reflection spectroscopy of fused silica pumped by an intense laser pulse. Plasma mirror reflection is used as an ultrafast optical switch, which enables us to measure frequency-resolved optical gating (FROG) traces. The VUV temporal waveform can be retrieved from the measured FROG trace using principal component generalized projections algorithm with modification. The temporal profile of the plasma mirror reflectivity is also extracted simultaneously.
ABSTRACT
The two dissociative ionization channels of ethanol (C2H5OH) induced by an intense near-infrared laser pulse (λ ~ 783 nm), C2H5OH â CH2OH(+) + CH3 + e(-) and C2H5OH â C2H5(+) + OH + e(-), are investigated using photoelectron-photoion coincidence method. It is shown that both the electronic ground state and the first electronically excited state of C2H5OH(+) are produced at the moment of photoelectron emission. From the observed correlation between the electronic states of C2H5OH(+) prepared at the moment of photoelectron emission and the kinetic energy release of the fragment ions, it is revealed that C2H5OH(+) prepared in the electronic ground state at the photoelectron emission gains larger internal energy in the end than that prepared in the electronically excited state. The averaged internal energy of C2H5OH(+) just before the dissociation is found to increase when the laser field intensity increases from 9 to 23 TW∕cm(2) and when the laser pulse duration increases from 35 to 800 fs.
Subject(s)
Ethanol/chemistry , Lasers , Electrons , Photochemical ProcessesABSTRACT
We investigate coherent correlation between nonadiabatic rotational excitation and angle-dependent ionization of NO in intense laser fields in the state-resolved manner. When neutral NO molecules are partly ionized in intense laser fields (I(0) > 35 TW/cm(2)), a hole in the rotational wave packet of the remaining neutral NO is created because of the ionization rate depending on the alignment angle of the molecular axis with respect to the laser polarization direction. Rotational state distributions of NO are experimentally observed, and then the characteristic feature that the population at higher J levels is increased by the ionization can be identified. Numerical calculation for solving time-dependent rotational Schrödinger equations including the effect of the ionization is carried out. The numerical results suggest that NO molecules aligned perpendicular to the laser polarization direction are dominantly ionized at the peak intensity of I(0) = 42 TW/cm(2), where the multiphoton ionization is preferred rather than the tunneling ionization.
ABSTRACT
We propose a simple scheme to characterize attosecond extreme ultraviolet (XUV) pulses. A broadband ultraviolet (UV) approximately vacuum ultraviolet (VUV) pump pulse creates a coherent superposition of atomic bound states, from which photoionization takes place by the time-delayed attosecond XUV probe pulse. Information on the spectral phase of the XUV pulse can be extracted from the phase offset of the interference beating in the photoelectron spectra using a standard SPIDER (spectral phase interferometry for direct electric-field reconstruction) algorithm. We further discuss the influence of the chirp and polychromaticity of the pump pulse, and show that they do not spoil the reconstruction process. Since our scheme is applicable for various simple atoms such as H, He, and Cs, etc., and capable of characterizing attosecond XUV pulses with a pulse duration of a few hundred attoseconds or even less, it can be an alternative technique to characterize attosecond XUV pulses. Specific numerical examples are presented for the H atom utilizing the 2p and 3p states.
ABSTRACT
Two-body Coulomb explosion with the C-O bond breaking of methanol induced by intense laser pulses with the duration of Delta t=7 and 21 fs is investigated by the coincidence momentum imaging method. When Delta t=7 fs, the angular distribution of recoil vectors of the fragment ions for the direct C-O bond breaking pathway, CH(3)OH(2+)-->CH(3) (+)+OH(+), exhibits a peak deflected from the laser polarization direction by 30 degrees -45 degrees , and the corresponding angular distribution for the migration pathway, CH(2)OH(2) (+)-->CH(2) (+)+H(2)O(+), in which one hydrogen migrates from the carbon site to the oxygen site prior to the C-O bond breaking, exhibits almost the same profile. When the laser pulse duration is stretched to Delta t=21 fs, the angular distributions for the direct and migration pathways exhibit a broad peak along the laser polarization direction probably due to the dynamical alignment and/or the change in the double ionization mechanism; that is, from the nonsequential double ionization to the sequential double ionization. However, the extent of the anisotropy in the migration pathway is smaller than that in the direct pathway, exhibiting a substantial effect of hydrogen atom migration in the dissociative ionization of methanol interacting with the linearly polarized intense laser field.
ABSTRACT
The relative yield of the C-O bond breaking with respect to the C-C bond breaking in ethanol cation C2H5OH+ is maximized in intense laser fields (10(13)-10(15) Wcm2) by open-loop and closed-loop optimization procedures. In the open-loop optimization, a train of intense laser pulses are synthesized so that the temporal separation between the first and last pulses becomes 800 fs, and the number and width of the pulses within a train are systematically varied. When the duration of 800 fs is filled with laser fields by increasing the number of pulses or by stretching all pulses in a triple pulse train, the relative yield of the C-O bond breaking becomes significantly large. In the closed-loop optimization using a self-learning algorithm, the four dispersion coefficients or the phases of 128 frequency components of an intense laser pulse are adopted as optimized parameters. From these optimization experiments it is revealed that the yield ratio of the C-O bond breaking is maximized as far as the total duration of the intense laser field reaches as long as approximately 1 ps and that the intermittent disappearance of the laser field within a pulse does not affect the relative yields of the bond breaking pathways.
