The transient signals derived from femtosecond pump-probe experiments are analyzed in terms of the coherent evolution of the energy levels perturbed by the excitation pulse. The model system is treated as the sum of independent two-level subsystems that evolve adiabatically or are permanently excited, depending on the detuning from the central wavelength of the excitation laser. This approach will allow us to explain numerically and analytically the convergence between the coherent and incoherent (rate equations) treatments for complex multi-level systems. It will be also shown that the parameter that determines the validity of the incoherent treatment is the distribution of states outside and inside the laser bandwidth, rather than the density of states as it is commonly accepted.
The standard model of femtosecond filamentation is based on phenomenological assumptions which suggest that the ionization-induced carriers can be treated as free according to the Drude model, while the nonlinear response of the bound carriers follows the all-optical Kerr effect. Here, we demonstrate that the additional plasma generated at a multiphoton resonance dominates the saturation of the nonlinear refractive index. Since resonances are not captured by the standard model, we propose a modification of the latter in which ionization enhancements can be accounted for by an ionization rate o…
Ionization-free femtosecond UV pulse filamentation resulting from non-perturbative Kerr effect saturation due to transient photoexcitation of molecules
P.N. Lebedev Physical Institute of the Russian Academy of Sciences（俄罗斯科学院列别杰夫物理研究所）
Femtosecond high-order harmonic transient absorption spectroscopy is used to resolve the complete |j,m> quantum state distribution of Xe+ produced by optical strong-field ionization of Xe atoms at 800nm. Probing at the Xe N_4/5 edge yields a population distribution rho_j,|m| of rho_3/2,1/2 : rho_1/2,1/2 : rho_3/2,3/2 = 75 +- 6 : 12 +- 3 : 13 +- 6 %. The result is compared to a tunnel ionization calculation with the inclusion of spin-orbit coupling, revealing nonadiabatic ionization behavior. The sub-50-fs time resolution paves the way for table-top extreme ultraviolet absorption probing of ult…
We propose and demonstrate the method of population transfer by piecewise adiabatic passage between two quantum states. Coherent excitation of a two-level system with a train of ultrashort laser pulses is shown to reproduce the effect of an adiabatic passage, conventionally achieved with a single frequency-chirped pulse. By properly adjusting the amplitudes and phases of the pulses in the excitation pulse train, we achieve complete and robust population transfer to the target state. The effect is demonstrated experimentally by observing piecewise excitation of Rubidium atoms from 5s_1/2 to 5p_…
Photoassociation of ultracold rubidium atoms with femtosecond laser pulses is studied theoretically. The spectrum of the pulses is cut off in order to suppress pulse amplitude at and close to the atomic resonance frequency. This leads to long tails of the laser pulse as a function of time giving rise to coherent transients in the photoassociation dynamics. They are studied as a function of cutoff position and chirp of the pulse. Molecule formation in the electronically excited state is attributed to off-resonant excitation in the strong-field regime.
We present and implement a new scheme for independent control of both the final and the transient population utilizing the symmetry properties of the system. By proper pulse shaping, utilizing the invariance of the two-photon absorption to specific phase transformations of the pulse, different time evolutions of the transient population are photo-induced for a given (fixed) final state population. The model system is the Na atom. The work is conducted in the weak-field regime for which the transient two-photon excitation is described by second-order perturbation theory. One most attractive cas…
We experimentally investigate various processes present in the photoassociative interaction of an ultracold atomic sample with shaped femtosecond laser pulses. We demonstrate the photoassociation of pairs of rubidium atoms into electronically excited, bound molecular states using spectrally cut femtosecond laser pulses tuned below the rubidium D1 or D2 asymptote. Time-resolved pump-probe spectra reveal coherent oscillations of the molecular formation rate, which are due to coherent transient dynamics in the electronic excitation. The oscillation frequency corresponds to the detun-ing of the sp…
We simulate the transient absorption of attosecond pulses of infrared-laser-dressed atoms by considering a three-level system with the adiabatic approximation. The delay-dependent interference features are investigated from the perspective of the coherent interaction processes between the attosecond pulse and the quasi-harmonics. We find that many features of the interference fringes in the absorption spectra of the attosecond pulse can be attributed to the coherence phase difference. However, the modulation signals of laser-induced sidebands of the dark state is found related to the populatio…
We present the principle and experimental demonstration of Time Resolved Quantum State Holography. The quantum state of an excited state interacting with an ultrashort chirped laser pulse is measured during this interaction. This has been obtained by manipulating coherent transients created by the interaction of femtosecond shaped pulses and rubidium atoms.
This work investigates the utility of femtosecond pulse shaping in increasing the efficiency of Raman excitation of molecules in the strong-field interaction regime. We study experimentally and theoretically the effect of pulse shaping on the strength of non-resonant coherent anti-Stokes Raman scattering in iodine vapor at laser intensities exceeding $10^{13}$ W/cm$^2$. We show that unlike the perturbative case, shaping strong non-resonant laser pulses can increase the signal strength beyond that observed with the transform-limited excitation. Both adiabatic and non-adiabatic schemes of excita…
We apply attosecond transient absorption spectroscopy (ATAS) to explore the effects of a nonzero permanent dipole on electron dynamics at the subfemtosecond scale, exemplified in the polar LiF molecule. In contrast with nonpolar systems, a familiar feature of the ATA spectra--the light-induced structures--are observed adjacent to a bright state. Moreover, a previously unobserved ladder structure is identified. The new observations are analyzed in the context of a model based on fixed-nuclei adiabatic states, supported by full numerical simulations. Analytic calculations originating in the adia…
We present calculation of photoexcitation and high-harmonic generation in bulk diamond induced by intense near-infrared laser pulse of photon energy 1.55 eV, time duration of 15 fs and peak field strength $F=$ 0.4 V/Å. Depending on the laser polarization direction, the pulsed irradiation creates electron-hole pairs and transient density fluctuations in a localized region of the crystal momentum space. As a consequence energetic inter- and intra-band harmonics are generated with alternating phase during each half-cycle of the driving pulse. The corresponding inter- and intra-band currents are i…
This paper gives an account of our progress towards performing femtosecond time-resolved photoelectron diffraction on gas-phase molecules in a pump-probe setup combining optical lasers and an X-ray Free-Electron Laser. We present results of two experiments aimed at measuring photoelectron angular distributions of laser-aligned 1-ethynyl-4-fluorobenzene (C8H5F) and dissociating, laseraligned 1,4-dibromobenzene (C6H4Br2) molecules and discuss them in the larger context of photoelectron diffraction on gas-phase molecules. We also show how the strong nanosecond laser pulse used for adiabatically l…
A strong phase modulated coupling field leads to an amplitude modulation of a probe field in an electromagnetically induced transparency process. Time vs. detuning plots for different modulation frequencies reveals a transition between an adiabatic regime where a series of smooth pulses are created with a global phase dependent upon the detuning, and a non-adiabatic regime where a strong transient oscillating response is added to these pulses. In the extreme non-adiabatic regime, where the modulation frequency is higher than the transient decay time, a coherent interference pattern is revealed…
Diffraction-before-destruction imaging with single ultrashort X-ray pulses has the potential to visualise non-equilibrium processes, such as chemical reactions, at the nanoscale with sub-femtosecond resolution in the native environment without the need of crystallization. Here, a nanospecimen partially diffracts a single X-ray flash before sample damage occurs. The structural information of the sample can be reconstructed from the coherent X-ray interference image. State-of-art spatial resolution of such snapshots from individual heavy element nanoparticles is limited to a few nanometers. Furt…
Femtosecond high-order harmonic transient absorption spectroscopy is used to observe electromagnetically induced transparency-like behavior as well as induced absorption in the extreme ultraviolet by laser dressing of the He 2s2p (1Po) and 2p2 (1Se) double excitation states with an intense 800 nm field. Probing in the vicinity of the 1s2 \to 2s2p transition at 60.15 eV reveals the formation of an Autler-Townes doublet due to coherent coupling of the double excitation states. Qualitative agreement with the experimental spectra is obtained only when optical field ionization of both double excita…
We investigate the dynamics of molecular photoexcitation by unchirped femtosecond laser pulses using RbCs as a model system. This study is motivated by a goal of optimizing a two-color scheme of transferring vibrationally-excited ultracold molecules to their absolute ground state. In this scheme the molecules are initially produced by photoassociation or magnetoassociation in bound vibrational levels close to the first dissociation threshold. We analyze here the first step of the two-color path as a function of pulse intensity from the low-field to the high-field regime. We use two different a…
The chirped-pulse interaction in the adiabatic coupling regime induces cyclic permutations of the energy states of a three-level system in the $V$-type configuration, which process is known as the three-level chirped rapid adiabatic passage. Here we show that a spectral hole in a chirped pulse can turn on and off one of the two adiabatic crossing points of this process, reducing the system to an effective two-level system. The given hybrid adiabatic-nonadiabatic transition results in selective excitation of the three-level system, controlled by the laser intensity and spectral position of the …
