Control of de-excitation to selected vibrational levels in the ground state of NaH molecule using two broadband ultrashort pulses

We show that the de-excitation to different vibrational levels of the ground state in NaH molecule can be controlled by using two delayed ultrashort pulses (4 fs Gaussian). A vibrational wave packet generated on the excited A¹Σ⁺ state by the first pulse is de-excited back to the ground state by a second pulse after a time delay. The cross-section for de-excitation of the wave packet to different vibrational levels of the ground electronic state can be controlled by controlling the delay time between the two pulses as well as by choosing a pulse duration much shorter than the vibrational period of the molecule, such that the de-excited wave packet remains localized in the Franck–Condon region of a particular vibrational level of the ground state. Hence, the de-excitation to a particular vibrational level can be enhanced by suppressing that in others. In spite of the large bandwidth of the pulse which includes nine vibrational levels of the upper state and five vibrational levels of the ground state, one can selectively de-excite the molecule to any one or two vibrational levels of the ground state by carefully choosing the delay time between the pulses and the pulse duration. We are designing the wave packet in the ground state by two short pulses and selectively distributing the population in one or two levels at various values of the delay time. In light molecules having small vibrational period, this selectivity in de-excitation to one or two vibrational levels in the ground state can be achieved only by using ultrashort (4 fs) pulses in the presence of which the localization of the wave packet in the Franck–Condon region of the vibrational levels are particularly possible. It has been shown that the de-excitation cross-section to a particular vibrational level oscillates with delay between the pulses which can be realized as a time-dependent quantum gate.     

Quantum computation with vibrationally excited molecules

A new physical implementation for quantum computation is proposed. The vibrational modes of molecules are used to encode qubit systems. Global quantum logic gates are realized using shaped femtosecond laser pulses which are calculated applying optimal control theory. The scaling of the system is favorable; sources for decoherence can be eliminated. A complete set of one- and two-quantum gates is presented for a specific molecule. Detailed analysis regarding experimental realization shows that the structural resolution of today's pulse shapers is easily sufficient for pulse formation.     

Quantum interferometry by using delayed phase-locked ultrashort pulses: implementation of quantum gate operation in molecules

It will be shown that by using two phase-locked delayed ultrashort pulses of different durations one can selectively populate odd or even vibrational levels of an excited state of a molecule. One can control the enhancement or damping in a selective vibrational level by controlling the laser parameters e.g. delay, phase difference, temporal width and carrier frequency of two ultradhort pulses. Conversely by reading the population distribution In vibrational levels of an excited state of a molecule one can study the amplitude and the phase of the wavepacket generated by the interference of two wavepackets excited by two ultrashort pulses i.e. by quantum interferometry. It will be examined whether the information stored in a molecule by quantum computation can be retrieved efficiently by using quantum interferometry.     

Optimal laser pulse design for transferring the coherent nuclear wave packet of H+2

Within the Franck–Condon approximation, the single ionisation of H₂ leaves H⁺₂ in a coherent superposition of 19 nuclear vibrational states. We numerically design an optimal laser pulse train to transfer such a coherent nuclear wave packet to the ground vibrational state of H⁺₂. Frequency analysis of the designed optimal pulse reveals that the transfer principle is mainly an anti-Stokes transition, i.e. the H⁺₂ in 1sσ_g with excited nuclear vibrational states is first pumped to 2pσ_g state by the pulse at an appropriate time, and then dumped back to 1sσ_g with lower excited or ground vibrational states. The simulation results show that the population of the ground state after the transfer is more than 91%. To the best of our knowledge, this is the highest transition probability when the driving laser field is dozens of femtoseconds.     

Pulse shaping and its characterization of mid-infrared femtosecond pulses: Toward coherent control of molecules in the ground electronic states

We have examined a technique of complex shaping of mid-infrared femtosecond laser pulses towards accurate and precise control of rovibrational wave packets of molecules in the ground electronic state. A Germanium acousto-optics modulator was used as a device for the pulse shaping. In order to characterize the shaped pulses precisely, sum-frequency cross-correlation frequency-resolved optical gating was introduced for the analysis of both amplitude and phase of the electric fields. The mid-infrared pulses were shaped and characterized with a frequency resolution better than 4.5 cm⁻¹. Such a resolution is supposed to be sufficient for the realization of quantum gate operations with high fidelity, which is one of the most challenging applications of rovibrational wave packet manipulation of molecules. In order to demonstrate the precision of our method of shaping and its characterization, we have generated shaped pulses that will realize Hadamard and NOT quantum gates with rovibrational states of a CO molecule.     

Photoassociation of NaRb with an asymmetric laser pulse

We investigate the photoassociation dynamics of cold NaRb molecule controlled by an asymmetric laser pulse called slowly-turned-on and rapidly-turned-off (STRT) laser pulse. This new shaped laser pulse has a remarkable merit, compared with the typical Gauss-type pulses, so that we can efficiently associate molecules with the state expected instead of going back to the continuum state. Using the three-state model, we solve the quantum mechanical equation with the “split operator-Fourier transform” method under the rotating-wave approximation (RWA) in propagation of the wave packet. By the projection of the obtained wave function onto each vibrational state, we can get the vibrational population of the ground electronic state. The results reveal that, with the STRT laser pulse, an efficient photoassociation process can be achieved and the vibrational distribution in the ground state can be controlled by the laser parameters.     

Stacking chirped pulse optical parametric amplification

Stacking chirped pulse optical parametric amplification based on a home-built Yb³⁺-doped mode-locked fiber laser and an all-fiber pulse stacker has been demonstrated. Energic 11 mJ shaped pulses with pulse duration of 2.3 ns and a net total gain of higher than 1.1 × 10⁷ at fluctuation less than 2% rms are achieved by optical parametric amplification pumped by a Q-switched Nd:YAG frequency-doubled laser, which provides a simple and efficient amplification scheme for temporally shaped pulses by stacking chirped pulse.     

Radiative Transitions and Temperature Time Dependences in Pulse Excited Microwave Discharges – (N2, Ar + N2)

Quantitative spectral and microwave measurements of vibrational temperatures and electron densities were performed for 2400 MHz non-isothermic pulse excited discharges in flowing nitrogen and argon at pressures (60–2700) Pa. A detailed analysis of the N₂ vibrational states population for the N₂ C³Π_u, X¹Σ_g⁺ electronic states has been carried out. The basic difficulties encountered when comparing the spectroscopically determined values of vibrational temperatures with corresponding quantities of the ground electronics state are mentioned and the time resolved dependences of the translational gas temperature in N₂ during the microwave pulse is evaluated. The steady state in the nitrogen pulse excited microwave plasma is reached within 3 · 10^?4 s, but generally, this time depends on the gas pressure in the discharge tube. In the Ar + N₂ mixtures the excitation conditions are complicated by the metastable argon atoms (3P_2,0) creating the nonequilibrium populations of electronic, vibrational and rotational N₂ states.     

Rotational structure of the 000, 010, 100, 020, and 001 vibrational states of the D216O molecule: Spectroscopic assignment of rotational levels up to J, Ka = 30 and analysis of published data

The complete spectroscopic assignment of calculated Partridge-Schwenke rotational energy levels up to J, K _a = 30 is presented for the 000, 010, 100, 020, and 001 vibrational states of the D₂ ¹⁶O molecule. The nonpolynomial model of an effective rotational Hamiltonian is used to perform the assignment and to analyze the experimental energy levels available in the literature for these states. The results obtained are compared with the data calculated by other authors. The results of this study can be useful in searching for and identifying new, highly excited rotational levels of D₂ ¹⁶O, as well as in creating the databases of parameters of rovibrational transitions of the water molecule.     

Coherent excitation of molecular vibrational modes by high-power ultrashort infrared laser pulses

Coherent dynamics of multiphoton excitation of molecular vibrational modes by subpicosecond IR laser pulses differs greatly from that of picosecond pulse excitation. The resonance response of a molecule is primarily determined by the power broadening rather than the laser carrier frequency. Selective excitation of high vibrational levels is possible with the use of subpicosecond pulses.     

Vibrational excitation of diatomic molecular ions in strong field ionization of diatomic molecules

A model based on the strong-field and Born-Oppenheimer approximations qualitatively describes the distribution over vibrational states formed in a diatomic molecular ion following ionization of the neutral molecule by intense laser pulses. Good agreement is found with a recent experiment [X. Urbain et al., Phys. Rev. Lett. 92, 163004 (2004)]. In particular, the observed deviation from a Franck-Condon-like distribution is reproduced. Additionally, we demonstrate control of the vibrational distribution by a variation of the peak intensity or a change of frequency of the laser pulse.     

Tunable,sub-nanosecond KrF-Raman laser in the ultraviolet

A 0.5 cm^–1 bandwidth injection-locked KrF laser pumps a rare-gas Brillouin cell to produce a reflected pulse with a leading edge risetime of 1 ns, tunable from 248.1 to 248.7 nm. Consistent with Lamb theory of laser amplifiers, subsequent excimer amplification of this pulse produces an intense 500 ps spike on the pulse leading edge. Stimulated Raman scattering then separates the spike from the parent pulse, yielding a tunable short pulse at the first Stokes (S ₁) wavelength. Varying the Raman cell length results in a variable Raman threshold and an adjustable short pulse duration: 250 ps pulses at energies of 3–4 mJ at 268 nm with a 50 cm methane cell and 350 ps, 5 mJ pulses from a 100 cm cell are measured with a streak camera. First pass Raman conversion of the spike toS ₁ followed by second pass backward Raman amplification, where the parent 248 nm pulse serves as the pump beam for the reflectedS ₁ pulse, yields simultaneousS ₁ pulses of 20–25 mJ in the 800 ps range andS ₂ pulses of 550 ps at 5–6 mJ near 290 nm. This laser will avoid collision effects during laser excitation and enable quantitative, single pulse imaging of OH radicals in turbulent combustion because of its high pulse energy.     

The influence of femtosecond laser parameters on the wavepacket and population of the diabatic excited states of NaLi

Using the three-state model and time-dependent wavepacket method, the influence of the parameters of the intense femtosecond laser field on the wavepacket dynamic process of the double-minimum potential state 5¹Σ⁺ and the population of the ground and diabatic electronic states of NaLi are investigated. The calculations show that different femtosecond laser parameters result in different influences on the evolution of the wavepacket and the population of NaLi. With increasing laser intensity and wavelength the diabatic coupling strength between A and B states first strengthens and then weakens. The population interchanges between A and B states when the laser pulse disappears. The above results provide the suggestions and useful information for one to achieve quantum manipulation of the molecule in an experiment.     

Femtosecond dynamics of primary processes in visual pigment rhodopsin

The dynamics of the coherent photoisomerization of the 11-cis-retinal in bovine rhodopsin is studied by femtosecond time-resolved laser absorption spectroscopy with a resolution of 30 fs. Rhodopsin is excited with 500-, 535-, and 560-nm femtosecond pulses to produce different initial Franck-Condon states with different vibrational energies of the molecule in its electronically excited state. The time evolution of the photoinduced differential absorption spectra of rhodopsin is measured upon excitation with a femtosecond pulse in a spectral range from 400 to 720 nm. Oscillations in the time-resolved absorption of the rhodopsin photoproducts, such as photorhodopsin with a vibrationally excited all-trans-retinal and in its initial-state rhodopsin with a vibrationally excited 11-cis-retinal, are examined. It is demonstrated that these oscillations reflect the dynamics of coherent vibrational wavepackets. The Fourier transform of these oscillatory components yields frequencies, amplitudes, and initial phases of various vibrational modes involved in the motion the wavepackets in both photoproducts. The main vibrational modes manifest themselves at frequencies of 62 and 160 cm^?1 for photorhodopsin and 44 and 142 cm^?1 for initial-state rhodopsin. It is shown that these vibrational modes are directly involved in the coherent reaction under the study, with their amplitudes in the power spectrum produced by the Fourier transform of the kinetic curves being dependent on the wavelength of rhodopsin excitation.     

Theoretical exploration of asymmetric molecular harmonic emission and attosecond pulse generation in the presence of spatially inhomogeneous plasmon-enhanced field

Asymmetric molecular harmonic generation from HeH²⁺ ion in the presence of the spatially inhomogeneous plasmon-enhanced field has been theoretically investigated by solving the two-dimensional non-Born–Oppenheimer time-dependent Schrödinger equation (both the electron and nuclear motions are considered only along the laser polarisation axis). It shows that (1) for the normal homogeneous field, the harmonic cut-off from the asymmetric molecule is beyond the classical harmonic cut-off energy from the atom (I_p + 3.17 U_p). Further analyses show that the multi-channels ionisation–recombination process is responsible for the harmonic extension. (2) For the spatially inhomogeneous plasmon-enhanced field, the harmonic cut-off can be further enhanced, and an optimal 3.0 dB enhanced field with a 482 eV supercontinuum has been obtained. Quantum time-frequency harmonic analyses have been shown to explain the harmonic characteristics and the harmonic extension process. (3) Initial vibrational state and isotopic effects show that intense harmonics can be generated from higher initial vibrational state and the heavier molecule. Finally, by properly superposing the harmonics, a series of sub-30 as attosecond pulses can be obtained.     

Effects of electron relaxation on multiple harmonic generation from metal surfaces with femtosecond laser pulses

Calculations are presented for the first four (odd and even) harmonics of an 800 nm laser from a gold surface, with pulse widths ranging from 100 down to 14 fs. For peak laser intensities above 1 GW/cm² the harmonics are enhanced because of a partial depletion of the initial electron states. At 10¹¹ W/cm² of peak laser intensity the calculated conversion efficiency for 2nd-harmonic generation is 3 × 10⁻⁹, while for the 5th-harmonic it is 10⁻¹⁰. The generated harmonic pulses are broadened and delayed relative to the laser pulse because of the finite relaxation times of the excited electronic states. The finite electron relaxation times cause also the broadening of the autocorrelations of the laser pulses obtained from surface harmonic generation by two time-delayed identical pulses. Comparison with recent experimental results shows that the response time of an autocorrelator using nonlinear optical processes in a gold surface is shorter than the electron relaxation times. This seems to indicate that for laser pulses shorter than ∼30 fs, the fast nonresonant channel for multiphoton excitation via continuum-continuum transitions in metals becomes important as the resonant channel becomes slow (relative to the laser pulse) and less efficient.     

Absorption of CO2 laser pulses at different wavelengths by ground-state and vibrationally heated SF6

The absorption of CO₂ laser pulses by low pressure SF₆ gas has been investigated over a wide range of energy fluxes. For laser energy fluxes of 0.01–1 J cm^-2 the effective absorption cross section varies between 0.2 and 2 × 10^-18 cm². For each laser line an individual dependence on the energy is found and in some cases minor changes in the absorption behaviour seem to occur around 0.1 J cm^-2. SF₆ excited with an average vibrational energy content of up to 20 photons/molecule does not absorb measurable amounts of 9.4 μm laser light. The influence of various SF₆ and Ar pressures on the temporal shape of the transmitted pulses has been investigated.     

Picosecond laser ablation of thin copper films

The ablation process of thin copper films on fused silica by picosecond laser pulses is investigated. The ablation area is characterized using optical and scanning electron microscopy. The single-shot ablation threshold fluence for 40 ps laser pulses at 1053 nm has been determinated toF _thres = 172 mJ/cm². The ablation rate per pulse is measured as a function of intensity in the range of 5 × 10⁹ to 2 × 10¹¹ W/cm² and changes from 80 to 250 nm with increasing intensity. The experimental ablation rate per pulse is compared to heat-flow calculations based on the two-temperature model for ultrafast laser heating. Possible applications of picosecond laser radiation for microstructuring of different materials are discussed.     

A comparative study of the ionic keV X-ray line emission from plasma produced by the femtosecond,picosecond and nanosecond duration laser pulses

We report here an experimental study of the ionic keV X-ray line emission from magnesium plasma produced by laser pulses of three widely different pulse durations (FWHM) of 45 fs, 25 ps and 3 ns, at a constant laser fluence of ∼1.5 × 10⁴ J cm^− 2. It is observed that the X-ray yield of the resonance lines from the higher ionization states such as H- and He-like ions decreases on decreasing the laser pulse duration, even though the peak laser intensities of 3.5 × 10¹⁷ W cm^− 2 for the 45 fs pulses and 6.2 × 10¹⁴ W cm^− 2 for the 25 ps pulses are much higher than 5 × 10¹² W cm^− 2 for the 3 ns laser pulse. The results were explained in terms of the ionization equilibrium time for different ionization states in the heated plasma. The study can be useful to make optimum choice of the laser pulse duration to produce short pulse intense X-ray line emission from the plasma and to get the knowledge of the degree of ionization in the plasma.     

可调谐的调Q掺Yb3+双包层光纤激光器

利用双包层光纤中的受激布里渊散射和声光调Q器件,对掺Yb³⁺双包层光纤激光器进行了混合调Q的实验研究.在连续泵浦状态下,当入纤泵浦功率为1.24W时,在1080～1119nm的可调谐范围内,在国内首次获得了输出脉冲宽度小于6ns,重复频率1.5 kHz,脉冲能量高于80μJ,峰值功率高于13.3kW稳定调Q光纤激光器的脉冲输出.经计算,实验结果和理论计算值符合得很好.