Quantum beats in stimulated electronic raman scattering of ultrashort laser pulses

A theory of quantum beats in a Stokes signal observed in pump-probe experiments upon excitation of four-level atoms with two close upper lying levels by femtosecond laser pulses is developed. Quantum beats arise in the intensity of the Stokes field due to the interference of two atomic wave packets generated by ultrashort pump and probe pulses. An analytical solution of the non-steady-state Maxwell-Bloch equations is obtained, and the dependence of the Stokes radiation intensity on the delay time between two laser pulses is investigated. The theoretical results describe qualitatively well the observed features of quantum beats.     

Optical ramsey fringes in two-photon spectroscopy

Using two coherent time delayed short pulses, we have demonstrated that one can obtain, in the profile of Doppler-free two-photon resonances, interference fringes with a splitting 1/2T (T: delay time between the two pulses) much smaller than the spectral width 1/τ of each pulse (τ: duration of each pulse). Furthermore, by inducing a 90° phase shift between pairs of coherent time-delayed laser pulses, and subtracting the resulting fluorescence from pairs of coherent pulses with and without the phase shift, we have eliminated the diffraction background and isolated the Ramsey's interference fringes in the profile of Doppler-free two-photon resonances. This technique should lead to a number of important improvements in the presently available methods of ultra-high resolution laser spectroscopy of atoms, molecules, and crystals. Supported in part by the Joint Services Electronics Program.     

钡蒸气的受激喇曼散射及碰撞诱导受激辐射

在宽带XeCl激光泵浦的钡蒸气中,观察到波长分别为472.6nm,582.6nm和648.3nm的碰撞诱导受激辐射以及波长为475nm的受激喇曼散射.碰撞锈导受激辐射脉宽为3ns左右的自终止型短脉冲,其强度随缓冲气体压力的升高而上升.喇曼光脉冲前沿与泵浦光脉冲前沿之间有长20ns的时间延迟,喇曼转换效率随缓冲气体压力的升高而下降     

Multi-Particle Interference in an Electronic Mach–Zehnder Interferometer

The development of dynamic single-electron sources has made it possible to observe and manipulate the quantum properties of individual charge carriers in mesoscopic circuits. Here, we investigate multi-particle effects in an electronic Mach–Zehnder interferometer driven by a series of voltage pulses. To this end, we employ a Floquet scattering formalism to evaluate the interference current and the visibility in the outputs of the interferometer. An injected multi-particle state can be described by its first-order correlation function, which we decompose into a sum of elementary correlation functions that each represent a single particle. Each particle in the pulse contributes independently to the interference current, while the visibility (given by the maximal interference current) exhibits a Fraunhofer-like diffraction pattern caused by the multi-particle interference between different particles in the pulse. For a sequence of multi-particle pulses, the visibility resembles the diffraction pattern from a grid, with the role of the grid and the spacing between the slits being played by the pulses and the time delay between them. Our findings may be observed in future experiments by injecting multi-particle pulses into a Mach–Zehnder interferometer.     

块状介质超连续谱相位的相干特性

 块状介质超连续谱由一系列复杂的非线性过程产生。用两路飞秒泵浦光聚焦到熔石英玻璃上得到两束独立的超连续谱，实验上观察到它们形成的稳定干涉条纹；改变两路泵浦光的时间延迟，得到共线超连续谱形成的频率梳。实验证明，块状介质超连续谱的产生保持了泵浦光的相位锁定关系，泵浦光能量抖动和介质的缺陷都不会对超连续谱的相位带来明显的扰动。     

Dual-polarization and dual-wavelength diode-pumped laser operation from a birefringent Yb3+-doped GdAl3(BO3)4 nonlinear crystal

From two positions of the concave output mirror of the laser cavity, diode-pumped ordinary or extraordinary polarization lasing of an Yb³⁺-doped GdAl₃(BO₃)₄ nonlinear birefringent crystal is obtained. Translating the mirror at an intermediate position, simultaneous ordinary and extraordinary polarization lasing at 1046 (2.5 nm FWHM) and 1040 nm (2.2 nm FWHM), respectively, is obtained with up to 53% slope efficiency. Using a YAG:Cr⁴⁺ saturable absorber for passive Q-switching the cavity, ordinary and extraordinary pulses are obtained with an energy as high as 236 μJ and with about 30 ns duration. The two pulses of orthogonal polarizations can be separated by up to a few hundred ns, depending on the experimental conditions. The simultaneity of the pulses is observed but is difficult to maintain. A model constituted by two coupled equations reproduces reasonably well the experimental data. Repetition rates up to 3 kHz have been explored, corresponding to 4.65 W absorbed pump power. PACS 42.55.Xi; 42.60.Gd; 42.25.Ja     

Third-harmonic and sum-frequency generation in a quadratically nonlinear polymer by time-ordered ultrashort laser pulses

Third-harmonic and sum-frequency generation in quadratically nonlinear azopolymer films is experimentally studied using femtosecond chromium forsterite laser pulses. A noncollinear geometry of sum-frequency and third-harmonic generation developed and implemented in this work allows the influence of the time ordering of ultrashort laser pump pulses on nonlinear-optical phenomena to be experimentally observed. Femtosecond laser pulses induce transitions of azopolymer molecules to an electronically excited state and produce vibrational wave packets, leading to an asymmetry in the dependence of the efficiency of second-and third-order nonlinear-optical processes on the delay time between the pump pulses.     

Coherent control of the lattice dynamics of bismuth near the lindemann stability limit

The relative contributions of the anharmonicity of the lattice potential and the nonequilibrium concentration of charge carriers to the time dependence of the coherent A _1g phonon frequency in bismuth excited by high-energy ultrashort laser pulses are studied by the coherent control method. The contributions are separated by the pump-probe method in which excitation is performed by two pulses with a controlled time delay. It is shown that, depending on the relative delay between the pump pulses, both correlation and anticorrelation between the amplitude and the initial frequency of oscillations are observed while the chirp and the initial frequency of the coherent phonon are anticorrelated. In addition, it has been found that the contributions of the lattice and the electronic subsystem are always anticorrelated. Therefore, a certain phase can be assigned to an electronic excitation and it may be suggested that the time dependence of the phonon frequency is determined not only by instantaneous values of the lattice and electronic response but also by the phase relations between them.     

Optical control of the anisotropy of the orientation of molecules in a liquid

The control of the anisotropy of the orientation of molecules in pure 1,2-dichlorobenzene, C₆H₄Cl₂ at room temperature is demonstrated experimentally. To accomplish the optical control, the medium is exposed to non-resonant excitation with two successive linearly polarized laser pulses with a duration of 60 fs. The state of transient anisotropy is probed with the third pulse by detecting the ultrafast optical Kerr effect via optical heterodyne detection and synchronous demodulation. It is shown that variations in the two parameters, the delay time between two pump pulses, and the angle between the polarization directions of the pump pulses ensure the control of the anisotropy of the orientation of molecules in the subpicosecond region.     

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.     

Enhancement of coherent population transfer in a double Λ-type four-level system via a train of pulse pairs

We propose a flexible way to significantly enhance population transfer efficiency with a train of time-separated pump-Stokes pulse pairs when the non-adiabatic coupling between two degenerate adiabatic states exists in a double Λ-type four-level system, where the pump and Stokes pulses in each pair can be applied in either counterintuitive or intuitive order. It is shown that the needed Rabi frequency for achieving complete population transfer can be reduced dramatically with the increase of number of pump-Stokes pulse pairs, which results from temporal constructive quantum interference between the sequential transitions and subsequent coherent accumulation; moreover, an arbitrary coherent superposition between the two lower states can be realized by suitably tuning the Rabi frequency and the time delay between each pump-Stokes pair. The method may find applications in control of chemical reactions, quantum optics, and quantum information processing.     

Coherent and incoherent spectral broadening in a photonic crystal fiber

The coherence of the spectral broadening process is the key requisite for the application of supercontinua in frequency combs. We investigate the coherence of two subsequent supercontinuum pulses created in a photonic crystal fiber pumped by a femtosecond laser. We measure Young interference fringes from a Michelson-type interferometer at different wavelengths of the output spectrum and analyze their dependence on pump intensity and polarization. The visibility of these fringes is a direct measure of the coherence of the spectral broadening processes.     

Relative phase measurement of a stark wave packet in the vicinity of the saddle point

A gas of Rb atoms in a static electric field has been photoexcited to just above the classical ionization threshold by a phase-locked sequence of two far infrared pulses. A single laser pulse generates a series of ejected electron packets emerging at the saddle point of the potential; each of the ejected packets is characterized by a phase and a chirp. We calculate and measure these phases and chirps using the time dependent interference of the electronic wave function controlled by the delay between the two light pulses.     

Few‐cycle,broadband, mid‐infrared optical parametric oscillator pumped by a 20‐fs Ti:sapphire laser

A few‐cycle, broadband, singly‐resonant optical parametric oscillator (OPO) for the mid‐infrared based on MgO‐doped periodically‐poled LiNbO₃ (MgO:PPLN), synchronously pumped by a 20‐fs Ti:sapphire laser is reported. By using crystal interaction lengths as short as 250 µm, and careful dispersion management of input pump pulses and the OPO resonator, near‐transform‐limited, few‐cycle idler pulses tunable across the mid‐infrared have been generated, with as few as 3.7 optical cycles at 2682 nm. The OPO can be continuously tuned over 2179‐3732 nm (4589‐2680 cm^‐1) by cavity delay tuning, providing up to 33 mW of output power at 3723 nm. The idler spectra exhibit stable broadband profiles with bandwidths spanning over 422 nm (FWHM) recorded at 3732 nm. The effect of crystal length on spectral bandwidth and pulse duration is investigated at a fixed wavelength, confirming near‐transform‐limited idler pulses for all grating interaction lengths. By locking the repetition frequency of the pump laser to a radio‐frequency reference, and without active stabilization of the OPO cavity length, an idler power stability better than 1.6% rms over >2.75 hours is obtained when operating at maximum output power, in excellent spatial beam quality with TEM₀₀ mode profile. Photograph shows a multigrating MgO:PPLN crystal used as a nonlinear gain medium in the few‐cycle femtosecond mid‐IR OPO. The visible light is the result of non‐phase‐matched sum‐frequency mixing between the interacting beams.     

Femtosecond pulse generation using stimulated Raman scattering in integrated silicon optical waveguide device

To generate ultrafast femtosecond optical pulses, we propose a model of an integrated device consisting of a Mach-Zehnder interferometer (MZI) with two symmetric 3 dB directional couplers and a straight waveguide based on the single-mode silicon-on-insulator (SOI) optical waveguide. The principle of pulse generation in the presented device is based on the strong stimulated Raman scattering (SRS) in silicon; the center wavelength of the pulse generated is tunable by changing the center wavelength of the co-propagating pump pulse. Numerical results show that, when a continuous wave (CW) with a weak power at 1670 nm wavelength and a pump pulse with a high peak power at 1550 nm wavelength are co-propagating, a narrow femtosecond pulse with a pulse width (full width at half maximum, FWHM) of ∼60 fs (FWHM of the pump pulse is 166.5 fs) can be achieved in the device proposed. In addition, when the waveguide length, pump peak power, and pump-pulse width are fixed, the properties of generated femtosecond pulse depend strongly on the incident chirp of the pump pulse and the CW power.     

Temporal coherent control induced by wave packet interferences in one and two photon atomic transitions

The interaction of a sequence of two identical ultrashort laser pulses with an atomic system results in quantum interferences as in Ramsey fringes experiments. These interferences allow achievement of temporal coherent control of the excitation probability. We present the results of a temporal coherent control experiment on two different atomic systems: one-photon absorption in K (4s-4p) and two-photon absorption in Cs (6s-7d). In K, the quantum interferences between the two excitation paths associated with the laser pulses are revealed through rapid oscillations of the excitation probability as a function of the time delay between the two pulses. These oscillations take place at the transition frequency (period T = 2.56 fs). The interferences are modulated by beats (at about 580 fs) resulting from the doublet structure of the excited state (4p (² P _1/2 , ² P _3/2 )). Three complementary interpretations of this experiment are presented: in terms of beats of quantum interferences, of variation in the spectrum intensity, and of wave packet interferences. Whenever the two laser pulses are temporally overlapped, optical interferences are superimposed on to the quantum interferences. The distinction between these two types of interference is clearly revealed in the two-photon excitation scheme performed on Cs (6s-7d (² D _3/2 , ² D _5/2 )) because quantum interferences occur at twice the frequency of the optical interferences. Received: 30 December 1997 / Revised: 28 February 1998 / Accepted: 4 March 1998     

Temporally Correlated Narrowband Biphoton Interference Based on Mach–Zehnder Interferometer

Since early 1990s, Mach–Zehnder interferometer has been used to investigate the interference of biphoton wave packets. Due to subpicosecond time coherence of biphoton generated by spontaneous parametric downconversion process, some physical processes are ignored in the interferometer, most likely the biphoton time‐domain interference. Here, the two‐photon interference phenomenon based on the Mach–Zehnder interferometer is theoretically studied, where the correlated photon pairs are produced by the four‐wave mixing in atomic system. In particular, the quantum interference effect to effectively control the coherent time of two‐photon by adjusting the input delay is used. In the damped Rabi oscillation regime, two‐photon bunching and antibunching effects are observed. In addition, in the group‐delay regime, the interference between biphoton precursor, slow‐light wave packets and also in between the precursor and the slow‐light wave packets is observed, which had never been reported before. These results may have potential applications in the fields of biphoton shaping and quantum information processing.     

Frequency–time and time–space mappings with broadband and supercontinuum chirped pulses in coherent wave mixing and pump–probe techniques

Broadband and supercontinuum pulses with a linear chirp define a linear transform, mapping the difference between the instantaneous frequencies of pump pulses onto the delay time between these pulses. This delay between the pump pulses can be then mapped onto the spatial coordinate with the use of a broad-beam wave-mixing or pump–probe geometry. The new possibilities offered by these mappings for four-wave-mixing techniques are discussed. The spectral and temporal resolution of chirped-pulse wave-mixing and pump–probe techniques are examined. Single-shot multidimensional wave-mixing techniques using broadband and supercontinuum chirped pulses are discussed. PACS 42.65.Dr; 42.65.An     

Field-free molecular orientation induced by combined femtosecond single- and dual-color laser pulses：The role of delay time and quantum interference

The coherent control of field-free molecular orientation of CO with combined femtosecond single- and dual-color laser pulses has been theoretically studied. The effect of the delay time between the femtosecond single- and dual-color laser pulses is discussed, and the physical mechanism of the enhancement of molecular orientation with pre-alignment of the molecule is investigated. It is found that the basic mechanism is based on the creation of a rotational wave packet by the femtosecond single-color laser pulse. Furthermore, we investigate the interference between multiple rotational excitation pathways following pre-alignment with femtosecond single-color laser pulse. It is shown that such interference can lead to an enhancement of the orientation of CO molecule by a factor of 1.6.     

Imaging and control of interfering wave packets in a dissociating molecule

Using two identical 110 femtosecond (fs) optical pulses separated by 310 fs, we launch two dissociative wave packets in I2. We measure the square of the wave function as a function of both the internuclear separation, /Psi(R)/(2), and of the internuclear velocity, /Psi(v(R))/(2), by ionizing the dissociating molecule with an intense 20 fs probe pulse. Strong interference is observed in both /Psi(R)/(2) and in /Psi(v(R))/(2). The interference, and therefore the shape of the wave function, is controlled through the phase difference between the two dissociation pulses in good agreement with calculations.