Rabi Oscillations and Coherence Dynamics in Terahertz Streaking-Assisted Photoelectron Spectrum

We present an approach,a Terahertz streaking-assisted photoelectron spectrum(THz SAPS),to achieve direct observations of ultrafast coherence dynamics with timescales beyond the pulse duration.Using a 24 fs probe pulse,the THz SAPS enables us to well visualize Rabi oscillations of 11.76 fs and quantum beats of 2.62 fs between the 5S_1/2 and 5P_3/2 in rubidium atoms.The numerical results show that the THz SAPS can simultaneously achieve high resolution in both frequency and time domains without the limitation of Heisenberg uncertainty of the probe pulse.The long probe pulse promises sufficiently high frequency resolution in photoelectron spectroscopy allowing to observe Autler-Townes splittings,whereas the streaking THz field enhances temporal resolution for not only Rabi oscillations but also quantum beats between the ground and excited states.The THz SAPS demonstrates a potential applicability for observation and manipulation of ultrafast coherence processes in frequency and time domains.     

A femtosecond self-mode-locked Ti:sapphire laser with high stability of pulse-repetition frequency and its applications

The spectral characteristics and stability of a frequency of intermode beats of a fs self-mode-locked Ti:sapphire laser are investigated. An active method is used to obtain high stability. The frequency stability of intermode beats not lower than 1.27×10⁻¹² rms in 50 s is achieved. Possible applications of the setup, such as measurement of large frequency intervals in the optical range, creation of optical frequency synthesizers, etc., are proposed. The physical principles for the creation of an optical clock of a new type using a highly stable fs Ti:sapphire laser are considered. Received: 7 May 1999 / Published online: 27 October 1999     

液体水中O-H 弯曲振动能量弛豫的数值

应用分子动力学模拟方法研究了液相水中水分子O-H弯曲振动能量弛豫的机理. 采用刚性和柔性溶剂模型来探讨振动能量弛豫的不同通道. 研究发现，刚性溶剂中O?H弯曲振动泛频的弛豫时间为174 fs而柔性溶剂中为115 fs. O-H 弯曲振动泛频振动能量弛豫的主要途径是跃迁O?H 弯曲振动基频. O-H弯曲振动基频的弛豫时间为204 fs，与实验值170 fs符合得较好.     

Time-resolved refractive index and absorption mapping of light-plasma filaments in water

By means of a quantitative shadowgraphic method, we performed a space-time characterization of the refractive index variation and transient absorption induced by a light-plasma filament generated by a 120 fs laser pulse in water. The formation and evolution of the plasma channel in the proximity of the nonlinear focus were observed with a 23 fs time resolution.     

Ultrafast nonlinear optical response of squarylium dye J-aggregates spincoated films and an application to T bps demultiplexer

We have fabricated spincoated film of squarylium dye (SQ) J-aggregates exhibiting ultrafast nonlinear optical response at room temperature and shown a new serial-to-parallel demultiplexer for T bps optical signals using SQJ-aggregates film. Optical dynamics measurements reveal that saturable absorption of this SQJ-spincoated film exhibits a decay time of less than 100 fs at pump energy of 80 fJ/μm². With this ultrafast SQJ optical film, multi-output demultiplexing operations for T bps optical signals were demonstrated. A series of 4 pulses with 100 fs duration and 1 ps interval (corresponding to 1 T bps signals) were irradiated onto the SQJ film synchronized with a 100 fs gate pulse at a finite angle. Four demultiplexed signals were clearly observed at different areas on CCD camera.     

Spectroscopic investigations of femtosecond laser irradiated polystyrene and fabrication of microstructures

We report microfabrication of structures in bulk and thin films of polystyrene (PS) using femtosecond (fs) laser pulses. For the first time to our knowledge, we report emission from the fs laser modified regions of bulk and thin films of PS when excited at 458, 488, and 514 nm. Moreover, we report the existence of peroxide type free radicals, for the first time, in fs laser irradiated bulk PS. We observed the suppression of Raman modes in case of structures fabricated at higher energies and the same effect was noticed in central portion of the structures fabricated. No appreciable broadening was observed in the case of structures fabricated at low energies. Possible applications resulting from such structures are discussed briefly.     

Direct observation of sub-100 fs mobile charge generation in a polymer-fullerene film

The formation of mobile charges in a roll-to-roll processed poly-3-hexylthiophene-fullerene bulk heterojunction film is observed directly by using transient terahertz spectroscopy with sub-100?fs temporal resolution. The transient terahertz ac conductivity reveals that 20% of the incident pump photons are converted into highly delocalized charges within the 40?fs, 3.1?eV pump pulse duration, which then rapidly becomes localized within 120?fs. Approximately 2/3 of these carriers subsequently decay, possibly into an exciton, on a 1?ps time scale.     

Tunable second harmonic generation from a Kerr-lens mode-locked Yb:YCa_4O(BO_3)_3 femtosecond laser

We experimentally demonstrated a diode-pumped Kerr-lens mode-locked femtosecond(fs) laser with a self-frequency doubling Yb:YCa_4O(BO_3)_3 crystal.Sub-40 fs laser pulses were directly generated from the oscillator without extracavity compression.The central wavelength was tunable from 1039 nm to 1049 nm with a typical bandwidth of 35 nm and an average output power of 53 mW.For the first time,a self-frequency doubled second harmonic green laser with tunable range from 519 nm to 525 nm was observed.     

Optical phonon sidebands of electronic intersubband absorption in strongly polar semiconductor heterostructures

We present the first evidence for a distinct optical phonon progression in the linear and nonlinear intersubband absorption spectra of electrons in a GaN/Al(0.8)Ga(0.2)N heterostructure. Femtosecond two-color pump-probe experiments in the midinfrared reveal spectral holes on different vibronic transitions separated by the LO-phonon frequency. These features wash out with a decay time of 80 fs due to spectral diffusion. The remaining nonlinear transmission changes decay with a time constant of 380 fs. All results observed are described by the independent boson model.     

Raman study of phase transformation of TiO2 rutile single crystal irradiated by infrared femtosecond laser

Titanium dioxide (TiO₂) rutile single crystal was irradiated by infrared femtosecond (fs) laser pulses with repetition rate of 250 kHz and phase transformation of rutile TiO₂ was observed. Micro-Raman spectra show that the intensity of E_g Raman vibrating mode of rutile phase increases and that of A_1g Raman vibrating mode decreases apparently within the ablation crater after fs laser irradiation. With increasing of irradiation time, the Raman vibrating modes of anatase phase emerged. Rutile phase of TiO₂ single crystal is partly transformed into anatase phase. The anatase phase content transformed from rutile phase increased to a constant with increasing of fs pulse laser irradiation time. The study indicates the more stable rutile phase is transformed into anatase phase by the high pressure produced by fs pulse laser irradiation.     

Real-time observation of phase-controlled molecular wave-packet interference

The quantum interference of two molecular wave packets has been precisely controlled in the B electronic state of the I2 molecule by using a pair of fs laser pulses whose relative phase is locked within the attosecond time scale and its real-time evolution has been observed by another fs laser pulse. It is clearly observed that the temporal evolution changes drastically as a function of the relative phase between the locked pulses, allowing us to read both amplitude and phase information stored in the wave functions of the molecular ensemble.     

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.     

Time-resolved measurements of high order harmonics confined by polarization gating

We investigate the temporal confinement of high order harmonic pulses generated by a femtosecond (fs) infrared (IR) pulse with a time varying polarization. We use a set of two birefringent quartz plates to modulate the IR polarization. It produces a short temporal gate of linear polarization where harmonics are efficiently generated during a small fraction of the IR pulse. By rotating one of the plates, the gate width can be continuously varied between 70 fs down to 7 fs. The XUV pulse duration is measured by cross-correlation with a probe IR pulse of 12 fs. When the gate width is decreased, a clear temporal confinement of the XUV emission is observed through the cross correlation signal. This experiment is the first direct experimental evidence in the temporal domain that the polarization gating technique can be used to significantly shorten the harmonic pulse duration. PACS 32.80.Wr; 42.65.Ky; 42.65.Re     

Reduction of multi-photon ionization in dielectrics due to collisions

The collisional effect due to the multi-photon ionization process in dielectric material has been studied. We found that the breakdown threshold of fused silica is the same for both linearly and circularly polarized light at 55 fs and 100 fs, which we believe is an indication of the suppression of multi-photon ionization in solids. By numerically solving the time-dependent Schrödinger equation with scattering, for the first time, we have observed substantial reduction of the multi-photon ionization rate in dielectrics due to collisions.     

Dissection of dispersed off‐resonant femtosecond degenerate four‐wave mixing of O2

Simultaneous time and frequency detection in off‐resonant femtosecond degenerate four‐wave mixing (fs‐DFWM) experiments displays spectral features that are covered in standard, nondispersed, frequency‐integrated measurements. The application of laser fields with finite bandwidths, narrower than or comparable to the rotational Raman bands, affects the observed coherent signals. Information available from such experiments is split between the time and frequency domains and an improved measurement necessitates a combined detection. Rotational recurrences of oxygen (O₂), measured by dispersed fs‐DFWM at room temperature, exhibit spectral characteristics, using 800‐nm laser pulses with ∼100 fs duration. Analysis of the detected signals in both dimensions incorporating temporal and spectral trends can assist in the extraction and interpretation of chemicophysical quantities from the experiment. The dispersed recurrent signals are in accordance with simulations. Copyright © 2011 John Wiley & Sons, Ltd.     

Ultrafast motion of liquids C2H4Cl2 and C2H4Br2 studied with a femtosecond laser

Transient optical Kerr effect of liquids C₂H₄Cl₂ and C₂H₄Br₂ is investigated, for the first time to our knowledge, with a femtosecond (fs) probe laser delayed with respect to a coherent fs pump laser. Coherent coupling and electronic Kerr signals are observed around zero delay when pump and probe overlap. Persisting after the pump-probe overlap are Kerr signals arising from the torsional and other intramolecular vibrations of the trans and gauche conformations; Kerr signals arising from the intermolecular motion are also observed. Vibrational quantum interference is only observed in liquid C₂H₄Br₂ and the related beats data are fitted with the torsional vibrations, 91 cm⁻¹ (gauche) and 132 cm⁻¹ (trans), and the CCBr angle-bending vibrations, 231 cm⁻¹ (gauche) and 190 cm⁻¹ (trans), with dephasing times, 0.45 ps, 0.45 ps, 2 ps, and 1.5 ps, respectively. These vibrational frequencies agree with those obtained in the frequency-domain. That no vibrational mode is observed for C₂H₄Cl₂ might be attributed to ineffective Raman-pumping. Kerr signals observed after the pump-probe overlap are Fourier transformed to give the spectra of the intermolecular motion and the vibrational spectrum, which agrees with the one observed in the infrared absorption and/or Raman scattering heretofore.     

Ultrashort dephasing-time measurements in Nile Blue polymer films

Optical dephasing measurements using degenerate four-wave mixing (DFWM) were performed on thin dye-polymer films at room temperature. Incoherent light centered at 575 nm was used as a source for ultrafast measurements on the blue side of the inhomogeneous distribution of the oxazine dye Nile Blue. Under these conditions, a new form of interference was observed as a sinusoidal variation of the DFWM signal versus delay time. A measured interference period of 1.96+/-0.07 fs corresponds to the optical cycle time of the light source. Numerical solutions for the DFWM intensity confirm the oscillation effect and estimate a measured dephasing time of 2-3 fs.     

Two-step femtosecond laser pulse train fabrication of nanostructured substrates for highly surface-enhanced Raman scattering

A simple and repeatable method using femtosecond laser pulse train to fabricate nanostructured substrates with silver nanoparticles over a large area for surface-enhanced Raman scattering is reported. The method involves two steps: (1)?femtosecond laser pulse train micromachining and roughening and (2)?femtosecond laser processing of the substrates in a silver nitrate solution. Surface modification is investigated experimentally by varying the time delay of the double femtosecond laser pulse train. With time delay ranging from 200 to 600?fs, the different enhancement factors were observed. This study demonstrates that a maximum enhancement factor of 6.8×10⁶, measured by 10^-6 M Rhodamine 6G solution, can be achieved at the time delay of 400?fs.     

Oscillation of the refractive index at the focal region of a femtosecond laser pulse inside a glass

The temporal evolution of refractive-index change produced by a tightly focused femtosecond (fs) laser pulse inside a soda-lime glass plate was investigated by use of a transient lens method with subpicosecond time resolution. An oscillating behavior of the light intensity in the central region of the probe beam was observed 0-1500 ps after irradiation of the plate. The oscillation was interpreted in terms of a rapid temperature increase and the ensuing propagation of the pressure wave. This study is to our knowledge the first real-time observation of refractive-index change inside a glass induced by a fs laser pulse.     

Constructive and Destructive Two-Pulse Excitation Investigated with a White-Light Michelson Interferometer

Linear propagation of two pulses through methanol solution of aluminum phthalocyanine chloride is investigated using a modified white-light Michelson interferometer. The observed coherence time of the white light is 6 fs, and the separation between the two-excitation pulses is set to about 10 fs. The excitation is dependent on the phase-relation between the two pulses. We have observed an enhancement of the excitation when the two pulses are in-phase and strong suppression of the excitation when the two pulses are out of phase by π.