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.     

Generation of ultrabroadband terahertz radiation under optical breakdown of air by two femtosecond pulses of different frequencies

Experimental results on the generation of terahertz (THz) electromagnetic radiation under ionization of air by femtosecond pulses at fundamental and second-harmonic frequencies of a Ti-sapphire laser are presented. The mean power of the generated THz radiation as a function of the time delay between two pulses of different frequencies is found to be quasi-periodical. Theoretically, we show that efficient generation of THz radiation is governed by the inertial part of the nonlinear response of the medium, which is determined by the dynamics of population of highly excited states with subsequent emission of electrons.     

The dynamics of a THz Rydberg wavepacket

An optically excited Rydberg wavepacket can be generated by exciting the electron from a low-lying state to a coherent superposition of high-lying states with a short broadband optical pulse. A special kind of Rydberg wavepacket is generated in the case of a interaction of a weak THz half cycle pulse with a stationary Rydberg state, called the THz wavepacket. This THz wavepacket is a coherent superposition of the initial Rydberg state and its neighbouring states. We have investigated the time evolution of THz wavepackets by measuring the impact of two in time delayed half cycle pulses ( ≈ 200 V cm^-1) on the population of a stationary (n = 40) Rydberg state in rubidium. The first half cycle pulse creates the THz wavepacket and the second half cycle pulse probes the dynamics of the THz wavepacket. We support our experimental data by numerically solving the Schr?dinger equation and with a semi-classical picture. Whereas an optically excited wavepacket is initially localized, a THz wavepacket is initially delocalized and becomes localized after half a revival time. Received 23 August 2000 and Received in final form 27 March 2001     

Optical Absorption Spectra and Intraband Dynamics in Terahertz-Driven Semiconductor Superlattice

We have theoretically investigated the optical absorption spectrum and intraband dynamics by subjecting a superlattice to both a terahertz (THz)-frequency driving field and an optical pulse by using an excitonic basis.In the presence of a THz dc field, the satellite structures in the absorption spectra are presented. The satellite structure is a result from the THz nonlinear dynamics of Wannier-Stark ladder excitons. On the other hand, the coherent intraband polarization is investigated. We find that the excitonic Bloch oscillation is driven by the THz field and yields an intraband polarization that continues to oscillate at times much longer than the intraband dephasing time. The temporal evolution of the slowly varying components of the intraband polarization is dependent on the THz frequency.     

Excitation-density-dependent generation of broadband terahertz radiation in an asymmetrically excited photoconductive antenna

The generation of terahertz (THz) transients in photoconductive emitters has been studied by varying the spatial extent and density of the optically excited photocarriers in asymmetrically excited, biased low-temperature-grown GaAs antenna structures. We find a pronounced dependence of the THz pulse intensity and broadband (>6.0 THz) spectral distribution on the pump excitation density and simulate this with a three-dimensional carrier dynamics model. We attribute the observed variation in THz emission to changes in the strength of the screening field.     

Few-cycle THz spectroscopy of nanostructures

Optically excited plasma oscillations in n-doped GaAs epilayers emit intense THz pulses. Using a THz-pump and THz-probe technique we observe the response of the intersubband polarization in semiconductor quantum structures. THz Cross-correlation measurements of modulation doped semiconductor quantum structures allow to determine the absorption, the dispersion, and the dephasing times of the quantized electrons.     

Coherent optical phonons and parametrically coupled magnons induced by femtosecond laser excitation of the Gd(0001) surface

Coherent spin dynamics in the THz domain coupled to a coherent phonon is observed in the time-resolved second harmonic response of the Gd(0001) ferromagnetic metal surface. An LO phonon of 2.9 THz is excited by a transient charge displacement at the surface caused by resonant absorption of a fs laser pulse in the exchange-split surface state. This lattice vibration modulates the interlayer distance inducing a coherent variation of the exchange interaction between spins in adjacent layers. The resulting magnetization dynamics is considered as optical magnon wave packets coupled to the phonon.     

Infrared and far-infrared spectroscopy of CH3OH: TeraHertz laser lines and assignments

We use a ¹³CO₂ laser as optical pumping source to search for new THz laser lines generated from ¹³CH₃OH. Nineteen new THz laser lines (also identified as far-infrared, FIR) ranging from 42.3 μm (7.1 THz) to 717.7 μm (0.42 THz) are reported. They are characterized in wavelength, offset, relative polarization, relative intensity, and optimum working pressure. We have assigned eight laser lines to specific rotational energy levels in the excited state associated with the C-O stretching mode.     

多功能太赫兹超表面偏振控制器

本文提出了一种“金属栅-开口环/硅环-金属栅”结构的透射式超表面偏振控制器, 研究了入射角度和抽运光对该器件传输及偏振态控制性能的影响. 研究结果表明, 当线偏振太赫兹波垂直入射时, 可对0.39-1.11 THz频段的太赫兹波实现偏振方向90°旋转, 偏振旋转效率为99%, 损耗为1 dB. 对于斜入射的情况, 偏振转换性能在0-60°范围内基本保持不变, 且透过率达到90%以上. 同时, 通过调控抽运光强度的方式, 该器件能够实现对透射与反射太赫兹光束的强度调制, 调制深度均达到90%, 且可以实现太赫兹波偏振分束功能. 该器件可以作为未来太赫兹空间光通信和信息处理的宽带、角度不敏感、可调谐的偏振转换器和分束器.     

Oscillations at a difference frequency in the middle and far infrareds in GaP semiconductor waveguides

The feasibility of oscillation at a difference frequency in the middle and far infrareds is considered under the condition of phase matching between a nonlinear polarization wave and a difference mode produced by two fundamental modes with a wavelength near 1 μm excited in a GaP dielectric waveguide. With 10-W short-wave modes propagating in a 100-μm-wide planar waveguide, the power of the difference mode can be as high as 300 μW at 1–8 THz at room temperature. When the GaP waveguide leans upon a silicon substrate, the power of the difference mode may reach 5 mW at 10–14 THz at the same temperatures.     

Pulsed EPR spectrometer with injection-locked UCSB free-electron laser

We describe the first free-electron laser (FEL)-based pulsed electron paramagnetic resonance (EPR) system designed to study spin dynamics and structure changes of proteins in aqueous solution with nano-second of time resolution. This novel approach opens up the possibility for high-power sub-THz and THz pulsed EPR spectroscopy.     

All-optical ultrafast polarization switching of terahertz radiation by impulsive molecular alignment

We experimentally demonstrate ultrafast polarization switching of terahertz (THz) radiation generated by dual-color driving pulses composed of orthogonally polarized fundamental and second-harmonic waves, which can be controlled by field-free molecular alignment in air by modulating the relative phase between the two field components as a transient dynamic wave plate. By fine-tuning the time delay to properly match the molecular alignment revivals, a significant polarization modulation of the THz radiation is observed and both linearly and elliptically polarized THz radiations can be obtained.     

Asynchronous sampling for ultrafast experiments with low momentum compaction at the ANKA ring

A high‐repetition‐rate pump–probe experiment is presented, based on the asynchronous sampling approach. The low‐α mode at the synchrotron ANKA can be used for a time resolution down to the picosecond limit for the time‐domain sampling of the coherent THz emission as well as for hard X‐ray pump–probe experiments, which probe structural dynamics in the condensed phase. It is shown that a synchronization of better than 1 ps is achieved, and examples of phonon dynamics of semiconductors are presented.     

Terahertz polarization imaging with birefringent materials

We present a terahertz (THz) imaging method with a birefringent material which is sensitive to THz wave polarization. The subtle THz polarization modulations introduced by the target are extracted by the amplitudes of the two separated THz peaks passing through the birefringent material. The anisotropy of the industrial sprayed-on-foam-insulation (SOFI) is characterized by measuring its azimuthal angle dependent THz polarization response. This work demonstrated that this polarization sensitive THz imaging technique can be used for industrial inspection and biological related characterization.     

Nonstationary rotational diffusion in room temperature liquids measured by femtosecond three-pulse transient anisotropy

A femtosecond three-pulse chi((5)) polarization anisotropy experiment is used to examine the time dependence of the rotational diffusion of coumarin 153 in polar liquids. By probing the polarization anisotropy decay at various points during the molecule's excited state lifetime, a time-dependent diffusion coefficient is found in several solvents. This anomalous behavior is consistent with the relaxation of the solvent friction to accommodate the solute's excited state charge distribution. Rotational diffusion times measured immediately after photoexcitation by two-pulse chi((3)) experiments may reflect a nonstationary bath dynamics, rather than the equilibrium friction of the solvent.     

Terahertz radiation by spontaneous polarization fields in InN

Terahertz (THz) radiation is measured from InN excited by femtosecond optical pulses at 790 nm. The InN sample is grown by metalorganic chemical vapor deposition. The InN surface shows typical grain like morphology often observed in N-polar InN. The polarity of the THz radiation field from InN is opposite to that from p-InAs, whose radiation mechanism is dominated by the photo-Dember effect, and is same as that from p-GaAs indicating that the dominant radiation mechanism in InN is the drift current induced by the internal electric field at low-density excitation. In addition, since no azimuthal angle dependence of the THz radiation is observed, the optical rectification effect is ruled out. The lattice constant c=5.7091 Å for the InN epilayer is determined by θ–2θ scan of X-ray diffraction. This implies that the InN epilayer is fully relaxed. Therefore, there is no piezoelectric polarization, and the internal electric field in the InN epilayer results from spontaneous polarization. According to the direction of the spontaneous polarization, the N polarity of the InN sample is confirmed.     

THz wave polarization-controlled spectroscopic imaging for anisotropic materials

We present a polarization-controlled terahertz (THz) wave spectroscopic imaging modality to investigate the anisotropy of the detected materials. The polarization of the emitted THz wave is controlled by changing the relative phase between the fundamental and second-harmonic waves in the two-color laser-induced air plasma THz generation configuration. The THz wave polarization direction is extracted by measuring the two electric field amplitudes when the polarization of the incident wave is controlled to be horizontal and vertical. The anisotropy of the industrial Sprayed-On-Foam-Insulation (SOFI) is characterized by measuring its azimuthal angle dependent THz polarization response. This work demonstrates that THz wave polarization-controlled imaging technique can be used for highly sensitive industrial nondestructive inspection and biological related characterization.     

Ultra-fast dynamics of coherent lattice and spin excitations at the Gd(0001) surface

The Gd(0001) surface is investigated by pump–probe experiments using femtosecond laser pulses at 740–860 nm wavelength. Employing optical second-harmonic generation, spin and lattice dynamics are separated through the symmetry of optical field contributions that are even and odd with respect to magnetization reversal. A coherent phonon–magnon mode at a frequency of 3 THz that is excited through the exchange-split surface state is observed in the time domain. A magneto-elastic phonon–magnon interaction based on spin–orbit coupling is weak for Gd and a modulation of the exchange interaction mediated by the lattice vibration is proposed as a microscopic interaction mechanism of this coupled mode. In parallel, electron–electron and electron–phonon interactions and their magnetic counterparts lead to incoherent dynamics of the electron, lattice, and spin subsystems. Variation of the optical wavelength shows that for longer wavelengths up to 860 nm the coherent mode dominates, while for shorter ones (≥740 nm) incoherent contributions prevail. This dependence indicates that selective depopulation of the occupied surface state component drives the coherent excitation. However, temperature-dependent studies show that the oscillation amplitude of even and odd contributions scales with the spin polarization of the surface state, suggesting that the spin dependence of the ion potentials contributes as well. Furthermore, the frequency of the coherent mode presents a blue shift with a delay of 0.17 THz/ps that saturates at the static frequency of the respective bulk phonon. This behavior is a consequence of equilibration of the screened ion potential at the surface subsequent to the intense laser excitation. PACS 78.47.+p; 63.22.+m; 63.20.Ls; 75.30.Ds     

Generation of THz transients by photoexcited single-crystal GaAs meso-structures

We report a sub-picosecond photoresponse and THz transient generation of GaAs single-crystal mesoscopic platelets excited by femtosecond optical pulses. Our structures were fabricated by a top-down technique, by patterning an epitaxial, 500-nm-thick GaAs film grown on top of an AlAs sacrificial layer and then transferring the resulting etched away 10 × 20-μm² platelets onto an MgO substrate using a micropipette. The freestanding GaAs devices, incorporated into an Au coplanar strip line, exhibited extremely low dark currents and ~0.4 % detection efficiency at 10 V bias. The all-optical, pump–probe carrier dynamics analysis showed that, for 800-nm-wavelength excitation, the intrinsic relaxation of photocarriers featured a 310-fs-wide transient with a 290 fs fall time. We have also carried out a femtosecond, time-resolved electro-optic characterization of our devices and recorded along the transmission line the electrical transients as short as ~600 fs, when the platelet was excited by a train of 100-fs-wide, 800-nm-wavelength optical laser pulses. The platelets have been also demonstrated to be very efficient generators of free-space propagating THz transients with the spectral bandwidth exceeding 2 THz. The presented performance of the epitaxial, freestanding GaAs meso-structured photodevices makes them uniquely suitable for THz-frequency optoelectronic applications, ranging from ultrafast photodetectors to THz-bandwidth optical-to-electrical transducers and photomixers.     

非线性克尔效应对飞秒激光偏振的超快调制

研究了近红外飞秒激光的偏振在太赫兹频率的超快调制.利用抽运-探测光谱技术,通过改变两个脉冲之间的延迟时间可以控制光脉冲的旋转角.在Li：NaTb（WO₄）₂磁光晶体中观察到探测光的偏振随延迟时间变化的高速振荡,振荡信号的中心频率为0.19 THz.这种超快偏振调制现象可以解释为,抽运-探测实验构置中,前向传播的抽运光诱导的光学克尔非线性引起被晶体远端表面所反射的背向传播的探测光脉冲偏振面的额外旋转.通过改变抽运光的圆偏振旋性可以控制探测光调制信号的相位和振幅.实验结果表明,非线性光学克尔效应可以作为一种全新的手段,在磁光晶体中实现近红外飞秒激光以太赫兹频率的超快偏振调控.这将在超快磁光调制器等全光器件中得以应用.实验结果将有助于偏振依赖的超快动力学过程的研究.