Observation of ultrafast carrier dynamics in amorphous Ge2Sb2Te5 films induced by femtosecond laser pulses

The femtosecond pump-probe technique was used to study the carrier dynamics of amorphous Ge2Sb2Te5 films. With carrier density at around 10(20)-10(21) cm(-3), carriers were excited within 1 ps and recovered to the initial state for less than 3 ns. On the picosecond time scale, the carrier relaxation consists of two components: a fast process within 5 ps and a slow process after 5 ps. The relaxation time of the fast component is a function of carrier density, which increases from 1.9 to 4.3 ps for the carrier density changing from 9.7x10(20) cm(-3) to 3.1x10(21) cm(-3). A possible interpretation of the relaxation processes is elucidated. In the first 5 ps the relaxation process is dominated by an intraband carrier relaxation and the carrier trapping. It is followed by a recombination process of trapped carriers at later delay time. (c) 2007 American Institute of Physics.

Study of rapid carrier capture and relaxation in InAs/GaAs heterostructures

The rapid carrier capture and relaxation processes in InAs/GaAs quantum dots were studied at 77K by using a simple degenerate pump-probe technique. A rising process was observed in the transient reflectivity, following the initial fast relaxation associated with GaAs bulk matrix, and this rising process was assigned to be related to the carrier capture from the GaAs barriers to InAs layers. The assignment was modeled using Kramers-Kronig relation. By analyzing the rising process observed in the transient reflectivity, the carrier capture time constants were obtained. The measured capture times decrease with the increase of carrier concentration.

Ultrafast low-temperature grown AlGaAs/GaAs photorefractive quantum wells using point defects as capture centers

At a medium substrate temperature of 400 degrees C and a lower As flux, we have grown an ultrafast AlGaAs/GaAs photorefractive multiple quantum well (MQW) structure by molecular beam epitaxy. The as-grown sample exhibits strong photorefractive effect under the transverse Frantz-Keldysh geometry. A peak electroabsorption of 2100 cm(-1) is measured in the as-grown sample in an 11 kV/cm dc electric field, and the peak photorefractive diffraction efficiency can be 1.2%. After postgrowth annealing, the photorefractive effect becomes weak and disappears in samples annealed above 700 degrees C. Using optical transient current spectroscopy, deep levels are measured in these samples. It is found that deep levels are stable against annealing until 700 degrees C. Using a pump-probe technique, carrier lifetimes are measured at room temperature. We find that the as-grown sample has a lifetime of 20 ps, while the 700 degrees C annealed sample has a lifetime of more than 200 ps. The ultrafast lifetime in the as-grown sample is caused by point defects, not by As clusters. Our result show that AlGaAs/GaAs MQW structure grown around 400 degrees C has better performance of the photorefractive effect. (C) 1999 American Institute of Physics. [S0003-6951(99)04036-X].

Observation of quantum beat in Rb by parametric four-wave mixing

Two coupled parametric four-wave-mixing processed in Rb atoms are studied using perturbation theory, which reveals clear evidence of the appearance of quantum beat at 608 cm(-1), corresponding to the energy difference of the 7s - 5d states of Rb atoms, in the parametric four-wave-mixing signals. A pump-probe technique is utilized to observe the quantum beat. Time-varying characteristics of the quantum beat are investigated using time-dependent Fourier transform. The results show that the time-varying characteristics of the quantum beat potential tool for monitoring the dissociation of molecules.

Dynamics of excited OCS investigated by resonance-enhanced multiphoton ionization

The predissociation decay behavior of molecule carbonyl sulfide (OCS) has been investigated by resonance-enhanced multiphoton ionization spectroscopy using the pump-probe technique of dichroic femtosecond lasers in real time. The lifetime of excited OCS around 74 720 cm(-1) by two-photon absorption of 268 nm, corresponding to upsilon(1)=1 of the Rydberg state [(2)Pi(1/2)]4ppi((1)Sigma(+)), is directly determined to be tau(D)=1071+/-11 fs. This picosecond decay process indicates that the excited state is predissociative. The temporal information of dissociation enriches the knowledge of the potential-energy surface of the associative excited state.

Anomalous variation of thermal lens signal with concentration from rhodamine B in methanol solution

Thermal lens signals in solutions of rhodamine B laser dye in methanol are measured using the dual beam pump-probe technique. The nature of variations of signal strength with concentration is found to be different for 514 and 488 nm Ar + laser excitations. However, both the pump wavelengths produce an oscillatory type variation of thermal lens signal amplitude with the concentration of the dye solution. Probable reasons for this peculiar behaviour (which is absent in the case of fluorescent intensity) are mentioned.

Ultrafast detection and control of molecular dynamics

Many elementary chemical and physical processes such as the breaking of a chemical bond or the vibrational motion of atoms within a molecule take place on a femtosecond (fs = 10−15 s) or picosecond (ps = 10−12 s) time scale. It is now possible to monitor these events as a function of time with temporal resolution well below 100 fs. This capability is based on the pump-probe technique where one optical pulse triggers a reaction and a second delayed optical pulse probes the changes that ensue. To illustrate this capability, the dynamics of ligand motion within a protein are presented. Moving beyond casual observation of a reaction to active control of its outcome requires additional experimental and theoretical effort. To illustrate the concept of control, the effect of optical pulse duration on the vibrational dynamics of a tri-atomic molecule are discussed. The experimental and theoretical resources currently available are poised to make the dream of reaction control a reality for certain molecular systems.

Enhanced sensitivity in detection of Kerr rotation by double modulation and time averaging based on Allan variance

Experiments in spintronics necessarily involve the detection of spin polarization. The sensitivity of this detection becomes an important factor to consider when extending the low temperature studies on semiconductor spintronic devices to room temperature, where the spin signal is weaker. In pump-probe experiments, which optically inject and detect spins, the sensitivity is often improved by using a photoelastic modulator (PEM) for lock-in detection. However, spurious signals can arise if diode lasers are used as optical sources in such experiments, along with a PEM. In this work, we eliminated the spurious electromagnetic coupling of the PEM onto the probe diode laser, by the double modulation technique. We also developed a test for spurious modulated interference in the pump-probe signal, due to the PEM. Besides, an order of magnitude enhancement in the sensitivity of detection of spin polarization by Kerr rotation, to 3x10(-8) rad was obtained by using the concept of Allan variance to optimally average the time series data over a period of 416 s. With these improvements, we are able to experimentally demonstrate at room temperature, photoinduced steady-state spin polarization in bulk GaAs. Thus, the advances reported here facilitate the use of diode lasers with a PEM for sensitive pump-probe experiments. They also constitute a step toward detection of spin-injection in Si at room temperature.

Measurement of Electron Density Profile Behind Strong Shock Waves with a Langmuir Probe

At the shock velocity range of 7~9km/s, the variations of electron density behind strong normal shock waves are measured in a low-density shock tube by using the Langmuir electrostatic probe technique. The electron temperature, calculated based on Park’s three-temperature model, is used in interpreting the probe current data. The peak electron densities determined in the present experiment are shown to be in a good agreement with those predicted by Lin’s calculation. The experimentally obtained ratios of the characteristic ionization distance to the mean free path of freestream ahead of the shock wave are found to be in a good agreement with the existing experiments and Park’s calculation.

Time-resolved investigation of low-density plasma channels produced by a kilohertz femtosecond laser in air

By employing pump-probe back longitudinal diffractometry, the electron density and decay dynamics of a weak plasma channel created by a 1-KHz fs laser in air has been investigated. With ultrashort laser pulses of 50 fs and low energy of 0.6 mJ, we observe weak plasma channels with a length similar to 2 cm in air. An analytical reconstruction method of electron density has been analyzed, which is sensitive to the phase shift and channel size. The electron density in the weak plasma channel is extracted to be about 4x10(16) cm(-3). The diameters of the plasma channel and the filament are about 50 and 150 mu m, respectively, and the measurable electron density can be extended to less than 10(15) cm(-3). Moreover, a different time-frequency technique called linearly chirped longitudinal diffractometry is proposed to time-resolved investigate ultrafast ionization dynamics of laser-irradiated gas, laser interaction with cluster beam, etc.

All-optical signal processing using semiconductor optical amplifiers for next generation optical networks

This thesis details an experimental and simulation investigation of some novel all-optical signal processing techniques for future optical communication networks. These all-optical techniques include modulation format conversion, phase discrimination and clock recovery. The methods detailed in this thesis use the nonlinearities associated with semiconductor optical amplifiers (SOA) to manipulate signals in the optical domain. Chapter 1 provides an introduction into the work detailed in this thesis, discusses the increased demand for capacity in today’s optical fibre networks and finally explains why all-optical signal processing may be of interest for future optical networks. Chapter 2 discusses the relevant background information required to fully understand the all-optical techniques demonstrated in this thesis. Chapter 3 details some pump-probe measurement techniques used to calculate the gain and phase recovery times of a long SOA. A remarkably fast gain recovery is observed and the wavelength dependent nature of this recovery is investigated. Chapter 4 discusses the experimental demonstration of an all-optical modulation conversion technique which can convert on-off- keyed data into either duobinary or alternative mark inversion. In Chapter 5 a novel phase sensitive frequency conversion scheme capable of extracting the two orthogonal components of a quadrature phase modulated signal into two separate frequencies is demonstrated. Chapter 6 investigates a novel all-optical clock recovery technique for phase modulated optical orthogonal frequency division multiplexing superchannels and finally Chapter 7 provides a brief conclusion.

Ultrafast coherent control and quantum encoding of molecular vibrations in D2+ using intense laser pulses

Intense, few-femtosecond pulse technology has enabled studies of the fastest vibrational relaxation processes. The hydrogen group vibrations can be imaged and manipulated using intense infrared pulses. Through numerical simulation, we demonstrate an example of ultrafast coherent control that could be effected with current experimental facilities, and observed using high-resolution time-of-flight spectroscopy. The proposal is a pump-probe-type technique to manipulate the D2+ ion with ultrashort pulse sequences. The simulations presented show that vibrational selection can be achieved through pulse delay. We find that the vibrational system can be purified to a two-level system thus realizing a vibrational qubit. A novel scheme for the selective transfer of population between these two levels, based on a Raman process and conditioned upon the delay time of a second control-pulse is outlined, and may enable quantum encoding with this system.

Attosecond phase locking of harmonics emitted from laser-produced plasmas

Laser-driven coherent extreme-ultraviolet (XUV) sources provide pulses lasting a few hundred attoseconds(1,2), enabling real-time access to dynamic changes of the electronic structure of matter(3,4), the fastest processes outside the atomic nucleus. These pulses, however, are typically rather weak. Exploiting the ultrahigh brilliance of accelerator-based XUV sources(5) and the unique time structure of their laser-based counterparts would open intriguing opportunities in ultrafast X-ray and high-field science, extending powerful nonlinear optical and pump-probe techniques towards X-ray frequencies, and paving the way towards unequalled radiation intensities. Relativistic laser-plasma interactions have been identified as a promising approach to achieve this goal(6-13). Recent experiments confirmed that relativistically driven overdense plasmas are able to convert infrared laser light into harmonic XUV radiation with unparalleled efficiency, and demonstrated the scalability of the generation technique towards hard X-rays(14-19). Here we show that the phases of the XUV harmonics emanating from the interaction processes are synchronized, and therefore enable attosecond temporal bunching. Along with the previous findings concerning energy conversion and recent advances in high-power laser technology, our experiment demonstrates the feasibility of confining unprecedented amounts of light energy to within less than one femtosecond.

Langmuir probe measurements of plasma parameters in the late stages of a laser ablated plume

A simple Langmuir probe technique has been used to measure the electron density, electron temperature, and plasma potential in the late stages (>5 mu s) of a laser ablated plasma plume. In the plasma, formed following 248 nm laser irradiation of a copper target, in vacuum at a laser fluence of 2.5 J cm(-2), electron densities of similar to 10(18) m(-3) and temperatures of similar to 0.5 eV were measured. These values are comparable with those reported previously using Faraday cup detectors and optical emission spectroscopy, respectively. (C) 1997 American Institute of Physics.