The two-dimensional IR nonlinear spectroscopy of a cyclic penta-peptide in relation to its three-dimensional structure

A form of two-dimensional (2D) vibrational spectroscopy, which uses two ultrafast IR laser pulses, is used to examine the structure of a cyclic penta-peptide in solution. Spectrally resolved cross peaks occur in the off-diagonal region of the 2D IR spectrum of the amide I region, analogous to those in 2D NMR spectroscopy. These cross peaks measure the coupling between the different amide groups in the structure. Their intensities and polarizations relate directly to the three-dimensional structure of the peptide. With the help of a model coupling Hamiltonian, supplemented by density functional calculations, the spectra of this penta-peptide can be regenerated from the known solution phase structure. This 2D-IR measurement, with an intrinsic time resolution of less than 1 ps, could be used in all time regimes of interest in biology.

The relaxation dynamics of the excited electronic states of retinal in bacteriorhodopsin by two-pump-probe femtosecond studies

We present the results of two-pump and probe femtosecond experiments designed to follow the relaxation dynamics of the lowest excited state (S1) populated by different modes. In the first mode, a direct (S0 → S1) radiative excitation of the ground state is used. In the second mode, an indirect excitation is used where the S1 state is populated by the use of two femtosecond laser pulses with different colors and delay times between them. The first pulse excites the S0 → S1 transition whereas the second pulse excites the S1 → Sn transition. The nonradiative relaxation from the Sn state populates the lowest excited state. Our results suggest that the S1 state relaxes faster when populated nonradiatively from the Sn state than when pumped directly by the S0 → S1 excitation. Additionally, the Sn → S1 nonradiative relaxation time is found to change by varying the delay time between the two pump pulses. The observed dependence of the lowest excited state population as well as its dependence on the delay between the two pump pulses are found to fit a kinetic model in which the Sn state populates a different surface (called S′1) than the one being directly excited (S1). The possible involvement of the Ag type states, the J intermediate, and the conical intersection leading to the S0 or to the isomerization product (K intermediate) are discussed in the framework of the proposed model.

Ultrafast coherent spectroscopy of the Fermi edge singularity

Paper submitted to the XVI Sitges Conference on Statistical Mechanics, Sitges, Barcelona, Spain, 7-11 June 1999.

Optical spin transfer in ferromagnetic semiconductors

Circularly polarized laser pulses that excite electron-hole pairs across the band gap of (III,Mn)V ferromagnetic semiconductors can be used to manipulate and to study collective magnetization dynamics. The initial spin orientation of a photocarrier in a (III,V) semiconductors is determined by the polarization state of the laser. We show that the photocarrier spin can be irreversibly transferred to the collective magnetization, whose dynamics can consequently be flexibly controlled by suitably chosen laser pulses. As illustrations we demonstrate the feasibility of all optical ferromagnetic resonance and optical magnetization reorientation.

Many-body quantum dynamics of polarization squeezing in optical fibers

We report new experiments that test quantum dynamical predictions of polarization squeezing for ultrashort photonic pulses in a birefringent fiber, including all relevant dissipative effects. This exponentially complex many-body problem is solved by means of a stochastic phase-space method. The squeezing is calculated and compared to experimental data, resulting in excellent quantitative agreement. From the simulations, we identify the physical limits to quantum noise reduction in optical fibers. The research represents a significant experimental test of first-principles time-domain quantum dynamics in a one-dimensional interacting Bose gas coupled to dissipative reservoirs.

Passive nonlinear pulse shaping in normally dispersive fiber

We propose a simple method for passive nonlinear optical pulse shaping that utilizes pulse prechirping and nonlinear propagation in a normally dispersive nonlinear fiber to generate various temporal waveforms of practical interest from conventional laser pulses.

Continuous-wave ultraviolet light induced fiber Bragg gratings in few- and single-mode microstructured polymer optical fibers

Reported are observations and measurements of the inscription of fibre Bragg gratings in two different types of microstructured polymer optical fibre: few-moded and endlessly single mode. Contrary to FBG inscription in silica microstructured fibre, where high energy laser pulses are a prerequisite, we have successfully used a low power CW laser source operating at 325nm to produce 1-cm long gratings with a reflection peak at 1570 nm. Peak reflectivities of more than 10% have been observed.

Strong long-period fiber gratings recorded at 352 nm

We describe long-period grating inscription in hydrogenated telecom fibers by use of high-intensity femto-second 352 nm laser pulses. We show that this technique allows us to fabricate high-quality 30 dB gratings of 300 μm period and 2 cm length by use of a three-photon absorption mechanism. © 2005 Optical Society of America.

Nonlinear diffraction in sub-critical femtosecond inscription

Material processing using high-intensity femtosecond (fs) laser pulses is a fast developing technology holding potential for direct writing of multi-dimensional optical structures in transparent media. In this work we re-examine nonlinear diffraction theory in context of fs laser processing of silica in sub-critical (input power less than the critical power of self-focusing) regime. We have applied well known theory, developed by Vlasov, Petrishev and Talanov, that gives analytical description of the evolution of a root-mean-square beam (not necessarily Gaussian) width RRMS(z) in medium with the Kerr nonlinearity.

Autosoliton propagation and mapping problem in optical fiber lines with lumped nonlinear devices

A theoretical model is developed to describe the propagation of ultrashort optical pulses in fiber transmission systems in the quasilinear regime, with periodically inserted in-line nonlinear optical devices.

Fabrication and characterisation of 45º and Ex 45º:tilted fibre gratings and their applications in fibre lasers and sensors

In this thesis, I present the studies on fabrication, spectral and polarisation characterisation of fibre gratings with tilted structures at 45º and > 45º (namely 45º- TFGs and ex 45º-TFGs throughout this thesis) and a range of novel applications with these two types of grating. One of the major contributions made in this thesis is the systematic investigation of the grating structures, inscription analysis and spectral and polarisation properties of both types of TFGs. I have inscribed 45º-TFGs in standard telecom and polarisation maintaining (PM) fibres. Two wavelength regions of interest have been explored including 1.55 µm and 1.06 µm. Detailed analysis on fabrication and characterisation of 45º-TFGs on PM fibres have also been carried out for the first time. For ex 45º- TFGs, fabrication has been investigated only on low-cost standard telecom fibre. Furthermore, thermal responses have been measured and analysed showing that both types of TFG have low responsivity to temperature change. More importantly, their refractive index (RI) responses have been characterised to verify the high responsivity to surrounding medium. Based on the unique polarisation properties, both types of TFG have been applied in fibre laser systems to improve the laser performance, which forms another major contribution of the research presented in this thesis. The integration of a 45º-TFG to the Erbium doped fibre laser (EDFL) enables single polarisation laser output at a single wavelength. When combing with ex 45º-TFGs, the EDFL can be transformed to a multi-wavelength switchable laser with single polarisation output. Furthermore, by utilising the polarisation property of the TFGs, a 45º-TFG based mode locked fibre laser is implemented. This laser can produce laser pulses at femtosecond scale and is the first application of TFG in the field of nonlinear optics. Another important contribution from the studies is the development of TFG based passive and active optical sensor systems. An ex 45º-TFG has been successfully developed into a liquid level sensor showing high sensitivity to water based solvents. Strain and twist sensors have been demonstrated via a fibre laser system using both 45°- and ex 45º-TFG with capability identifying not just the twist rate but also the direction. The sensor systems have shown the added advantage of low cost signal demodulation. In addition, load sensor applications have been demonstrated using the 45º-TFG based single polarisation EDFL and the experimental results show good agreement with the theoretical simulation.

Ultra-long mode-locked Er-droped fibre lasers

The development of ultra-long (UL) cavity (hundreds of meters to several kilometres) mode-locked fibre lasers for the generation of high-energy light pulses with relatively low (sub-megahertz) repetition rates has emerged as a new rapidly advancing area of laser physics. The first demonstration of high pulse energy laser of this type was followed by a number of publications from many research groups on long-cavity Ytterbium and Erbium lasers featuring a variety of configurations with rather different mode-locked operations. The substantial interest to this new approach is stimulated both by non-trivial underlying physics and by the potential of high pulse energy laser sources with unique parameters for a range of applications in industry, bio-medicine, metrology and telecommunications. It is well known, that pulse generation regimes in mode-locked fibre lasers are determined by the intra-cavity balance between the effects of dispersion and non-linearity, and the processes of energy attenuation and amplification. The highest per-pulse energy has been achieved in normal-dispersion UL fibre lasers mode-locked through nonlinear polarization evolution (NPE) for self-modelocking operation. In such lasers are generated the so-called dissipative optical solitons. The uncompensated net normal dispersion in long-cavity resonatorsusually leads to very high chirp and, consequently, to a relatively long duration of generated pulses. This thesis presents the results of research Er-doped ultra-long (more than 1 km cavity length) fibre lasers mode-locked based on NPE. The self-mode-locked erbium-based 3.5-km-long all-fiber laser with the 1.7 µJ pulse energy at a wavelength of 1.55 µm was developed as a part of this research. It has resulted in direct generation of short laser pulses with an ultralow repetition rate of 35.1 kHz. The laser cavity has net normal-dispersion and has been fabricated from commercially-available telecom fibers and optical-fiber elements. Its unconventional linear-ring design with compensation for polarization instability ensures high reliability of the self-mode-locking operation, despite the use of a non polarization-maintaining fibers. The single pulse generation regime in all-fibre erbium mode-locking laser based on NPE with a record cavity length of 25 km was demonstrated. Modelocked lasers with such a long cavity have never been studied before. Our result shows a feasibility of stable mode-locked operation even for an ultra-long cavity length. A new design of fibre laser cavity – “y-configuration”, that offers a range of new functionalities for optimization and stabilization of mode-locked lasing regimes was proposed. This novel cavity configuration has been successfully implemented into a long-cavity normal-dispersion self-mode-locked Er-fibre laser. In particular, it features compensation for polarization instability, suppression of ASE, reduction of pulse duration, prevention of in-cavity wave breaking, and stabilization of the lasing wavelength. This laser along with a specially designed double-pass EDFA have allowed us to demonstrate anenvironmentally stable all-fibre laser system able to deliver sub-nanosecond high-energy pulses with low level of ASE noise.

Autosoliton propagation and mapping problem in optical fiber lines with lumped nonlinear devices

A theoretical model is developed to describe the propagation of ultrashort optical pulses in fiber transmission systems in the quasilinear regime, with periodically inserted in-line nonlinear optical devices. © 2005 The American Physical Society.

Nonlinear diffraction in sub-critical femtosecond inscription

Material processing using high-intensity femtosecond (fs) laser pulses is a fast developing technology holding potential for direct writing of multi-dimensional optical structures in transparent media. In this work we re-examine nonlinear diffraction theory in context of fs laser processing of silica in sub-critical (input power less than the critical power of self-focusing) regime. We have applied well known theory, developed by Vlasov, Petrishev and Talanov, that gives analytical description of the evolution of a root-mean-square beam (not necessarily Gaussian) width RRMS(z) in medium with the Kerr nonlinearity.

Passive nonlinear pulse shaping in normally dispersive fiber

We propose a simple method for passive nonlinear optical pulse shaping that utilizes pulse prechirping and nonlinear propagation in a normally dispersive nonlinear fiber to generate various temporal waveforms of practical interest from conventional laser pulses.