A novel scheme for ultrashort terahertz pulse generation over a gapless wide spectral range: Raman-resonance-enhanced four-wave mixing.

Ultrashort energetic terahertz (THz) pulses have created an exciting new area of research on light interactions with matter. For material studies in small laboratories, widely tunable femtosecond THz pulses with peak field strength close to MV cm-1 are desired. Currently, they can be largely acquired by optical rectification and difference frequency generation in crystals without inversion symmetry. We describe in this paper a novel scheme of THz pulse generation with no frequency tuning gap based on Raman-resonance-enhanced four-wave mixing in centrosymmetric media, particularly diamond. We show that we could generate highly stable, few-cycle pulses with near-Gaussian spatial and temporal profiles and carrier frequency tunable from 5 to >20 THz. They had a stable and controllable carrier-envelop phase and carried ~15 nJ energy per pulse at 10 THz (with a peak field strength of ~1 MV cm-1 at focus) from a 0.5-mm-thick diamond. The measured THz pulse characteristics agreed well with theoretical predictions. Other merits of the scheme are discussed, including the possibility of improving the THz output energy to a much higher level.

Greater than 50 times compression of 1030 nm Yb:KGW laser pulses to single-cycle duration.

Generation of octave-spanning spectrum that spans from 570 nm to 1300 nm utilizing 1030 nm 170 fs pulses from a Yb:KGW laser and a two-stage multiple-plate arrangement is demonstrated. 3.21 fs sub-single-cycle pulses are obtained after dispersion compensation. The high compression ratio of more than 50 times is achieved for two scenarios with widely different parameters including high input peak power at 1 kHz repetition rate and modest peak power at a high repetition rate of 100 kHz. The output pulses have good spatial mode quality and exhibit long-term stability. The achieved compression ratio and flexibility are unprecedented in ultrafast pulse compression to single-cycle regime. The experiments demonstrate that the technique of multiple-plate pulse compression is versatile and applicable for a wide range of laser pulse parameters.

Sub-4 fs laser pulses at high average power and high repetition rate from an all-solid-state setup.

The generation of high average power, carrier-envelope phase (CEP) stable, near-single-cycle pulses at a repetition rate of 100 kHz is demonstrated using an all solid-state setup. By exploiting self-phase modulation in thin quartz plates and air, the spectrum of intense pulses from a high-power, high repetition rate non-collinear optical parametric chirped pulse amplifier (NOPCPA) is extended to beyond one octave, and pulse compression down to 3.7 fs is achieved. The octave-spanning spectrum furthermore allows performing straightforward f-to-2f interferometry by frequency-doubling the long-wavelength part of the spectrum. Excellent CEP-stability is demonstrated for extended periods of time. A full spatio-spectral characterization of the compressed pulses shows only minor asymmetries between the two perpendicular beam axes. We believe that the completed system represents the first laser system satisfying all requirements for performing high repetition rate attosecond pump-probe experiments with fully correlated detection of all ions and electrons produced in the experiment.

Supercontinuum generation in a multi-plate medium.

We analyze femtosecond supercontinuum generation in a distribution of thin solid plates to show that the distributed scheme inhibits processes leading to pulse breakup while allowing spectral expansion to proceed as desired. We introduce basic criteria for setting the plate thickness or initial laser intensity and the location of each plate in the laser beam path and confirm that under these conditions a fully-coherent and intense supercontinuum can be generated for input peak power of as much as two thousand times the critical power for self-focusing of the solid medium.

Generation of octave-spanning supercontinuum by Raman-assisted four-wave mixing in single-crystal diamond.

An octave-spanning coherent supercontinuum is generated by non-collinear Raman-assisted four-wave mixing in single-crystal diamond using 7.7 fs laser pulses that have been chirped to about 420 fs in duration. The use of ultrabroad bandwidth pulses as input results in substantial overlap of the generated spectrum of the anti-Stokes sidebands, creating a phase-locked supercontinuum when all the sidebands are combined to overlap in time and space. The overall bandwidth of the generated supercontinuum is sufficient to support its compression to isolated few-to-single cycle attosecond transients. The significant spectral overlap of adjacent anti-Stokes sidebands allows the utilization of straight-forward spectral interferometry to test the relative phase coherence of the anti-Stokes outputs and is demonstrated here for two adjacent pairs of sidebands. The method can subsequently be employed to set the relative phase of the sidebands for pulse compression and for the synthesis of arbitrary field transients.

Compact optical function generator.

We demonstrate the use of a nonlinear photonic crystal to generate a harmonic comb and an ultrabroad-band acousto-optic modulator for the field amplitudes and phases of the comb to succeed in synthesizing femtosecond and subfemtosecond optical field waveforms. Nonsinusoidal fields of various shapes are synthesized and verified using shaper-assisted linear cross-correlation. The compact all-solid-state system could lead to the realization of a portable arbitrary optical waveform synthesizer that is analogous in many aspects to an RF function generator.

Non-invasive characterization of the domain boundary and structure properties of periodically poled ferroelectrics.

Shaping the ferroelectric domains as waveguide, grating, lens, and prism are key to the successful penetration of periodically-poled ferroelectrics on various wavelength conversion applications. The complicated structures are, however, difficult to be fully characterized, especially the unexpected index contrast at the anti-parallel domain boundaries are typical in the order of 10(-4) or less. An ultrahigh resolution optical coherence tomography was employed to fully characterize the domain boundary and structure properties of a periodically-poled lithium niobate (PPLN) waveguide with an axial resolution of 0.68 µm, an transversal resolution of 3.2 µm, and an index contrast sensitivity of 4x10(-7). The anti-parallel domain uniformity can clearly be seen non-invasively. Dispersion of the ferroelectric material was also obtained from 500 to 750 nm.

Synthesis and measurement of ultrafast waveforms from five discrete optical harmonics.

Achieving the control of light fields in a manner similar in sophistication to the control of electromagnetic fields in the microwave and radiofrequency regimes has been a major challenge in optical physics research. We manipulated the phase and amplitude of five discrete harmonics spanning the blue to mid-infrared frequencies to produce instantaneous optical fields in the shape of square, sawtooth, and subcycle sine and cosine pulses at a repetition rate of 125 terahertz. Furthermore, we developed an all-optical shaper-assisted linear cross-correlation technique to retrieve these fields and thereby verified their shapes and confirmed the critical role of carrier-envelope phase in Fourier synthesis of optical waveforms.

Upconversion blue laser by intracavity frequency self-doubling of periodically poled lithium tantalate parametric oscillator.

We report a design for upconversion 435 nm blue lasers based on simultaneously fulfilling the nonlinear processes of optical parametric oscillation (OPO) and second-harmonic generation (SHG) in a 7.9 mum periodically poled lithium tantalate (PPLT). The uncoated 15-mm-long PPLT device exhibits a low threshold of 150 mW and a differential slope efficiency of 22.6%, rendering 56 mW blue generation when pumped by a pulsed 532 nm green laser with an average power rating of 400 mW. These observations were attributed to a quasi-phase-matching (QPM) structural design with a 75% domain duty cycle to ensure the concurrence of frequency doubling with the first-order QPM-OPO PPLT device via the second-order QPM-SHG process.

Generation of multi-octave-spanning laser harmonics by cascaded quasi-phase matching in a monolithic ferroelectric crystal.

We report the generation of the second to the sixth harmonics of a fundamental frequency covering two and a half octaves in a multiply-periodically poled lithium tantalate crystal by cascaded quasi-phase-matched frequency mixing. A frequency comb that is composed of these harmonics will permit the synthesis of a train of periodic subcycle subfemtosecond pulses in a compact setting.

Arbitrary waveform synthesis by multiple harmonics generation and phasing in aperiodic optical superlattices.

The process of generating periodic optical waveforms includes the generation and phasing of several harmonics of a fundamental frequency. In this work, we show that simultaneous generation and phasing of the harmonics can be performed in a monolithic aperiodic optical superlattice (AOS). Stable periodic waveforms can thus be delivered to a predetermined location by simply sending a laser beam through a properly designed and fabricated AOS crystal. A detailed mathematical description for generating the domain pattern in such an AOS crystal is given and the process is numerically demonstrated. The waveform that is generated from a monolithic AOS is highly reproducible and phase stable. We also use propagation in air as an example to show how any predictable phase and amplitude modifications such as air dispersion that will alter the desired waveform can be pre-compensated in the design phase of the AOS crystal.

Controlling the carrier-envelope phase of Raman-generated periodic waveforms.

We demonstrate control of the carrier-envelope phase of ultrashort periodic waveforms that are synthesized from a Raman-generated optical frequency comb. We generated the comb by adiabatically driving a molecular vibrational coherence with a beam at a fundamental frequency plus its second harmonic. Heterodyne measurements show that full interpulse phase locking of the comb components is realized. The results set the stage for the synthesis of periodic arbitrary waveforms in the femtosecond and subfemtosecond regimes with full control.

Substantial gain enhancement for optical parametric amplification and oscillation in two-dimensional chi(2) nonlinear photonic crystals.

We have analyzed optical parametric interaction in a 2D NPC. While in general the nonlinear coefficient is small compared to a 1D NPC, we show that at numerous orientations a multitude of reciprocal vectors contribute additively to enhance the gain in optical parametric amplification and oscillation in a 2D patterned crystal. In particular, we have derived the effective nonlinear coefficients for common-signal amplification and common-idler amplification for a tetragonal inverted domain pattern. We show that in the specific case of signal amplification with QPM by both G(10) and G(11), symmetry of the crystal results in coupled interaction with the corresponding signal amplification by G(10) and G(1,-1). As a consequence, this coupled utilization of all three reciprocal vectors leads to a substantial increase in parametric gain. Using PPLN we demonstrate numerically that a gain that comes close to that of a 1D QPM crystal could be realized in a 2D NPC with an inverted tetragonal domain pattern. This special mechanism produces two pairs of identical signal and idler beams propagating in mirror-imaged forward directions. In conjunction with this gain enhancement and multiple beams output we predict that there is a large pulling effect on the output wavelength due to dynamic signal build-up in the intrinsic noncollinear geometry of a 2D NPC OPO.

Sub-single-cycle optical pulse train with constant carrier envelope phase.

We describe the synthesis of periodic waveforms consisting of a train of pulses that are 0.83 cycles long and have an electric field pulse width of 0.44 fs using 7 Raman sidebands generated by molecular modulation in H2. We verify by optical correlation that the carrier-envelope phase is constant in these waveforms when they are synthesized from commensurate sidebands. The estimated overall shift of the carrier-envelope phase is less than 0.18 cycles from the first to the last pulse of nearly 10(6) pulses in the pulse train.

Broadly tunable ultraviolet light generation in a compact MgO-doped periodically-poled stoichiometric lithium tantalate optical parametric oscillator with a high-Q cavity.

A compact tunable UV laser source based on intracavity sum frequency generation in a MgO-doped periodically-poled stoichiometric lithium tantalate optical parametric oscillator is reported. UV output at an approximately 1 mW level of power over the range of 364 to 378 nm with a bandwidth of 0.5 nm was obtained with a crystal that has just one periodically-poled grating period. The full tuning range can be as much as approximately 68 nm, from 324 to 392 nm by varying the crystal temperature from room temperature to 250 degrees C. This will cover nearly the entire UVA range.

Optical interference in nonlinear photonic crystals.

A model to analyze the interaction of the parametric fields being generated in a two-dimensional nonlinear photonic crystal has been developed. The analysis provides details of the interference of the generated wave(s) both inside and in the region just outside the crystal. The results are verified by second-harmonic generation in a LiNbO3 crystal that has been poled with a tetragonal inverted domain structure.

Green-pumped high-power optical parametric oscillator based on periodically poled MgO-doped stoichiometric LiTaO3.

A high-power 532 nm-pumped multikilohertz nanosecond optical parametric oscillator using a periodically poled 1.0 mol.% MgO-doped stoichiometric lithium tantalate crystal that could be operated from room temperature to 200 degrees C without damage is reported. A broad continuous tuning range from 855 to 1410 nm was achieved within a single domain period. Efficient operation of high peak power and watt level average power with a power conversion of 62.5% was measured. These results show that a high-resolution high average power visible tunable source can be realized.

Dissociation of heme from gaseous myoglobin ions studied by infrared multiphoton dissociation spectroscopy and Fourier-transform ion cyclotron resonance mass spectrometry.

Detachment of heme prosthetic groups from gaseous myoglobin ions has been studied by collision-induced dissociation and infrared multiphoton dissociation in combination with Fourier-transform ion cyclotron resonance mass spectrometry. Multiply charged holomyoglobin ions (hMbn+) were generated by electrospray ionization and transferred to an ion cyclotron resonance cell, where the ions of interest were isolated and fragmented by either collision with Ar atoms or irradiation with 3 mum photons, producing apomyoglobin ions (aMbn+). Both charged heme loss (with [Fe(III)-heme]+ and aMb(n-1)+ as the products) and neutral heme loss (with [Fe(II)-heme] and aMbn+ as the products) were detected concurrently for hMbn+ produced from a myoglobin solution pretreated with reducing reagents. By reference to Ea = 0.9 eV determined by blackbody infrared radiative dissociation for charged heme loss of ferric hMbn+, an activation energy of 1.1 eV was deduced for neutral heme loss of ferrous hMbn+ with n = 9 and 10.

Multipass acoustically open photoacoustic detector for trace gas measurements.

What we believe to be a novel multipass, acoustically open photoacoustic detector designed for fast-response, high-sensitivity detection of trace gases and pollutants in the atmosphere is demonstrated. The acoustic pulses generated by the absorption of the light pulses of a tunable optical parametric oscillator by target molecules are detected by an ultrasonic sensor at 40 kHz. The photoacoustic signal is enhanced by an optical multipass arrangement and by concentration of the acoustic energy to the surface of the ultrasonic sensor. The detection sensitivity, estimated from CO2 measurements around a 2 microm wavelength, is approximately 3.3 x 10(-9) W cm(-1).