Generation of tunable octave-spanning mid-infrared pulses by filamentation in gas media

The continued development of femtosecond mid-infrared (IR) sources with ultrabroad spectral width is critical for probing and controlling complex molecular structural dynamics on an ultrafast timescale. We report on a sub-20 fs, coherent mid-IR source with an octave-spanning spectral bandwidth (>2000 cm(-1)) tunable from 2-8 micrometers (37.5-150 THz), with energy >0.4 μJ/pulse at 1 kHz. The mid-IR pulses are generated by four-wave mixing during the filamentation of intense 800 nm and 400 nm pulses in various gas media. Spectral tunability is achieved by the choice of gas, pressure and input 800 nm pulse energy.     

Chirped pulse amplification in single mode Tm:fiber using a chirped Bragg grating

We report femtosecond pulse generation and chirped pulse amplification in Tm:fiber. A mode-locked oscillator operating in the soliton regime produced 800 fs pulses with 5 nm spectral bandwidth, at 40 pJ pulse energy. This oscillator seeded a pre-amplifier that utilizes a Raman soliton self-frequency shift to produce wavelength tunable pulses with 3 nJ energy, reduced pulse duration of 150 fs, and increased bandwidth of 30 nm. For further amplification, the pulses were stretched up to 160 ps using a chirped Bragg grating (CBG). Stretched pulses were amplified to 85 nJ after compression in single-mode Tm:fiber and recompressed with the CBG as short as 400 fs. Compressed pulses were coupled into a highly nonlinear tellurite fiber to investigate the potential of this ultrashort pulse 2-μm fiber source as a pump for mid-IR supercontinuum generation.     

Broadband femtosecond transient infrared spectroscopy using a 256 x 256 element indium antimonide focal-plane detector

Application and characterization of large-format IR focal-plane arrays as detectors for ultrafast, high-resolution IR spectroscopy are discussed. We also present generation of broadband IR probe-reference pulses by use of collinear non-phase-matched geometry and shot-to-shot dual-track normalization to obtain transient spectra from broadly absorbing hydrogen-bonded systems. As much as 400-cm(-1)-wide coverage with 15-cm(-1) FWHM spectral resolution and +/-6.4 x 10(-4)(DOD = 3 x 10(-4)) baseline standard deviation (+/-1sigmas) is demonstrated near 2.9 microm.     

Generation of narrowband subpicosecond mid-infrared pulses via difference frequency mixing of chirped near-infrared pulses

The widely used setup for the generation of femtosecond infrared (IR) pulses based on parametric amplifiers (OPAs) and difference frequency mixing (DFM) is extended to produce tunable narrowband mid-IR pulses. The insertion of pairs of silicon prisms after the OPA induces adjustable chirp, which leads to the generation of narrowband pulses in the DFM stage. Rapid tunability of the mid-IR wavelength via a computer-controllable actuator can be achieved in a range of approximately 200 cm(-1) at a bandwidth of the IR-pulses between approximately 15 and approximately 50 cm(-1) and pulse energies up to 0.4 microJ. The narrowband mid-IR pulses are well suited for 2D IR spectroscopy.     

Mid-IR femtosecond pulse generation on the microjoule level up to 5 μm at high repetition rates

We show efficient generation of mid-IR pulses tunable between 1 and 5?μm from 100?kHz class femtosecond systems. The concept can be applied to various sources, particularly based on Ti:sapphire and the newly evolving Yb+ lasers. The mid-IR pulses are generated as the idler of a collinear optical parametric amplifier pumped by the laser fundamental. The seed for this amplifier is the idler of a previous amplification stage pumped with the second harmonic and seeded with a visible continuum. This enhances the energy and allows us to influence the bandwidth of the final output. Pulses with microjoule energy and Fourier limits of 50?fs are achieved.     

90 GW peak power few-cycle mid-infrared pulses from an optical parametric amplifier

We demonstrate a compact 20 Hz repetition-rate mid-IR OPCPA system operating at a central wavelength of 3900 nm with the tail-to-tail spectrum extending over 600 nm and delivering 8 mJ pulses that are compressed to 83 fs (<7 optical cycles). Because of the long optical period (～13 fs) and a high peak power, the system opens a range of unprecedented opportunities for tabletop ultrafast science and is particularly attractive as a driver for a highly efficient generation of ultrafast coherent x-ray continua for biomolecular and element specific imaging.     

Femtosecond high-sensitivity, chirp-free transient absorption spectroscopy using kilohertz lasers

A simple method is demonstrated for high-sensitivity, chirp-free measurements of femtosecond (fs) transient absorption over the entire bandwidth of a white-light continuum probe. This technique uses phase-sensitive detection, with spectral scanning and simultaneous adjustment of the time delay between pump and probe pulses; it permits a direct measurement of spectra undistorted by chirp at all time scales, limited only by the resolution of the fs source. The method is applied to study the ultrafast relaxation dynamics of pi-conjugated oligomers and semiconductor nanocrystals.     

Generation of ultrashort coherent vacuum ultraviolet pulses using electron storage rings: a new bright light source for experiments

We demonstrate for the first time that seeded harmonic generation on electron storage rings can produce coherent optical pulses in the vacuum ultraviolet spectral range. The experiment is performed at Elettra, where coherent pulses are generated at 132 nm, with a duration of about 100 fs. The light source has a repetition rate of 1 kHz and adjustable polarization; it is very bright, with a peak power several orders of magnitude above that of spontaneous synchrotron radiation. Owing to high stability, the source is used in a test photoemission electron microscopy experiment. We anticipate that seeded harmonic generation on storage rings can lead to unprecedented developments in time-resolved femtosecond spectroscopy and microscopy.     

Simultaneous fs pulse spectral broadening and third harmonic generation in highly nonlinear fibre: experiments and simulations

Experiments and numerical simulations are used to study non-phasematched single-mode third harmonic generation occurring simultaneously with fs pulse spectral broadening in highly nonlinear fibre. Pump pulses around 100 fs at 1560 nm injected into sub-5 cm lengths of commercially-available highly nonlinear fibre are observed to undergo spectral broadening spanning over 700 nm at the -30 dB level, and to simultaneously generate third harmonic radiation around 520 nm. Simulations based on a generalized nonlinear envelope equation are shown to well reproduce the spectral structure of the broadened pump pulses and the generated third harmonic signal. PACS 42.65.-k; 42.81.Dp     

Ultrafast intrachain photoexcitation of polymeric semiconductors

We report on excited state dynamics in isolated poly(9,9-dioctylfluorene) chains obtained by embedding the polymer in an inert plastic matrix. Early events (<300 fs) of intrachain photophysics are detected by pump-probe spectroscopy using tunable UV 25-fs pump pulses and sub-10-fs visible probe pulses. We show that higher-lying optical states, reached by multiphoton transitions, give rise to on-chain charge separation on the ultrafast time scale. The intrachain charge pair decays geminately within 500 fs to the lowest singlet state. Characteristic time scales for internal conversion and intramolecular vibrational redistribution are also determined.     

Enhancement and broadening of extreme-ultraviolet supercontinuum in a relative phase controlled two-color laser field

We experimentally demonstrate the generation of an extreme-ultraviolet (XUV) supercontinuum in argon with a two-color laser field consisting of an intense 7 fs pulse at 800 nm and a relatively weak 37 fs pulse at 400 nm. By controlling the relative time delay between the two laser pulses, we observe enhanced high-order harmonic generation as well as spectral broadening of the supercontinuum. A method to produce isolated attosecond pulses with variable width and intensity is proposed.     

High energy femtosecond OPA pumped by 1030 nm Yb:KGW laser.

We present a traveling-wave-type optical parametric amplifier (OPA) pumped at 1.03 μm by a Yb:KGW laser that produces tunable high-energy pulses of 6.5–4 μJ in the mid-infrared (mid-IR) region from 3.6 to 7 μm. Pumping with negatively chirped pulses generates nearly transform-limited (TL) mid-IR pulses of 300–330 fs length. Pumping with TL pulses of 200 fs not only decreases the output energy by a factor of 1.5, but also decreases the mid-IR pulse-length to 160 fs after additional compression. The compact and simple OPA setup is ideal for femtosecond infrared experiments in the fingerprint region.     

Generation of an isolated sub-100 attosecond pulse in the water-window spectral region

We propose a scheme to generate isolated attosecond pulses in the water-window spectral region. Based on the numerical solutions of the single active electron model, we investigate high-order harmonic generation in helium atoms driven by a multi-cycle two-colour optical field synthesized by an intense 2000 nm, 20 fs pulse and its frequency-doubled pulse. When the latter is slightly detuned and properly phase shifted with respect to the fundamental laser pulse, an ultra-broad extreme ultraviolet supercontinuum with a spectral width of 130~eV can be generated in the 270--400~eV spectral regions. A supercontinuum from 280--340~eV in the water window can be selected to yield an isolated 67 attosecond pulse without employing any phase compensation. This water window coherent x-ray pulse with less than 100 attosecond duration is a potential tool for studying the ultrafast electronic dynamics of biological samples in water.     

KTiOPO4, KTiOAsO4, and KNbO3 crystals for mid-infrared femtosecond optical parametric amplifiers: analysis and comparison

We have designed a simple mid-IR femtosecond OPA seeded by a white-light continuum and delivering very stable, largely tunable and energetic output pulses. This OPA requires fewer than 200 7J of 120-fs Ti:sapphire pump pulses as energy. This system allowed us to experimentally compare the performances of potassium crystals (KTP, KTA, and KNbO₃) for the generation of up to 100-fs Fourier-transform-limited pulses tunable in 1-4.6 7m mid-IR wavelengths.     

连续光谱飞秒光脉冲的产生

本文报道了在较低的泵浦功率密度（１０＾１０Ｗ／ｃｍ＾２）产生光谱连续覆盖（４００～８７０）ｎｍ，持续时间为８０ｆｓ，重复频率为８ｋＨｚ的高重复频率“白光”超短脉冲的实际实验系统。     

Pulse synthesis in the single-cycle regime from independent mode-locked lasers using attosecond-precision feedback

We report the synthesis of a nearly single-cycle (3.7?fs), ultrafast optical pulse train at 78?MHz from the coherent combination of a passively mode-locked Ti:sapphire laser (6?fs pulses) and a fiber supercontinuum (1-1.4?μm, with 8?fs pulses). The coherent combination is achieved via orthogonal, attosecond-precision synchronization of both pulse envelope timing and carrier envelope phase using balanced optical cross-correlation and balanced homodyne detection, respectively. The resulting pulse envelope, which is only 1.1 optical cycles in duration, is retrieved with two-dimensional spectral shearing interferometry (2DSI). To our knowledge, this work represents the first stable synthesis of few-cycle pulses from independent laser sources.     

Vacuum ultraviolet pulses of 11 fs from fifth-harmonic generation of a Ti:sapphire laser

We demonstrate that in a short Ar cell, generation of the fifth harmonic from 12 fs pulses at 810 nm directly results in ultrashort vacuum UV pulses at 162 nm. They have a spectral width of approximately 5 nm and a duration of 11+/-1 fs (1.4 times the transform limit), as measured by cross correlation with the fundamental pulses. Their energy (estimated to 4 nJ) turned out to be sufficient for use as a pump in time-resolved experiments.     

Generation of single-cycle THz transients with high electric-field amplitudes

Single-cycle terahertz (THz) transients in the frequency range 0.3-7 THz with electric-field amplitudes of more than 400 kV/cm are generated by four-wave mixing of the fundamental and the second harmonic of 25 fs pulses from a Ti:sapphire amplifier in ionized air. These transients are fully characterized by electro-optic sampling with ZnTe and GaP crystals. One can tune the center frequency of the THz transients by varying the length of the incident pulse. The electric-field amplitude increases linearly with the incident pulse energy.     

Femtosecond properties of photorefractive polymers

Photorefractive polymers allow to reversibly record holograms over a broad spectral range. This capability offers the possibility to store the information contained in ultrafast optical pulses (i.e., time domain) in the frequency domain. We demonstrate a storage bandwidth of >80 nm around 800 nm (i.e., >36 THz), giving a temporal resolution for Gaussian pulses of 13 fs at room temperature. Time reversal of a pulse train of 130 fs pulses confirms these capabilities.     

Cross-validation of theoretically quantified fiber continuum generation and absolute pulse measurement by MIIPS for a broadband coherently controlled optical source

The predicted spectral phase of a fiber continuum pulsed source rigorously quantified by the scalar generalized nonlinear Schrödinger equation is found to be in excellent agreement with that measured by multiphoton intrapulse interference phase scan (MIIPS) with background subtraction. This cross-validation confirms the absolute pulse measurement by MIIPS and the transform-limited compression of the fiber continuum pulses by the pulse shaper performing the MIIPS measurement, and permits the subsequent coherent control on the fiber continuum pulses by this pulse shaper. The combination of the fiber continuum source with the MIIPS-integrated pulse shaper produces compressed transform-limited 9.6 fs (FWHM) pulses or arbitrarily shaped pulses at a central wavelength of 1020 nm, an average power over 100 mW, and a repetition rate of 76 MHz. In comparison to the 229-fs pump laser pulses that generate the fiber continuum, the compressed pulses reflect a compression ratio of 24.