Femtosecond Pump Pulses Research Articles

All-fiber coherent supercontinuum generation in a cascade of silica, fluoride, and chalcogenide fibers

Abstract We present an all-fiber coherent supercontinuum spanning the spectral range of 1.7–5.0 µm from a cascade of silica, ZBLAN, and chalcogenide (ChG) nonlinear fibers (NLFs). Coherence is maintained by the combined use of femtosecond pump pulses as well as by allowing deterministic spectral broadening mechanism at every stage of the cascade. The use of femtosecond pump pulses enables avoiding modulation instability (MI) at the onset of the supercontinuum generation process and thus prevent subsequent MI-seeded random noise. Once in the NLF cascade, the pump pulse is instead converted into a soliton of order maintained at N < 6 in the silica and ZBLAN NLFs, ensuring soliton fission followed by self-frequency shift of a few solitons. Finally, in the ChG NLF, spectral broadening is facilitated through self-phase modulation and dispersive wave generation. The deterministic nature of these nonlinear phenomena results in the generation of a coherent supercontinuum. The supercontinuum delivers an average power of 54 mW from an average pump power of 300 mW, yielding a power conversion efficiency of 18%. The experimental results closely align with numerical simulations, from which coherence is estimated. Such a coherent supercontinuum with a megahertz repetition rate is essential for spectroscopic systems based on optical frequency combs and applications in high-precision optical coherence tomography.

Temporal reflection from short pump pulses inside a dispersive nonlinear medium: the impact of pump parameters

We have studied, through a series of experiments and numerical simulations, how temporal reflection from an intense pump pulse inside a photonic crystal fiber is affected by parameters of the pump pulse used to form a moving high-index boundary. We used femtosecond pump pulses, which slow down inside the fiber as their spectrum red-shifts because of intrapulse Raman scattering. Temporal reflection of probe pulses occurs from such decelerating pump pulses. We changed the width and chirp of our pump pulses with a 4f pulse shaper capable of providing both spectral filtering and frequency chirping. We found that temporal refection exhibited novel features, to our knowledge, when pump pulses were made wider or chirped. In both cases, two or more reflected pulses were produced at different wavelengths in a specific range of the initial pump-probe delays. Numerical simulations reveal that the origin of such novel features is related to the complex nonlinear evolution of pump pulses inside optical fibers.

Ultrafast dynamics of exciton-polariton fluids at non-zero momenta

In this study, we have explored the ultrafast formation and decay dynamics of exciton-polariton fluids at non-zero momenta, non-resonantly excited by a small-spot femtosecond pump pulse in a ZnO microcavity. Using the femtosecond angle-resolved spectroscopic imaging technique, multidimensional dynamics in both the energy and momentum degrees of freedom have been obtained. Two distinct regions with different decay rate in the energy dimension and various decay-channels in the momentum dimension can be well-resolved. Theoretical simulations based on the generalized Gross–Pitaevskii equation can reach a qualitative agreement with the experimental observations, demonstrating the significance of the initial potential barrier induced by the pump pulse during the decay process. The finding of our study can provide additional insights into the fundamental understanding of exciton-polariton condensates, enabling further advancements for controlling the fluids and practical applications.

Quantum optical tomography based on time-resolved and mode-selective single-photon detection by femtosecond up-conversion

We developed an optical time-of-flight measurement system using a time-resolved and mode-selective up-conversion single-photon detector for acquiring tomographic images of a mouse brain. The probe and pump pulses were spectrally carved from a 100-femtosecond mode-locked fiber laser at 1556 nm using 4f systems, so that their center wavelengths were situated at either side of the phase matching band separated by 30 nm. We demonstrated a sensitivity of 111 dB which is comparable to that of shot-noise-limited optical coherence tomography and an axial resolution of 57 μm (a refractive index of 1.37) with 380 femtosecond probe and pump pulses whose average powers were 1.5 mW and 30 μW, respectively. The proposed technique will open a new way of non-contact and non-invasive three-dimensional structural imaging of biological specimens with ultraweak optical irradiation.

Selective Detection in Impulsive Low-Frequency Raman Imaging Using Shaped Probe Pulses

Impulsive stimulated Raman scattering (ISRS) using a single short femtosecond pump pulse to excite molecular vibrations offers an elegant pump-probe approach to perform vibrational imaging below $200\phantom{\rule{0.2em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. One shortcoming of ISRS is its inability to offer vibrational selectivity as all the vibrational bonds whose frequencies lie within the short pump-pulse bandwidth are excited. To date, several coherent control techniques have been explored to address this issue and selectively excite a specific molecular vibration by shaping the pump pulse. There has not been any systematic work that reports an analogous shaping of the probe pulse to implement preferential detection. In this work, we focus on vibrational imaging and report vibrational selective detection by shaping the probe pulse in time. We demonstrate numerically and experimentally two pulse-shaping strategies with one functioning as a vibrational notch filter and the other functioning as a vibrational low-pass filter. This enables fast ($25\phantom{\rule{0.2em}{0ex}}\text{\ensuremath{\mu}}\mathrm{s}/$pixel) and selective hyperspectral imaging in the low-frequency regime ($<200\phantom{\rule{0.2em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$).

Effects of initial three-dimensional electron energy distribution on terahertz Bloch oscillations in a biased semiconductor superlattice

We investigate how the initial three-dimensional energy distribution of electrons created by femtosecond pump pulses in a biased semiconductor superlattice affects terahertz Bloch oscillations, which imitate a step response to a bias electric field. The emitted terahertz waveforms are well reproduced from a damped oscillation current with capacitive nature, exhibiting shorter relaxation times and worse temporal resolutions for central pump photon energies that are outside the range of ordinary electron excitation into the conduction first miniband. This indicates that in-plane excess energy changes the relaxation time via scattering processes, while partial use of the pump pulse spectrum reduces the temporal resolution.

Mid Infrared supercontinuum generation in a silicon germanium photonic waveguide

We report simulations of pulse evolution along a 5 cm long silicon germanium (SiGe) photonic waveguide. Femtosecond laser pulses of duration 210 fs and wavelength of 4.7 µm close to the first zero dispersion wavelength (ZDW) of SiGe situated at 4.6 µm were used in pumping the SiGe photonic waveguide. Simulations were made by solving the generalised nonlinear Schrödinger equation for the femtosecond pump pulse evolution along the length of SiGe photonic waveguide using the fourth order Runge-Kutta in the interaction picture method. The simulated supercontinum spans the 2.5–8.5 µm spectral region comprising of molecular signatures for most hazardous and greenhouse gases making it attractive for environmental monitoring applications.

Effect of molecular orientation on predissociation of NaI molecules

Based on the time-depend quantum wave packet method, a scheme is proposed to investigate the effect of the molecular orientation on the predissociation of NaI molecules. The molecular orientation in the ground state is steered by THz half-cycle pulse. Then the oriented molecule is excited by femtosecond pump pulse. Molecular orientation has a significant effect on the angular distribution of wave packets. The excited wave packet is distributed in a more narrow region with the increase of molecular orientation degree. The angular distribution of dissociated products is essentially consistent with the angular distribution of excited wave packet. The dissociation probability is proportional to the excitation probability of pump pulse, which is related to the molecular orientations. Compared with the result of predissociation without molecular orientation, the maximal dissociation probability can increase by 6.5% in our work. The electric field intensity of the pump pulse also has a significant influence on dissociation probability.

Ultra-high intensity temporally oscillatory optical Kerr effect in Carbon Disulfide arising from electronic and molecular distortions

Temporal oscillatory structure of Kerr induced birefringence is revealed in Carbon Disulfide (CS2) using an intense femtosecond optical pump pulse. The optical Kerr effect using temporal gates were experimentally investigated using a 300 fs 600 nm probe and a 1200 nm pump pulses. Several input pump powers and focusing lenses were used to show how the oscillator nature of Kerr Gating scales with input pump intensity. Temporal curves were also simulated using the two primary Kerr (n2) mechanisms: the ultrafast electron cloud (n2(e)) and the slower molecular motion (n2(m)) distortions. Results reveal high level oscillatory structure in CS2 that had been previously unreported and show the influence of pulse duration on relaxation processes. The discrepancies between high intensity gates and corresponding simulated curves display the impactful role of plasma generation in Kerr processes at extreme intensities.

Buildup dynamics of room-temperature polariton condensation

By using the femtosecond angle-resolved spectroscopic imaging technique, the ultrafast buildup dynamics of room-temperature polariton condensation is explicitly visualized in a ZnO whispering gallery mode microcavity. The buildup time of polariton condensation with respect to the arrival of the femtosecond pump pulse decreases with the increasing pump power and reaches a lower limit of about 4 ps. Simulation results by numerically solving the open-dissipative Gross-Pitaevskii equation coupled to an incoherent reservoir are in quantitative agreement with the experimental observations, showing that the scattering from exciton reservoir to the lower polariton branches and the decay from these branches dominate the buildup process.

Time resolved transient transmission spectroscopy of TiCl4 and SnCl4

Herewith, for the first time, we present the vibrational spectra collected for liquid TiCl4 and liquid SnCl4 by use of time resolved transient transmission spectroscopy. Of our interest is the isotopically split isotropic ν1 intramolecular vibrational band, the shape of which is very sensitive to intermolecular interactions. The high resolution spectra, obtained as fast Fourier transforms of the time domain signals acquired in transient transmission experiment, are compared with spontaneous Raman spectra. The dependence of the spectrum shape on intermolecular interactions has been established by diluting TiCl4 and SnCl4 in CS2 at different concentrations. Fitting the simplified oscillatory model of a liquid to FFTs of time domain signals in transient transmission experiment we have found intermolecular force constants and decoherence lifetimes for all concentrations. Application of the pump–probe spectroscopic technique and windowed fast Fourier transform procedure allowed us to observe the evolution of the spectral shape, and thus of the intermolecular forces, after the liquid has been perturbed by the femtosecond pump pulse.

Femtosecond Rotational Dynamics of D_{2} Molecules in Superfluid Helium Nanodroplets.

Rotational dynamics of D_{2} molecules inside helium nanodroplets is induced by a moderately intense femtosecond pump pulse and measured as a function of time by recording the yield of HeD^{+} ions, created through strong-field dissociative ionization with a delayed femtosecond probe pulse. The yield oscillates with a period of 185fs, reflecting field-free rotational wave packet dynamics, and the oscillation persists for more than 500periods. Within the experimental uncertainty, the rotational constant B_{He} of the in-droplet D_{2} molecule, determined by Fourier analysis, is the same as B_{gas} for an isolated D_{2} molecule. Our observations show that the D_{2} molecules inside helium nanodroplets essentially rotate as free D_{2} molecules.

Time-resolved vibrational-pump visible-probe spectroscopy for thermal conductivity measurement of metal-halide perovskites.

Understanding thermal transport at the microscale to the nanoscale is crucially important for a wide range of technologies ranging from device thermal management and protection systems to thermal-energy regulation and harvesting. In the past decades, non-contact optical methods, such as time-domain and frequency-domain thermoreflectance, have emerged as extremely powerful and versatile thermal metrological techniques for the measurement of material thermal conductivities. Here, we report the measurement of thermal conductivity of thin films of CH3NH3PbI3 (MAPbI3), a prototypical metal-halide perovskite, by developing a time-resolved optical technique called vibrational-pump visible-probe (VPVP) spectroscopy. The VPVP technique relies on the direct thermal excitation of MAPbI3 by femtosecond mid-infrared optical pump pulses that are wavelength-tuned to a vibrational mode of the material, after which the time dependent optical transmittance across the visible range is probed in the ns to the μs time window using a broadband pulsed laser. Using the VPVP method, we determine the thermal conductivities of MAPbI3 thin films deposited on different substrates. The transducer-free VPVP method reported here is expected to permit spectrally resolving and spatiotemporally imaging of the dynamic lattice temperature variations in organic, polymeric, and hybrid organic-inorganic semiconductors.

Algorithm for subcycle terahertz scanning tunneling spectroscopy

Terahertz scanning tunneling microscopy (THz-STM) enables ultrafast measurements of surfaces, single molecules, and nanostructures with simultaneous subpicosecond temporal resolution and atomic spatial resolution. In pump-probe THz-STM experiments employing femtosecond optical pump pulses, lightwave-driven tunneling by a time-delayed THz probe pulse accesses the evolving differential conductance of the tunnel junction following photoexcitation. However, a general theoretical approach to extract the time- and voltage-dependent differential conductance from THz-STM measurements is lacking. Here, we introduce an algorithm for pump-probe THz scanning tunneling spectroscopy (THz-STS) analysis. Our approach allows us to reliably reconstruct the tunnel junction's differential conductance in steady-state or time-dependent scenarios from simulated THz-STS data. The algorithm achieves subcycle time resolution, which we demonstrate by retrieving dynamics faster than the bandwidth of the input THz voltage transient. Subcycle THz-STS will make lightwave-driven microscopy yet more powerful as a tool for characterizing \aa{}ngstr\"om-scale ultrafast dynamics in novel materials.

Investigation of Nonlinear Optical Properties of Quantum Dots Deposited onto a Sample Glass Using Time-Resolved Inline Digital Holography.

We report on the application of time-resolved inline digital holography in the study of the nonlinear optical properties of quantum dots deposited onto sample glass. The Fresnel diffraction patterns of the probe pulse due to noncollinear degenerate phase modulation induced by a femtosecond pump pulse were extracted from the set of inline digital holograms and analyzed. The absolute values of the nonlinear refractive index of both the sample glass substrate and the deposited layer of quantum dots were evaluated using the proposed technique. To characterize the inhomogeneous distribution of the samples’ nonlinear optical properties, we proposed plotting an optical nonlinearity map calculated as a local standard deviation of the diffraction pattern intensities induced by noncollinear degenerate phase modulation.

Rotational echo spectroscopy for accurate measurement of molecular alignment.

We measure the molecular alignment induced in gas using molecular rotational echo spectroscopy. Our results show that the echo intensity and the time interval between the local extremas of the echo responses depend sensitively on the pump intensities and the initial molecular rotational temperature, respectively. This allows us to accurately extract these experimental parameters from the echo signals and then further determine the molecular alignment in experiments. The accuracy of our method has been verified by comparing the simulation with the extracted parameters from the molecular alignment experiment performed with a femtosecond pump pulse.

Investigation of supercontinuum generation in photonic crystal fiber using bursts of femtosecond pulses

Results of experimental and numerical investigation of supercontinuum generation in polarization maintaining photonic crystal fiber using a burst of two orthogonal polarization femtosecond pump pulses are presented. The initial pump pulse source was a mode-locked Yb:KGW laser generating 52 nJ energy 90 fs duration pulses at 1033 nm with 76 MHz repetition rate. Analysis of cross-correlation frequency-resolved optical gating traces and numerical simulation results reveal that there are slight changes in supercontinuum generation when temporal delay between pump pulses in the burst is changed. Weak dependence of supercontinuum characteristics on temporal distance between the pump pulses is related to supercontinuum generation dynamics which is analyzed in detail.

Re-excitation dynamics of a “cold” charge transfer state at organic donor/acceptor interfaces

By employing a femtosecond electric pump pulse, we theoretically investigate the re-excitation dynamics of a “cold” charge transfer (CCT) state at organic donor/acceptor (D/A) interfaces. It is demonstrated that a relaxed CCT state can be pushed to different “hot” CT (HCT) states via experiencing electron (HCT1 state) and/or hole (HCT2 state) higher-energy transitions, where the transition modes and probabilities are primarily determined by the pulse energy. Without the assistance of a charge driving field, both the two HCT states relax to the initial CCT state through different internal conversion processes, whose dynamics are clearly clarified in this work. However, after a driving field is applied, we find that both of the HCT states can be dissociated into free charges before their relaxations. In particular, the HCT2 state is very easily dissociated compared to the HCT1 state, as well as the CCT state, due to the more delocalized hole charge distribution along the donor. In addition, by enhancing the pulse intensity, we can further improve the hole delocalization along the donor so that the pulsed HCT2 state is more favorable to be dissociated. This work underlines the importance of charge delocalization for the interfacial charge dynamics, including both the internal conversion and charge separation, mediated by different intermediate HCT states in organic solar cells.

Plasma-assisted temporal shifts of bichromatic femtosecond laser pulses in air

Terahertz and third-harmonic generation by tightly focused bichromatic femtosecond pump pulses with comparable input intensities in air is studied both experimentally and theoretically. Plasma-assisted temporal shifts in the field of intense laser pulses are shown to lead to the time delay between the pump pulses in the vicinity of the focus. This delay can be compensated by the initial time delay that is evidenced by the measured as well as calculated correlation functions of the fundamental and second harmonics. The possibility to characterize the plasma channel length from the correlation function is discussed.

Analysis of the active medium parameters of molecular nitrogen ions in ambient air.

In this Letter, we report the direct streak camera measurements of the duration of a lasing pulse from molecular nitrogen ions under various focusing conditions of 10 mJ, 950 nm femtosecond pump pulse in atmospheric pressure air. The parameters of the active medium are analyzed, and a mechanism for formation of picosecond lasing pulse duration at femtosecond seed pulse duration is proposed.