Gouy phase effects on photocurrents in plasmonic nanogaps driven by single-cycle pulses.

The investigation of optical phenomena in the strong-field regime requires few-cycle laser pulses at field strengths exceeding gigavolts per meter (GV/m). Surprisingly, such conditions can be reached by tightly focusing pJ-level pulses with nearly octave spanning optical bandwidth onto plasmonic nanostructures, exploiting the field-enhancement effect. In this situation, the Gouy phase of the focused beam can deviate significantly from the monochromatic scenario. Here, we study the effect of the Gouy phase of a pulse exploited to drive coherent strong-field photocurrents within a plasmonic gap nanoantenna. While the influence of the specific Gouy phase profile in the experiment approaches the monochromatic case closely, this scheme may be utilized to identify more intricate phase profiles at sub-diffraction scale. Our results pave the way for Gouy phase engineering at picojoule (pJ) pulse energy levels, enabling the optimization of strong-field optical phenomena.

Controlling intracavity dual-comb soliton motion in a single-fiber laser.

Ultrafast science builds on dynamic compositions of precisely timed light pulses, and evolving groups of pulses are observed in almost every mode-locked laser. However, the underlying physics has rarely been controlled or used until now. Here, we demonstrate a general approach to control soliton motion inside a dual-comb laser and the programmable synthesis of ultrashort pulse patterns. Introducing single-pulse modulation inside an Er:fiber laser, we rapidly shift the timing between two temporally separated soliton combs. Their superposition outside the cavity yields ultrashort soliton sequences. On the basis of real-time spectral interferometry, we observe the deterministic switching of intersoliton separation arising from the interplay of attracting and repulsing forces via ultrafast nonlinearity and laser gain dynamics. Harnessing these insights, we demonstrate the high-speed all-optical synthesis of nano- to picosecond pump-probe delays and programmable free-form soliton trajectories. This concept may pave the way to a new class of all-optical delay generators for ultrafast measurements at unprecedented high tuning, cycling, and acquisition speeds.

Electric-Field Fluctuations as the Cause of Spectral Instabilities in Colloidal Quantum Dots.

Spectral diffusion (SD) represents a substantial obstacle toward implementation of solid-state quantum emitters as a source of indistinguishable photons. By performing high-resolution emission spectroscopy for individual colloidal quantum dots at cryogenic temperatures, we prove the causal link between the quantum-confined Stark effect and SD. Statistically analyzing the wavelength of emitted photons, we show that increasing the sensitivity of the transition energy to an applied electric field results in amplified spectral fluctuations. This relation is quantitatively fit to a straightforward model, indicating the presence of a stochastic electric field on a microscopic scale, whose standard deviation is 9 kV/cm, on average. The current method will enable the study of SD in multiple types of quantum emitters such as solid-state defects or organic lead halide perovskite quantum dots, for which spectral instability is a critical barrier for applications in quantum sensing.

Quantitative Ultrafast Magnetoacoustics at Magnetic Metasurfaces.

Femtosecond (fs) time-resolved magneto-optics is applied to investigate laser-excited ultrafast dynamics of one-dimensional nickel gratings on fused silica and silicon substrates for a wide range of periodicities Λ = 400-1500 nm. Multiple surface acoustic modes with frequencies up to a few tens of GHz are generated. Nanoscale acoustic wavelengths Λ/n have been identified as nth-spatial harmonics of Rayleigh surface acoustic wave (SAW) and surface skimming longitudinal wave (SSLW), with acoustic frequencies and lifetimes being in agreement with theoretical calculations. Resonant magnetoelastic excitation of the ferromagnetic resonance (FMR) by SAW's third spatial harmonic, and, most interestingly fingerprints of the parametric resonance at 1/2 SAW frequency have been observed. Numerical solutions of Landau-Lifshitz-Gilbert (LLG) equation magnetoelastically driven by complex polychromatic acoustic fields quantitatively reproduce all resonances at once. Thus, our results provide a solid experimental and theoretical base for a quantitative understanding of ultrafast fs-laser-driven magnetoacoustics and tailoring the magnetic-grating-based metasurfaces at the nanoscale.

Dissection of DNA damage and repair pathways in live cells by femtosecond laser microirradiation and free-electron modeling.

Understanding and predicting the outcome of the interaction of light with DNA has a significant impact on the study of DNA repair and radiotherapy. We report on a combination of femtosecond pulsed laser microirradiation at different wavelengths, quantitative imaging, and numerical modeling that yields a comprehensive picture of photon-mediated and free-electron-mediated DNA damage pathways in live cells. Laser irradiation was performed under highly standardized conditions at four wavelengths between 515 nm and 1,030 nm, enabling to study two-photon photochemical and free-electron-mediated DNA damage in situ. We quantitatively assessed cyclobutane pyrimidine dimer (CPD) and γH2AX-specific immunofluorescence signals to calibrate the damage threshold dose at these wavelengths and performed a comparative analysis of the recruitment of DNA repair factors xeroderma pigmentosum complementation group C (XPC) and Nijmegen breakage syndrome 1 (Nbs1). Our results show that two-photon-induced photochemical CPD generation dominates at 515 nm, while electron-mediated damage dominates at wavelengths ≥620 nm. The recruitment analysis revealed a cross talk between nucleotide excision and homologous recombination DNA repair pathways at 515 nm. Numerical simulations predicted electron densities and electron energy spectra, which govern the yield functions of a variety of direct electron-mediated DNA damage pathways and of indirect damage by •OH radicals resulting from laser and electron interactions with water. Combining these data with information on free electron-DNA interactions gained in artificial systems, we provide a conceptual framework for the interpretation of the wavelength dependence of laser-induced DNA damage that may guide the selection of irradiation parameters in studies and applications that require the selective induction of DNA lesions.

Tracing attosecond electron emission from a nanometric metal tip.

Solids exposed to intense electric fields release electrons through tunnelling. This fundamental quantum process lies at the heart of various applications, ranging from high brightness electron sources in d.c. operation1,2 to petahertz vacuum electronics in laser-driven operation3-8. In the latter process, the electron wavepacket undergoes semiclassical dynamics9,10 in the strong oscillating laser field, similar to strong-field and attosecond physics in the gas phase11,12. There, the subcycle electron dynamics has been determined with a stunning precision of tens of attoseconds13-15, but at solids the quantum dynamics including the emission time window has so far not been measured. Here we show that two-colour modulation spectroscopy of backscattering electrons16 uncovers the suboptical-cycle strong-field emission dynamics from nanostructures, with attosecond precision. In our experiment, photoelectron spectra of electrons emitted from a sharp metallic tip are measured as function of the relative phase between the two colours. Projecting the solution of the time-dependent Schrödinger equation onto classical trajectories relates phase-dependent signatures in the spectra to the emission dynamics and yields an emission duration of 710 ± 30 attoseconds by matching the quantum model to the experiment. Our results open the door to the quantitative timing and precise active control of strong-field photoemission from solid state and other systems and have direct ramifications for diverse fields such as ultrafast electron sources17, quantum degeneracy studies and sub-Poissonian electron beams18-21, nanoplasmonics22 and petahertz electronics23.

Passively phase-locked Er:fiber source of single-cycle pulses in the near infrared with electro-optic timing modulation for field-resolved electron control.

A single-cycle light source in the near infrared is demonstrated enabling sensitive applications of ultrafast optical field control of electronic transport. The compact Er:fiber system generates passively phase-locked pulses with broadband spectra covering 150 THz to 350 THz at a duration of 4.2 fs and 40 MHz repetition rate. A second output arm is equipped with an electro-optic modulator (EOM) that switches the arrival time of the pulses by 700 ps at arbitrary frequencies up to 20 MHz, enabling timing modulation of the pump pulse without changing the average intensity. As a benchmark demonstration, we investigate the carrier relaxation dynamics in low-temperature-grown InGaAs (LT-InGaAs) using quantum interference currents (QuICs).

Ultrabroadband suppression of mid-infrared reflection losses of a layered semiconductor by nanopatterning with a focused ion beam.

Moth-eye structures are patterned onto gallium selenide surfaces with sub-micrometer precision. In this way, Fresnel reflection losses are suppressed to below one percent within an ultrabroad optical bandwidth from 15 to 65 THz. We tune the geometry by rigorous coupled-wave analysis. Subsequently, ablation with a Ga+ ion beam serves to write optimized structures in areas covering 30 by 30 µm. The benefits are demonstrated via optical rectification of femtosecond laser pulses under tight focusing, resulting in emission of phase-stable transients in the mid-infrared. We analyze the performance of antireflection coating directly in the time domain by ultrabroadband electro-optic sampling.

Low-field onset of Wannier-Stark localization in a polycrystalline hybrid organic inorganic perovskite.

Methylammonium lead iodide perovskite (MAPbI3) is renowned for an impressive power conversion efficiency rise and cost-effective fabrication for photovoltaics. In this work, we demonstrate that polycrystalline MAPbI3s undergo drastic changes in optical properties at moderate field strengths with an ultrafast response time, via transient Wannier Stark localization. The distinct band structure of this material - the large lattice periodicity, the narrow electronic energy bandwidths, and the coincidence of these two along the same high-symmetry direction - enables relatively weak fields to bring this material into the Wannier Stark regime. Its polycrystalline nature is not detrimental to the optical switching performance of the material, since the least dispersive direction of the band structure dominates the contribution to the optical response, which favors low-cost fabrication. Together with the outstanding photophysical properties of MAPbI3, this finding highlights the great potential of this material in ultrafast light modulation and novel photonic applications.

Ultrafast Control of Magnetic Anisotropy by Resonant Excitation of 4f Electrons and Phonons in Sm_{0.7}Er_{0.3}FeO_{3}.

We compare the ultrafast dynamics of the spin reorientation transition in the orthoferrite Sm_{0.7}Er_{0.3}FeO_{3} following two different pumping mechanisms. Intense few-cycle pulses in the midinfrared selectively excite either the f-f electronic transition of Sm^{3+} or optical phonons. With phonon pumping, a finite time delay exists for the spin reorientation, reflecting the energy transfer between the lattice and 4f system. In contrast, an instantaneous response is found for resonant f-f excitation. This suggests that 4f electronic pumping can directly alter the magnetic anisotropy due to the modification of 4f-3d exchange at femtosecond timescales, without involving lattice thermalization.

Passive elimination of correlated amplitude fluctuations in ultrabroadband supercontinua from highly nonlinear fibers by three-wave mixing.

The nonlinear transformation of fluctuations by frequency broadening is found to produce strong anti-correlations in the spectral output. This effect is investigated by dispersive Fourier transform measurements. We exploit the anti-correlations in order to cancel the intensity noise in a subsequent sum-frequency mixing step. This principle allows for the generation of tunable visible pulses by cascaded nonlinear mixing whilst maintaining the same intensity noise performance as the input pulses. In addition, we demonstrate that the power fluctuations occurring in the process of passive stabilization of the carrier-envelope phase locking via difference frequency generation may be cancelled by an analogous strategy.

Up to 70 THz bandwidth from an implanted Ge photoconductive antenna excited by a femtosecond Er:fibre laser.

Phase-stable electromagnetic pulses in the THz frequency range offer several unique capabilities in time-resolved spectroscopy. However, the diversity of their application is limited by the covered spectral bandwidth. In particular, the upper frequency limit of photoconductive emitters - the most widespread technique in THz spectroscopy - reaches only up to 7 THz in the regular transmission mode due to absorption by infrared-active optical phonons. Here, we present ultrabroadband (extending up to 70 THz) THz emission from an Au-implanted Ge emitter that is compatible with mode-locked fibre lasers operating at wavelengths of 1.1 and 1.55 µm with pulse repetition rates of 10 and 20 MHz, respectively. This result opens up the possibility for the development of compact THz photonic devices operating up to multi-THz frequencies that are compatible with Si CMOS technology.

Dynamics of electron-emission currents in plasmonic gaps induced by strong fields.

The dynamics of ultrafast electron currents triggered by femtosecond laser pulse irradiation of narrow gaps in a plasmonic dimer is studied using quantum mechanical Time-Dependent Density Functional Theory (TDDFT). The electrons are injected into the gap due to the optical field emission from the surfaces of the metal nanoparticles across the junction. Further evolution of the electron currents in the gap is governed by the locally enhanced electric fields. The combination of TDDFT and classical modelling of the electron trajectories allows us to study the quiver motion of the electrons in the gap region as a function of the Carrier Envelope Phase (CEP) of the incident pulse. In particular, we demonstrate the role of the quiver motion in establishing the CEP-sensitive net electric transport between nanoparticles.

Plasmonic mid-infrared third harmonic generation in germanium nanoantennas.

We demonstrate third harmonic generation in plasmonic antennas consisting of highly doped germanium grown on silicon substrates and designed to be resonant in the mid-infrared frequency range that is inaccessible with conventional nonlinear plasmonic materials. Owing to the near-field enhancement, the result is an ultrafast, subdiffraction, coherent light source with a wavelength tunable between 3 and 5 µm, and ideally overlapping with the fingerprint region of molecular vibrations. To observe the nonlinearity in this challenging spectral window, a high-power femtosecond laser system equipped with parametric frequency conversion in combination with an all-reflective confocal microscope setup is employed. We demonstrate spatially resolved maps of the linear scattering cross section and the nonlinear emission of single isolated antenna structures. A clear third-order power dependence as well as mid-infrared emission spectra prove the nonlinear nature of the light emission. Simulations support the observed resonance length of the double-rod antenna and demonstrate that the field enhancement inside the antenna material is responsible for the nonlinear frequency mixing.

Highly standardized multicolor femtosecond fiber system for selective microphotomanipulation of deoxyribonucleic acid and chromatin.

We present a three-color femtosecond Er/Yb:fiber laser enabling highly specific and standardized nonlinear optical manipulation of live cells. The system simultaneously provides bandwidth-limited 80-fs pulses with identical intensity envelope centered at wavelengths of 515, 775, and 1035 nm in the focus of a confocal microscope. We achieve this goal by combining high-order dispersion control via, for example, chirped fiber Bragg gratings with proper bandwidth management in each nonlinear conversion step. Wavelength-selective and noninterfering induction of deoxyribonucleic acid (DNA) photoproducts and DNA strand breaks, as well as fluorescence photoactivation of a photoactivatable green fluorescent protein (PA-GFP)-histone fusion protein, are demonstrated. The capability to introduce different types of DNA lesions and perform photoswitching experiments in a selective manner is essential for quantitative studies on DNA repair and chromatin dynamics.

Coherent field transients below 15 THz from phase-matched difference frequency generation in 4H-SiC.

We experimentally demonstrate tunable, phase-matched difference frequency generation covering the spectral region below 15 THz using 4H-SiC as a nonlinear crystal. This material combines a non-centrosymmetric lattice and strong birefringence with broadband transparency at low optical frequencies. Thorough refractive index measurements in the terahertz spectral range allow us to calculate phase-matching conditions for any near-infrared pump laser source. 4H-SiC is also exploited as a detector crystal for electro-optic sampling. The results allow us to estimate the effective second-order nonlinear coefficient.

Ultrabroadband out-of-loop characterization of the carrier-envelope phase noise of an offset-free Er:fiber frequency comb.

Recent demonstrations of passively phase-locked fiber-based combs motivate broadband characterization of the noise associated with the stabilized carrier-envelope offset frequency. In our study, we analyze the phase noise of a 100 MHz Er:fiber system in a wide range spanning from microhertz to the Nyquist frequency. An interferometric detection method enables analysis of the high-frequency output of an f-to-2f interferometer. The dominant contribution of a broadband white noise floor at high frequencies attests quantum-limited performance. An out-of-loop measurement of the carrier-envelope phase reveals its jitter to be as low as 250 mrad when integrated over 12 orders of magnitude of the radio-frequency spectrum.

Multicolor lasers using birefringent filters: experimental demonstration with Cr:Nd:GSGG and Cr:LiSAF.

In this study, we numerically and experimentally investigate application of birefringent filters (BRFs) as frequency selective elements in multicolor lasers. A BRF plate made out of crystalline quartz with an arbitrarily oriented optical axis has been explored. Simulation results have shown that compared to regular BRFs where the optical axis lies in the plane of the plates surface, a BRF with an optical axis pointing out of its surface enables design flexibility in filter parameters, providing access to a wider set of free spectral range and bandwidth values. As a result, multicolor operation could be obtained in many wavelength pairs using a single BRF plate. In the experiments a 3-mm thick quartz BRF with an optical axis 45° to the surface plane has been used. With Cr:Nd:GSGG as a laser medium two-color and three-color cw laser operation has been demonstrated in 11 and 3 different transition combinations, respectively. Moreover, two-color laser operation has been demonstrated in 10 different wavelength pairs in Cr:LiSAF. To our knowledge, this study is the first detailed investigation and experimental demonstration of BRFs with tilted optical axis for multicolor operation of solid-state lasers. Compared to other methods, BRFs enable a rich selection of transition pairs and also the ratio of the power in each line could be regulated by fine adjustment of the rotation angle. Implementation of tilted-axis BRFs should boost development of efficient and low-cost multicolor lasers in other gain media as well.

Coupling of Excitons and Discrete Acoustic Phonons in Vibrationally Isolated Quantum Emitters.

The photoluminescence emission by mesoscopic condensed matter is ultimately dictated by the fine-structure splitting of the fundamental exciton into optically allowed and dipole-forbidden states. In epitaxially grown semiconductor quantum dots, nonradiative equilibration between the fine-structure levels is mediated by bulk acoustic phonons, resulting in asymmetric spectral broadening of the excitonic luminescence. In isolated colloidal quantum dots, spatial confinement of the vibrational motion is expected to give rise to an interplay between the quantized electronic and phononic degrees of freedom. In most cases, however, zero-dimensional colloidal nanocrystals are strongly coupled to the substrate such that the charge relaxation processes are still effectively governed by the bulk properties. Here we show that encapsulation of single colloidal CdSe/CdS nanocrystals into individual organic polymer shells allows for systematic vibrational decoupling of the semiconductor nanospheres from the surroundings. In contrast to epitaxially grown quantum dots, simultaneous quantization of both electronic and vibrational degrees of freedom results in a series of strong and narrow acoustic phonon sidebands observed in the photoluminescence. Furthermore, an individual analysis of more than 200 compound particles reveals that enhancement or suppression of the radiative properties of the fundamental exciton is controlled by the interaction between fine-structure states via the discrete vibrational modes. For the first time, pronounced resonances in the scattering rate between the fine-structure states are directly observed, in good agreement with a quantum mechanical model. The unambiguous assignment of mediating acoustic modes to the observed scattering resonances complements the experimental findings. Thus, our results form an attractive basis for future studies on subterahertz quantum opto-mechanics and efficient laser cooling at the nanoscale.

Optical Activation of Germanium Plasmonic Antennas in the Mid-Infrared.

Impulsive interband excitation with femtosecond near-infrared pulses establishes a plasma response in intrinsic germanium structures fabricated on a silicon substrate. This direct approach activates the plasmonic resonance of the Ge structures and enables their use as optical antennas up to the mid-infrared spectral range. The optical switching lasts for hundreds of picoseconds until charge recombination redshifts the plasma frequency. The full behavior of the structures is modeled by the electrodynamic response established by an electron-hole plasma in a regular array of antennas.