Sub-cycle Time Resolution Research Articles

Ultra-Nonlinear Subcycle Photoemission of Few-Electron States from Sharp Gold Nanotapers.

The generation of ultrashort electron wavepackets is crucial for the development of ultrafast electron microscopes. Recent studies on Coulomb-correlated few-electron number states, photoemitted from sharp metallic tapers, have shown emission nonlinearities in the multiphoton photoemission regime which scale with the electron number. Here, we study few-electron photoemission from gold nanotapers triggered by few-cycle near-infrared pulses, demonstrating extreme 20th-order nonlinearities for electron triplets. We report interferometric autocorrelation traces of the electron yield that are quenched to a single emission peak with subfemtosecond duration due to these high nonlinearities. The modulation of the emission yield by the carrier-envelope phase suggests that electron emission predominantly occurs during a single half cycle of the driving laser field. When applying a bias voltage to the tip, recollisions in the electron trajectories are suppressed and coherent subcycle electron beams are generated with promising prospects for ultrafast electron microscopy with subcycle time resolution.

Phase-resolved measurement and control of ultrafast dynamics in terahertz electronic oscillators

As a key component for next-generation wireless communications (6 G and beyond), terahertz (THz) electronic oscillators are being actively developed. Precise and dynamic phase control of ultrafast THz waveforms is essential for high-speed beam steering and high-capacity data transmission. However, measurement and control of such ultrafast dynamic process is beyond the scope of electronics due to the limited bandwidth of the electronic equipment. Here we surpass this limit by applying photonic technology. Using a femtosecond laser, we generate offset-free THz pulses to phase-lock the electronic oscillators based on resonant tunneling diode. This enables us to perform phase-resolved measurement of the emitted THz electric field waveform in time-domain with sub-cycle time resolution. Ultrafast dynamic response such as anti-phase locking behaviour is observed, which is distinct from in-phase stimulated emission observed in laser oscillators. We also show that the dynamics follows the universal synchronization theory for limit cycle oscillators. This provides a basic guideline for dynamic phase control of THz electronic oscillators, enabling many key performance indicators to be achieved in the new era of 6 G and beyond.

Field-resolved space–time characterization of few-cycle structured light pulses

Accompanied by the rapid development of ultrafast laser platforms in recent decades, the spatiotemporal manipulation of ultrashort laser pulses has attracted much attention due to the potential for cutting-edge applications of structured light, including optical tweezers, optical communications, super-resolution imaging, time-resolved spectroscopy in molecules and quantum materials, and strong-field physics. Today, techniques capable of characterizing the full spatial, temporal, and polarization state properties of structured light are strongly desired. Here, we demonstrate a technique, termed 3D TIPTOE, for characterizing structured mid-infrared waveforms, which uses only a two-dimensional silicon-based image sensor as both the detector and the nonlinear medium. By combining the advantages of the sub-cycle time resolution afforded by nonlinear excitation and the spatial resolution inherent to the two-dimensional sensor, the 3D TIPTOE technique allows full characterization of structured electric fields, significantly reducing the complexity of detection compared to other techniques. The validity of the technique is established by measuring both few-cycle Bessel–Gaussian pulses and radially polarized femtosecond vector beams.

Build-up and dephasing of Floquet-Bloch bands on subcycle timescales.

Strong light fields have created opportunities to tailor novel functionalities of solids1-5. Floquet-Bloch states can form under periodic driving of electrons and enable exotic quantum phases6-15. On subcycle timescales, lightwaves can simultaneously drive intraband currents16-29 and interband transitions18,19,30,31, which enable high-harmonic generation16,18,19,21,22,25,28-30 and pave the way towards ultrafast electronics. Yet, the interplay of intraband and interband excitations and their relation to Floquet physics have been key open questions as dynamical aspects of Floquet states have remained elusive. Here we provide this link by visualizing the ultrafast build-up of Floquet-Bloch bands with time-resolved and angle-resolved photoemission spectroscopy. We drive surface states on a topological insulator32,33 with mid-infrared fields-strong enough for high-harmonic generation-and directly monitor the transient band structure with subcycle time resolution. Starting with strong intraband currents, we observe how Floquet sidebands emerge within a single optical cycle; intraband acceleration simultaneously proceeds in multiple sidebands until high-energy electrons scatter into bulk states and dissipation destroys the Floquet bands. Quantum non-equilibrium calculations explain the simultaneous occurrence of Floquet states with intraband and interband dynamics. Our joint experiment and theory study provides a direct time-domain view of Floquet physics and explores the fundamental frontiers of ultrafast band-structure engineering.

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.

Generation of 5.2 fs, energy scalable blue pulses.

In this Letter, ultrashort blue pulses spanning 350-500 nm are generated by combining the broadband frequency doubling technology with the two-stage multiplate continuum (MPC) generation scheme. We prepare relatively broadband input pulses and use a two-stage configuration for MPC generation, allowing us to employ thinner and less solid plates for further spectral broadening. Therefore, the deteriorations of the spectral phase, energy conversion efficiency, and beam quality, which occur more easily for 400 nm pulses, are effectively suppressed. After fine dispersion management, we obtain clean 5.2 fs blue pulses with a root-mean-square energy stability of 0.69% over one hour and excellent beam quality. Furthermore, lower than 8% energy loss during the spectral broadening process at each stage is achieved. The overall optimized performances and energy scalability of this blue pulse, as well as the possibility of further compressing the pulse duration, are likely to motivate more strong-field research with sub-cycle time resolution in this extended wavelength range.

Clocking Dissociative Above-Threshold Double Ionization of H_{2} in a Multicycle Laser Pulse.

The dissociative above-threshold double ionization (ATDI) of H_{2} in strong laser fields involves the sequential releasing of two electrons at specific instants with the stretching of the molecular bond. By mapping the releasing instants of two electrons to their emission directions in a multicycle polarization-skewed femtosecond laser pulse, we experimentally clock the dissociative ATDI of H_{2} via distinct photon-number-resolved pathways, which are distinguished in the kinetic energy release spectrum of two protons measured in coincidence. The timings of the experimentally resolved dissociative ATDI pathways are in good accordance with the classical predictions. Our results verify the multiphoton scenario of the dissociative ATDI of H_{2} in both time and energy fashion, strengthening the understanding of the strong-field phenomenon and providing a robust tool with a subcycle time resolution to clock abundant ultrafast dynamics of molecules.

Terahertz Scanning Tunneling Microscopy for Visualizing Ultrafast Electron Motion in Nanoscale Potential Variations

Studying the microscopic behavior of free carriers in materials at an ultrashort time scale is critical to developing semiconductor, optoelectronic, and other technologies satisfying the ever-increasing requirements for smaller sizes and higher speeds. Understanding the effect of local potential modulations and localized states due to nanoscale microstructures on carrier dynamics is essential to realize these requirements. Here, we used time-resolved scanning tunneling microscopy/spectroscopy (STM/STS) combined with a carrier-envelope phase (CEP)-controlled subcycle THz electric field, THz-STM, to probe the ultrafast motion of electrons photoinjected into C60 multilayer structures grown on Au substrate. We have succeeded in demonstrating the time-resolved measurement of ultrafast electron dynamics with sub-nanoscale spatial resolution and subcycle time resolution for the first time and successfully visualized the electron motion triggered by the spatial variation in the lowest unoccupied molecular orbital (LUMO). The difference in the effects of molecular defects, such as a molecular vacancy and orientational disorder, was also clearly distinguished with single-molecular-level spatial resolution. This method is expected to play an important role in the precise evaluation of local electronic structures and dynamics for the future development of new functional materials and device elements.

Sub-cycle time resolution of multi-photon momentum transfer in strong-field ionization

During multi-photon ionization of an atom it is well understood how the involved photons transfer their energy to the ion and the photoelectron. However, the transfer of the photon linear momentum is still not fully understood. Here, we present a time-resolved measurement of linear momentum transfer along the laser pulse propagation direction. We can show that the linear momentum transfer to the photoelectron depends on the ionization time within the laser cycle using the attoclock technique. We can mostly explain the measured linear momentum transfer within a classical model for a free electron in a laser field. However, corrections are required due to the parent-ion interaction and due to the initial momentum when the electron enters the continuum. The parent-ion interaction induces a negative attosecond time delay between the appearance in the continuum of the electron with minimal linear momentum transfer and the point in time with maximum ionization rate.

Temporal evolution of electron density and temperature in low pressure transient Ar/N2 plasmas estimated by optical emission spectroscopy

A recently published method for the analysis of phase-resolved optical emission spectra was extended in order to permit estimation of time-resolved electron density profiles. The previously presented method combined collisional-radiative modelling with a self-absorption method to estimate the evolution of Te with sub-cycle time-resolution. However, it was not capable to give similar profiles for ne as the model was insensitive to its variations. The extensions proposed in this work describe a way to also estimate the electron density with sub-cycle time resolution from the changing rates of the argon Paschen 1s states. The method was applied to a low-pressure DBD-jet operated with argon and several argon–nitrogen mixtures with up to 4% N2. Good agreement among evaluation of ne from changing rates of individual 1s states was observed during the collisional phase and the full-cycle temporal profile could be calculated from relative changes in light emission. Electron densities exhibited a drop for larger admixtures of nitrogen and ranged from 1017 m−3 to 1018 m−3. As assumed in a previous work, the electron temperature model worked without explicit consideration of additional processes even when N2 affected the plasma. However, presumably due to collisional quenching by nitrogen, two argon Paschen 2p levels were found to be inappropriate for Te estimation and had to be removed. Values for electron temperature from the remaining levels remained at a similar value as for pure argon.

Ultrafast transition between exciton phases in van der Waals heterostructures.

Heterostructures of atomically thin van der Waals bonded monolayers have opened a unique platform to engineer Coulomb correlations, shaping excitonic1-3, Mott insulating4 or superconducting phases5,6. In transition metal dichalcogenide heterostructures7, electrons and holes residing in different monolayers can bind into spatially indirect excitons1,3,8-11 with a strong potential for optoelectronics11,12, valleytronics1,3,13, Bose condensation14, superfluidity14,15 and moiré-induced nanodot lattices16. Yet these ideas require a microscopic understanding of the formation, dissociation and thermalization dynamics of correlations including ultrafast phase transitions. Here we introduce a direct ultrafast access to Coulomb correlations between monolayers, where phase-locked mid-infrared pulses allow us to measure the binding energy of interlayer excitons in WSe2/WS2 hetero-bilayers by revealing a novel 1s-2p resonance, explained by a fully quantum mechanical model. Furthermore, we trace, with subcycle time resolution, the transformation of an exciton gas photogenerated in the WSe2 layer directly into interlayer excitons. Depending on the stacking angle, intra- and interlayer species coexist on picosecond scales and the 1s-2p resonance becomes renormalized. Our work provides a direct measurement of the binding energy of interlayer excitons and opens the possibility to trace and control correlations in novel artificial materials.

Subcycle observation of lightwave-driven Dirac currents in a topological surface band.

Harnessing the carrier wave of light as an alternating-current bias may enable electronics at optical clock rates1. Lightwave-driven currents have been assumed to be essential for high-harmonic generation in solids2-6, charge transport in nanostructures7,8, attosecond-streaking experiments9-16 and atomic-resolution ultrafast microscopy17,18. However, in conventional semiconductors and dielectrics, the finite effective mass and ultrafast scattering of electrons limit their ballistic excursion and velocity. The Dirac-like, quasi-relativistic band structure of topological insulators19-29 may allow these constraints to be lifted and may thus open a new era of lightwave electronics. To understand the associated, complex motion of electrons, comprehensive experimental access to carrier-wave-driven currents is crucial. Here we report angle-resolved photoemission spectroscopy with subcycle time resolution that enables us to observe directly how the carrier wave of a terahertz light pulse accelerates Dirac fermions in the band structure of the topological surface state of Bi2Te3. While terahertz streaking of photoemitted electrons traces the electromagnetic field at the surface, the acceleration of Dirac states leads to a strong redistribution of electrons in momentum space. The inertia-free surface currents are protected by spin-momentum locking and reach peak densities as large as two amps per centimetre, with ballistic mean free paths of several hundreds of nanometres, opening up a realistic parameter space for all-coherent lightwave-driven electronic devices. Furthermore, our subcycle-resolution analysis of the band structure may greatly improve our understanding of electron dynamics and strong-field interaction in solids.

Attosecond transient absorption spectrum of argon at the L2,3 edge

Progress in high-harmonic generation has led to high-energy attosecond pulses with cutoff above the carbon $1s$ edge (283.8 eV). These pulses are essential to extend time-resolved spectroscopies to the water window in order to control electron dynamics in solvated organic species. Here we report a step towards this goal: the measurement, with subcycle time resolution, of the attosecond transient absorption spectrum of argon at the $2{p}^{\ensuremath{-}1} {L}_{2,3}$ edge ($\ensuremath{\sim}250$ eV) in the presence of a short-wave infrared control pulse. The measurements, supported by theoretical simulations, demonstrate the concurrent role of Auger decay and tunnel ionization in the driven evolution of inner-valence holes of polyelectronic atoms.

Fast time-resolved electrostatic force microscopy: Achieving sub-cycle time resolution.

The ability to measure microsecond- and nanosecond-scale local dynamics below the diffraction limit with widely available atomic force microscopy hardware would enable new scientific studies in fields ranging from biology to semiconductor physics. However, commercially available scanning-probe instruments typically offer the ability to measure dynamics only on time scales of milliseconds to seconds. Here, we describe in detail the implementation of fast time-resolved electrostatic force microscopy using an oscillating cantilever as a means to measure fast local dynamics following a perturbation to a sample. We show how the phase of the oscillating cantilever relative to the perturbation event is critical to achieving reliable sub-cycle time resolution. We explore how noise affects the achievable time resolution and present empirical guidelines for reducing noise and optimizing experimental parameters. Specifically, we show that reducing the noise on the cantilever by using photothermal excitation instead of piezoacoustic excitation further improves time resolution. We demonstrate the discrimination of signal rise times with time constants as fast as 10 ns, and simultaneous data acquisition and analysis for dramatically improved image acquisition times.

Detection of subfemtosecond transients by means of nonlinear Raman scattering

Ultrafast transient processes are shown to qualitatively modify the nonlinear-optical response of a Raman-active medium. Fast processes with phase relaxation times shorter than the laser field cycle T 0 = 2π/ω, where ω is the carrier frequency of the laser field, can be detected via modulation of the dipole moment at the frequency 2ω. This modulation is observed in the nonlinear-optical response of the medium against a background of a conventional, Raman part of the signal. Nonlinear Raman scattering can thus help to record ultrafast transients with a subcycle time resolution.

Sampling a terahertz dipole transition with subcycle time resolution

We present a time-resolved technique to measure optical excitation processes with a time resolution shorter than the oscillation period of the exciting light. Our terahertz (THz) experiments fully resolve the polarization dynamics of electrons in semiconductor heterostructures when they are excited by a THz pulse. The time resolution of the polarization enables us to deduce the population dynamics of the excited state, which includes the dynamics of a virtual population in the case of off-resonant excitation.