Subcycle Temporal Resolution Research Articles

Probing phonon-driven symmetry alterations in graphene via high-order-harmonic spectroscopy

High-order-harmonic spectroscopy has become an essential ingredient in probing various ultrafast electronic processes in solids with subcycle temporal resolution. Despite its immense importance, the sensitivity of high-order-harmonic spectroscopy to phonon dynamics in solids is not well known. This work addresses this critical question and demonstrates the potential of high-order-harmonic spectroscopy to probe the impact of coherent phonons on electron dynamics in solids. A pump pulse excites in-plane optical phonon modes in monolayer graphene, and a circularly polarized pulse is employed to probe the excited phonon dynamics that generates higher-order harmonics. We show that the coherent phonon dynamics alters the dynamical symmetry of graphene with the probe pulse and leads to the generation of symmetry-forbidden harmonics. Moreover, sidebands associated with the prominent harmonic peaks are generated as a result of the coherent dynamics. It is found that the symmetries and the characteristic timescale of the excited phonon mode determine the polarization and positions of these sidebands. This paper opens an avenue in time-resolved probing of phonon-driven dynamical symmetries in solids with subcycle temporal resolution.

Field-resolved THz-pump laser-probe measurements with CEP-unstable THz light sources

Radiation sources with a stable carrier-envelope phase (CEP) are highly demanded tools for field-resolved studies of light-matter interaction, providing access both to the amplitude and phase information of dynamical processes. At the same time, many coherent light sources, including those with outstanding power and spectral characteristics lack CEP stability, and so far could not be used for this type of research. In this work, we present a method enabling linear and non-linear phase-resolved terahertz (THz) -pump laser-probe experiments with CEP-unstable THz sources. THz CEP information for each pulse is extracted using a specially designed electro-optical detection scheme. The method correlates the extracted CEP value for each pulse with the THz-induced response in the parallel pump-probe experiment to obtain an absolute phase-resolved response after proper sorting and averaging. As a proof-of-concept, we demonstrate experimentally field-resolved THz time-domain spectroscopy with sub-cycle temporal resolution using the pulsed radiation of a CEP-unstable infrared free-electron laser (IR-FEL) operating at 13 MHz repetition rate. In spite of the long history of IR-FELs and their unique operational characteristics, no successful realization of CEP-stable operation has been demonstrated yet. Being CEP-unstable, IR-FEL radiation has so far only been used in non-coherent measurements without phase resolution. The technique demonstrated here is robust, operates easily at high-repetition rates and for short THz pulses, and enables common sequential field-resolved time-domain experiments. The implementation of such a technique at IR-FEL user end-stations will facilitate a new class of linear and non-linear experiments for studying coherent light-driven phenomena with increased signal-to-noise ratio.

Asymmetric double-pulse interferometric FROG for visible-wavelength time-domain spectroscopy.

To extend the detection range of time-domain spectroscopy into the challenging visible frequencies, we propose an interferometry-type frequency-resolved optical gating (FROG). Our numerical simulation shows that, when operating in a double-pulse scheme, a unique phase-locking mechanism can be activated and preserves both zero- and first-order phases (φ0, φ1)-indispensable for phase-sensitive spectroscopic study-that are otherwise inaccessible to standard FROG measurement. Followed by time-domain signal reconstruction and analysis protocol, we show that time-domain spectroscopy with sub-cycle temporal resolution is enabled and well suits the need of a ultrafast-compatible and ambiguity-free method for complex dielectric function measurement at visible wavelengths.

Probing phonon dynamics with multidimensional high harmonic carrier-envelope-phase spectroscopy

We explore pump-probe high harmonic generation (HHG) from monolayer hexagonal-boron-nitride, where a terahertz pump excites coherent optical phonons that are subsequently probed by an intense infrared pulse that drives HHG. We find, through state-of-the-art ab initio calculations, that the structure of the emission spectrum is attenuated by the presence of coherent phonons and no longer comprises discrete harmonic orders, but rather a continuous emission in the plateau region. The HHG yield strongly oscillates as a function of the pump-probe delay, corresponding to ultrafast changes in the lattice such as specific bond compression or stretching dynamics. We further show that in the regime where the excited phonon period and the pulse duration are of the same order of magnitude, the HHG process becomes sensitive to the carrier-envelope phase (CEP) of the driving field, even though the pulse duration is so long that no such sensitivity is observed in the absence of coherent phonons. The degree of CEP sensitivity versus pump-probe delay is shown to be a highly selective measure for instantaneous structural changes in the lattice, providing an approach for ultrafast multidimensional HHG spectroscopy. Remarkably, the obtained temporal resolution for phonon dynamics is ∼1 femtosecond, which is much shorter than the probe pulse duration because of the inherent subcycle contrast mechanism. Our work paves the way toward routes of probing phonons and ultrafast material structural changes with subcycle temporal resolution and provides a mechanism for controlling the HHG spectrum.

Subcycle contact-free nanoscopy of ultrafast interlayer transport in atomically thin heterostructures

Tunnelling is one of the most fundamental manifestations of quantum mechanics. The recent advent of lightwave-driven scanning tunnelling microscopy has revolutionized ultrafast nanoscience by directly resolving electron tunnelling in electrically conducting samples on the relevant ultrashort length- and timescales. Here, we introduce a complementary approach based on terahertz near-field microscopy to perform ultrafast nano-videography of tunnelling processes even in insulators. The central idea is to probe the evolution of the local polarizability of electron–hole pairs with evanescent terahertz fields, which we detect with subcycle temporal resolution. In a proof of concept, we resolve femtosecond interlayer transport in van der Waals heterobilayers and reveal pronounced variations of the local formation and annihilation of interlayer excitons on deeply subwavelength, nanometre scales. Such contact-free nanoscopy of tunnelling-induced dynamics should be universally applicable to conducting and non-conducting samples and reveal how ultrafast transport processes shape functionalities in a wide range of condensed matter systems.

Electro-optic interface for ultrasensitive intracavity electric field measurements at microwave and terahertz frequencies

Electro-optic quantum coherent interfaces map the amplitude and phase of a quantum signal directly to the phase or intensity of a probe beam. At terahertz frequencies, a fundamental challenge is not only to sense such weak signals (due to a weak coupling with a probe in the near-infrared) but also to resolve them in the time domain. Cavity confinement of both light fields can increase the interaction and achieve strong coupling. Using this approach, current realizations are limited to low microwave frequencies. Alternatively, in bulk crystals, electro-optic sampling was shown to reach quantum-level sensitivity of terahertz waves. Yet, the coupling strength was extremely weak. Here, we propose an on-chip architecture that concomitantly provides subcycle temporal resolution and an extreme sensitivity to sense terahertz intracavity fields below 20 V/m. We use guided femtosecond pulses in the near-infrared and a confinement of the terahertz wave to a volume of V T H z ∼ 10 − 9 ( λ T H z / 2 ) 3 in combination with ultraperformant organic molecules ( r 33 = 170 p m / V ) and accomplish a record-high single-photon electro-optic coupling rate of g e o = 2 π × 0.043 G H z , 10,000 times higher than in recent reports of sensing vacuum field fluctuations in bulk media. Via homodyne detection implemented directly on chip, the interaction results into an intensity modulation of the femtosecond pulses. The single-photon cooperativity is C 0 = 1.6 × 10 − 8 , and the multiphoton cooperativity is C = 0.002 at room temperature. We show > --> 70 d B dynamic range in intensity at 500 ms integration under irradiation with a weak coherent terahertz field. Similar devices could be employed in future measurements of quantum states in the terahertz at the standard quantum limit, or for entanglement of subsystems on subcycle temporal scales, such as terahertz and near-infrared quantum bits.

Probing Molecular Dynamics by Laser-Induced Backscattering Holography.

We use differential holography to overcome the forward scattering problem in strong-field photoelectron holography. Our differential holograms of H_{2} and D_{2} molecules exhibit a fishbonelike structure, which arises from the backscattered part of the recolliding photoelectron wave packet. We demonstrate that the backscattering hologram can resolve the different nuclear dynamics between H_{2} and D_{2} with subangstrom spatial and subcycle temporal resolution. In addition, we show that attosecond electron dynamics can be resolved. These results open a new avenue for ultrafast studies of molecular dynamics in small molecules.

Ultrafast Infrared Nanoscopy with Sub-Cycle Temporal Resolution

Ultrafast microscopy of surfaces with simultaneous nanometer spatial resolution and femtosecond temporal resolution can be achieved by coupling ultrafast optical pulses to sharp metal tips [1-10]. In the case of scattering-type near-field scanning optical microscopy (s-NSOM), evanescent fields scattered from the tip apex provide a window into a drastically subwavelength world. Moreover, since these scattered fields can be measured using established far-field technologies, ultrafast infrared pulses emerging from a nanoscale volume can be detected with the best possible time resolution: faster than a single optical oscillation cycle [1].

Advanced terahertz electric near-field measurements at sub-wavelength diameter metallic apertures

Using terahertz-light excitation, we have measured with sub-wavelength spatial, and sub-cycle temporal resolution the time- and frequency-dependent electric-field and surface-charge density in the vicinity of small metallic holes. In addition to a singularity like concentration of the electric field near the hole edges, we observe, that holes can act as differential operators whose near-field output is the time-derivative of the incident electric field. Our results confirm the well-known predictions made by Bouwkamp, Philips Res. Rep. 5, 321-332 (1950), and reveal, with unprecedented detail, what physically happens when light passes through a small hole.