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Christian Heide

Publications and source records attributed to Christian Heide.

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Nonresonant optomechanical control of structural phases

Optical tweezers demonstrate how light can exert forces to trap, repel, and manipulate microscopic particles without absorption. Recent theory has suggested that such forces can extend beyond particle manipulation to drive structural phase transitions in solids. Here we apply this optomechanical principle to tin selenide (SnSe), a material where proximity to several different structural phases gives rise to its high thermoelectric figure of merit and makes it a candidate for a switchable topological crystalline insulator. Whereas the force for standard optical tweezers arises from a gradient in the intensity of a light field, the optomechanical force is mediated by a gradient in the dielectric constant as a function of phonon coordinate. Unlike conventional methods that rely on resonant excitation and absorption through the imaginary part of the dielectric function, this approach operates dispersively through the real part and can be directly driven by Raman processes, enabling selective transitions with reduced energy cost and ultrafast response. Using time-domain Raman scattering, we show that above a critical mid-infrared field strength the $A_g$ Raman modes disappear abruptly without softening, signaling the formation of a new structural phase. This phase, distinct from those induced by heating or carrier excitation, exhibits large-amplitude and long-lived modulations in its optical response. Complementing this observation, we show also evidence for an equivalent DC-field-driven structural phase transformation to a higher symmetry phase, as observed by atom probe tomography. Our study demonstrates the concept of nonresonant optomechanical phase control and defines novel opportunities for synthesizing hidden structural phases with unique functional properties.

physics.optics

Nonresonant Raman control of ferroelectric polarization

Important advances have recently been made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light-matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes has been experimentally observed and proposed for dynamic material control, but the resulting atomic excursion has been limited to perturbative levels. Here, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds.

physics.optics

Attosecond vortices in semiconductor materials

We present the first theoretical results on the generation of short-wavelength attosecond vortex beams in semiconductors through their interactions with an intense Laguerre-Gauss beam, in the limit where non-perturbative high-order harmonics are generated. We exploit the details of the novel microscopic mechanism for high-order harmonic generation (HHG) in condensed matter, such as the use of dephasing time included in semiconductor Bloch equations (SBE), the combination of the SBE model with the thin slab model, and the use of experimentally verified scaling laws for various harmonic orders. For our test, we use a zinc oxide crystal as our standard sample, and our vortex beam is characterized by a topological charge of $l=1$. Our time-domain analysis shows that harmonics within the plateau region specifically contribute to the generation of the attosecond vortex beam. Our findings have implications for advancing the understanding of solid-state HHG and leveraging its strengths, such as the use of thin and dense media, for the efficient generation of short-wavelength attosecond vortex beams.

physics.atom-ph

Optical control of electrons in a Floquet topological insulator

Light-dressed materials hold enormous potential for generating new electronic properties. The band structure resulting from light-dressing can exhibit starkly different quantum and topological phenomena. So far, optical control of charge within a light-dressed band structure has been elusive. Here, we demonstrate optical control of electrons in light-dressed graphene. By focusing circularly polarized femtosecond laser pulses at 1550 nm on monolayer graphene, we generate a Floquet topological insulator (FTI). With a phase-locked second harmonic field, we dynamically control electrons in this FTI state. For the first time, we observe photocurrent circular dichroism, the all-optical anomalous Hall effect, and FTI valley-polarized currents. The photocurrents show strong sub-cycle phase-sensitivity, opening the door to ultrafast control within topologically protected electronics (topotronics), spectroscopy, and attosecond physics in novel quantum materials.

physics.optics

Strong-Field Bloch Electron Interferometry for Band Structure Retrieval

When Bloch electrons in a solid are exposed to a strong optical field, they are coherently driven in their respective bands where they acquire a quantum phase as the imprint of the band shape. If an electron approaches an avoided crossing formed by two bands, it may be split by undergoing a Landau-Zener transition. We here employ subsequent Landau-Zener transitions to realize strong-field Bloch electron interferometry (SFBEI), allowing us to reveal band structure information. In particular, we measure the Fermi velocity (band slope) of graphene in the vicinity of the K points as (1.07$\pm$0.04) nm fs$^{-1}$. We expect SFBEI for band structure retrieval to apply to a wide range of material systems and experimental conditions, making it suitable for studying transient changes in band structure with femtosecond temporal resolution at ambient conditions.

physics.optics

Giant room-temperature nonlinearities from a monolayer Janus topological semiconductor

Nonlinear optical materials possess wide applications, ranging from terahertz and mid-infrared detection to energy harvesting. Recently, the correlations between nonlinear optical responses and topological properties, such as Berry curvature and the quantum metric tensor, have stimulated great interest. Here, we report giant room-temperature nonlinearities in an emergent non-centrosymmetric two-dimensional topological material, the Janus transition metal dichalcogenides in the 1T' phase, which are synthesized by an advanced atomic-layer substitution method. High harmonic generation, terahertz emission spectroscopy, and second harmonic generation measurements consistently reveal orders-of-the-magnitude enhancement in terahertz-frequency nonlinearities of 1T' MoSSe (e.g., > 50 times higher than 2H MoS$_2$ for 18th order harmonic generation; > 20 times higher than 2H MoS$_2$ for terahertz emission). It is elucidated that such colossal nonlinear optical responses come from topological band mixing and strong inversion symmetry breaking due to the Janus structure. Our work defines general protocols for designing materials with large nonlinearities and preludes the applications of topological materials in optoelectronics down to the monolayer limit. This two-dimensional form of topological materials also constitute a unique platform for examining origin of the anomalous high-harmonic generation, with potential applications as building blocks for scalable attosecond sources.

cond-mat.mes-hall

High-harmonic generation from artificially stacked 2D crystals

We report a coherent layer-by-layer high-order harmonic generation (HHG) build-up in artificially stacked transition metal dichalcogenides (TMDC) crystals in their various stacking configurations. In the experiments, millimeter-sized single crystalline monolayers are synthesized using the gold foil-exfoliation method, followed by artificially stacking on a transparent substrate. High-order harmonics up to the 19th order are generated by the interaction with an ultrafast mid-infrared (MIR) driving laser. We find that the generation is sensitive to the number of layers and their relative orientation. For AAAA stacking configuration, both odd- and even-orders exhibit a quadratic increase in intensity as a function of the number of layers, which is a signature of constructive interference of high-harmonic emission from successive layers. Particularly, we observe some deviations from this scaling at photon energies above the bandgap, which is explained by self-absorption effects. For AB and ABAB stacking, even-order harmonics remain below the detection level, consistent with the presence of inversion symmetry. Our study confirms the capability of producing non-perturbative high-order harmonics from stacked layered materials subjected to intense MIR fields without damaging samples. It has implications for optimizing solid-state HHG sources at the nano-scale and developing high-harmonics as an ultrafast probe of artificially stacked layered materials. Because the HHG process is a strong-field driven process, it has the potential to probe high-momentum and energy states in the bandstructure combined with atomic-scale sensitivity in real space, making it an attractive probe of novel material structures such as the Moiré pattern.

physics.optics

Floquet engineering of strongly-driven excitons in monolayer tungsten disulfide

Interactions of quantum materials with strong-laser fields can induce exotic nonequilibrium electronic states. Monolayer transition-metal dichalcogenides, a new class of direct-gap semiconductors with prominent quantum confinement, offer exceptional opportunities toward Floquet engineering of quasiparticle electron-hole states, or excitons. Strong-field driving has a potential to achieve enhanced control of electronic band structure, thus a possibility to open a new realm of exciton light-matter interactions. However, experimental implementation of strongly-driven excitons has so far remained out of reach. Here, we use mid-infrared laser pulses below the optical bandgap to excite monolayer tungsten disulfide up to a field strength of 0.3 V/nm, and demonstrate strong-field light dressing of excitons in the excess of a hundred millielectronvolt. Our high-sensitivity transient absorption spectroscopy further reveals formation of a virtual absorption feature below the 1s-exciton resonance, which is assigned to a light-dressed sideband from the dark 2p-exciton state. Quantum-mechanical simulations substantiate the experimental results and enable us to retrieve real-space movies of the exciton dynamics. This study advances our understanding of the exciton dynamics in the strong-field regime, and showcases the possibility of harnessing ultrafast, strong-field phenomena in device applications of two-dimensional materials.

cond-mat.mtrl-sci

Light-field control of real and virtual charge carriers

Light-driven electronic excitation is a cornerstone for energy and information transfer. In the interaction of intense and ultrafast light fields with solids, electrons may be excited irreversibly, or transiently during illumination only. As the transient electron population cannot be observed after the light pulse is gone it is referred to as virtual, while the population remaining excited is called real. Virtual charge carriers have recently been associated with high-harmonic generation and transient absorption, while photocurrent generation may stem from real as well as virtual charge carriers. Yet, a link between the carrier types in their generation and importance for observables up to technological relevance is missing. Here we show that real and virtual carriers can be excited and disentangled in the optical generation of currents in a gold-graphene-gold heterostructure using few-cycle laser pulses. Depending on the waveform used for photoexcitation, real carriers receive net momentum and propagate to the gold electrodes, while virtual carriers generate a polarization response read out at the gold-graphene interfaces. Based on these insights, we further demonstrate a proof of concept of a logic gate for future lightwave electronics. Our results offer a direct means to monitor and excite real and virtual charge carriers. Individual control over each type will dramatically increase the integrated circuit design space and bring closer to reality petahertz signal processing.

physics.optics

Probing Electron-Hole Coherence in Strongly-Driven Solids

High-harmonic generation (HHG) is a coherent optical process in which the incident photon energy is up-converted to the multiples of its initial energy. In solids, under the influence of a strong laser field, electron-hole (e-h) pairs are generated and subsequently driven to high energy and momentum within a fraction of the optical cycle. These dynamics encode the band structure, including non-trivial topological properties of the source material, through both intraband current and interband polarization, into the high harmonic spectrum. In the course of this process, dephasing between the driven electron and the hole can significantly reduce the HHG efficiency. Here, we exploit this feature and turn it into a measurement of e-h coherence in strongly driven solids. Utilizing a pre-pump pulse, we first photodope monolayer molybdenum disulfide and then examine the HHG induced by an intense infrared pulse. We observe clear suppression of the HH intensity, which becomes more pronounced with increasing order. Based on quantum simulations, we attribute this monotonic order dependence as a signature of ultrafast electron-hole dephasing, which leads to an exponential decay of the inter-band polarization, proportional to the sub-cycle excursion time of the e-h pair. Our results demonstrate the importance of many-body effects, such as density-dependent decoherence in HHG and provide a novel platform to probe electron-hole coherence in strongly driven systems.

physics.optics

Electronic coherence and coherent dephasing in the optical control of electrons in graphene

Electronic coherence is of utmost importance for the access and control of quantum-mechanical solid-state properties. Using a purely electronic observable, the photocurrent, we measure an electronic coherence time of 22 +/- 4 fs in graphene. The photocurrent is ideally suited to measure electronic coherence as it is a direct result of quantum path interference, controlled by the delay between two ultrashort two-color laser pulses. The maximum delay for which interference between the population amplitude injected by the first pulse interferes with that generated by the second pulse determines the electronic coherence time. In particular, numerical simulations reveal that the experimental data yield a lower boundary on the electronic coherence time and that coherent dephasing masks a lower coherence time. We expect that our results will significantly advance the understanding of coherent quantum-control in solid-state systems ranging from excitation with weak fields to strongly driven systems.

cond-mat.mes-hall

Adiabaticity parameters for the categorization of light-matter interaction -- from weak to strong driving

We investigate theoretically and numerically the light-matter interaction in a two-level system (TLS) as a model system for excitation in a solid-state band structure. We identify five clearly distinct excitation regimes, categorized with well-known adiabaticity parameters: (1) the perturbative multiphoton absorption regime for small driving field strengths, and four light field-driven regimes, where intraband motion connects different TLS: (2) the impulsive Landau-Zener (LZ) regime, (3) the non-impulsive LZ regime, (4) the adiabatic regime and (5) the adiabatic-impulsive regime for large electric field strengths. This categorization is tremendously helpful to understand the highly complex excitation dynamics in any TLS, in particular when the driving field strength varies, and naturally connects Rabi physics with Landau-Zener physics. In addition, we find an insightful analytical expression for the photon orders connecting the perturbative multiphoton regime with the light field-driven regimes. Moreover, in the adiabatic-impulsive regime, adiabatic motion and impulsive LZ transitions are equally important, leading to an inversion symmetry breaking of the TLS when applying few-cycle laser pulses. This categorization allows a deep understanding of driven TLS in a large variety of settings ranging from cold atoms and molecules to solids and qubits, and will help to find optimal driving parameters for a given purpose.

quant-ph

Sub-cycle temporal evolution of light-induced electron dynamics in hexagonal 2D materials

Two-dimensional materials with hexagonal symmetry such as graphene and transition metal dichalcogenides} are unique materials to study light-field-controlled electron dynamics inside of a solid. Around the $K$-point, the dispersion relation represents an ideal system to study intricately coupled intraband motion and interband (Landau-Zener) transitions driven by the optical field of phase-controlled few-cycle laser pulses. Based on the coupled nature of the intraband and interband processes, we have recently observed in graphene repeated coherent Landau-Zener transitions between valence and conduction band separated by around half an optical period of ~1.3 fs [Higuchi et al., Nature 550, 224 (2017)]. Due to the low temporal symmetry of the applied laser pulse, a residual current density and a net electron polarization are formed. Here we show extended numerical data on the temporal evolution of the conduction band population of 2D materials with hexagonal symmetry during the light-matter interaction, yielding deep insights to attosecond-fast electron dynamics. In addition, we show that a residual ballistic current density is formed, which strongly increases when a band gap is introduced. Both, the sub-cycle electron dynamics and the resulting residual current are relevant for the fundamental understanding and future applications of strongly driven electrons in two-dimensional materials, including graphene or transition metal dichalcogenide monolayers.

physics.optics

Attosecond-fast internal photoemission

The photoelectric effect has a sister process relevant in optoelectronics called internal photoemission. Here an electron is photoemitted from a metal into a semiconductor. While the photoelectric effect takes place within less than 100 attoseconds, the attosecond time scale has so far not been measured for internal photoemission. Based on the new method CHArge transfer time MEasurement via Laser pulse duration-dependent saturation fluEnce determinatiON, CHAMELEON, we show that the atomically thin semi-metal graphene coupled to bulk silicon carbide, forming a Schottky junction, allows charge transfer times as fast as (300 $\pm$ 200) attoseconds. These results are supported by a simple quantum mechanical model simulation. With the obtained cut-off bandwidth of 3.3 PHz for the charge transfer rate, this semimetal-semiconductor interface represents the first functional solid-state interface offering the speed and design space required for future light-wave signal processing.

physics.app-ph

CEP-stable soliton-based pulse compression to 4.4 fs and UV generation at 800 kHz repetition rate

We report generation of a femtosecond supercontinuum extending from the ultraviolet to the near-infrared and detection of its carrier-envelope phase variation by f-to-2f interferometry. The spectrum is generated in a gas-filled hollow-core photonic crystal fiber where soliton dynamics allows CEP-stable self-compression of OPCPA pump pulses at 800 nm to a duration of 1.7 optical cycles, followed by dispersive wave emission. The source provides up to 1 μJ of pulse energy at 800 kHz repetition rate resulting in 0.8 W of average power, and can be extremely useful for example in strong-field physics, pump-probe measurements and ultraviolet frequency comb metrology.

physics.optics

Interaction of carrier envelope phase-stable laser pulses with graphene: the transition from the weak-field to the strong-field regime

Ultrafast control of electron dynamics in solid state systems has recently found particular attention. By increasing the electric field strength of laser pulses, the light-matter interaction in solids might turn from a perturbative into a novel non-perturbative regime, where interband transitions from the valence to the conduction band become strongly affected by intraband motion. We have demonstrated experimentally and numerically that this combined dynamics can be controlled in graphene with the electric field waveform of phase-stabilized few-cycle laser pulses. Here we show new experimental data and matching simulation results at comparably low optical fields, which allows us to focus on the highly interesting transition regime where the light-matter interaction turns from perturbative to non-perturbative. We find a 5th order power-law scaling of the laser induced waveform-dependent current at low optical fields, which breaks down for higher optical fields, indicating the transition.

physics.optics

Coherent electron trajectory control in graphene

We investigate coherent electron dynamics in graphene, interacting with the electric field waveform of two orthogonally polarized, few-cycle laser pulses. Recently, we demonstrated that linearly polarized driving pulses lead to sub-optical-cycle Landau-Zener quantum path interference by virtue of the combination of intraband motion and interband transition [Higuchi $\textit{et al.}$, Nature $\textbf{550}$, 224 (2017)]. Here we introduce a pulsed control laser beam, orthogonally polarized to the driving pulses, and observe the ensuing electron dynamics. The relative delay between the two pulses is a tuning parameter to control the electron trajectory, now in a complex fashion exploring the full two-dimensional reciprocal space in graphene. Depending on the relative phase, the electron trajectory in the reciprocal space can, for example, be deformed to suppress the quantum path interference resulting from the driving laser pulse. Intriguingly, this strong-field-based complex matter wave manipulation in a two-dimensional conductor is driven by a high repetition rate \textit{laser oscillator}, rendering unnecessary complex and expensive amplified laser systems.

cond-mat.mes-hall

Light-field driven currents in graphene

Ultrafast electron dynamics in solids under strong optical fields has recently found particular attention. In dielectrics and semiconductors, various light-field-driven effects have been explored, such as high-harmonic generation, sub-optical-cycle interband population transfer and nonperturbative increase of transient polarizability. In contrast, much less is known about field-driven electron dynamics in metals because charge carriers screen an external electric field in ordinary metals. Here we show that atomically thin monolayer Graphene offers unique opportunities to study light-field-driven processes in a metal. With a comparably modest field strength of up to 0.3 V/Å, we drive combined interband and intraband electron dynamics, leading to a light-field-waveform controlled residual conduction current after the laser pulse is gone. We identify the underlying pivotal physical mechanism as electron quantum-path interference taking place on the 1-femtosecond ($10^{-15}$ second) timescale. The process can be categorized as Landau-Zener-Stückelberg interferometry. These fully coherent electron dynamics in graphene take place on a hitherto unexplored timescale faster than electron-electron scattering (tens of femtoseconds) and electron-phonon scattering (hundreds of femtoseconds). These results broaden the scope of light-field control of electrons in solids to an entirely new and eminently important material class -- metals -- promising wide ramifications for band structure tomography and light-field-driven electronics.

physics.optics