arXiv subjects

I. Gierz

Publications and source records attributed to I. Gierz.

14 recordsLinked to original sources

arXiv2021

On the survival of Floquet-Bloch states in the presence of scattering

Floquet theory has spawned many exciting possibilities for electronic structure control with light with enormous potential for future applications. The experimental realization in solids, however, largely remains pending. In particular, the influence of scattering on the formation of Floquet-Bloch states remains poorly understood. Here we combine time- and angle-resolved photoemission spectroscopy with time-dependent density functional theory and a two-level model with relaxation to investigate the survival of Floquet-Bloch states in the presence of scattering. We find that Floquet-Bloch states will be destroyed if scattering -- activated by electronic excitations -- prevents the Bloch electrons from following the driving field coherently. The two-level model also shows that Floquet-Bloch states reappear at high field intensities where energy exchange with the driving field dominates over energy dissipation to the bath. Our results clearly indicate the importance of long scattering times combined with strong driving fields for the successful realization of various Floquet phenomena.

cond-mat.mtrl-sci↗

arXiv2020

Microscopic understanding of ultrafast charge transfer in van-der-Waals heterostructures

Van-der-Waals heterostructures show many intriguing phenomena including ultrafast charge separation following strong excitonic absorption in the visible spectral range. However, despite the enormous potential for future applications in the field of optoelectronics, the underlying microscopic mechanism remains controversial. Here we use time- and angle-resolved photoemission spectroscopy combined with microscopic many-particle theory to reveal the relevant microscopic charge transfer channels in epitaxial WS$_2$/graphene heterostructures. We find that the timescale for efficient ultrafast charge separation in the material is determined by direct tunneling at those points in the Brillouin zone where WS$_2$ and graphene bands cross, while the lifetime of the charge separated transient state is set by defect-assisted tunneling through localized sulphur vacanices. The subtle interplay of intrinsic and defect-related charge transfer channels revealed in the present work can be exploited for the design of highly efficient light harvesting and detecting devices.

cond-mat.mes-hall↗

arXiv2020

Floquet states in dissipative open quantum systems

We theoretically investigate basic properties of nonequilibrium steady states of periodically-driven open quantum systems based on the full solution of the Maxwell-Bloch equation. In a resonantly driving condition, we find that the transverse relaxation, also known as decoherence, significantly destructs the formation of Floquet states while the longitudinal relaxation does not directly affect it. Furthermore, by evaluating the quasienergy spectrum of the nonequilibrium steady states, we demonstrate that the Rabi splitting can be observed as long as the decoherence time is as short as one third of the Rabi-cycle. Moreover, we find that Floquet states can be formed even under significant dissipation when the decoherence time is substantially shorter than the cycle of driving, once the driving field strength becomes strong enough. In an off-resonant condition, we demonstrate that the Floquet states can be realized even in weak field regimes because the system is not excited and the decoherence mechanism is not activated. Once the field strength becomes strong enough, the system can be excited by nonlinear processes and the decoherence process becomes active. As a result, the Floquet states are significantly disturbed by the environment even in the off-resonant condition. Thus, we show here that the suppression of heating is a key condition for the realization of Floquet states in both on and off-resonant conditions not only because it prevents material damage but also because it contributes to preserving coherence.

cond-mat.mes-hall↗

arXiv2019

Direct evidence for efficient ultrafast charge separation in epitaxial WS$_2$/graphene heterostructure

We use time- and angle-resolved photoemission spectroscopy (tr-ARPES) to investigate ultrafast charge transfer in an epitaxial heterostructure made of monolayer WS$_2$ and graphene. This heterostructure combines the benefits of a direct gap semiconductor with strong spin-orbit coupling and strong light-matter interaction with those of a semimetal hosting massless carriers with extremely high mobility and long spin lifetimes. We find that, after photoexcitation at resonance to the A-exciton in WS$_2$, the photoexcited holes rapidly transfer into the graphene layer while the photoexcited electrons remain in the WS$_2$ layer. The resulting charge transfer state is found to have a lifetime of $\sim1$\,ps. We attribute our findings to differences in scattering phase space caused by the relative alignment of WS$_2$ and graphene bands as revealed by high resolution ARPES. In combination with spin-selective excitation using circularly polarized light the investigated WS$_2$/graphene heterostructure might provide a new platform for efficient optical spin injection into graphene.

cond-mat.mtrl-sci↗

arXiv2018

Charge density wave melting in one-dimensional wires with femtosecond sub-gap excitation

Charge density waves (CDWs) are symmetry-broken ground states that commonly occur in low-dimensional metals due to strong electron-electron and/or electron-phonon coupling. The non-equilibrium carrier distribution established via photodoping with femtosecond laser pulses readily quenches these ground states and induces an ultrafast insulator-to-metal phase transition. To date, CDW melting has been mainly investigated in the single-photon and tunneling regimes, while the intermediate multi-photon regime has received little attention. Here we excite one-dimensional indium wires with a CDW gap of ~300meV with mid-infrared pulses at 190meV with MV/cm field strength and probe the transient electronic structure with time- and angle-resolved photoemission spectroscopy (tr-ARPES). We find that the CDW gap is filled on a timescale short compared to our temporal resolution of 300fs and that the phase transition is completed within ~1ps. Supported by a minimal theoretical model we attribute our findings to multi-photon absorption across the CDW gap.

cond-mat.mtrl-sci↗

arXiv2018

Band Structure Dynamics in Indium Wires

One-dimensional Indium wires grown on Si(111) substrates, which are metallic at high temperatures, become insulating below $\sim100$ K due to the formation of a Charge Density Wave (CDW). The physics of this transition is not conventional and involves a multiband Peierls instability with strong interband coupling. This CDW ground state is readily destroyed with femtosecond laser pulses resulting in a light-induced insulator-to-metal phase transition. The current understanding of this transition remains incomplete, requiring measurements of the transient electronic structure to complement previous investigations of the lattice dynamics. Time- and angle-resolved photo\-emission spectroscopy with extreme ultra-violet radiation is applied to this end. We find that the transition from the insulating to the metallic band structure occurs within $\sim660$ fs that is a fraction of the amplitude mode period. The long life time of the transient state ($>100$ ps) is attributed to trapping in a metastable state in accordance with previous work.

cond-mat.mtrl-sci↗

arXiv2017

Ultrafast Momentum Imaging of Pseudospin-Flip Excitations in Graphene

The pseudospin of Dirac electrons in graphene manifests itself in a peculiar momentum anisotropy for photo-excited electron-hole pairs. These interband excitations are in fact forbidden along the direction of the light polarization, and are maximum perpendicular to it. Here, we use time- and angle-resolved photoemission spectroscopy to investigate the resulting unconventional hot carrier dynamics, sampling carrier distributions as a function of energy and in-plane momentum. We first show that the rapidly-established quasi-thermal electron distribution initially exhibits an azimuth-dependent temperature, consistent with relaxation through collinear electron-electron scattering. Azimuthal thermalization is found to occur only at longer time delays, at a rate that depends on the substrate and the static doping level. Further, we observe pronounced differences in the electron and hole dynamics in n-doped samples. By simulating the Coulomb- and phonon-mediated carrier dynamics we are able to disentangle the influence of excitation fluence, screening, and doping, and develop a microscopic picture of the carrier dynamics in photo-excited graphene. Our results clarify new aspects of hot carrier dynamics that are unique to Dirac materials, with relevance for photo-control experiments and optoelectronic device applications.

cond-mat.mes-hall↗

arXiv2017

Enhanced electron-phonon coupling in graphene with periodically distorted lattice

Electron-phonon coupling directly determines the stability of cooperative order in solids, including superconductivity, charge and spin density waves. Therefore, the ability to enhance or reduce electron-phonon coupling by optical driving may open up new possibilities to steer materials' functionalities, potentially at high speeds. Here we explore the response of bilayer graphene to dynamical modulation of the lattice, achieved by driving optically-active in-plane bond stretching vibrations with femtosecond mid-infrared pulses. The driven state is studied by two different ultrafast spectroscopic techniques. Firstly, TeraHertz time-domain spectroscopy reveals that the Drude scattering rate decreases upon driving. Secondly, the relaxation rate of hot quasi-particles, as measured by time- and angle-resolved photoemission spectroscopy, increases. These two independent observations are quantitatively consistent with one another and can be explained by a transient three-fold enhancement of the electron-phonon coupling constant. The findings reported here provide useful perspective for related experiments, which reported the enhancement of superconductivity in alkali-doped fullerites when a similar phonon mode was driven.

cond-mat.mtrl-sci↗

arXiv2015

Tracking primary thermalization events in graphene with photoemission at extreme timescales

Direct and inverse Auger scattering are amongst the primary processes that mediate the thermalization of hot carriers in semiconductors. These two processes involve the annihilation or generation of an electron-hole pair by exchanging energy with a third carrier, which is either accelerated or decelerated. Inverse Auger scattering is generally suppressed, as the decelerated carriers must have excess energies higher than the band gap itself. In graphene, which is gapless, inverse Auger scattering is instead predicted to be dominant at the earliest time delays. Here, $<8$ femtosecond extreme-ultraviolet pulses are used to detect this imbalance, tracking both the number of excited electrons and their kinetic energy with time- and angle-resolved photoemission spectroscopy. Over a time window of approximately 25 fs after absorption of the pump pulse, we observe an increase in conduction band carrier density and a simultaneous decrease of the average carrier kinetic energy, revealing that relaxation is in fact dominated by inverse Auger scattering. Measurements of carrier scattering at extreme timescales by photoemission will serve as a guide to ultrafast control of electronic properties in solids for PetaHertz electronics.

cond-mat.mtrl-sci↗

arXiv2015

Angle-resolved photoemission spectroscopy with 9-eV photon-energy pulses generated in a gas-filled hollow-core photonic crystal fiber

A recently developed source of ultraviolet radiation, based on optical soliton propagation in a gas-filled hollow-core photonic crystal fiber, is applied here to angle-resolved photoemission spectroscopy (ARPES). Near-infrared femtosecond pulses of only few μJ energy generate vacuum ultraviolet (VUV) radiation between 5.5 and 9 eV inside the gas-filled fiber. These pulses are used to measure the band structure of the topological insulator Bi2Se3 with a signal to noise ratio comparable to that obtained with high order harmonics from a gas jet. The two-order-of-magnitude gain in efficiency promises time-resolved ARPES measurements at repetition rates of hundreds of kHz or even MHz, with photon energies that cover the first Brillouin zone of most materials.

physics.optics↗

arXiv2014

Optically enhanced coherent transport in YBa2Cu3O6.5 by ultrafast redistribution of interlayer coupling

Nonlinear optical excitation of infrared active lattice vibrations has been shown to melt magnetic or orbital orders and to transform insulators into metals. In cuprates, this technique has been used to remove charge stripes and promote superconductivity, acting in a way opposite to static magnetic fields. Here, we show that excitation of large-amplitude apical oxygen distortions in the cuprate superconductor YBa2Cu3O6.5 promotes highly unconventional electronic properties. Below the superconducting transition temperature (Tc = 50 K), interbilayer coherence is transiently enhanced at the expense of intra-bilayer coupling. Strikingly, even above Tc a qualitatively similar effect is observed up to room temperature, with transient inter-bilayer coherence emerging from the incoherent ground state and similar transfer of spectral weight from high to low frequency. These observations are compatible with previous reports of an inhomogeneous normal state that retains important properties of a superconductor, in which light may be melting competing orders or dynamically synchronizing the interlayer phase. The transient redistribution of coherence discussed here could lead to new strategies to enhance superconductivity in steady state.

cond-mat.supr-con↗

arXiv2014

Optically induced coherent transport far above Tc in underdoped YBa2Cu3O6+x

We report on a photo-induced transient state of YBa2Cu2O6+x in which transport perpendicular to the Cu-O planes becomes highly coherent. This effect is achieved by excitation with mid-infrared optical pulses, tuned to the resonant frequency of apical oxygen vibrations, which modulate both lattice and electronic properties. Below the superconducting transition temperature Tc, the equilibrium signatures of superconducting interlayer coupling are enhanced. Most strikingly, the optical excitation induces a new reflectivity edge at higher frequency than the equilibrium Josephson plasma resonance, with a concomitant enhancement of the low frequency imaginary conductivity. Above Tc, the incoherent equilibrium conductivity becomes highly coherent, with the appearance of a reflectivity edge and a positive imaginary conductivity that increases with decreasing frequency. These features are observed up to room temperature in YBa2Cu2O6.45 and YBa2Cu2O6.5. The data above Tc can be fitted by hypothesizing that the light re-establishes a transient superconducting state over only a fraction of the solid, with a lifetime of a few picoseconds. Non-superconducting transport could also explain these observations, although one would have to assume transient carrier mobilities near 10^4 cm^2/(V.sec) at 100 K, with a density of charge carriers similar to the below Tc superfluid density. Our results are indicative of highly unconventional non-equilibrium physics and open new prospects for optical control of complex solids.

cond-mat.supr-con↗

arXiv2013

Possible observation of parametrically amplified coherent phasons in K0.3MoO3 using time-resolved extreme-ultraviolet ARPES

We use time- and angle-resolved photoemission spectroscopy (tr-ARPES) in the Extreme Ultraviolet (EUV) to measure the time- and momentum-dependent electronic structure of photo-excited K0.3MoO3. Prompt depletion of the Charge Density Wave (CDW) condensate launches coherent oscillations of the amplitude mode, observed as a 1.7-THz-frequency modulation of the bonding band position. In contrast, the anti-bonding band oscillates at about half this frequency. We attribute these oscillations to coherent excitation of phasons via parametric amplification of phase fluctuations.

cond-mat.str-el↗

arXiv2009

Silicon surface with giant spin-splitting

We demonstrate the induction of a giant Rashba-type spin-splitting on a semiconducting substrate by means of a Bi trimer adlayer on a Si(111) wafer. The in-plane inversion symmetry is broken so that the in-plane potential gradient induces a giant spin-splitting with a Rashba energy of about 140 meV, which is more than an order of magnitude larger than what has previously been reported for any semiconductor heterostructure. The separation of the electronic states is larger than their lifetime broadening, which has been directly observed with angular resolved photoemission spectroscopy. The experimental results are confirmed by relativistic first-principles calculations. We envision important implications for basic phenomena as well as for the semiconductor based technology.

cond-mat.mtrl-sci↗