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) inter-bilayer 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.
Full text
Available for:
IJS, IZUM, KILJ, KISLJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
Floquet states in dissipative open quantum systems Sato, S A; De Giovannini, U; Aeschlimann, S ...
Journal of physics. B, Atomic molecular and optical physics/Journal of physics. B, Atomic, molecular and optical physics,
11/2020, Volume:
53, Issue:
22
Journal Article
Peer reviewed
Open access
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 resonant ...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 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 multi-photon absorption 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 energy transfer from light to matter 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.
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 fs 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 time scales by photoemission will serve as a guide to ultrafast control of electronic properties in solids for petahertz electronics.
Full text
Available for:
CMK, CTK, FMFMET, IJS, NUK, PNG, UM
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 vacancies. 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.
Full text
Available for:
CMK, CTK, FMFMET, IJS, NUK, PNG, UM
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 nonequilibrium 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 regime with pump photon energies bigger than the gap size. The recent development of strong-field midinfrared sources now enables the investigation of CDW dynamics following subgap excitation. Here we excite prototypical one-dimensional indium wires with a CDW gap of ∼300 meV with midinfrared pulses at ℏω=190 meV with MV/cm field strength and probe the transient electronic structure with time- and angle-resolved photoemission spectroscopy. We find that the CDW gap is filled on a timescale short compared to our temporal resolution of 300 fs and that the band structure changes are completed within ∼1 ps. Supported by a minimal theoretical model we attribute our findings to multiphoton absorption across the CDW gap.
Full text
Available for:
CMK, CTK, FMFMET, IJS, NUK, PNG, UM
We demonstrate 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 inducing a giant spin ...splitting with a Rashba energy of about 140 meV, much 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.
Full text
Available for:
CMK, CTK, FMFMET, IJS, NUK, PNG, UM
•tr-ARPES is used to investigate carrier thermalization in photo-excited graphene.•Photo-excitation builds up a non-thermal carrier distribution.•Lifetime of non-thermal carriers depends on their ...number.•<10fs dynamics dominated by impact ionization.
The dynamics of photo-generated electron–hole pairs in solids are dictated by many-body interactions such as electron–electron and electron–phonon scattering. Hence, understanding and controlling these scattering channels is crucial for many optoelectronic applications, ranging from light harvesting to optical amplification. Here we measure the formation and relaxation of the photo-generated non-thermal carrier distribution in monolayer graphene with time- and angle-resolved photoemission spectroscopy. Using sub-10fs pulses we identify impact ionization as the primary scattering channel, which dominates the dynamics for the first 25fs after photo-excitation. Auger recombination is found to set in once the carriers have accumulated at the Dirac point with time scales between 100 and 250fs, depending on the number of non-thermal carriers. Our observations help in gauging graphene's potential as a solar cell and TeraHertz lasing material.
Full text
Available for:
GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK, ZRSKP
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 midinfrared pulses. The driven state is studied by two different ultrafast spectroscopic techniques. First, terahertz time-domain spectroscopy reveals that the Drude scattering rate decreases upon driving. Second, the relaxation rate of hot quasiparticles, 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 threefold 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.
Full text
Available for:
CMK, CTK, FMFMET, IJS, NUK, PNG, UM
The pseudospin of Dirac electrons in graphene manifests itself in a peculiar momentum anisotropy for photoexcited 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 quasithermal 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 photoexcited graphene. Our results clarify new aspects of hot carrier dynamics that are unique to Dirac materials, with relevance for photocontrol experiments and optoelectronic device applications.
Full text
Available for:
CMK, CTK, FMFMET, IJS, NUK, PNG, UM
PDF
