218 research outputs found
Electronic-structural dynamics in graphene
We review our recent time- and angle-resolved photoemission spectroscopy experiments, which measure the transient electronic structure of optically driven graphene. For pump photon energies in the near infrared (ℏωpump = 950 meV), we have discovered the formation of a population-inverted state near the Dirac point, which may be of interest for the design of THz lasing devices and optical amplifiers. At lower pump photon energies (ℏωpump pump = 200 meV), a transient enhancement of the electron-phonon coupling constant is observed, providing interesting perspective for experiments that report light-enhanced superconductivity in doped fullerites in which a similar lattice mode was excited. All the studies reviewed here have important implications for applications of graphene in optoelectronic devices and for the dynamical engineering of electronic properties with light
Band Structure Dynamics in Indium Wires
One-dimensional Indium wires grown on Si(111) substrates, which are metallic
at high temperatures, become insulating below 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 fs that is a fraction of the amplitude mode
period. The long life time of the transient state ( ps) is attributed to
trapping in a metastable state in accordance with previous work.Comment: 14 pages, 7 figure
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.Comment: 23 pages, 12 figure
Direct evidence for efficient ultrafast charge separation in epitaxial WS/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 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, the photoexcited holes
rapidly transfer into the graphene layer while the photoexcited electrons
remain in the WS layer. The resulting charge transfer state is found to
have a lifetime of \,ps. We attribute our findings to differences in
scattering phase space caused by the relative alignment of WS and graphene
bands as revealed by high resolution ARPES. In combination with spin-selective
excitation using circularly polarized light the investigated WS/graphene
heterostructure might provide a new platform for efficient optical spin
injection into graphene.Comment: 28 pages, 14 figure
Direct evidence for efficient ultrafast charge separation in epitaxial WS<sub>2</sub>/graphene heterostructures
We use time- and angle-resolved photoemission spectroscopy (tr-ARPES) to investigate ultrafast charge transfer in an epitaxial heterostructure made of monolayer WS2 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 WS2, the photoexcited holes rapidly transfer into the graphene layer while the photoexcited electrons remain in the WS2 layer. The resulting charge-separated transient state is found to have a lifetime of ∼1 ps. We attribute our findings to differences in scattering phase space caused by the relative alignment of WS2 and graphene bands as revealed by high-resolution ARPES. In combination with spin-selective optical excitation, the investigated WS2/graphene heterostructure might provide a platform for efficient optical spin injection into graphene
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, 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.Comment: 16 pages, 8 figure
Population Inversion in Monolayer and Bilayer Graphene
The recent demonstration of saturable absorption and negative optical
conductivity in the Terahertz range in graphene has opened up new opportunities
for optoelectronic applications based on this and other low dimensional
materials. Recently, population inversion across the Dirac point has been
observed directly by time- and angle-resolved photoemission spectroscopy
(tr-ARPES), revealing a relaxation time of only ~ 130 femtoseconds. This
severely limits the applicability of single layer graphene to, for example,
Terahertz light amplification. Here we use tr-ARPES to demonstrate long-lived
population inversion in bilayer graphene. The effect is attributed to the small
band gap found in this compound. We propose a microscopic model for these
observations and speculate that an enhancement of both the pump photon energy
and the pump fluence may further increase this lifetime.Comment: 18 pages, 6 figure
Tuning independently Fermi energy and spin splitting in Rashba systems: Ternary surface alloys on Ag(111)
By detailed first-principles calculations we show that the Fermi energy and
the Rashba splitting in disordered ternary surface alloys (BiPbSb)/Ag(111) can
be independently tuned by choosing the concentrations of Bi and Pb. The
findings are explained by three fundamental mechanisms, namely the relaxation
of the adatoms, the strength of the atomic spin-orbit coupling, and band
filling. By mapping the Rashba characteristics,i.e.the splitting and the Rashba
energy, and the Fermi energy of the surface states in the complete range of
concentrations. Our results suggest to investigate experimentally effects which
rely on the Rashba spin-orbit coupling in dependence on spin-orbit splitting
and band filling.Comment: 11 pages, 3 figure
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
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