301 research outputs found
Revealing the role of electrons and phonons in the ultrafast recovery of charge density wave correlations in 1-TiSe
Using time- and angle-resolved photoemission spectroscopy with selective
near- and mid-infrared photon excitations, we investigate the femtosecond
dynamics of the charge density wave (CDW) phase in 1-TiSe, as well as
the dynamics of CDW fluctuations at 240 K. In the CDW phase, we observe the
coherent oscillation of the CDW amplitude mode. At 240 K, we single out an
ultrafast component in the recovery of the CDW correlations, which we explain
as the manifestation of electron-hole correlations. Our momentum-resolved study
of femtosecond electron dynamics supports a mechanism for the CDW phase
resulting from the cooperation between the interband Coulomb interaction, the
mechanism of excitonic insulator phase formation, and electron-phonon coupling.Comment: 9 pages, 6 figure
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
Evidence of reduced surface electron-phonon scattering in the conduction band of Bi_{2}Se_{3} by non-equilibrium ARPES
The nature of the Dirac quasiparticles in topological insulators calls for a
direct investigation of the electron-phonon scattering at the \emph{surface}.
By comparing time-resolved ARPES measurements of the TI Bi_{2}Se_{3} with
different probing depths we show that the relaxation dynamics of the electronic
temperature of the conduction band is much slower at the surface than in the
bulk. This observation suggests that surface phonons are less effective in
cooling the electron gas in the conduction band.Comment: 5 pages, 3 figure
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.Comment: 12 pages, 4 figure
Momentum resolved spin dynamics of bulk and surface excited states in the topological insulator
The prospective of optically inducing a spin polarized current for spintronic
devices has generated a vast interest in the out-of-equilibrium electronic and
spin structure of topological insulators (TIs). In this Letter we prove that
only by measuring the spin intensity signal over several order of magnitude in
spin, time and angle resolved photoemission spectroscopy (STAR-PES) experiments
is it possible to comprehensively describe the optically excited electronic
states in TIs materials. The experiments performed on
reveal the existence of a Surface-Resonance-State in the 2nd bulk band gap
interpreted on the basis of fully relativistic ab-initio spin resolved
photoemission calculations. Remarkably, the spin dependent relaxation of the
hot carriers is well reproduced by a spin dynamics model considering two
non-interacting electronic systems, derived from the excited surface and bulk
states, with different electronic temperatures.Comment: 5 pages and 4 figure
Probing the structure and dynamics of molecular clusters using rotational wavepackets
The chemical and physical properties of molecular clusters can heavily depend
on their size, which makes them very attractive for the design of new materials
with tailored properties. Deriving the structure and dynamics of clusters is
therefore of major interest in science. Weakly bound clusters can be studied
using conventional spectroscopic techniques, but the number of lines observed
is often too small for a comprehensive structural analysis. Impulsive alignment
generates rotational wavepackets, which provides simultaneous information on
structure and dynamics, as has been demonstrated successfully for isolated
molecules. Here, we apply this technique for the firsttime to clusters
comprising of a molecule and a single helium atom. By forcing the population of
high rotational levels in intense laser fields we demonstrate the generation of
rich rotational line spectra for this system, establishing the highly
delocalised structure and the coherence of rotational wavepacket propagation.
Our findings enable studies of clusters of different sizes and complexity as
well as incipient superfluidity effects using wavepacket methods.Comment: 5 pages, 6 figure
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.Comment: 4 figure
Ramifications of Optical Pumping on the Interpretation of Time-Resolved Photoemission Experiments on Graphene
In pump-probe time and angle-resolved photoemission spectroscopy (TR-ARPES)
experiments the presence of the pump pulse adds a new level of complexity to
the photoemission process in comparison to conventional ARPES. This is
evidenced by pump-induced vacuum space-charge effects and surface
photovoltages, as well as multiple pump excitations due to internal reflections
in the sample-substrate system. These processes can severely affect a correct
interpretation of the data by masking the out-of-equilibrium electron dynamics
intrinsic to the sample. In this study, we show that such effects indeed
influence TR-ARPES data of graphene on a silicon carbide (SiC) substrate. In
particular, we find a time- and laser fluence-dependent spectral shift and
broadening of the acquired spectra, and unambiguously show the presence of a
double pump excitation. The dynamics of these effects is slower than the
electron dynamics in the graphene sample, thereby permitting us to deconvolve
the signals in the time domain. Our results demonstrate that complex
pump-related processes should always be considered in the experimental setup
and data analysis.Comment: 9 pages, 4 figure
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