12 research outputs found
Establishing non-thermal regimes in pump-probe electron-relaxation dynamics
Time- and angle-resolved photoemission spectroscopy (TR-ARPES) accesses the
electronic structure of solids under optical excitation, and is a powerful
technique for studying the coupling between electrons and collective modes. One
approach to infer electron-boson coupling is through the relaxation dynamics of
optically-excited electrons, and the characteristic timescales of energy
redistribution. A common description of electron relaxation dynamics is through
the effective electronic temperature. Such a description requires that
thermodynamic quantities are well-defined, an assumption that is generally
violated at early delays. Additionally, precise estimation of the non-thermal
window -- within which effective temperature models may not be applied -- is
challenging. We perform TR-ARPES on graphite and show that Boltzmann rate
equations can be used to calculate the time-dependent electronic occupation
function, and reproduce experimental features given by non-thermal electron
occupation. Using this model, we define a quantitative measure of non-thermal
electron occupation and use it to define distinct phases of electron relaxation
in the fluence-delay phase space. More generally, this approach can be used to
inform the non-thermal-to-thermal crossover in pump-probe experiments.Comment: 18 pages, 10 figure
A versatile laser-based apparatus for time-resolved ARPES with micro-scale spatial resolution
We present the development of a versatile apparatus for a 6.2 eV laser-based
time and angle-resolved photoemission spectroscopy with micrometer spatial
resolution (time-resolved -ARPES). With a combination of tunable spatial
resolution down to 11 m, high energy resolution (11 meV),
near-transform-limited temporal resolution (280 fs), and tunable 1.55 eV
pump fluence up to 3 mJ/cm, this time-resolved -ARPES system
enables the measurement of ultrafast electron dynamics in exfoliated and
inhomogeneous materials. We demonstrate the performance of our system by
correlating the spectral broadening of the topological surface state of
BiSe with the spatial dimension of the probe pulse, as well as
resolving the spatial inhomogeneity contribution to the observed spectral
broadening. Finally, after in-situ exfoliation, we performed time-resolved
-ARPES on a 30 m few-layer-thick flake of transition metal
dichalcogenide WTe, thus demonstrating the ability to access ultrafast
electron dynamics with momentum resolution on micro-exfoliated and twisted
materials
Comparative Electronic Structures of the Chiral Helimagnets Cr1/3NbS2 and Cr1/3TaS2
Magnetic materials with noncollinear spin textures are promising for
spintronic applications. To realize practical devices, control over the length
and energy scales of such spin textures is imperative. The chiral helimagnets
Cr1/3NbS2 and Cr1/3TaS2 exhibit analogous magnetic phase diagrams with
different real-space periodicities and field dependence, positioning them as
model systems for studying the relative strengths of the microscopic mechanisms
giving rise to exotic spin textures. Here, we carry out a comparative study of
the electronic structures of Cr1/3NbS2 and Cr1/3TaS2 using angle-resolved
photoemission spectroscopy and density functional theory. We show that bands in
Cr1/3TaS2 are more dispersive than their counterparts in Cr1/3NbS2 and connect
this result to bonding and orbital overlap in these materials. We also
unambiguously distinguish exchange splitting from surface termination effects
by studying the dependence of their photoemission spectra on polarization,
temperature, and beam size. We find strong evidence that hybridization between
intercalant and host lattice electronic states mediates the magnetic exchange
interactions in these materials, suggesting that band engineering is a route
toward tuning their spin textures. Overall, these results underscore how the
modular nature of intercalated transition metal dichalcogenides translates
variation in composition and electronic structure to complex magnetism.Comment: 46 pages, 18 figures, 5 table
Direct determination of mode-projected electron-phonon coupling in the time-domain
Ultrafast spectroscopies have become an important tool for elucidating the
microscopic description and dynamical properties of quantum materials. In
particular, by tracking the dynamics of non-thermal electrons, a material's
dominant scattering processes -- and thus the many-body interactions between
electrons and collective excitations -- can be revealed. Here we present a new
method for extracting the electron-phonon coupling strength in the time domain,
by means of time and angle-resolved photoemission spectroscopy (TR-ARPES). This
method is demonstrated in graphite, where we investigate the dynamics of
photo-injected electrons at the K point, detecting quantized energy-loss
processes that correspond to the emission of strongly-coupled optical phonons.
We show that the observed characteristic timescale for spectral-weight-transfer
mediated by phonon-scattering processes allows for the direct quantitative
extraction of electron-phonon matrix elements, for specific modes, and with
unprecedented sensitivity.Comment: 19 pages, 4 figure
Nature of the current-induced insulator-to-metal transition in CaRuO as revealed by transport-ARPES
The Mott insulator CaRuO exhibits a rare insulator-to-metal
transition (IMT) induced by DC current. While structural changes associated
with this transition have been tracked by neutron diffraction, Raman
scattering, and x-ray spectroscopy, work on elucidating the response of the
electronic degrees of freedom is still in progress. Here we unveil the
current-induced modifications of the electronic states of CaRuO by
employing angle-resolved photoemission spectroscopy (ARPES) in conjunction with
four-probe transport. Two main effects emerge: a clear reduction of the Mott
gap and a modification in the dispersion of the Ru-bands. The changes in
dispersion occur exclusively along the high-symmetry direction, parallel
to the -axis where the greatest in-plane lattice change occurs. These
experimental observations are reflected in dynamical mean-field theory (DMFT)
calculations simulated exclusively from the current-induced lattice constants,
indicating a current driven structural transition as the primary mechanism of
the IMT. Furthermore, we demonstrate this phase is distinct from the
high-temperature zero-current metallic phase. Our results provide insight into
the elusive nature of the current-induced IMT of CaRuO and advance the
challenging, yet powerful, technique of transport-ARPES.Comment: 8 pages, 4 figure
Unveiling the underlying interactions in Ta2NiSe5 from photo-induced lifetime change
We present a generic procedure for quantifying the interplay of electronic
and lattice degrees of freedom in photo-doped insulators through a comparative
analysis of theoretical many-body simulations and time- and angle-resolved
photoemission spectroscopy (TR-ARPES) of the transient response of the
candidate excitonic insulator Ta2NiSe5. Our analysis demonstrates that the
electron-electron interactions dominate the electron-phonon ones. In
particular, a detailed analysis of the TRARPES spectrum enables a clear
separation of the dominant broadening (electronic lifetime) effects from the
much smaller bandgap renormalization. Theoretical calculations show that the
observed strong spectral broadening arises from the electronic scattering of
the photo-excited particle-hole pairs and cannot be accounted for in a model in
which electron-phonon interactions are dominant. We demonstrate that the
magnitude of the weaker subdominant bandgap renormalization sensitively depends
on the distance from the semiconductor/semimetal transition in the
high-temperature state, which could explain apparent contradictions between
various TR-ARPES experiments. The analysis presented here indicates that
electron-electron interactions play a vital role (although not necessarily the
sole one) in stabilizing the insulating state
Fano interference of the Higgs mode in cuprate high-Tc superconductors
Despite decades of search for the pairing boson in cuprate high-Tc
superconductors, its identity still remains debated to date. For this reason,
spectroscopic signatures of electron-boson interactions in cuprates have always
been a center of attention. For example, the kinks in the quasiparticle
dispersion observed by angle-resolved photoemission spectroscopy (ARPES)
studies have motivated a decade-long investigation of electron-phonon as well
as electron-paramagnon interactions in cuprates. On the other hand, the overlap
between the charge-order correlations and the pseudogap in the cuprate phase
diagram has also generated discussions about the potential link between them.
In the present study, we provide a fresh perspective on these intertwined
interactions using the novel approach of Higgs spectroscopy, i.e. an
investigation of the amplitude oscillations of the superconducting order
parameter driven by a terahertz radiation. Uniquely for cuprates, we observe a
Fano interference of its dynamically driven Higgs mode with another collective
mode, which we reveal to be charge density wave fluctuations from an extensive
doping- and magnetic field-dependent study. This finding is further
corroborated by a mean field model in which we describe the microscopic
mechanism underlying the interaction between the two orders. Our work
demonstrates Higgs spectroscopy as a novel and powerful technique for
investigating intertwined orders and microscopic processes in unconventional
superconductors
Control of atoms and molecules with shaped broadband pulses
The main goal of this PhD work is an experimental study of coherent excitation of atomic and molecular wavepackets, i.e. superpositions of many quantum eigenstates, by shaped femtosecond pulses. Approaches allowing nearly complete population transfer between quantum eigenstates were well studied in the past within the two level approximation. In this work we focus on adiabatic and non-adiabatic methods of population transfer beyond the two-level approximation.
Excitation of multi-level target states is possible due to broad spectrum of an ultrashort pulse which contains frequencies needed for multiple transitions to different states in the final superposition. At the same time, the spectrum of an ultrashort pulse can be modified, or ``shaped'', in order to affect the excitation process and control the amplitudes in the final superposition. Both non-adiabatic and quasi-adiabatic methods were first implemented and studied in electronic wavepackets in alkali atoms. The non-adiabatic approach revealed features linked to the strong-field perturbations of the energy level structure of the quantum system. An adiabatic method was implemented for the first time on a femtosecond time scale, and was thoroughly characterized. The control over complex amplitudes in the target superposition was demonstrated as well as completeness of the population transfer. In the second part of this work, we focused on coherent control of rotational wavepackets in diatomic molecules. Rotational excitation by a periodic train of femtosecond pulses was investigated in the context of ``delta-kicked'' rotor - a paradigm system for studying quantum chaos, and the effect of quantum resonance was demonstrated for the first time in a system of true quantum rotors. Control of uni-directional molecular rotation was proposed and demonstrated with a novel ``chiral pulse train'' - a sequence of femtosecond pulses with polarization rotating from pulse to pulse by a predefined angle. All the developed techniques offer new tools in coherent control of atomic and molecular wavepackets on an ultrashort time scale.Science, Faculty ofPhysics and Astronomy, Department ofGraduat
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Comparative Electronic Structures of the Chiral Helimagnets Cr1/3NbS2 and Cr1/3TaS2
Magnetic materials with noncollinear spin textures are promising for spintronic applications. To realize practical devices, control over the length and energy scales of such spin textures is imperative. The chiral helimagnets Cr1/3NbS2 and Cr1/3TaS2 exhibit analogous magnetic-phase diagrams with different real-space periodicities and field dependence, positioning them as model systems for studying the relative strengths of the microscopic mechanisms giving rise to exotic spin textures. Although the electronic structure of the Nb analogue has been experimentally investigated, the Ta analogue has received far less attention. Here, we present a comprehensive suite of electronic structure studies on both Cr1/3NbS2 and Cr1/3TaS2 using angle-resolved photoemission spectroscopy and density functional theory. We show that bands in Cr1/3TaS2 are more dispersive than their counterparts in Cr1/3NbS2, resulting in markedly different Fermi wavevectors. The fact that their qualitative magnetic phase diagrams are nevertheless identical shows that hybridization between the intercalant and host lattice mediates the magnetic exchange interactions in both of these materials. We ultimately find that ferromagnetic coupling is stronger in Cr1/3TaS2, but larger spin-orbit coupling (and a stronger Dzyaloshinskii-Moriya interaction) from the heavier host lattice ultimately gives rise to shorter spin textures