Hi everyone,
On Monday at 3:00 pm on the division room, Prof. Angel Rubio, Director of the Max Planck
for Structure and Dynamics of Matter will give a seminar (see the abstract below). Also
there are still some free spots for having lunch with him on Tuesday. Please let me know
if you wanna join
Best
David
QED-Chemistry and Materials: A new theoretical framework for the first principles
modelling of Light-Matter interactions, from weak to strong coupling
Angel Rubio
Max Planck Institute for the Structure and Dynamics of Matter, Hamburg, Germany
Email: angel.rubio@mpsd.mpg.de<mailto:angel.rubio@mpsd.mpg.de>
Computer simulations that predict the light-induced change in the physical and chemical
properties of complex systems, molecules, nanostructures and solids usually ignore the
quantum nature of light. Recent experiments at the interface between materials science
and quantum optics have uncovered situations where both the molecular system and the
photon field have to be treated in detail. In this talk, we show how theoretical
approaches have to be adapted to treat such coupled matter–photon problems and which
effects can be anticipated. We demonstrate how the effects of treating quantum-photons
can be properly included in such calculations. Our newly developed quantum electrodynamics
density-functional formalism (QED-TDDFT) provides this theoretical framework. The basic
idea is to treat the full QED system of particles and photons as a quantum fluid. Here the
particles are represented by a charge current, and the photons by a classical
electromagnetic field that acts on the current in a very complex manner. We will provide
an overview of how well-established concepts in the fields of quantum chemistry and
material sciences have to be adapted when the quantum nature of light becomes important in
correlated matter-photon problems. We analyse model systems in optical cavities, where
the matter-photon interaction is considered from the weak- to the strong coupling limit
and for individual photon modes as well as for the multi-mode case. We identify
fundamental changes in Born-Oppenheimer surfaces, spectroscopic quantities, conical
intersections and efficiency for quantum control. We apply the new
quantum-electrodynamical density-functional theory to single-photon emission and show how
a straightforward approximation accurately describes the correlated electron-photon
dynamics.
We will also address how periodic driving of many-body systems offers a platform to design
Floquet states of matter with tunable electronic properties on ultrafast time scales.
Based on the previous QED-TDDFT theoretical framework, we will introduce Floquet
time-dependent density functional theory (Floquet-TDDFT) as a general and robust first
principles method for predictive Floquet engineering of topological states of matter.
Using this scheme we show how femtosecond laser pulses with circularly polarised light can
be used to switch between Weyl semimetal, Dirac semimetal, and topological insulator
states in a prototypical 3D Dirac material, Na3Bi. Our findings are general and apply to
any 3D Dirac semimetal. Furthermore, we show that the concepts of Floquet analysis can be
applied to monitor electron photon and electron-phonon dressing in 2D materials . This
coupling leads to phonon- or photon-dressed quasi-particles (polarons or polaritons)
imprinting specific signatures in the spectrum of the electronic structure that can be
detected by time dependent ARPES as sidebands to the equilibrium band structure. Most
strikingly, we find that the non-equilibrium electronic structure created by coherent
dynamical dressing is the same for photon and phonon perturbations. We demonstrate that if
time-reversal symmetry is broken by the coherent lattice perturbations a topological phase
transition can be induced. The extension to spin-resolved ARPES can be used to predict
asymmetric dichroic response linked to the valley selective optical excitations in
monolayer transition metal dichalcogenides (TMDs). This work establishes that the recently
demonstrated concept of light-induced non-equilibrium Floquet phases can also be applied
when using coherent phonon modes for the dynamical control of material properties. The
present results are generic for bosonic time-dependent perturbations, therefore we
envision similar phenomena to be observed for example for plasmon, magnon or exciton
driven materials.
The new QED-TDDFT framework introduced here paves the road to describe matter-photon
interactions from first-principles and deal with emergent properties of matte, opening
the possibility to predict and control the change of material properties, selectively
trigger physicochemical processes, alter chemical reactions, and create new state of
matter due to the interaction with light from first principles.
References:
H. Hübener, U. de Giovannini, A. Rubio, Phonon driven Floquet matter,, (2017); H.
Hübener, M. A. Sentef, U. de Giovannini, A.F. Kemper, A. Rubio, Creating stable
Floquet-Weyl semimetals by laser-driving of 3D Dirac materials, Nature Communications 7,
13940 (2017)
N. Tancogne-Dejean, O. D. Mucke, F. X. Kartner , A. Rubio, Impact of the electronic band
structure in high-harmonic generation spectra of solids, Physical Review Letters 118,
087403 (2017)
U. De Giovannini, H. Hübener, A. Rubio, Monitoring electron-photion dressing in WSe2,
NanoLetters {\bf 16} 7993–7998 (2016)
Atoms and Molecules in Cavities: From Weak to Strong Coupling in QED Chemistry, J. Flick,
M. Ruggenthaler, H. Appel, A. Rubio, Proceedings of The National Academy of Sciences of
The United States of America 114, 3026–3034 (2017)
Kohn-Sham Approach to Quantum Electrodynamical Density Functional Theory: Exact
Time-Dependent Effective Potentials in Real Space J. Flick, M. Ruggenthaler, H. Appel, A.
Rubio
Proceedings of The National Academy of Sciences of The United States of America 112
15285-15290 (2015)
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