104,694 research outputs found
Floquet analysis of excitations in materials
No full textControlled excitation of materials can transiently induce changed or novel properties with many fundamental and technological implications. Especially, the concept of Floquet engineering and the manipulation of the electronic structure via dressing with external lasers have attracted some recent interest. Here we review the progress made in defining Floquet material properties and give a special focus on their signatures in experimental observables as well as considering recent experiments realizing Floquet phases in solid state materials. We discuss how a wide range of experiments with non-equilibrium electronic structure can be viewed by employing Floquet theory as an analysis tool providing a different view of excitations in solids
Phonon Driven Floquet Matter
No full textThe effect of electron-phonon coupling in materials can be interpreted as a dressing of the electronic structure by the lattice vibration, leading to vibrational replicas and hybridization of electronic states. In solids, a resonantly excited coherent phonon leads to a periodic oscillation of the atomic lattice in a crystal structure bringing the material into a nonequilibrium electronic configuration. Periodically oscillating quantum systems can be understood in terms of Floquet theory, which has a long tradition in the study of semiclassical light-matter interaction. Here, we show that the concepts of Floquet analysis can be applied to coherent lattice vibrations. This coupling leads to phonon-dressed quasi-particles imprinting specific signatures in the spectrum of the electronic structure. Such dressed electronic states can be detected by time- and angular-resolved photoelectron spectroscopy (ARPES) manifesting as sidebands to the equilibrium band structure. Taking graphene as a paradigmatic material with strong electron-phonon interaction and nontrivial topology, we show how the phonon-dressed states display an intricate sideband structure revealing the electron-phonon coupling at the Brillouin zone center and topological ordering of the Dirac bands. We demonstrate that if time-reversal symmetry is broken by the coherent lattice perturbations a topological phase transition can be induced. This work establishes that the recently demonstrated concept of light-induced nonequilibrium Floquet phases can also be applied when using coherent phonon modes for the dynamical control of material properties
Ab initio simulation of attosecond transient absorption spectroscopy in two-dimensional materials
No full textWe extend the first-principles analysis of attosecond transient absorption spectroscopy to two-dimensional materials. As an example of two-dimensional materials, we apply the analysis to monolayer hexagonal boron nitride (h-BN) and compute its transient optical properties under intense few-cycle infrared laser pulses. Nonadiabatic features are observed in the computed transient absorption spectra. To elucidate the microscopic origin of these features, we analyze the electronic structure of h-BN with density functional theory and investigate the dynamics of specific energy bands with a simple two-band model. Finally, we find that laser-induced intraband transitions play a significant role in the transient absorption even for the two-dimensional material and that the nonadiabatic features are induced by the dynamical Franz-Keldysh effect with an anomalous band dispersion
A first-principles time-dependent density functional theory framework for spin and time-resolved angular-resolved photoelectron spectroscopy in periodic systems
No full textWe present a novel theoretical approach to simulate spin, time, and angular-resolved photoelectron spectroscopy (ARPES) from first-principles that is applicable to surfaces, thin films, few layer systems, and low-dimensional nanostructures. The method is based on a general formulation in the framework of time-dependent density functional theory (TDDFT) to describe the real time-evolution of electrons escaping from a surface under the effect of any external (arbitrary) laser field. By extending the so-called t-SURFF method to periodic systems one can calculate the final photoelectron spectrum by collecting the flux of the ionization current trough an analyzing surface. The resulting approach, that we named t-SURFFP, allows us to describe a wide range of irradiation conditions without any assumption on the dynamics of the ionization process allowing for pump-probe simulations on an equal footing. To illustrate the wide scope of applicability of the method we present applications to graphene, monolayer, and bilayer WSe2, and hexagonal BN (hBN) under different laser configurations
Monitoring Electron-Photon Dressing in WSe2
No full textOptical pumping of solids creates a nonequilibrium electronic structure where electrons and photons combine to form quasiparticles of dressed electronic states. The resulting shift of electronic levels is known as the optical Stark effect, visible as a red shift in the optical spectrum. Here we show that in a pump-probe setup we can uniquely define a nonequilibrium quasiparticle bandstructure that can be directly measurable with photoelectron spectroscopy. The dynamical photon-dressing (and undressing) of the many-body electronic states can be monitored by pump-probe time and angular-resolved photoelectron spectroscopy (tr-ARPES) as the photon-dressed bandstructure evolves in time depending on the pump-probe pulse overlap. The computed tr-ARPES spectrum agrees perfectly with the quasi-energy spectrum of Floquet theory at maximum overlap and goes to the equilibrium bandstructure as the pump-probe overlap goes to zero. Additionally, we show how this time-dependent nonequilibrium quasiparticle structure can be understood to be the bandstructure underlying the optical Stark effect. 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). These results establish the photon dressed nonequilibrium bandstructures as the underlying quasiparticle structure of light-driven steady-state quantum phases of matter
Phonoritons as Hybridized Exciton-Photon-Phonon Excitations in a Monolayer h -BN Optical Cavity
No full textA phonoriton is an elementary excitation that is predicted to emerge from hybridization between exciton, phonon, and photon. Besides the intriguing many-particle structure, phonoritons are of interest as they could serve as functional nodes in devices that utilize electronic, phononic, and photonic elements for energy conversion and thermal transport applications. Although phonoritons are predicted to emerge in an excitonic medium under intense electromagnetic wave irradiation, the stringent condition for their existence has eluded direct observation in solids. In particular, on-resonance, intense pumping schemes have been proposed, but excessive photoexcitation of carriers prevents optical detection. Here, we theoretically predict the appearance of phonoritonic features in monolayer hexagonal boron nitride (h-BN) embedded in an optical cavity. The coherent superposition nature of phonoriton states is evidenced by the hybridization of exciton-polariton branches with phonon replicas that is tunable by the cavity-matter coupling strength. This finding simultaneously provides an experimental pathway for observing the predicted phonoritons and opens a new avenue for tuning materials properties
First-principles modelling for time-resolved ARPES under different pump–probe conditions
No full textFirst-principles methods for time-resolved angular resolved photoelectron spectroscopy play a pivotal role in providing interpretation and microscopic understanding of the complex experimental data and in exploring novel observables or observation conditions that may be achieved in future experiments. Here we describe an efficient, reliable and scalable first-principles method for tr-ARPES based on time-dependent density functional theory including propagation and surface effects usually discarded in the widely used many-body techniques based on computing the non-equilibrium spectral function and discuss its application to a variety of pump–probe conditions. We identify four conditions, depending on the length of the probe relative to the excitation in the materials on the one hand and on the overlap between pump and probe on the other hand. Within this paradigm different examples of observables of time-resolved ARPES are discussed in view of the newly developed and highly accurate time-resolved experimental spectroscopies
Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light
No full textWe derive here a highly selective photoelectron-based chirality-sensing technique that utilizes "locally chiral"laser pulses. We show that this approach results in strong chiral discrimination, where the standard forwards/backwards asymmetry of photoelectron circular dichroism (PECD) is lifted. The resulting dichroism is larger and more robust than conventional PECD (especially in the high-energy part of the spectrum), is found in all hemispheres, and is not symmetric or antisymmetric with respect to any symmetry operator. Remarkably, chiral dichroism of up to 10% survives in the angularly integrated above-threshold ionization (ATI) spectra, and chiral dichroism of up to 5% survives in the total ionization rates. We demonstrate these results through ab initio calculations in the chiral molecules bromochlorofluoromethane, limonene, fenchone, and camphor. We also explore the parameter space of the locally chiral field and show that the observed dichroism is strongly correlated to the degree of chirality of the light, validating it as a measure for chiral-interaction strengths. Our results pave the way for highly selective probing of ultrafast chirality in ATI and motivate the use of locally chiral light for enhancing ultrafast spectroscopies. Most importantly, the technique can be implemented to achieve all-optical enantiopurification of chiral samples
Direct Measurement of Electron-Phonon Coupling with Time-Resolved ARPES
No full textTime- and angular- resolved photoelectron spectroscopy is a powerful technique to measure electron dynamics in solids. Recent advances in this technique have facilitated band and energy resolved observations of the effect that excited phonons, have on the electronic structure. Here, we show with the help of ab initio simulations that the Fourier analysis of the time-resolved measurements of solids with excited phonon modes enables the determination of the band- and mode-resolved electron-phonon coupling directly from the experimental data without any additional input from theory. Such an observation is not restricted to regions of strong electron-phonon coupling and does not require strongly excited or hot phonons, but can be employed to monitor the dynamical renormalization of phonons in driven phases of matter
Phonon-driven spin-Floquet magneto-valleytronics in MoS 2
No full textTwo-dimensional materials equipped with strong spin-orbit coupling can display novel electronic, spintronic, and topological properties originating from the breaking of time or inversion symmetry. A lot of interest has focused on the valley degrees of freedom that can be used to encode binary information. By performing ab initio time-dependent density functional simulation on MoS 2 , here we show that the spin is not only locked to the valley momenta but strongly coupled to the optical E′′ phonon that lifts the lattice mirror symmetry. Once the phonon is pumped so as to break time-reversal symmetry, the resulting Floquet spectra of the phonon-dressed spins carry a net out-of-plane magnetization (≈0.024μ B for single-phonon quantum) even though the original system is non-magnetic. This dichroic magnetic response of the valley states is general for all 2H semiconducting transition-metal dichalcogenides and can be probed and controlled by infrared coherent laser excitation
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