Magnetic phases of two-component ultracold bosons in an optical lattice

We investigate spin-order of ultracold bosons in an optical lattice by means of Dynamical Mean-Field Theory. A rich phase diagram with anisotropic magnetic order is found, both for the ground state and at finite temperatures. Within the Mott insulator, a ferromagnetic to antiferromagnetic transition can be tuned using a spin-dependent optical lattice. In addition we find a supersolid phase, in which superfluidity coexists with antiferromagnetic spin order. We present detailed phase diagrams at finite temperature for the experimentally realized heteronuclear 87Rb - 41K mixture in a three-dimensional optical lattice.Comment: 6 pages, 4 figures, revised and published versio

A first-principles time-dependent density functional theory framework for spin and time-resolved angular-resolved photoelectron spectroscopy in periodic systems

We 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

Phonon Driven Floquet Matter

The 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

Monitoring Electron-Photon Dressing in WSe2

Optical 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

First-principles simulations for attosecond photoelectron spectroscopy based on time-dependent density functional theory

We develop a first-principles simulation method for attosecond time-resolved photoelectron spectroscopy. This method enables us to directly simulate the whole experimental processes, including excitation, emission and detection on equal footing. To examine the performance of the method, we use it to compute the reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) experiments of gas-phase Argon. The computed RABBITT photoionization delay is in very good agreement with recent experimental results from [Klünder et al., Phys. Rev. Lett. 106, 143002 (2011)] and [Guénot et al., Phys. Rev. A 85, 053424 (2012)]. This indicates the significance of a fully-consistent theoretical treatment of the whole measurement process to properly describe experimental observables in attosecond photoelectron spectroscopy. The present framework opens the path to unravel the microscopic processes underlying RABBITT spectra in more complex materials and nanostructures

Strong chiral dichroism and enantiopurification in above-threshold ionization with locally chiral light

We 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

Time- 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

Ab initio simulation of attosecond transient absorption spectroscopy in two-dimensional materials

We 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

Cavity Control of Excitons in Two-Dimensional Materials

We propose a robust and efficient way of controlling the optical spectra of two-dimensional materials and van der Waals heterostructures by quantum cavity embedding. The cavity light-matter coupling leads to the formation of exciton-polaritons, a superposition of photons and excitons. Our first-principles study demonstrates a reordering and mixing of bright and dark excitons spectral features and in the case of a type II van-der-Waals heterostructure an inversion of intra- and interlayer excitonic resonances. We further show that the cavity light-matter coupling strongly depends on the dielectric environment and can be controlled by encapsulating the active two-dimensional (2D) crystal in another dielectric material. Our theoretical calculations are based on a newly developed nonperturbative many-body framework to solve the coupled electron-photon Schrödinger equation in a quantum-electrodynamical extension of the Bethe-Salpeter approach. This approach enables the ab initio simulations of exciton-polariton states and their dispersion from weak to strong cavity light-matter coupling regimes. Our method is then extended to treat van der Waals heterostructures and encapsulated 2D materials using a simplified Mott-Wannier description of the excitons that can be applied to very large systems beyond reach for fully ab initio approaches

Light-Driven Extremely Nonlinear Bulk Photogalvanic Currents

We predict the generation of bulk photocurrents in materials driven by bichromatic fields that are circularly polarized and corotating. The nonlinear photocurrents have a fully controllable directionality and amplitude without requiring carrier-envelope-phase stabilization or few-cycle pulses, and can be generated with photon energies much smaller than the band gap (reducing heating in the photoconversion process). We demonstrate with ab initio calculations that the photocurrent generation mechanism is universal and arises in gaped materials (Si, diamond, MgO, hBN), in semimetals (graphene), and in two- and three-dimensional systems. Photocurrents are shown to rely on sub-laser-cycle asymmetries in the nonlinear response that build-up coherently from cycle to cycle as the conduction band is populated. Importantly, the photocurrents are always transverse to the major axis of the co-circular lasers regardless of the material's structure and orientation (analogously to a Hall current), which we find originates from a generalized time-reversal symmetry in the driven system. At high laser powers (∼1013 W/cm2) this symmetry can be spontaneously broken by vast electronic excitations, which is accompanied by an onset of carrier-envelope-phase sensitivity and ultrafast many-body effects. Our results are directly applicable for efficient light-driven control of electronics, and for enhancing sub-band-gap bulk photogalvanic effects