Related papers: First-principles approach to ultrafast pump-probe …
We introduce two-quantum (2Q) fluorescence-detected pump-probe (F-PP) spectroscopy as a tool to probe ultrafast multiparticle interactions in many-body systems. We describe a pulse-shaper-based fully collinear setup utilizing phase cycling…
We analyze the optical pump-probe reflection and transmission coefficients when the photoinduced response depends nonlinearly on the incident pump intensity. Under these conditions, we expect the photoconductivity depth profile to change…
By means of first-principles methods we analyze the optical response of transparent dense sodium as a function of applied pressure. We discover an unusual kind of charge-transfer exciton that proceeds from the interstitial distribution of…
Inorganic van der Waals bonded semiconductors like transition metal dichalcogenides are subject of intense research due to their electronic and optical properties which are promising for next-generation optoelectronic devices. In this…
The primary steps of photosynthesis rely on the generation, transport, and trapping of excitons in pigment-protein complexes (PPCs). Generically, PPCs possess highly structured vibrational spectra, combining many discrete intra-pigment…
We explore the nonlinear response of ultrafast strong-field driven excitons in a one-dimensional solid with ab initio simulations. We demonstrate from our simulations and analytical model that a finite population of excitons imprints unique…
Single molecule spectroscopy aims at unveiling often hidden but potentially very important contributions of single entities to a system's ensemble response. Albeit contributing tremendously to our ever growing understanding of molecular…
Excitons are key quasiparticles determining the optical properties of solids. As such, they can be utilized to coherently control the electronic structure of materials using optical femtosecond pulses. Identifying the decoherence mechanism…
The complex interaction dynamics of intense femtosecond (fs) pulses and their picosecond (ps)-long leading edge with nanostructured solids occur at both the nanometer and the femtosecond scales, making them extremely difficult to measure…
Despite major experimental progresses in time-resolved and angle-resolved photoemission spectroscopy, a quantitative, microscopic framework for interpreting exciton-induced modifications of electronic band structures -- applicable even…
In strongly correlated transition metal dichalcogenides, an intricate interplay of polaronic distortions, stacking arrangement, and electronic correlations determines the nature of the insulating state. Here, we study the response of the…
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…
In the last two decades, the three-beams pump-push-probe (PPP) technique has become a well-established tool for investigating the multidimensional configurational space of a molecule, as it permits to disclose precious information about the…
Exciting electrons in solids with intense light pulses offers the possibility of generating new states of matter through nonthermal means and controlling their macroscopic properties on femto- to picosecond timescales. One way to manipulate…
We report the lattice dynamics of transition metal thin films by using the ultrafast electron diffraction. We observe a suppression of the diffraction intensity in a few picosecond after the photoexcitation, which is directly interpreted as…
Attosecond nonlinear Fourier transform (NFT) pump probe spectroscopy is an experimental technique which allows investigation of the electronic excitation, ionization, and unimolecular dissociation processes. The NFT spectroscopy utilizes…
Ultrafast pump-probe measurements of plasmonic nanostructures probe the non-equilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements…
Strong light-matter coupling to form exciton- and vibropolaritons is increasingly touted as a powerful tool to alter the fundamental properties of organic materials. It is proposed that these states and their facile tunability can be used…
Transient absorption spectroscopy (TAS) is among the most common ultrafast photochemical experiments, but its interpretation remains challenging. In this work, we present an efficient and robust method for simulating TAS signals from first…
The ultrafast nonadiabatic internal conversion in azomethane is explored by the on-the-fly trajectory surface-hopping simulations of photoinduced dynamics and femtosecond transient absorption (TA) pump-probe (PP) spectra at three…