Related papers: Two-dimensional electronic spectroscopy from first…
Within the well-established optical response function formalism, a new strategy with the central idea of employing the forward-backward stochastic Schr\"{o}dinger equations in a segmented way to accurately obtain the two-dimensional (2D)…
Two-dimensional electronic spectroscopy (2DES) provides a detailed picture of electronically nonadiabatic dynamics that can be interpreted with the aid of simulations. Here, we develop and contrast trajectory-based nonadiabatic dynamics…
We show how vibronic spectra in molecular systems can be simulated in an efficient and accurate way using first principles approaches without relying on the explicit use of multiple Born-Oppenheimer potential energy surfaces. We demonstrate…
We present details of our effective computational methods based on the real-space finite-difference formalism to elucidate electronic and magnetic properties of the two-dimensional (2D) materials within the framework of the density…
Raman spectroscopy is a widely-used non-destructive material characterization method, which provides information about the vibrational modes of the material and therefore of its atomic structure and chemical composition. Interpretation of…
Two-dimensional electronic spectroscopy provides information on coupling and energy transfer between excited states on ultrafast timescales. Only recently, incoherent fluorescence detection has made it possible to combine this method with…
X-ray absorption and its dependence on the polarization of light is a powerful tool to investigate the orbital and spin moments of magnetic materials and their orientation relative to crystalline axes. Here, we present a program for the…
The atomistic resolution recently achieved by ultrafast spectroscopies demands corresponding theoretical advances. Real-time time-dependent density-functional theory (RT-TDDFT) with Ehrenfest dynamics offers an optimal trade-off between…
Electron microscopy is a powerful tool for studying the properties of materials down to their atomic structure. In many cases, the quantitative interpretation of images requires simulations based on atomistic structure models. These…
Ultra-fast and multi-dimensional spectroscopy gives a powerful looking glass into the dynamics of molecular systems. In particular two-dimensional electronic spectroscopy (2DES) provides a probe of coherence and the flow of energy within…
Ab initio computation of two-dimensional electronic spectra is an expanding field, whose goal is improving upon simple, few-dimensional models often employed to explain experiments. Here, we propose an accurate and computationally…
We present a first-principles-based (second-principles) scheme that permits large-scale materials simulations including both atomic and electronic degrees of freedom on the same footing. The method is based on a predictive…
Spectroscopy is the most important method for probing the structure of molecules. However, predicting molecular spectra on classical computers is computationally expensive, with the most accurate methods having a cost that grows…
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.…
Methods for reconstructing the spectral density of a vibrational environment from experimental data can yield key insights into the impact of the environment on molecular function. Although such experimental methods exist, they generally…
Quantum embedding schemes have the potential to significantly reduce the computational cost of first principles calculations, whilst maintaining accuracy, particularly for calculations of electronic excitations in complex systems. In this…
Two-dimensional electronic spectroscopy (2DES) provides rich information about how the electronic states of molecules, proteins, and solid-state materials interact with each other and their surrounding environment. Atomistic molecular…
Simulating electron-ion dynamics using time-dependent density functional theory within an Ehrenfest dynamics scheme can be done in two ways that are in principle exact and identical: propagating time-dependent electronic Kohn-Sham equations…
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…
A recently developed dynamical mean-field theory in the iterated perturbation theory approximation was used as a basis for construction of the "first principles" calculation scheme for investigating electronic structure of strongly…