Related papers: Two-dimensional electronic spectroscopy in the con…
Two-dimensional electronic spectroscopy (2DES) has enabled significant discoveries in both biological and synthetic energy-transducing systems. Although deriving chemical information from 2DES is a complex task, machine learning (ML) offers…
Electronically excited states of molecules are at the heart of photochemistry, photophysics, as well as photobiology and also play a role in material science. Their theoretical description requires highly accurate quantum chemical…
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…
Two-dimensional electronic spectroscopy has become one of the main experimental tools for analyzing the dynamics of excitonic energy transfer in large molecular complexes. Simplified theoretical models are usually employed to extract model…
How atoms and electrons in a molecule move during a chemical reaction and how rapidly energy is transferred to or from the surroundings can be studied with flashes of laser light. However, despite prolonged efforts to develop various…
Two-dimensional electronic spectroscopy (2DES) is one of the most powerful spectroscopic techniques, capable of attaining a nearly complete picture of a quantum system including its couplings, quantum coherence properties and its real-time…
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…
Machine-learning interatomic potentials (MLIPs) have enabled molecular dynamics at near ab initio accuracy, yet remain limited to energies and forces by construction, leaving electronic observables such as dipole moments and…
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…
In this study, we explore the potential of machine learning for modeling molecular electronic spectral intensities as a continuous function in a given wavelength range. Since presently available chemical space datasets provide excitation…
The presence of solvent tunes many properties of a molecule, such as its ground and excited state geometry, dipole moment, excitation energy, and absorption spectrum. Because the energy of the system will vary depending on the solvent…
The excited state dynamics of chromophores in complex environments determine a range of vital biological and energy capture processes. Time-resolved, multidimensional optical spectroscopies provide a key tool to investigate these processes.…
We propose an excited-state molecular dynamics simulation method based on variational quantum algorithms at a computational cost comparable to that of ground-state simulations. We utilize the feature that excited states can be obtained as…
Modern laboratory techniques like ultrafast laser excitation and shock compression can bring matter into highly nonequilibrium states with complex structural transformation, metallization and dissociation dynamics. To understand and model…
Selecting distinct quantum pathways in two-dimensional electronic spectroscopy (2DES) can give particularly deep insights into coherent and incoherent interactions and quantum dynamics in various materials. This includes isolating rephasing…
The local density of states (LDOS) of the adsorbate induced two-dimensional electron system (2DES) on n-InAs(110) is studied by low-temperature scanning tunneling spectroscopy. The LDOS exhibits irregular structures with fluctuation lengths…
Atomistic simulations using accurate energy functions can provide molecular-level insight into functional motions of molecules in the gas- and in the condensed phase. Together with recently developed and currently pursued efforts in…
Data-driven techniques are increasingly used to replace electronic-structure calculations of matter. In this context, a relevant question is whether machine learning (ML) should be applied directly to predict the desired properties or be…
Understanding the reactivity and spectroscopy of aqueous solutions at the atomistic level is crucial for the elucidation and design of chemical processes. However, the simulation of these systems requires addressing the formidable…
Vibrational coherences in ultrafast pump-probe (PP) and 2D electronic spectroscopy (2DES) provide insight into the excited state dynamics of molecules. Femtosecond coherence spectra (FCS) and 2D beat maps yield information about…