相关论文: Complete Reconstruction of the Wavefunction of a R…
We propose a two-step protocol for inverting ultrafast spectroscopy experiments on a molecular aggregate to extract the time-evolution of the excited state density matrix. The first step is a deconvolution of the experimental signal to…
Excited-state vibrational dynamics in molecules can be studied by an electronically off-resonant Raman process induced by a probe pulse with variable delay with respect to an actinic pulse. We establish the connection between several…
We propose a method to reconstruct the vibrational quantum state of molecules excited by a general excitation laser pulse. Unlike existing methods, we do not require the molecules before excitation to be in a pure state, allowing us to…
We calculate the eigenstates of a diatomic molecule in a range of model mean-field potentials, and evaluate the evolution of their associated Raman spectra with field strength. We demonstrate that dramatic changes in the appearance of the…
Vibrational motions in electronically excited states can be observed by either time and frequency resolved infrared absorption or by off resonant stimulated Raman techniques. Multipoint correlation function expressions are derived for both…
This paper describes a method to do ab initio molecular dynamics in electronically excited systems within the random phase approximation (RPA). Using a dynamical variational treatment of the RPA frequency, which corresponds to the…
The complete measurement of the quantum state of two correlated photons requires reconstructing the amplitude and phase of the biphoton wavefunction. We show how, by means of spatially resolved single photon detection, one can infer the…
Excited-state vibrations are crucial for determining photophysical and photochemical properties of molecular compounds. Stimulated Raman scattering can coherently stimulate and probe molecular vibrations with optical pulses, but it is…
Causality implies that by measuring an absorption spectrum, the time-dependent linear response function can be retrieved. Recent experiments suggest a link between the shape of spectral lines observed in absorption spectroscopy with the…
Photophysical and photochemical processes are ruled by the interplay between transient vibrational and electronic degrees of freedom, which are ultimately determined by the multidimensional potential energy surfaces (PESs). Differences…
A systematic method for determining correlated wavefunctions of extended systems in the ground and excited states is presented. It allows to fully exploit the power of quantum-chemical programs designed for correlation calculations of…
By employing single charge injections with an atomic force microscope, we investigated redox reactions of a molecule on a multilayer insulating film. First, we charged the molecule positively by attaching a single hole. Then we neutralized…
In this work we discuss the rotational structure of Rydberg molecules. We calculate the complete wave function in a laboratory fixed frame and derive the transition matrix elements for the pho- toassociation of free ground state atoms. We…
In this work, we extend the x-ray constrained wavefunction fitting approach, a key method in quantum crystallography for charge density reconstruction, to incorporate experimental observables beyond x-ray diffraction. Unlike traditional…
Multi-molecular excited states accompanied by an intra- and inter-molecular geometric relaxation are commonly encountered in optical and electrooptical studies and applications of organic semiconductors as, for example excimers or charge…
The description of excited state dynamics in multichromophoric systems constitutes both a theoretical and experimental challenge in modern physical chemistry. An experimental protocol which can systematically characterize both coherent and…
Molecular laser cooling and trapping requires addressing all spontaneous decays to excited vibrational states that occur at the $\gtrsim 10^{-4} - 10^{-5}$ level, which is accomplished by driving repumping transitions out of these states.…
Excited states of molecules lie in the heart of photochemistry and chemical reactions. The recent development in quantum computational chemistry leads to inventions of a variety of algorithms that calculate the excited states of molecules…
Time-dependent response theories are foundational to the development of algorithms that determine quantum properties of electronic excited states of molecules and periodic systems. They are employed in wave-function, density-functional, and…
We formulate the theory for a diatomic molecule in a spatially degenerate electronic state interacting with a non-resonant laser field and investigate its rovibrational structure in the presence of the field. We report on \textit{ab initio}…