Real-Time Time-Dependent Density Functional Theory for Pump-Probe Spectroscopies
Fuente:
arXiv
Guardado en:
| Autor principal: | |
|---|---|
| Formato: | Preprint |
| Publicado: |
2026
|
| Materias: | |
| Acceso en línea: | |
| Etiquetas: |
Agregar Etiqueta
Sin Etiquetas, Sea el primero en etiquetar este registro!
|
| _version_ | 1866916050625363968 |
|---|---|
| author | Moitra, Torsha |
| author_facet | Moitra, Torsha |
| contents | The last decade has witnessed a rapid advancement in laser technology, enabling the direct monitoring and control of electronic motion on its natural attosecond to sub-femtosecond timescales. Ultrafast processes are conventionally studied using pump-probe spectroscopic techniques, where a pump pulse drives the molecule out of equilibrium and a time-delayed probe pulse records the response of the coherent non-stationary state. Since, these processes are non-linear and non-perturbative in nature, real-time formalisms provide a suitable theoretical framework for studying ultrafast light-induced dynamics. In addition, relativistic effects can play an important role in such simulations, either because the external field lies in the XUV to soft-X-ray region targeting core-level excitations, or because the molecular system contains heavy elements. In this chapter, we provide an overview of recent developments in real-time time-dependent density functional theory for simulating pump-probe spectroscopies (namely, transient absorption and transient electronic circular dichroism) at both non-relativistic and relativistic Hamiltonian levels. In order to further interpret these spectroscopic signals, we analyze several spectroscopically relevant time-dependent sub-observables, such as induced electronic densities and induced dipole moments as well as analytical formulations of generalized non-equilibrium response functions. We provide examples to show that the framework can be used to investigate and design new light-induced phenomena that emerge only in the attosecond regime. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2605_27252 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Real-Time Time-Dependent Density Functional Theory for Pump-Probe Spectroscopies Moitra, Torsha Chemical Physics The last decade has witnessed a rapid advancement in laser technology, enabling the direct monitoring and control of electronic motion on its natural attosecond to sub-femtosecond timescales. Ultrafast processes are conventionally studied using pump-probe spectroscopic techniques, where a pump pulse drives the molecule out of equilibrium and a time-delayed probe pulse records the response of the coherent non-stationary state. Since, these processes are non-linear and non-perturbative in nature, real-time formalisms provide a suitable theoretical framework for studying ultrafast light-induced dynamics. In addition, relativistic effects can play an important role in such simulations, either because the external field lies in the XUV to soft-X-ray region targeting core-level excitations, or because the molecular system contains heavy elements. In this chapter, we provide an overview of recent developments in real-time time-dependent density functional theory for simulating pump-probe spectroscopies (namely, transient absorption and transient electronic circular dichroism) at both non-relativistic and relativistic Hamiltonian levels. In order to further interpret these spectroscopic signals, we analyze several spectroscopically relevant time-dependent sub-observables, such as induced electronic densities and induced dipole moments as well as analytical formulations of generalized non-equilibrium response functions. We provide examples to show that the framework can be used to investigate and design new light-induced phenomena that emerge only in the attosecond regime. |
| title | Real-Time Time-Dependent Density Functional Theory for Pump-Probe Spectroscopies |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2605.27252 |