Revealing possible long-living coherence in ultrafast processes allows detecting genuine quantum mechanical effects in molecules. To investigate such effects from a quantum chemistry perspective, we have developed a method for simulating the time evolution of molecular systems based on ab initio calculations, which includes relaxation and environment-induced dephasing of the molecular wave function whose rates are external parameters. The proposed approach combines a quantum chemistry description of the molecular target with a real-time propagation scheme within the time-dependent stochastic Schrödinger equation. Moreover, it allows a quantitative characterization of the state and dynamics coherence through the l1-norm of coherence and the linear entropy, respectively. To test the approach, we have simulated femtosecond pulse-shaping ultrafast spectroscopy of terrylenediimide, a well-studied fluorophore in single-molecule spectroscopy. Our approach is able to reproduce the experimental findings [R. Hildner et al., Nat. Phys. 7, 172 (2011)], confirming the usefulness of the approach and the correctness of the implementation.
Skip Nav Destination
Article navigation
28 May 2018
Research Article|
May 30 2018
Probing quantum coherence in ultrafast molecular processes: An ab initio approach to open quantum systems
Emanuele Coccia
;
Emanuele Coccia
a)
1
Department of Chemical Sciences, University of Padova
, via Marzolo 1, Padova, Italy
2
CNR Institute of Nanoscience
, via Campi 213/A, Modena, Italy
a)Authors to whom correspondence should be addressed: emanuele.coccia@unipd.it and stefano.corni@unipd.it
Search for other works by this author on:
Filippo Troiani;
Filippo Troiani
2
CNR Institute of Nanoscience
, via Campi 213/A, Modena, Italy
Search for other works by this author on:
Stefano Corni
Stefano Corni
a)
1
Department of Chemical Sciences, University of Padova
, via Marzolo 1, Padova, Italy
2
CNR Institute of Nanoscience
, via Campi 213/A, Modena, Italy
a)Authors to whom correspondence should be addressed: emanuele.coccia@unipd.it and stefano.corni@unipd.it
Search for other works by this author on:
a)Authors to whom correspondence should be addressed: emanuele.coccia@unipd.it and stefano.corni@unipd.it
J. Chem. Phys. 148, 204112 (2018)
Article history
Received:
January 19 2018
Accepted:
May 11 2018
Citation
Emanuele Coccia, Filippo Troiani, Stefano Corni; Probing quantum coherence in ultrafast molecular processes: An ab initio approach to open quantum systems. J. Chem. Phys. 28 May 2018; 148 (20): 204112. https://doi.org/10.1063/1.5022976
Download citation file:
Sign in
Don't already have an account? Register
Sign In
You could not be signed in. Please check your credentials and make sure you have an active account and try again.
Pay-Per-View Access
$40.00
Citing articles via
DeePMD-kit v2: A software package for deep potential models
Jinzhe Zeng, Duo Zhang, et al.
A theory of pitch for the hydrodynamic properties of molecules, helices, and achiral swimmers at low Reynolds number
Anderson D. S. Duraes, J. Daniel Gezelter
Electronic structure simulations in the cloud computing environment
Eric J. Bylaska, Ajay Panyala, et al.
Related Content
Stochastic Schrödinger equation for hot-carrier dynamics in plasmonic systems
J. Chem. Phys. (September 2024)
Controlling the nonadiabatic dynamics of the charge-transfer process with chirped pulses: Insights from a double-pump time-resolved fluorescence spectroscopy scheme
J. Chem. Phys. (January 2024)
A pair natural orbital implementation of the coupled cluster model CC2 for excitation energies
J. Chem. Phys. (August 2013)
Hierarchy of stochastic Schrödinger equation towards the calculation of absorption and circular dichroism spectra
J. Chem. Phys. (May 2017)
Two-dimensional coherent electronic spectrometer with switchable multi-color configurations
Rev. Sci. Instrum. (February 2024)