PCCP Seminar with Nancy Makri

Physical Chemistry/Chemical Physics seminar presented by Nancy Makri of UIUC.

Real-Time Path Integral Simulations of

Electron-Vibration Dynamics in Large Molecular Aggregates

 

Nancy Makri

Department of Chemistry, Department of Physics, and

Illinois Quantum Information Science and Technology Center

University of Illinois at Urbana-Champaign

           

 

            The unfavorable scaling of wavefunction storage severely impacts the feasibility of quantum dynamical calculations in the condensed phase. Feynman’s path integral formulation offers an attractive alternative, replacing wavefunctions by a sum of quantum mechanical amplitudes along all possible paths. However, the path sum involves astronomical numbers of terms, and stochastic methods are unable to deal with the oscillatory quantum phase.

A series of developments have led to efficient real-time path integral methods for a variety of processes. The quasi-adiabatic propagator path integral (QuAPI) for system-bath dynamics achieves linear scaling with the number of time steps by propagating a tensor that spans the memory interval. Recent work showed that one can further disentangle the variables through the small matrix decomposition of the path integral (SMatPI), thereby enabling the simulation of long-memory processes and multistate systems.  A different decomposition leads to the modular path integral (MPI) for extended systems, which allows the inclusion of any number of finite-temperature vibrational modes and scales linearly system length.  In addition to these numerically exact methods, the quantum-classical path integral (QCPI) offers a rigorous formulation of nonadiabatic dynamics in solution or biological environments.

These methods are used to investigate quantum coherence and its destruction in charge, proton, and energy transfer processes in a variety of systems, as well as the dynamics of coupled qubits. This seminar will focus on the intricate mechanistic details of excitation energy transfer (EET) in large molecular aggregates. Besides generating the populations and coherences of electronic/spin states over a range of temperatures, the path integral simulations track the evolution of electronic-vibrational densities, vibrational amplitudes and mode energies, offering a clear picture of nonadiabatic dynamics and mode-mode interactions in these systems. The coherence and spreading of energy in light harvesting bacteriochlorophyll complexes and in J aggregates of a perylene bisimide (PBI) will be discussed.

Dial-In Information

Contact chemistry@colorado.edu for registration and connecting.

Friday, January 28 at 4:00pm

Virtual Event
Event Type

Colloquium/Seminar

Interests

Science & Technology, Research & Innovation

Audience

Students, Faculty, General Public, Postdoc

College, School & Unit

Arts & Sciences

Group
Chemistry
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