Details
| Original language | English |
|---|---|
| Pages (from-to) | 11427-11433 |
| Number of pages | 7 |
| Journal | Journal of Physical Chemistry A |
| Volume | 116 |
| Issue number | 46 |
| Publication status | Published - 20 Sept 2012 |
Abstract
Extending the Shin-Metiu two-electron Hamiltonian, we construct a new Hamiltonian with effective singlet-triplet couplings. The Born-Oppenheimer electronic potentials and couplings are obtained for different parameters, and the laser-free dynamics is calculated with the full Hamiltonian and in the adiabatic limit. We compare the dynamics of the system using nuclear wave packets for different numbers of Born-Oppenheimer potentials and vibronic wave packets on a full 3-dimensional (two electron coordinates plus one nuclear coordinate) grid. Using strong fields, we show that it is possible to dynamically lock the spin state of the system by decoupling the singlet-triplet transition via a nonresonant dynamic Stark effect in the adiabatic limit. Although a similar spin-locking mechanism is observed in the dynamics of vibronic wave packets, multiphoton ionization cannot be neglected leading to the breakdown of the control scheme.
ASJC Scopus subject areas
- Chemistry(all)
- Physical and Theoretical Chemistry
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In: Journal of Physical Chemistry A, Vol. 116, No. 46, 20.09.2012, p. 11427-11433.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Quantum wave-packet dynamics in spin-coupled vibronic states
AU - Falge, Mirjam
AU - Engel, Volker
AU - Lein, Manfred
AU - Vindel-Zandbergen, Patricia
AU - Chang, Bo Y.
AU - Sola, Ignacio R.
N1 - Copyright: Copyright 2013 Elsevier B.V., All rights reserved.
PY - 2012/9/20
Y1 - 2012/9/20
N2 - Extending the Shin-Metiu two-electron Hamiltonian, we construct a new Hamiltonian with effective singlet-triplet couplings. The Born-Oppenheimer electronic potentials and couplings are obtained for different parameters, and the laser-free dynamics is calculated with the full Hamiltonian and in the adiabatic limit. We compare the dynamics of the system using nuclear wave packets for different numbers of Born-Oppenheimer potentials and vibronic wave packets on a full 3-dimensional (two electron coordinates plus one nuclear coordinate) grid. Using strong fields, we show that it is possible to dynamically lock the spin state of the system by decoupling the singlet-triplet transition via a nonresonant dynamic Stark effect in the adiabatic limit. Although a similar spin-locking mechanism is observed in the dynamics of vibronic wave packets, multiphoton ionization cannot be neglected leading to the breakdown of the control scheme.
AB - Extending the Shin-Metiu two-electron Hamiltonian, we construct a new Hamiltonian with effective singlet-triplet couplings. The Born-Oppenheimer electronic potentials and couplings are obtained for different parameters, and the laser-free dynamics is calculated with the full Hamiltonian and in the adiabatic limit. We compare the dynamics of the system using nuclear wave packets for different numbers of Born-Oppenheimer potentials and vibronic wave packets on a full 3-dimensional (two electron coordinates plus one nuclear coordinate) grid. Using strong fields, we show that it is possible to dynamically lock the spin state of the system by decoupling the singlet-triplet transition via a nonresonant dynamic Stark effect in the adiabatic limit. Although a similar spin-locking mechanism is observed in the dynamics of vibronic wave packets, multiphoton ionization cannot be neglected leading to the breakdown of the control scheme.
UR - http://www.scopus.com/inward/record.url?scp=84870033337&partnerID=8YFLogxK
U2 - 10.1021/jp306566x
DO - 10.1021/jp306566x
M3 - Article
C2 - 22946899
AN - SCOPUS:84870033337
VL - 116
SP - 11427
EP - 11433
JO - Journal of Physical Chemistry A
JF - Journal of Physical Chemistry A
SN - 1089-5639
IS - 46
ER -