PMID- 29985004
OWN - NLM
STAT- PubMed-not-MEDLINE
DCOM- 20180803
LR  - 20180803
IS  - 1520-5215 (Electronic)
IS  - 1089-5639 (Linking)
VI  - 122
IP  - 30
DP  - 2018 Aug 2
TI  - Spectral Filtering as a Tool for Two-Dimensional Spectroscopy: A Theoretical 
      Model.
PG  - 6206-6213
LID - 10.1021/acs.jpca.8b03339 [doi]
AB  - Two-dimensional optical spectroscopy is a powerful technique for the probing of 
      coherent quantum superpositions. Recently, the finite width of the laser spectrum 
      has been employed to selectively tune experiments for the study of particular 
      coherences. This involves the exclusion of certain transition frequencies, which 
      results in the elimination of specific Liouville pathways. The rigorous analysis 
      of such experiments requires the use of ever more sophisticated theoretical 
      models for the optical spectroscopy of electronic and vibronic systems. Here we 
      develop a nonimpulsive and non-Markovian model, which combines an explicit 
      definition of the laser spectrum, via the equation of motion-phase matching 
      approach (EOM-PMA), with the hierarchical equations of motion (HEOM). This 
      theoretical framework is capable of simulating the 2D spectroscopy of vibronic 
      systems with low frequency modes, coupled to environments of intermediate and 
      slower time scales. In order to demonstrate the spectral filtering of vibronic 
      coherences, we examine the elimination of lower energy peaks from the 2D spectra 
      of a zinc porphyrin monomer upon blue-shifting the laser spectrum. The filtering 
      of Liouville pathways is revealed through the disappearance of peaks from the 
      amplitude spectra for a coupled vibrational mode.
FAU - Green, Dale
AU  - Green D
AUID- ORCID: 0000-0002-2549-0486
AD  - School of Chemistry , University of East Anglia , Norwich Research Park, Norwich 
      NR4 7TJ , U.K.
FAU - V A Camargo, Franco
AU  - V A Camargo F
AD  - School of Chemistry , University of East Anglia , Norwich Research Park, Norwich 
      NR4 7TJ , U.K.
AD  - CAPES Foundation , Ministry of Education of Brazil , Brasilia DF 70040-202 , 
      Brazil.
FAU - Heisler, Ismael A
AU  - Heisler IA
AD  - School of Chemistry , University of East Anglia , Norwich Research Park, Norwich 
      NR4 7TJ , U.K.
FAU - Dijkstra, Arend G
AU  - Dijkstra AG
AD  - School of Chemistry , University of Leeds , Leeds LS2 9JT , U.K.
FAU - Jones, Garth A
AU  - Jones GA
AUID- ORCID: 0000-0003-2984-1711
AD  - School of Chemistry , University of East Anglia , Norwich Research Park, Norwich 
      NR4 7TJ , U.K.
LA  - eng
PT  - Journal Article
DEP - 20180723
PL  - United States
TA  - J Phys Chem A
JT  - The journal of physical chemistry. A
JID - 9890903
EDAT- 2018/07/10 06:00
MHDA- 2018/07/10 06:01
CRDT- 2018/07/10 06:00
PHST- 2018/07/10 06:00 [pubmed]
PHST- 2018/07/10 06:01 [medline]
PHST- 2018/07/10 06:00 [entrez]
AID - 10.1021/acs.jpca.8b03339 [doi]
PST - ppublish
SO  - J Phys Chem A. 2018 Aug 2;122(30):6206-6213. doi: 10.1021/acs.jpca.8b03339. Epub 
      2018 Jul 23.