Relaxation Dynamics of Chlorophyll b in the Sub-ps Ultrafast Timescale Measured by 2D Electronic Spectroscopy

Abstract

A thorough characterization of the early time sub-100 fs relaxation dynamics of biologically relevant chromophores is of crucial importance for a complete understanding of the mechanisms regulating the ultrafast dynamics of the relaxation processes in more complex multichromophoric light-harvesting systems. While chlorophyll a has already been the object of several investigations, little has been reported on chlorophyll b, despite its pivotal role in many functionalities of photosynthetic proteins. Here the relaxation dynamics of chlorophyll b in the ultrafast regime have been characterized using 2D electronic spectroscopy. The comparison of experimental measurements performed at room temperature and 77 K allows the mechanisms and the dynamics of the sub-100 fs relaxation dynamics to be characterized, including spectral diffusion and fast internal conversion assisted by a specific set of vibrational modes.

The Physical Chemistry and Chemical Physics (PCCP) Section of the International Journal of Molecular Sciences in Its Publications: The First 300 Thematic Articles in the First 3 Years

“…This area is the largest in terms of the number of related publications and includes 91 articles, namely [ 1 , 2 , 3 , 102 , 103 , 104 , 105 , 106 , 107 , 108 , 109 , 110 , 111 , 112 , 113 , 114 , 115 , 116 , 117 , 118 , 119 , 120 , 121 , 122 , 123 , 124 , 125 , 126 , 127 , 128 , 129 , 130 , 131 , 132 , 133 , 134 , 135 , 136 , 137 , 138 , 139 , 140 , 141 , 142 , 143 , 144 , 145 , 146 , 147 , 148 , 149 , 150 , 151 , 152 , 153 ,…”

“…The last one seems to be the most detailed, and it is precisely this that we will try to implement in the course of our narrative. As it should be expected, a priori, most of the publications in this direction are devoted to organic compounds, and primarily organic molecules; these include, with varying degrees of correctness, publications [ 1 , 2 , 3 , 102 , 103 , 104 , 106 , 108 , 112 , 117 , 118 , 119 , 121 , 124 , 127 , 128 , 130 , 131 , 132 , 133 , 135 , 138 , 139 , 140 , 141 , 142 , 143 , 144 , 146 , 147 , 148 , 151 , 153 , 154 , 156 , 157 , 164 , 165 , 166 , 168 , 171 , 172 , 174 , 176 , 178 , 180 , 183 , 185 , 186 ]. Much less space is occupied by the works related to polymeric (in fact, to a high molecular weight) compounds [ 113 , …”

Advances in the Chemistry of Porphyrins and Related Macrocycles

“…This class of compounds is especially versatile, being engaged in a wide multitude of today’s core applications ranging from biology to medicine and material science. The Special Issue entitled “Advances in the Chemistry of Porphyrins and Related Macrocycles“ collects featured research papers providing an overview of the recent developments and advances related to some topic aspects of porphyrin and porphyrinoid chemistry, including biological and biomedical applications [ 1 , 2 , 3 , 4 , 5 , 6 , 7 ], photophysics [ 8 ], supramolecular chemistry [ 9 ], and sensing materials [ 10 , 11 , 12 ]. The Special Issue welcomed the submission of original full research articles [ 1 , 3 , 4 , 6 , 7 , 8 , 9 , 10 , 11 ], as well as some review articles [ 2 , 5 , 12 ] aiming to provide a comprehensive foundation on some of the above-mentioned research field, highlighting the current state of knowledge.…”

“…The Special Issue entitled “Advances in the Chemistry of Porphyrins and Related Macrocycles“ collects featured research papers providing an overview of the recent developments and advances related to some topic aspects of porphyrin and porphyrinoid chemistry, including biological and biomedical applications [ 1 , 2 , 3 , 4 , 5 , 6 , 7 ], photophysics [ 8 ], supramolecular chemistry [ 9 ], and sensing materials [ 10 , 11 , 12 ]. The Special Issue welcomed the submission of original full research articles [ 1 , 3 , 4 , 6 , 7 , 8 , 9 , 10 , 11 ], as well as some review articles [ 2 , 5 , 12 ] aiming to provide a comprehensive foundation on some of the above-mentioned research field, highlighting the current state of knowledge. Several researchers from many research institutions, by virtue of their qualified scientific expertise, have contributed to the success of this Special Issue, and their scientific contributions are summarized here.…”

“…Within photophysical studies of biologically relevant chromophores, Fresch and Collini [ 8 ] performed a detailed and systematic survey on the relaxation dynamics in the ultrafast timescale of chlorophyll b (chl b ), a naturally important photosynthetic pigment whose role is pivotal in many functionalities of photosynthetic proteins. Relaxation dynamics have been characterized by 2D electronic spectroscopy (2DES) at room temperature (RT) and at 77 K to undercover the short time dynamics (≈100 fs).…”