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Award Abstract #1255084

CAREER: Mechanistic Investigations of the Excited-State Dynamics in Thiobase and Pterin UVA Sensitizers and in Their DNA Constructs

NSF Org: CHE
Division Of Chemistry
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Initial Amendment Date: March 12, 2013
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Latest Amendment Date: June 29, 2016
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Award Number: 1255084
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Award Instrument: Continuing grant
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Program Manager: James Lisy
CHE Division Of Chemistry
MPS Direct For Mathematical & Physical Scien
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Start Date: April 1, 2013
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End Date: March 31, 2018 (Estimated)
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Awarded Amount to Date: $606,590.00
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Investigator(s): Carlos Crespo-Hernandez carlos.crespo@case.edu (Principal Investigator)
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Sponsor: Case Western Reserve University
Nord Hall, Suite 615
CLEVELAND, OH 44106-4901 (216)368-4510
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NSF Program(s): Chem Struct,Dynmcs&Mechansms B
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Program Reference Code(s): 1982, 5918, 9161, 9251, AMPP, 1045
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Program Element Code(s): 9102

ABSTRACT

Through this CAREER award, supported by the Chemical Structure, Dynamics and Mechanisms-B Program of the Division of Chemistry, Prof. Carlos E. Crespo-Hernández of Case Western Reserve University will develop an integrated research and education program based upon investigations of the excited-state dynamics in UVA-sensitizers and of the photosensitized reactions that underlay DNA damage. This information along with the techniques used to obtain it are central to understanding a host of biological processes, including cell death and skin cancer, and for developing therapeutics for a range of disorders. The research, by providing an understanding of these reactions, will scrutinize fundamental ideas in the fields of organic photochemistry and photobiology. The educational objectives seek to motivate students at various educational levels to enter and persist in science and technology studies and careers by: developing modules that teach fundamental concepts in photochemistry and time-resolved spectroscopy and that incorporate active learning strategies; providing research opportunities for high school and undergraduate students; and mentoring and serving as a role model for underrepresented and disadvantaged students.

Photochemistry involves the study of the interaction of light with matter. Such interactions are paramount in vision, photosynthesis, solar energy conversion and storage, and photonic/optoelectronic devices. In addition, photochemistry of biologically related molecules is paramount for the prevention and treatment of skin cancer. In skin cancer, light causes damage to DNA by various mechanisms that are not fully understood. DNA damage in skin exposed to ultraviolet light emanating from the sun primarily depends on non-DNA biomolecules acting as energy transfer units. It is a goal of the Crespo-Hernández group to investigate the reactions in DNA that are initiated by these biomolecules when acting as energy/charge transfer units. The educational aspects of the CAREER plan involves the design of concept-centered modules and laboratory sessions for undergraduate and graduate courses that systematically incorporate active learning and teaching strategies to enhance student learning and retention. These activities will also contribute to a broader understanding of the variables that affect the performance and continuing interest of students in science and technology fields. Exposure of pre-college and postsecondary students, including underrepresented and disadvantaged students, to multidisciplinary research, modern photochemistry, spectroscopy, and computational methods will motivate their participation in science, spark their interest in important areas of science and technology, and contribute to the nation's scientific workforce and economic competitiveness.


PUBLICATIONS PRODUCED AS A RESULT OF THIS RESEARCH

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Pollum, M.; Jockusch, S.; Crespo-Hernández, C. E.. "2,4-Dithiothymine as a Potent UVA Chemotherapeutic Agent," Journal of the American Chemical Society, v.136, 2014, p. 17930. 

Reichardt, C.; Wen, C.; Vogt, R. A.; Crespo-Hernández, C. E.*. "Role of intersystem crossing in the fluorescence quenching of 2-aminopurine 2'-deoxyriboside in solution," Photochem. Photobiol. Sci., v.12, 2013, p. 1341. 

Pollum, M.; Crespo-Hernández, C. E.. "Communication: The dark singlet state as a doorway state in the ultrafast and efficient intersystem crossing dynamics in 2-thiothymine and 2-thiouracil," J. Chem. Phys., v.140, 2014, p. 071101. 

M. Pollum; S. Jockusch; C. E. Crespo-Hernández. "Increase in the Photoreactivity of Uracil Derivatives by Doubling Thionation," Phys. Chem. Chem. Phys., v.17, 2015, p. 27851. 

Brister, M.; Crespo-Hernández, C. E.. "Direct Observation of Triplet-State Population Dynamics in the RNA Uracil Derivative 1-Cyclohexyluracil," J. Phys. Chem. Lett., v.6, 2015, p. 4404. 

Pollum, M.; Ortiz-Rodríguez, L. A.; Jockusch, S.; Crespo-Hernández, C. E.. "The Triplet State of 6-Thio-2?-deoxyguanosine: Intrinsic Properties and Reactivity toward Molecular Oxygen," Photochem. Photobiol., v.92, 2016, p. 286. 

C. E. Crespo-Hernández; L. Martínez-Fernández.; C. Rauer; C. Reichardt; S. Mai; M. Pollum; L. Marquetand; L. González; I. Corral. "Electronic and Structural Elements that Regulate the Excited-State Dynamics in Purine Nucleobase Derivatives," J. Am. Chem. Soc., v.137, 2015, p. 4368-4381. 

 

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