Probing two-photon properties of molecules: Large non-condon effects dominate the resonance hyper-Raman scattering of rhodamine 6G

Chris B. Milojevich; Daniel W. Silverstein; Lasse Jensen; Jon P. Camden

doi:10.1021/ja2054622

Probing two-photon properties of molecules: Large non-condon effects dominate the resonance hyper-Raman scattering of rhodamine 6G

Chris B. Milojevich
, Daniel W. Silverstein
, Lasse Jensen
, Jon P. Camden

Chemistry

Research output: Contribution to journal › Article › peer-review

42 Scopus citations

Abstract

Experimentally measured resonance hyper-Raman (RHR) spectra spanning the S ₁ ← S ₀, S ₂ ← S ₀, and S ₃ ← S ₀ transitions in rhodamine 6G (R6G) have been recorded. These spectra are compared to the results of first-principles calculations of the RHR intensity that include both Franck-Condon (A-term) and non-Condon (B-term) scattering effects. Good agreement between the experimental and theoretical results is observed, demonstrating that first-principles calculations of hyper-Raman intensities are now possible for large molecules such as R6G. Such agreement indicates that RHR spectroscopy will now be a routine aid for probing multiphoton processes. This work further shows that optimization of molecular properties to enhance either A- or B-term scattering might yield molecules with significantly enhanced two-photon properties.

Original language	English (US)
Pages (from-to)	14590-14592
Number of pages	3
Journal	Journal of the American Chemical Society
Volume	133
Issue number	37
DOIs	https://doi.org/10.1021/ja2054622
State	Published - Sep 21 2011

All Science Journal Classification (ASJC) codes

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

Access to Document

10.1021/ja2054622

Cite this

@article{bb7b050d21e14c898d1f5f90f3779a6f,

title = "Probing two-photon properties of molecules: Large non-condon effects dominate the resonance hyper-Raman scattering of rhodamine 6G",

abstract = "Experimentally measured resonance hyper-Raman (RHR) spectra spanning the S 1 ← S 0, S 2 ← S 0, and S 3 ← S 0 transitions in rhodamine 6G (R6G) have been recorded. These spectra are compared to the results of first-principles calculations of the RHR intensity that include both Franck-Condon (A-term) and non-Condon (B-term) scattering effects. Good agreement between the experimental and theoretical results is observed, demonstrating that first-principles calculations of hyper-Raman intensities are now possible for large molecules such as R6G. Such agreement indicates that RHR spectroscopy will now be a routine aid for probing multiphoton processes. This work further shows that optimization of molecular properties to enhance either A- or B-term scattering might yield molecules with significantly enhanced two-photon properties.",

author = "Milojevich, \{Chris B.\} and Silverstein, \{Daniel W.\} and Lasse Jensen and Camden, \{Jon P.\}",

year = "2011",

month = sep,

day = "21",

doi = "10.1021/ja2054622",

language = "English (US)",

volume = "133",

pages = "14590--14592",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

number = "37",

}

TY - JOUR

T1 - Probing two-photon properties of molecules

T2 - Large non-condon effects dominate the resonance hyper-Raman scattering of rhodamine 6G

AU - Milojevich, Chris B.

AU - Silverstein, Daniel W.

AU - Jensen, Lasse

AU - Camden, Jon P.

PY - 2011/9/21

Y1 - 2011/9/21

N2 - Experimentally measured resonance hyper-Raman (RHR) spectra spanning the S 1 ← S 0, S 2 ← S 0, and S 3 ← S 0 transitions in rhodamine 6G (R6G) have been recorded. These spectra are compared to the results of first-principles calculations of the RHR intensity that include both Franck-Condon (A-term) and non-Condon (B-term) scattering effects. Good agreement between the experimental and theoretical results is observed, demonstrating that first-principles calculations of hyper-Raman intensities are now possible for large molecules such as R6G. Such agreement indicates that RHR spectroscopy will now be a routine aid for probing multiphoton processes. This work further shows that optimization of molecular properties to enhance either A- or B-term scattering might yield molecules with significantly enhanced two-photon properties.

AB - Experimentally measured resonance hyper-Raman (RHR) spectra spanning the S 1 ← S 0, S 2 ← S 0, and S 3 ← S 0 transitions in rhodamine 6G (R6G) have been recorded. These spectra are compared to the results of first-principles calculations of the RHR intensity that include both Franck-Condon (A-term) and non-Condon (B-term) scattering effects. Good agreement between the experimental and theoretical results is observed, demonstrating that first-principles calculations of hyper-Raman intensities are now possible for large molecules such as R6G. Such agreement indicates that RHR spectroscopy will now be a routine aid for probing multiphoton processes. This work further shows that optimization of molecular properties to enhance either A- or B-term scattering might yield molecules with significantly enhanced two-photon properties.

UR - https://www.scopus.com/pages/publications/80052789506

UR - https://www.scopus.com/pages/publications/80052789506#tab=citedBy

U2 - 10.1021/ja2054622

DO - 10.1021/ja2054622

M3 - Article

C2 - 21851085

AN - SCOPUS:80052789506

SN - 0002-7863

VL - 133

SP - 14590

EP - 14592

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 37

ER -

Probing two-photon properties of molecules: Large non-condon effects dominate the resonance hyper-Raman scattering of rhodamine 6G

Abstract

All Science Journal Classification (ASJC) codes

Access to Document

Other files and links

Fingerprint

Cite this