TY - JOUR A1 - Banerjee, Shiladitya A1 - Stüker, Tony A1 - Saalfrank, Peter T1 - Vibrationally resolved optical spectra of modified diamondoids obtained from time-dependent correlation function methods JF - Physical chemistry, chemical physics : PCCP ; a journal of European chemical societies N2 - Optical properties of modified diamondoids have been studied theoretically using vibrationally resolved electronic absorption, emission and resonance Raman spectra. A time-dependent correlation function approach has been used for electronic two-state models, comprising a ground state (g) and a bright, excited state (e), the latter determined from linear-response, time-dependent density functional theory (TD-DFT). The harmonic and Condon approximations were adopted. In most cases origin shifts, frequency alteration and Duschinsky rotation in excited states were considered. For other cases where no excited state geometry optimization and normal mode analysis were possible or desired, a short-time approximation was used. The optical properties and spectra have been computed for (i) a set of recently synthesized sp2/sp3 hybrid species with C[double bond, length as m-dash]C double-bond connected saturated diamondoid subunits, (ii) functionalized (mostly by thiol or thione groups) diamondoids and (iii) urotropine and other C-substituted diamondoids. The ultimate goal is to tailor optical and electronic features of diamondoids by electronic blending, functionalization and substitution, based on a molecular-level understanding of the ongoing photophysics. Y1 - 2015 U6 - https://doi.org/10.1039/C5CP02615F SN - 1463-9084 SN - 1463-9076 VL - 17 IS - 29 SP - 19656 EP - 19669 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Banerjee, Shiladitya A1 - Stueker, Tony A1 - Saalfrank, Peter T1 - Vibrationally resolved optical spectra of modified diamondoids obtained from time-dependent correlation function methods JF - Physical chemistry, chemical physics : a journal of European Chemical Societies N2 - Optical properties of modified diamondoids have been studied theoretically using vibrationally resolved electronic absorption, emission and resonance Raman spectra. A time-dependent correlation function approach has been used for electronic two-state models, comprising a ground state (g) and a bright, excited state (e), the latter determined from linear-response, time-dependent density functional theory (TD-DFT). The harmonic and Condon approximations were adopted. In most cases origin shifts, frequency alteration and Duschinsky rotation in excited states were considered. For other cases where no excited state geometry optimization and normal mode analysis were possible or desired, a short-time approximation was used. The optical properties and spectra have been computed for (i) a set of recently synthesized sp(2)/sp(3) hybrid species with CQC double-bond connected saturated diamondoid subunits, (ii) functionalized (mostly by thiol or thione groups) diamondoids and (iii) urotropine and other C-substituted diamondoids. The ultimate goal is to tailor optical and electronic features of diamondoids by electronic blending, functionalization and substitution, based on a molecular-level understanding of the ongoing photophysics. Y1 - 2015 U6 - https://doi.org/10.1039/c5cp02615f SN - 1463-9076 SN - 1463-9084 VL - 17 IS - 29 SP - 19656 EP - 19669 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Banerjee, Shiladitya A1 - Saalfrank, Peter T1 - Vibrationally resolved absorption, emission and resonance Raman spectra of diamondoids: a study based on time-dependent correlation functions JF - Physical chemistry, chemical physics : a journal of European Chemical Societies Y1 - 2014 U6 - https://doi.org/10.1039/c3cp53535e SN - 1463-9076 SN - 1463-9084 VL - 16 IS - 1 SP - 144 EP - 158 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Banerjee, Shiladitya A1 - Saalfrank, Peter T1 - Vibrationally resolved absorption, emission and resonance Raman spectra of diamondoids : a study based on time- dependent correlation functions Y1 - 2014 UR - http://pubs.rsc.org/en/content/articlehtml/2014/cp/c3cp53535e U6 - https://doi.org/10.1039/C3CP53535E ER - TY - JOUR A1 - Banerjee, Shiladitya A1 - Kröner, Dominik A1 - Saalfrank, Peter T1 - Resonance Raman and vibronic absorption spectra with Duschinsky rotation from a time-dependent perspective application to beta-carotene JF - The journal of chemical physics : bridges a gap between journals of physics and journals of chemistr N2 - The time-dependent approach to electronic spectroscopy, as popularized by Heller and co-workers in the 1980s, is applied here in conjunction with linear-response, time-dependent density functional theory to study vibronic absorption and resonance Raman spectra of beta-carotene, with and without a solvent. Two-state models, the harmonic and the Condon approximations are used in order to do so. A new code has been developed which includes excited state displacements, vibrational frequency shifts, and Duschinsky rotation, i.e., mode mixing, for both non-adiabatic spectroscopies. It is shown that Duschinsky rotation has a pronounced effect on the resonance Raman spectra of beta-carotene. In particular, it can explain a recently found anomalous behaviour of the so-called nu(1) peak in resonance Raman spectra [N. Tschirner, M. Schenderlein, K. Brose, E. Schlodder, M. A. Mroginski, C. Thomsen, and P. Hildebrandt, Phys. Chem. Chem. Phys. 11, 11471 (2009)], which shifts with the change in excitation wavelength. Y1 - 2012 U6 - https://doi.org/10.1063/1.4748147 SN - 0021-9606 VL - 137 IS - 22 PB - American Institute of Physics CY - Melville ER -