Simulation of structured 4T1→6A1 emission bands of Mn2+ impurity in Zn2SiO4: A first-principle methodology

Kretov, M. K.; Iskandarova, I. M.; Потапкин, Б. В.; Scherbinin, A. V.; Srivastava, A.M.; Stepanov, N. F.

doi:10.1016/j.jlumin.2012.03.067

Cited by 44 publications

(27 citation statements)

References 43 publications

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“…The line width G f is taken from the generation function for the simulation of the profile of the vibration spectra within the Lax-Pekar model. [47][48][49] The calculated value for G f is about 1.6 Â 10 14 s À1 for the S 1 state of the studied molecules.…”

Section: Huang-rhys Factors and Vibrational Relaxation Widthsmentioning

confidence: 79%

First-principles method for calculating the rate constants of internal-conversion and intersystem-crossing transitions

Valiev

Cherepanov

Baryshnikov

et al. 2018

Phys. Chem. Chem. Phys.

100

161

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A method for calculating the rate constants for internal-conversion (k) and intersystem-crossing (k) processes within the adiabatic and Franck-Condon (FC) approximations is proposed. The applicability of the method is demonstrated by calculation of k and k for a set of organic and organometallic compounds with experimentally known spectroscopic properties. The studied molecules were pyrromethene-567 dye, psoralene, hetero[8]circulenes, free-base porphyrin, naphthalene, and larger polyacenes. We also studied fac-Alq and fac-Ir(ppy), which are important molecules in organic light emitting diodes (OLEDs). The excitation energies were calculated at the multi-configuration quasi-degenerate second-order perturbation theory (XMC-QDPT2) level, which is found to yield excitation energies in good agreement with experimental data. Spin-orbit coupling matrix elements, non-adiabatic coupling matrix elements, Huang-Rhys factors, and vibrational energies were calculated at the time-dependent density functional theory (TDDFT) and complete active space self-consistent field (CASSCF) levels. The computed fluorescence quantum yields for the pyrromethene-567 dye, psoralene, hetero[8]circulenes, fac-Alq and fac-Ir(ppy) agree well with experimental data, whereas for the free-base porphyrin, naphthalene, and the polyacenes, the obtained quantum yields significantly differ from the experimental values, because the FC and adiabatic approximations are not accurate for these molecules.

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Section: Huang-rhys Factors and Vibrational Relaxation Widthsmentioning

confidence: 79%

First-principles method for calculating the rate constants of internal-conversion and intersystem-crossing transitions

Valiev

Cherepanov

Baryshnikov

et al. 2018

Phys. Chem. Chem. Phys.

100

161

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“…To produce additional insights, we have also calculated ω  S ( ) (equation (5)) and ω  L ( ) (equation (2)) with an additional assumption, namely that phonon modes that contribute to the luminescence lineshape are those of the unperturbed host [51,52]. For this purpose we have determined the vibrational modes of bulk diamond using density functional perturbation theory [53], reproducing earlier calculations [54].…”

Section: First-principles Approachmentioning

confidence: 99%

First-principles theory of the luminescence lineshape for the triplet transition in diamond NV centres

et al. 2014

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In this work we present theoretical calculations and analysis of the vibronic structure of the spin-triplet optical transition in diamond nitrogen-vacancy (NV) centres. The electronic structure of the defect is described using accurate firstprinciples methods based on hybrid functionals. We devise a computational methodology to determine the coupling between electrons and phonons during an optical transition in the dilute limit. As a result, our approach yields a smooth spectral function of electron-phonon coupling and includes both quasi-localized and bulk phonons on equal footings. The luminescence lineshape is determined via the generating function approach. We obtain a highly accurate description of the luminescence band, including all key parameters such as the Huang-Rhys factor, the Debye-Waller factor, and the frequency of the dominant phonon mode. More importantly, our work provides insight into the vibrational structure of NV centres, in particular the role of local modes and vibrational resonances. In particular, we find that the pronounced mode at 65 meV is a vibrational resonance, and we quantify localization properties of this mode. These excellent results for the benchmark diamond (NV) centre provide confidence that the procedure can be applied to other defects, including alternative systems that are being considered for applications in quantum information processing.

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“…[1][2][3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19][20] These approaches have been successfully applied to calculations of spectral band shapes for a large number of systems containing both inorganic [3][4][5][6][7] and organic [21][22][23][24][25][26][27][28] chromophores. However, this information can hardly be extracted directly from experimental data.…”

Section: Introductionmentioning

confidence: 99%

Vibronic bandshape of the absorption spectra of dibenzoylmethanatoboron difluoride derivatives: analysis based on ab initio calculations

Rukin

Freidzon

Scherbinin

et al. 2015

Phys. Chem. Chem. Phys.

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The nature of absorption bandshapes of dibenzoylmethanatoboron difluoride (DBMBF2) dye substituted in ortho-, meta-, and para-positions of the phenyl ring is investigated using DFT and TDDFT with the range-separated hybrid CAM-B3LYP functional and the 6-311G(d,p) basis set. The solvent effects are taken into account within the polarized continuum model. The vibronic bandshape is simulated using a time-dependent linear coupling model with a vertical gradient approach through an original code. For flexible chromophores, the spectra of individual conformers are summed up with Boltzmann factors. It is shown that the long-wavelength absorption bandshape of DBMBF2 derivatives is determined by three factors: the relative statistical weights of conformers with different electronic absorption patterns, the relative position and intensity of the second low-energy electronic transition, and the vibronic structure of individual electronic peaks. The latter is governed by the relationship between the hard vibrational modes, which contribute to vibronic progression, and soft modes, which provide broadening of the peaks. The simulated spectra of the dyes in the study are generally consistent with the available experimental data and explain the observed spectral features.

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Simulation of structured 4T1→6A1 emission bands of Mn2+ impurity in Zn2SiO4: A first-principle methodology

Cited by 44 publications

References 43 publications

First-principles method for calculating the rate constants of internal-conversion and intersystem-crossing transitions

First-principles method for calculating the rate constants of internal-conversion and intersystem-crossing transitions

First-principles theory of the luminescence lineshape for the triplet transition in diamond NV centres

Vibronic bandshape of the absorption spectra of dibenzoylmethanatoboron difluoride derivatives: analysis based on ab initio calculations

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