Franck–Condon Blockade and Aggregation‐Modulated Conductance in Molecular Devices Using Aggregation‐Induced Emission‐Active Molecules

Tian, Guangjun; Sun, Dexian; Zhang, Yuegang; Yu, Xi

doi:10.1002/anie.201900731

Cited by 41 publications

(16 citation statements)

References 41 publications

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“…The fluorescence spectra were calculated by the well-known mirror-image rule (47) from absorbance, where the energies of 0-0 transitions were slightly blue-shifted by 62 meV to match the experimental observations. All vibrational integrals were calculated by the DynaVib software (48).…”

Section: Ab Initio Calculationmentioning

confidence: 99%

Real-time detection of single-molecule reaction by plasmon-enhanced spectroscopy

Duan

et al. 2020

Sci. Adv.

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Determining structural transformations of single molecules (SMs) is an important fundamental scientific endeavor. Optical spectroscopies are the dominant tools used to unravel the physical and chemical features of individual molecules and have substantially contributed to surface science and biotechnology. In particular, Raman spectroscopy can identify reaction intermediates and reveal underlying reaction mechanisms; however, SM Raman experiments are subject to intrinsically weak signal intensities and considerable signal attenuation within the spectral dispersion systems of the spectrometer. Here, to monitor the structural transformation of an SM on the millisecond time scale, a plasmonic nanocavity substrate has been used to enable Raman vibrational and fluorescence spectral signals to be simultaneously collected and correlated, which thus allows a detection of photo-induced bond cleavage between the xanthene and phenyl group of a single rhodamine B isothiocyanate molecule in real time. This technique provides a novel method for investigating light-matter interactions and chemical reactions at the SM level.

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Section: Ab Initio Calculationmentioning

confidence: 99%

Real-time detection of single-molecule reaction by plasmon-enhanced spectroscopy

Duan

et al. 2020

Sci. Adv.

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“…[1b] Meanwhile,the radiative and nonradiative decay from T 1 to S 0 also needs to be effectively suppressed to improve the phosphorescence efficiency. [7] There are several strategies in terms of molecular design to realize organic RTP: 1) Introducing the carbonyl units, [4,8] heteroatoms, [9] heavy atoms, [10] or resonance-induced spin flipping [11] to subsequently induce the strong spin-orbit coupling (SOC) effect, which contributes to higher k ISC ,r esulting in the larger population of triplet excitons;2 )effectively suppressing the non-radiative decay of low-lying triplet excitons through inhibiting the molecular nonradiative decay,e ither through crystallization, [12] one of the most commonly adopted methods; [13] or via halogenbonding, [14] intramolecular H-aggregation, [15] aromatic guest inclusion in supramolecular host, [16] and so on.…”

mentioning

confidence: 99%

Organic Room‐Temperature Phosphorescence with Strong Circularly Polarized Luminescence Based on Paracyclophanes

et al. 2019

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Pure organic materials with intrinsic room‐temperature phosphorescence typically rely on heavy atoms or heteroatoms. Two different strategies towards constructing organic room‐temperature phosphorescence (RTP) species based upon the through‐space charge transfer (TSCT) unit of [2.2]paracyclophane (PCP) were demonstrated. Materials with bromine atoms, PCP‐BrCz and PPCP‐BrCz, exhibit RTP lifetime of around 100 ms. Modulating the PCP core with non‐halogen‐containing electron‐withdrawing units, PCP‐TNTCz and PCP‐PyCNCz, successfully elongate the RTP lifetime to 313.59 and 528.00 ms, respectively, the afterglow of which is visible for several seconds under ambient conditions. The PCP‐TNTCz and PCP‐PyCNCz enantiomers display excellent circular polarized luminescence with dissymmetry factors as high as −1.2×10−2 in toluene solutions, and decent RTP lifetime of around 300 ms for PCP‐TNTCz enantiomers in crystalline state.

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“…This implies overall the absence of electronic correlation between the tunneling events, although the electrons may encounter inelastic collisions. Poissonian behavior of the shot noise at the molecular scale may be construed within the Franck-Condon picture stemming from the resonant electronic transport between diverse charging states [79,80,81]. Following the charge stability plots, as demonstrated in Figure 7(e-f), there is no overlap in the Coulomb diamond edges around the zero bias.…”

Section: Shot Noise Characteristicsmentioning

confidence: 86%

Conformation controllable inelastic charge transport and shot noise behavior in metal-string single molecular devices

Roy

Sen

2020

Applied Surface Science

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It is often intriguing experimentally to take stock of how conformational changes in the device configuration may impact the overall charge transport behavior of single-molecule junctions. Based on the allied approach of density functional theory and non-equilibrium Green's function formalism, we explore here the effect of junction heterogeneity on inelastic charge transport in various metal-string based single-molecule devices. The constituent active elements being sensitive to the resonant levels, transition metal centers are found to influence stretching, bending, and torsional excitation modes, while rocking and scissoring modes are controlled largely by the axial ligands. For certain molecular conformations and electrode orientations, phonon-assisted quantum interference effect may crop up, leading to the suppression of higher wavenumber vibrational modes. The resulting inelastic spectra are likely to take the shape of dominant Fano resonance or anti-resonance, depending on whether phonons are emitted or absorbed. Such nanoscale quantum interference effect is manifested especially in those metal-string molecular junctions for which the energy gap (between localized and delocalized virtual states) lies well within the optical phonon energies (∆E |HOM O−LU M O| < 40 meV). It also turns out that single molecular shot noise can exhibit nearly Poissonian behavior if the inter-channel tunneling through frontier orbitals is accompanied by phonon absorption or emission following a slow relaxation process. Our results thus suggest that charge transport properties across metal-string complexes can be potentially tuned by selective architecture of the metal centers and also, by preferred orientation of nanoscale electrodes in a bid to build up molecular devices with desirable controllability.

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Franck–Condon Blockade and Aggregation‐Modulated Conductance in Molecular Devices Using Aggregation‐Induced Emission‐Active Molecules

Cited by 41 publications

References 41 publications

Real-time detection of single-molecule reaction by plasmon-enhanced spectroscopy

Real-time detection of single-molecule reaction by plasmon-enhanced spectroscopy

Organic Room‐Temperature Phosphorescence with Strong Circularly Polarized Luminescence Based on Paracyclophanes

Conformation controllable inelastic charge transport and shot noise behavior in metal-string single molecular devices

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