Detection of heating in current-carrying molecular junctions by Raman scattering

Ioffe, Z. M.; Shamai, Tamar; Ophir, Ayelet; Noy, Gilad; Yutsis, Ilan; Kfir, Kobi; Cheshnovsky, Ori; Selzer, Yoram

doi:10.1038/nnano.2008.304

Cited by 247 publications

(292 citation statements)

References 30 publications

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“…The functionality and stability of electron-conducting molecular junctions are directly linked to heating and cooling effects experienced by molecular vibrational modes in biased situations [4,[35][36][37][38][39][40][41]. In particular, junction heating and breakdown may occur once the bias voltage exceeds typical molecular vibrational frequencies, when the electronic levels are situated within the bias window, if energy dissipation from the molecule to its environment is not efficient.…”

Section: Application: Molecular Rectifiermentioning

confidence: 99%

Path-integral simulations with fermionic and bosonic reservoirs: Transport and dissipation in molecular electronic junctions

Simine¹,

Segal²

2013

The Journal of Chemical Physics

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We expand iterative numerically-exact influence functional path-integral tools and present a method capable of following the nonequilibrium time evolution of subsystems coupled to multiple bosonic and fermionic reservoirs simultaneously. Using this method, we study the real-time dynamics of charge transfer and vibrational mode excitation in an electron conducting molecular junction. We focus on nonequilibrium vibrational effects, particularly, the development of vibrational instability in a current-rectifying junction. Our simulations are performed by assuming large molecular vibrational anharmonicity (or low temperature). This allows us to truncate the molecular vibrational mode to include only a two-state system. Exact numerical results are compared to perturbative Master equation calculations demonstrating an excellent agreement in the weak electron-phonon coupling regime. Significant deviations take place only at strong coupling. Our simulations allow us to quantify the contribution of different transport mechanisms, coherent dynamics and inelastic transport, in the overall charge current. This is done by studying two model variants: The first admits inelastic electron transmission only, while the second one allows for both coherent and incoherent pathways.

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Section: Application: Molecular Rectifiermentioning

confidence: 99%

Path-integral simulations with fermionic and bosonic reservoirs: Transport and dissipation in molecular electronic junctions

Simine¹,

Segal²

2013

The Journal of Chemical Physics

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“…Vibrational signatures of molecular bridges have also been observed in inelastic electron tunneling spectroscopy. [35][36][37] New experimental techniques, [47][48][49] e.g., based on Raman spectroscopy, allow the characterization of the nonequilibrium state of the vibrational degrees of freedom in a molecular junction. The experimental progress has stimulated much interest in the theoretical modeling and simulation of vibrationally coupled electron transport in molecular junctions.…”

Section: Introductionmentioning

confidence: 99%

Numerically exact, time-dependent treatment of vibrationally coupled electron transport in single-molecule junctions

Wang

Pshenichnyuk

Härtle

et al. 2011

The Journal of Chemical Physics

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The multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) theory within second quantization representation of the Fock space, a novel numerically exact methodology to treat manybody quantum dynamics for systems containing identical particles, is applied to study the effect of vibrational motion on electron transport in a generic model for single-molecule junctions. The results demonstrate the importance of electronic-vibrational coupling for the transport characteristics. For situations where the energy of the bridge state is located close to the Fermi energy, the simulations show the time-dependent formation of a polaron state that results in a pronounced suppression of the current corresponding to the phenomenon of phonon blockade. We show that this phenomenon cannot be explained solely by the polaron shift of the energy but requires methods that incorporate the dynamical effect of the vibrations on the transport. The accurate results obtained with the ML-MCTDH in this parameter regime are compared to results of nonequilibrium Green's function theory.

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“…More recently, noise (23)(24)(25)(26), nonlinear response (e.g., negative differential heat conductance), and control by external stimuli (27,28) have been examined. An important driving factor in this growing interest is the development of experimental capabilities that greatly improve on the ability to gauge temperatures (and "effective" temperatures in nonequilibrium systems) with high spatial and thermal resolutions (29)(30)(31)(32)(33)(34)(35)(36)(37)(38)(39)(40)(41)(42)(43) and to infer from such measurement the underlying heat transport processes. In particular, vibrational energy transport/ heat conduction in molecular layers and junctions has recently been characterized using different probes (6,19,(44)(45)(46)(47)(48)(49)(50)(51)(52).…”

mentioning

confidence: 99%

Electron transfer across a thermal gradient

Craven

Nitzan

2016

Proc. Natl. Acad. Sci. U.S.A.

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Charge transfer is a fundamental process that underlies a multitude of phenomena in chemistry and biology. Recent advances in observing and manipulating charge and heat transport at the nanoscale, and recently developed techniques for monitoring temperature at high temporal and spatial resolution, imply the need for considering electron transfer across thermal gradients. Here, a theory is developed for the rate of electron transfer and the associated heat transport between donor-acceptor pairs located at sites of different temperatures. To this end, through application of a generalized multidimensional transition state theory, the traditional Arrhenius picture of activation energy as a single point on a free energy surface is replaced with a bithermal property that is derived from statistical weighting over all configurations where the reactant and product states are equienergetic. The flow of energy associated with the electron transfer process is also examined, leading to relations between the rate of heat exchange among the donor and acceptor sites as functions of the temperature difference and the electronic driving bias. In particular, we find that an open electron transfer channel contributes to enhanced heat transport between sites even when they are in electronic equilibrium. The presented results provide a unified theory for charge transport and the associated heat conduction between sites at different temperatures. T he study of electronic transport in molecular nanojunctions naturally involves consideration of inelastic transport, where the transporting electron can exchange energy with underlying nuclear motions (1, 2). Such studies have been motivated by the use of inelastic tunneling spectroscopy, and more recently Raman spectroscopy, as diagnostic tools on one hand, and by considerations of junction stability on the other. In parallel, there has been an increasing interest in vibrational heat transport in nanostructures and their interfaces with bulk substrates (3-11) focusing on structure-transport correlations (12-15), moleculesubstrate coupling (16-18), ballistic and diffusive transport processes (11,19), and rectification (20-22). More recently, noise (23-26), nonlinear response (e.g., negative differential heat conductance), and control by external stimuli (27, 28) have been examined. An important driving factor in this growing interest is the development of experimental capabilities that greatly improve on the ability to gauge temperatures (and "effective" temperatures in nonequilibrium systems) with high spatial and thermal resolutions (29-43) and to infer from such measurement the underlying heat transport processes. In particular, vibrational energy transport/ heat conduction in molecular layers and junctions has recently been characterized using different probes (6,19,(44)(45)(46)(47)(48)(49)(50)(51)(52).The interplay between charge and energy (electronic and nuclear) transport (53-60) is of particular interest as it pertains to the performance of energy-conversion devices, such as therm...

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Detection of heating in current-carrying molecular junctions by Raman scattering

Cited by 247 publications

References 30 publications

Path-integral simulations with fermionic and bosonic reservoirs: Transport and dissipation in molecular electronic junctions

Path-integral simulations with fermionic and bosonic reservoirs: Transport and dissipation in molecular electronic junctions

Numerically exact, time-dependent treatment of vibrationally coupled electron transport in single-molecule junctions

Electron transfer across a thermal gradient

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