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T Seideman

Publications and source records attributed to T Seideman.

11 recordsLinked to original sources
PubMed2006

Quantifying desorption of saturated hydrocarbons from silicon with quantum calculations and scanning tunneling microscopy.

Electron stimulated desorption of cyclopentene from the Si(100)-(2 x 1) surface is studied experimentally with cryogenic UHV STM and theoretically with transport, electronic structure, and dynamical calculations. Unexpectedly for a saturated hydrocarbon on silicon, desorption is observed at bias magnitudes as low as 2.5 V, albeit the desorption yields are a factor of 500 to 1000 lower than previously reported for unsaturated molecules on silicon. The low threshold voltage for desorption is attributed to hybridization of the molecule with the silicon surface, which results in low-lying ionic resonances within 2-3 eV of the Fermi level. These resonances are long-lived, spatially localized, and displaced in equilibrium with respect to the neutral state. This study highlights the importance of nuclear dynamics in silicon-based molecular electronics and suggests new guidelines for the control of such dynamics.

Journal Article↗
PubMed2005

Intrinsically biased electrocapacitive catalysis.

We propose the application of the contact potential from metal-metal junctions or the built-in potential of semiconductor p-n junctions to induce or catalyze chemical reactions. Free of external sources, this intrinsic potential across microscale and nanoscale vacuum gaps establishes electric fields in excess of 10(7) Vm. The electrostatic potential energy of these fields can be converted into useful chemical energy. As an example, we focus on the production of superthermal gas ions to drive reactions. Analysis indicates that this intrinsically biased electrocapacitive catalysis can achieve locally directed ion energies up to a few electron volts and local gas temperature boosts in excess of 10(4) K. Practical considerations for implementation and experimental tests are considered.

Journal Article↗
PubMed2001

Above-threshold dissociative ionization in the intermediate intensity regime.

The problem of dissociative ionization at intermediate intensities ( 10(10)-10(12) W cm(-2)) was studied using the example of I2 and the technique of velocity map imaging. Several new phenomena were observed, including a continuous distribution of recoil energies peaked at zero-kinetic energy, a set of constant dissociative ionic states, and strong anisotropy of the fragment velocity distribution that is diminished by intermediate resonances.

Journal Article↗
PubMed2000

Inducing desorption of organic molecules with a scanning tunneling microscope: theory and experiments.

A scanning-tunneling microscope has been used to induce efficient local desorption of benzene from Si(100) at low currents (<100 pA), sample biases (approximately -2.4 V) and temperatures (22 K). A theoretical model based upon first principles electronic structure calculations and quantum mechanical wave packet dynamics describes this process as occurring via transient ionization of a pi state of the adsorbed molecule. This model accounts for the unexpected efficiency and sharp threshold of the yield.

Adsorption↗
PubMed2000

Three dimensional alignment of molecules using elliptically polarized laser fields

We demonstrate, theoretically and experimentally, that an intense, elliptically polarized, nonresonant laser field can simultaneously force all three axes of a molecule to align along given axes fixed in space, thus inhibiting the free rotation in all three Euler angles. Theoretically, the effect is illustrated through time dependent quantum mechanical calculations. Experimentally, 3, 4-dibromothiophene molecules are aligned with a nanosecond laser pulse. The alignment is probed by 2D ion imaging of the fragments from a 20 fs laser pulse induced Coulomb explosion.

Journal Article↗
PubMed2000

Direct observation of a breit-wigner phase of a wave function

The Breit-Wigner phase of a wave function was obtained by measuring the interference between two independent ionization paths of a molecule. The state of interest was present in only one of the paths, thereby producing a phase shift in the observed signal. An analytical theory was used to determine the phase of the wave function from the observable.

Journal Article↗
PubMed2000

Towards disentangling coupled electronic-vibrational dynamics in ultrafast non-adiabatic processes

Femtosecond time-resolved photoelectron spectroscopy is emerging as a new technique for investigating polyatomic excited state dynamics. Due to the sensitivity of photoelectron spectroscopy to both electronic configurations and vibrational dynamics, it is well suited to the study of non-adiabatic processes such as internal conversion, which often occur on sub-picosecond time scales. We discuss the technical requirements for such experiments, including lasers systems, energy- and angle-resolved photoelectron spectrometers and new detectors for coincidence experiments. We present a few examples of these methods applied to problems in diatomic wavepacket dynamics and ultrafast non-adiabatic processes in polyatomic molecules.

Journal Article↗
PubMed2000

Controlling organic reactions on silicon surfaces with a scanning tunneling microscope: theoretical and experimental studies of resonance-mediated desorption.

The dynamics of tip-induced, resonance-mediated bond-breaking in complex organic adsorbates is studied theoretically and experimentally. Desorption of benzene from a Si(100) surface is found to be efficient and sensitive to voltage, the measured yield rising from below 10(-10) to ca. 10(-6) per electron within a ca. 0.8 V range at low (< 100 pA) current. A theoretical model, based upon first principles electronic structure calculations and quantum mechanical wavepacket simulations, traces these observations to multi-mode dynamics triggered by a transition into a cationic resonance. The model is generalized to provide understanding of, and suggest a means of control over, the behaviour of different classes of organic adsorbates under tunneling current.

Journal Article↗