TY  - JOUR
A1  - Beyvers, Stephanie
A1  - Ohtsuki, Y
A1  - Saalfrank, Peter
T1  - Optimal control in a dissipative system : vibrational excitation of CO/Cu(100) by IR pulses
N2  - The question as to whether state-selective population of molecular vibrational levels by shaped infrared laser pulses is possible in a condensed phase environment is of central importance for such diverse fields as time-resolved spectroscopy, quantum computing, or "vibrationally mediated chemistry." This question is addressed here for a model system, representing carbon monoxide adsorbed on a Cu(100) surface. Three of the six vibrational modes are considered explicitly, namely, the CO stretch vibration, the CO-surface vibration, and a frustrated translation. Optimized infrared pulses for state-selective excitation of "bright" and "dark" vibrational levels are designed by optimal control theory in the framework of a Markovian open-system density matrix approach, with energy flow to substrate electrons and phonons, phase relaxation, and finite temperature accounted for. The pulses are analyzed by their Husimi "quasiprobability" distribution in time-energy space.
Y1  - 2006
UR  - http://jcp.aip.org/
U6  - https://doi.org/10.1063/1.2206593
SN  - 0021-9606
ER  - 
TY  - JOUR
A1  - Saalfrank, Peter
A1  - Nest, Mathias
A1  - Andrianov, Igor V.
A1  - Klamroth, Tillmann
A1  - Kroner, Dominic
A1  - Beyvers, Stephanie
T1  - Quantum dynamics of laser-induced desorption from metal and semiconductor surfaces, and related phenomena
N2  - Recent progress towards a quantum theory of laser-induced desorption and related phenomena is reviewed, for specific examples. These comprise the photodesorption of NO from Pt(111), the scanning tunnelling microscope and laser- induced desorption and switching of H at Si(100), and the electron stimulated desorption and dissociation of CO at Ru(0001). The theoretical methods used for nuclear dynamics range from open-system density matrix theory over nonadiabatically coupled multi-state models to electron-nuclear wavepackets. Also, aspects of time-dependent spectroscopy to probe ultrafast nonadiabatic processes at surfaces will be considered for the example of two-photon photoemission of solvated electrons in ice layers on Cu(111)
Y1  - 2006
UR  - http://iopscience.iop.org/0953-8984/18/30/S05/pdf/0953-8984_18_30_S05.pdf
U6  - https://doi.org/10.1088/0953-8984/18/30/S05
SN  - 1361-648X
SN  - 0953-8984
VL  - 18
IS  - 30
SP  - S1425
EP  - S1459
PB  - IOP Publ.
CY  - Bristol
ER  -