Details
| Original language | English |
|---|---|
| Article number | 043202 |
| Journal | Physical review letters |
| Volume | 127 |
| Issue number | 4 |
| Early online date | 20 Jul 2021 |
| Publication status | Published - 23 Jul 2021 |
Abstract
The vibrational motion of molecules represents a fundamental example of an anharmonic oscillator. Using a prototype molecular system, HeH+, we demonstrate that appropriate laser pulses make it possible to drive the nuclear motion in the anharmonic potential of the electronic ground state, increasing its energy above the potential barrier and facilitating dissociation by purely vibrational excitation. We find excellent agreement between the frequency-dependent response of the helium hydride molecular cation to both classical and quantum mechanical simulations, thus removing any ambiguities through electronic excitation. Our results provide access to the rich dynamics of anharmonic quantum oscillator systems and pave the way to state-selective control schemes in ground-state chemistry by the adequate choice of the laser parameters.
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In: Physical review letters, Vol. 127, No. 4, 043202, 23.07.2021.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Laser-Driven Anharmonic Oscillator
T2 - Ground-State Dissociation of the Helium Hydride Molecular Ion by Midinfrared Pulses
AU - Wustelt, Philipp
AU - Oppermann, Florian
AU - Mhatre, Saurabh
AU - Kübel, Matthias
AU - Sayler, A. Max
AU - Lein, Manfred
AU - Gräfe, Stefanie
AU - Paulus, Gerhard G.
N1 - Funding Information: The authors acknowledge funding by the Deutsche Forschungsgemeinschaft (DFG) in the frame of the Schwerpunktprogramm (SPP) 1840, Quantum Dynamics in Tailored Intense Fields. We thank L. Yue and W. Pfeiffer for fruitful discussions. We thank T. Weber and F. Ronneberger for technical assistance.
PY - 2021/7/23
Y1 - 2021/7/23
N2 - The vibrational motion of molecules represents a fundamental example of an anharmonic oscillator. Using a prototype molecular system, HeH+, we demonstrate that appropriate laser pulses make it possible to drive the nuclear motion in the anharmonic potential of the electronic ground state, increasing its energy above the potential barrier and facilitating dissociation by purely vibrational excitation. We find excellent agreement between the frequency-dependent response of the helium hydride molecular cation to both classical and quantum mechanical simulations, thus removing any ambiguities through electronic excitation. Our results provide access to the rich dynamics of anharmonic quantum oscillator systems and pave the way to state-selective control schemes in ground-state chemistry by the adequate choice of the laser parameters.
AB - The vibrational motion of molecules represents a fundamental example of an anharmonic oscillator. Using a prototype molecular system, HeH+, we demonstrate that appropriate laser pulses make it possible to drive the nuclear motion in the anharmonic potential of the electronic ground state, increasing its energy above the potential barrier and facilitating dissociation by purely vibrational excitation. We find excellent agreement between the frequency-dependent response of the helium hydride molecular cation to both classical and quantum mechanical simulations, thus removing any ambiguities through electronic excitation. Our results provide access to the rich dynamics of anharmonic quantum oscillator systems and pave the way to state-selective control schemes in ground-state chemistry by the adequate choice of the laser parameters.
UR - http://www.scopus.com/inward/record.url?scp=85111532549&partnerID=8YFLogxK
U2 - 10.1103/PhysRevLett.127.043202
DO - 10.1103/PhysRevLett.127.043202
M3 - Article
C2 - 34355921
AN - SCOPUS:85111532549
VL - 127
JO - Physical review letters
JF - Physical review letters
SN - 0031-9007
IS - 4
M1 - 043202
ER -