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Title: Quantum coherent control of H3+ formation in strong fields

Journal Article · · Journal of Chemical Physics
DOI: https://doi.org/10.1063/1.5070067 · OSTI ID:1610694

Quantum coherent control (QCC) has been successfully demonstrated experimentally and theoretically for two- and three-photon optical excitation of atoms and molecules. Here, we explore QCC using spectral phase functions with a single spectral phase step for controlling the yield of H3+ from methanol under strong laser field excitation. We observe a significant and systematic enhanced production of H3+ when a negative 3/4 $$π$$ phase step is applied near the low energy region of the laser spectrum and when a positive 3/4 $$π$$ phase step is applied near the high energy region of the laser spectrum. In some cases, most notably the HCO+ fragment, we found the enhancement exceeded the yield measured for transform limited pulses. The observation of enhanced yield is surprising and far from the QCC prediction of yield suppression. The observed QCC enhancement implies an underlying strong field process responsible for polyatomic fragmentation controllable by easy to reproduce shaped pulses.

Research Organization:
Michigan State Univ., East Lansing, MI (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0002325
OSTI ID:
1610694
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 4 Vol. 150; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

References (32)

Control of Molecular Fragmentation Using Binary Phase-Shaped Femtosecond Laser Pulses journal October 2006
The fragmentation of doubly charged methanol journal March 1992
Wavepacket dancing: Achieving chemical selectivity by shaping light pulses journal December 1989
Stimulated Emission Enhancement Using Shaped Pulses journal March 2016
Coherence chemistry: controlling chemical reactions [with lasers] journal December 1989
Photodissociation Dynamics of Acetophenone and Its Derivatives with Intense Nonresonant Femtosecond Pulses journal March 2011
Coherent quantum control of two-photon transitions by a femtosecond laser pulse journal November 1998
H2 roaming chemistry and the formation of H3+ from organic molecules in strong laser fields journal December 2018
Mechanisms and time-resolved dynamics for trihydrogen cation (H3 +) formation from organic molecules in strong laser fields journal July 2017
Efficient ejection of H3+ from hydrocarbon molecules induced by ultrashort intense laser fields journal September 2008
Theoretical study of unimolecular decomposition of allene cations journal December 2008
Population and coherence control by three-pulse four-wave mixing journal September 1999
Molecular π pulses: Population inversion with positively chirped short pulses journal August 2000
Substituent effects on H 3 + formation via H 2 roaming mechanisms from organic molecules under strong-field photodissociation journal December 2018
Excitation of H + 2 with one-cycle laser pulses: shaped post-laser-field electronic oscillations, generation of higher- and lower-order harmonics journal December 2016
High-harmonic generation and correlated two-electron multiphoton ionization with elliptically polarized light journal November 1994
Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses journal August 1999
Coherent phase control of resonance-mediated ( 2 + 1 ) three-photon absorption journal March 2007
High-order-harmonic generation from coherent electron wave packets in atoms and molecules as a tool for monitoring attosecond electrons journal March 2012
Steering Proton Migration in Hydrocarbons Using Intense Few-Cycle Laser Fields journal May 2016
Teaching lasers to control molecules journal March 1992
Plasma perspective on strong field multiphoton ionization journal September 1993
Precision Measurement of Strong Field Double Ionization of Helium journal August 1994
Role of Electron Localization in Intense-Field Molecular Ionization journal October 1995
Temporal Coherent Control in Two-Photon Transitions: From Optical Interferences to Quantum Interferences journal April 1997
Transform-Limited Pulses Are Not Optimal for Resonant Multiphoton Transitions journal January 2001
Two Photon Absorption and Coherent Control with Broadband Down-Converted Light journal July 2004
Quantitative investigation of the multiphoton intrapulse interference phase scan method for simultaneous phase measurement and compensation of femtosecond laser pulses journal January 2006
Interference without an interferometer: a different approach to measuring, compressing, and shaping ultrashort laser pulses journal January 2008
Photon-echo detection by six-wave mixing journal January 1988
Transform-Limited Pulses Are Not Optimal for Resonant Multiphoton Transitions text January 2001
Excitation of H$_{2}^{+}$ with one-cycle laser pulses: Shaped post-laser-field electronic oscillations, generation of higher- and lower-order harmonics text January 2016

Cited By (1)

Strong-field control of H3+ production from methanol dications: Selecting between local and extended formation mechanisms journal February 2020