Control of photodissociation with the dynamic Stark effect induced by THz pulses
We demonstrate how dynamic Stark control can be achieved on molecular photodissociation in the dipole limit, using single-cycle (full width at half maximum) laser pulses in the terahertz (THz) regime. As the laser-molecule interaction follows the instantaneous electric field through the permanent di...
| Main Authors: | , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
American Physical Society
2020-03-01
|
| Series: | Physical Review Research |
| Online Access: | http://doi.org/10.1103/PhysRevResearch.2.013338 |
| _version_ | 1797211519725862912 |
|---|---|
| author | A. Tóth A. Csehi G. J. Halász Á. Vibók |
| author_facet | A. Tóth A. Csehi G. J. Halász Á. Vibók |
| author_sort | A. Tóth |
| collection | DOAJ |
| description | We demonstrate how dynamic Stark control can be achieved on molecular photodissociation in the dipole limit, using single-cycle (full width at half maximum) laser pulses in the terahertz (THz) regime. As the laser-molecule interaction follows the instantaneous electric field through the permanent dipoles, the molecular potentials dynamically oscillate and so do the crossings between them. In this paper, we consider rotating-vibrating diatomic molecules (two-dimensional description) and reveal the interplay between the dissociating wave packet and the dynamically fluctuating crossing seam located in the configuration space of the molecules spanned by the R vibrational and θ rotational coordinates. Our showcase example is the widely studied lithium fluoride molecule for which the two lowest Σ states are nonadiabatically coupled at an avoided crossing (AC); furthermore a low-lying pure repulsive Π state is energetically close. Optical pumping of the system in the ground state thus results in two dissociation channels: one indirect route via the AC in the ground Σ state and one direct path in the Π state. We show that applying THz control pulses with specific time delays relative to the pumping can significantly alter the population dynamics, as well as the kinetic energy and angular distribution of the photofragments. |
| first_indexed | 2024-04-24T10:27:47Z |
| format | Article |
| id | doaj.art-2a4541f8e27b42769237396fd0a811a3 |
| institution | Directory Open Access Journal |
| issn | 2643-1564 |
| language | English |
| last_indexed | 2024-04-24T10:27:47Z |
| publishDate | 2020-03-01 |
| publisher | American Physical Society |
| record_format | Article |
| series | Physical Review Research |
| spelling | doaj.art-2a4541f8e27b42769237396fd0a811a32024-04-12T16:51:40ZengAmerican Physical SocietyPhysical Review Research2643-15642020-03-012101333810.1103/PhysRevResearch.2.013338Control of photodissociation with the dynamic Stark effect induced by THz pulsesA. TóthA. CsehiG. J. HalászÁ. VibókWe demonstrate how dynamic Stark control can be achieved on molecular photodissociation in the dipole limit, using single-cycle (full width at half maximum) laser pulses in the terahertz (THz) regime. As the laser-molecule interaction follows the instantaneous electric field through the permanent dipoles, the molecular potentials dynamically oscillate and so do the crossings between them. In this paper, we consider rotating-vibrating diatomic molecules (two-dimensional description) and reveal the interplay between the dissociating wave packet and the dynamically fluctuating crossing seam located in the configuration space of the molecules spanned by the R vibrational and θ rotational coordinates. Our showcase example is the widely studied lithium fluoride molecule for which the two lowest Σ states are nonadiabatically coupled at an avoided crossing (AC); furthermore a low-lying pure repulsive Π state is energetically close. Optical pumping of the system in the ground state thus results in two dissociation channels: one indirect route via the AC in the ground Σ state and one direct path in the Π state. We show that applying THz control pulses with specific time delays relative to the pumping can significantly alter the population dynamics, as well as the kinetic energy and angular distribution of the photofragments.http://doi.org/10.1103/PhysRevResearch.2.013338 |
| spellingShingle | A. Tóth A. Csehi G. J. Halász Á. Vibók Control of photodissociation with the dynamic Stark effect induced by THz pulses Physical Review Research |
| title | Control of photodissociation with the dynamic Stark effect induced by THz pulses |
| title_full | Control of photodissociation with the dynamic Stark effect induced by THz pulses |
| title_fullStr | Control of photodissociation with the dynamic Stark effect induced by THz pulses |
| title_full_unstemmed | Control of photodissociation with the dynamic Stark effect induced by THz pulses |
| title_short | Control of photodissociation with the dynamic Stark effect induced by THz pulses |
| title_sort | control of photodissociation with the dynamic stark effect induced by thz pulses |
| url | http://doi.org/10.1103/PhysRevResearch.2.013338 |
| work_keys_str_mv | AT atoth controlofphotodissociationwiththedynamicstarkeffectinducedbythzpulses AT acsehi controlofphotodissociationwiththedynamicstarkeffectinducedbythzpulses AT gjhalasz controlofphotodissociationwiththedynamicstarkeffectinducedbythzpulses AT avibok controlofphotodissociationwiththedynamicstarkeffectinducedbythzpulses |