Convenient 1+1 Probing of S( D) for OCS Photodissociation:

its Applications to Coincidence Imaging

1

Chaya Weeraratna , Chandika Amarasinghe , Suk Kyoung Lee , Wen Li , Arthur G. Suits
1
Department of Chemistry, University of Missouri, Columbia, MO 65211 USA
2
Department of Chemistry, Wayne State University, Detroit MI 48202 USA
1

VUV absorption of OCS

Three-dimensional Detection

Introduction

Three dimensional imaging is a new technique which was

We introduced a convenient 1+1 probe of S( D) through the (4s

introduced as a modification to velocity map imaging. A novel

S ) state, and apply it in one-color experiments to investigate

approach to this technique was implemented by Li and

the underlying dissociation dynamics of carbonyl sulfide at

coworkers3,4 for strong field ionization and electron imaging.

216.9nm. Our results on OCS show a bimodal distribution

It requires a high speed digitizer and a computer algorithm

corresponding to two dissociation channels in the parent

designed using Labview language in addition to other

molecule, which agrees well with previous observations. The

components used in velocity map imaging.

same experiment was applied in validating our coincidence

imaging approach, which was introduced as a modification to
the velocity map imaging

Results

OCS (X ) + h CO (X ) + S ( D2) or S ( PJ)

1

The dipole transition from ground state to excited state is forbidden

We are developing it in our lower repetition rate ion imaging

in linear geometry but weakly allowed in bent geometry.

experiments. Three labview programs were used:

Three excited states are involved:

A" arise from Cs deformation of 1- state

1. Data acquisition: The camera captures positional

Two Renner-Teller components A' and A" arise from 1 state

In earlier studies S (1D2) was probed by 2+1 REMPI through 4(1P)

times of each and every ion

information while the high speed digitizer, records the arrival

or 4(1F) states at 291.5nm and 288.2nm1, and the resultant image

shows two speed components corresponding to bimodal rotational
distributions of CO fragment. The faster, low-J components are
more isotropic affirming the dissociation is from an admixture of A'
and A" states, while the slower high-J component shows a purely

2. Correlation: Due to intensity variations of ion spots, a

parallel transition.

correlation could be made and it is possible to assign each

ion spot position with their respective arrival times, thereby
constructing a 3D distribution of the expanding ion sphere.

Experiment
One color experiment at 216.9nm and 1+1 REMPI scheme2
OCS (X1+) CO (X1+) + S (1D)
D0 = (3460824) cm-1
S (1D) (3s23p4) + S (3S) (3s23p3 (4S) 4s) +

S+ (3s23p3 (4S))

Total translational energy distribution

Speed and anisotropy parameter distributions

The angular distribution is characterized by I() = (4)1

[1+P2(cos )] where is the anisotropy parameter. The
anisotropy parameters for two velocity regions separately are,

The DC slice imaging technique with improved ion optics

1.20 and 2 for faster and slower components respectively.

assembly was used to detect S ( D) fragments.

Therefore, the earlier explained bimodal distribution is exhibited

3. Slicing: Both time and spatial slicing could be achieved

with time gates as low as 4ns and 1 pixel respectively.

in our image along with an excellent resolution, fully rotationally

resolved. The sensitivity of the probe transition to the laser

S (1D)

polarization was studied with a two color experiment, using two

CO

linearly polarized lasers, 222nm for photodissociation and

CO2

216.9nm probe. We observed no sensitivity of the probe

polarization to atomic orbital alignment.

References and Acknowledgment

1.
2.
3.
4.

Experimental apparatus and the ion optics setup

T. P. Rakitzis, Phys. Rev. Lett. 87 (2001) 123001

C. Weeraratna, Chem. Phys. Lett. 657 (2016) 162-166
S. K. Lee, Rev. of Sci. Instrum. 83 (2014) 123303
S. K. Lee, J. Chem. Phys. 141 (2014) 221101

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