This wouldn't really help as hitting CO2 or CH4 with a laser would produce molecules and radicals (CO and CH3 mainly) that feature in the natural atmospheric oxidation of hydrocarbons, you would just be speeding up photochemical ozone production (tropospheric ozone as well as being a component of smog is also a greenhouse gas...). If you are going to speculate along these lines you really need to understand what products you will form and what will happen to them in the atmosphere, section 2 in this link (
Tropospheric Chemistry) is a good starting point.