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[Music]

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so my presentation will mostly deal with

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reactivity and all the results issue

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from theoretical computations so I won't

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give any details about the methods

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because I'm pretty sure that you don't

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care about that

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so I am working on prebiotic chemistry

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which basically aims at understanding

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how life could appear on an earth

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originally in organic planet considering

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that it is ruled mainly by organic

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chemistry to solve this issue two main

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hypotheses have been made the first one

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is based on an endogenous synthesis

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theory here in this case the building

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blocks of life that are amino acids

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nucleic acid bases or simple sugars for

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example were thought to have been

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synthesized on the atmosphere of the

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early Earth based on the compounds that

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were found at that time that are methane

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nitrogen or ammonia for example this

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theory is supported by the miller-urey

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experiment in which they simulated the

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atmosphere of early Earth and discovered

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after some time that five different

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amino acids had been synthesized this

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experiment had been have been performed

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in 1962 fifty two and a couple of years

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ago they realized the mixture and found

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20 amino acids so it's a good thing for

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this theory however they just found

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amino acid they didn't find any sugars

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or whatsoever this is also why now some

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people are looking for are looking on

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Titan's atmosphere because it is thought

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to be very similar to that atmosphere of

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early Earth the second theory is based

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on an exogenous delivery of these

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building blocks of life that would be

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synthesized in interstellar medium and

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then brought back to brought back

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to hurt thanks to comets or asteroids

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for example and this is supported by the

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fact that we actually find some building

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blocks of life on comets I will focus on

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that so so far as it was mentioned

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before around 200 compounds have been

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detected in interstellar medium they are

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mainly molecules with 2 to 12 atoms and

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among them around 60 can be called

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complex organic molecules they are very

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important in providing chemistry because

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they can be considered either as

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precursors or as intermediate in the

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synthesis four of the building blocks of

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life the question is how can they be

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formed in interstellar medium

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considering that the environment there

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is very harsh the temperature and the

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pressure are really low just so you know

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the two molecules I will talk about

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later have been detected there here

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there is the formamide and cyano

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so the reactivity in interstellar medium

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is very different from the one we can

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find on earth because this very low

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temperature condition will lead to the

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fact that the only energy that is

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available for a reaction comes from the

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reactants so we can we cannot have any

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reaction that would exhibit a barrier

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the very low pressure as far as it is

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concerned will lead to the fact that

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three bodies won't be able to meet there

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so we have to focus only on two body

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reactions the study of this reactivity

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in interstellar medium can be split in

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two parts

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the first one is the dust grain

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chemistry here so in that case the

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reaction would occur at the surface of

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just grain that is composed of

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carbonaceous or silicate silicate core

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surrounded by Isis of carbon monoxide

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water and so on

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in that case these reactions on surface

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can help to reduce the potential

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barriers that a reaction could see and

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it can also is the encounter between the

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reactants because they are not far from

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each other since they are all adsorbed

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on the dust however it can also involve

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some physical processes such as a

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absorption and desorption that can be

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problematic in some regions that are

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cold or dark for example the other field

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is just phase chemistry so in that case

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we again have the same conditions no

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barrier no three-body collisions but in

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addition in the case of multi slit multi

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step reactions we cannot overpass the

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energy that comes from the reactants

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because of the very low temperature this

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chemistry can involve ion ion ion

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neutral or neutral neutral reaction and

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in my case I will focus on gas phase

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chemistry involving neutral neutral

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reactions so let's start with formula

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which is here so it's very important in

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prebiotic chemistry because it is the

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simplest amide and it can be a precursor

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in via biotic amino acid synthesis and

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perhaps also in that of the nucleic acid

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bases this makes it a central compound

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that could connect both metabolism that

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is ruled by proteins and genetics that

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is ruled by DNA and RNA it was detected

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also in interstellar medium in several

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galactic central sources in an active

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site of high style of highest mass star

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formation and more recently even in a

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product in a solar type Prada store so

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the question is how did it get there the

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first thing I try to form formamide

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was using the radical OAH and

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methylamine here as pressure source and

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I got this

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reaction path which is very complicated

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I won't describe it but what we can see

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is that the first steps here are barrier

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less so we're good and all the energies

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of all the involve compounds are always

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below the energy of the reactants this

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makes it a viable path in interstellar

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medium the problem is in the case is

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that we have a lot of products including

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soap former former mine here but also

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the two isomers of metonymic acid

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formaldehyde and here H 2 Zn so we need

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to know the amount of every product and

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the relative of the proportion of them

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to do so we did some kinetic theory and

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we got these results so here we have the

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rate constant as a function of

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temperature for the formation of several

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products here we have h 2 Zn and the two

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isomers of cyano method of metonymic

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acid and the plain line represents the

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back dissociation into the reactants and

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we can see that at low temperature which

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are the temperature of interest the main

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product is H 2 Zn so it's not formamide

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we were set and when we increase the

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energies the back dissociation becomes

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prevailing so unfortunately the form of

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mod and formaldehyde rate constants were

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not shown on the figure because the rate

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constants were found negligible so

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that's not what we wanted but it can be

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understood by the fact that a lot of

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steps are required to obtain them and we

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need to overpass this very high

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transition state so since the first

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reaction you don't work in forming

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formamide we started other reactants

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that are NH 2 and formaldehyde and

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actually we took the problem the other

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way around because they are formed in

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this reaction and instead

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of considering them as products we

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consider them as reactants and in that

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case we obtain this a lot simpler

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reaction path that also doesn't have any

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barrier and has energies that are below

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the energy of the reactants so in that

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case we were happy formamide is the only

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species that is formed by that path so

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we wanted to know how much of it was

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formed this is why we did the kinetics

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Theory the kinetics study thanks to our

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KN theory and we obtained that the rate

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constant as a function of temperature

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again of the formation of formalised

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using the different methods but it's

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only the formation of formamide and in

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that case we found that at low energy

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the formamide was actually formed

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largely more than the back dissociation

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into the reactants so that's good and

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moreover when we put those reactors rate

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constants into actual chemical models we

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had matching abundances so we were happy

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in that in order to further validate

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this we studied the deuterated formamide

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so there are three types of deuterated

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formalized because there are three

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hydrogens i think i won't have time to

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talk a lot about it but let's just say

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that again the kinetic studies based on

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this reaction studying the deuterated

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formamide also gave matching observe

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also match the observed abundances so

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this means that our path seems to be

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reliable now let's move on to sino

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methylamine so it exists under the form

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of three isomers the e Z and n here in

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prebiotic chemistry it's important

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because it's an i n h ZN dimer while

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adenine which is one of bases of eight

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of the GNA is the pentamer so maybe this

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compound can be an

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remediate in its formation surprisingly

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only the e isomer has been detected in

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interstellar medium thanks to microwave

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spike spectroscopy so the question is

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how is informed in is M and are also the

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other isomers formed and if they are why

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can't we detect them so the reactivity I

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started from those two precursors the

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radical CN and methylamine here

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if the CN adds to the carbon atom here

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it goes to the C isomers that are in NZ

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and if it adds on the nitrogen atom here

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it goes through the N is over here is

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the full reaction path starting so from

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the precursors that are here so again I

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don't just describe it so much but still

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still no barrier here and everything is

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below the energy of the reactants so

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again this can occur in interstellar

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medium now the question is how much of n

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is formed

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regarding the C and the Z so kinetics

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study and we got that so in red here we

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have the formation of Z in a black of e

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in green of N and in blue of the back

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dissociation into the reactants we can

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see that here at every temperature the Z

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isomer should be formed more than the

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and the N here should be formed only as

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traces this can be explained by the fact

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that the transition states that lead to

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Z are always a bit lower in energy than

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the one leading to so now thanks to that

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we said that all the three isomers

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should be formed more on Z more than E

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and everything more than n a lot more

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than n so why only the e isomers has

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been detected the first thing I tried

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was to investigate decay

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path that only Z and n could undergo but

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they were all find energy energetically

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too high so they cannot occur in

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interstellar medium the second thing I

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thought of was to question the means of

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detection because the microwave

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spectroscopy is highly depends on the

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mode of the dipole moment value of the

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investigated compound so to check that I

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looked at the dipole moment values of

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all the three isomers and we can see

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here that e has a larger dipole moment

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than the Z which could explain why she

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was not detected there and has a large

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enough dipole moment value but we saw

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that it was it should be formed only as

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traces and some transitions that were

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that were found could match with n but

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it wasn't enough to make a definitive

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detection so to conclude gas phase

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chemistry can also explain some comes

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formations but there are still a lot of

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compounds to try in the case of

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formamide

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to formation paths were proposed and

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while the the second I shown was effect

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was shown to be effective the first one

280
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didn't lead to form a body it led more

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to other compounds of prebiotic

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interests and in the case of sino

283
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methylamine isomers we showed a path

284
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that seemed to work we also considered

285
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the ISO cyano methylamine which is

286
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exactly the same but the CN moiety here

287
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is linked through the nitrogen atom

288
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instead of the carbon atom but in that

289
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case it was too energetic so we gave up

290
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on that and the conclusion of that is

291
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that Z should before more than E and a

292
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lot more than n but maybe the detection

293
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tool was not efficient not efficient as

294
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efficient enough to detect them

295
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I would like to thank all of those

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people and you for your attention very

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first how did you calculate the dipole

298
00:16:03,790 --> 00:16:00,800
moment dipole moment yeah yeah with the

299
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the frequency calculations it is the

300
00:16:09,189 --> 00:16:07,190
Indians put of the it's in out in the

301
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output of the frequency calculation the

302
00:16:14,829 --> 00:16:12,800
informations are inside variations and

303
00:16:20,050 --> 00:16:14,839
could you please go back to slide number

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three number three number two loss so

305
00:16:38,290 --> 00:16:34,180
and before you go back to that how did

306
00:16:41,980 --> 00:16:38,300
you match abundances but you say when

307
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you calculate our or our km rate

308
00:16:46,389 --> 00:16:43,940
constant then you match it with

309
00:16:49,199 --> 00:16:46,399
abundances of them yes actually the the

310
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rate constants that are obtained are

311
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implemented in a stroke Emma Cole model

312
00:16:57,280 --> 00:16:55,250
that calculates the abundances that we

313
00:17:01,120 --> 00:16:57,290
should have depending on the temperature

314
00:17:03,490 --> 00:17:01,130
and the environment that's what why we

315
00:17:05,079 --> 00:17:03,500
could say that they match the observed

316
00:17:09,370 --> 00:17:05,089
want but I didn't do that

317
00:17:11,799 --> 00:17:09,380
oh you didn't okay all right and the

318
00:17:17,049 --> 00:17:11,809
last question sorry I'm being selfish

319
00:17:20,350 --> 00:17:17,059
and the second option for decade you say

320
00:17:22,210 --> 00:17:20,360
involves physical processes that can be

321
00:17:25,090 --> 00:17:22,220
problematic what's the problem again I

322
00:17:26,829 --> 00:17:25,100
didn't understand that part because for

323
00:17:28,900 --> 00:17:26,839
example methanol we talked about that

324
00:17:33,460 --> 00:17:28,910
earlier with a note remember who

325
00:17:37,150 --> 00:17:33,470
methanol was we can find the reaction

326
00:17:40,060 --> 00:17:37,160
process it's found but it's also

327
00:17:45,039 --> 00:17:40,070
detected in very cold and dark places

328
00:17:47,980 --> 00:17:45,049
and we don't know yet how it can go from

329
00:17:50,500 --> 00:17:47,990
the dust grain to the gas phase because

330
00:17:53,049 --> 00:17:50,510
it's it's very cold and very dark so

331
00:17:55,270 --> 00:17:53,059
there is no UV there is no energy and

332
00:18:06,780 --> 00:17:55,280
it's not known yet so it can be a

333
00:18:13,630 --> 00:18:10,600
um thank you for your talk I'm quite

334
00:18:16,420 --> 00:18:13,640
curious about your methods yeah okay so

335
00:18:21,520 --> 00:18:16,430
for formamide

336
00:18:25,570 --> 00:18:21,530
all the optimizations were done with b2

337
00:18:27,850 --> 00:18:25,580
Pullip g3 and ml/cc pivot is did you

338
00:18:30,130 --> 00:18:27,860
know them or do you want me to so it's a

339
00:18:33,510 --> 00:18:30,140
double hits a double hybrid functional

340
00:18:37,270 --> 00:18:33,520
with dispersion effects in addition to a

341
00:18:40,810 --> 00:18:37,280
triple databases stats and all the

342
00:18:43,600 --> 00:18:40,820
energies are revaluated using CCS DT and

343
00:18:46,090 --> 00:18:43,610
a complete basis set extrapolation in

344
00:18:49,240 --> 00:18:46,100
that case so it's very precise in the

345
00:18:54,520 --> 00:18:49,250
case of cyano autonomy is just CBS QB 3

346
00:18:56,640 --> 00:18:54,530
it's a hybrid methods using a complete

347
00:19:02,140 --> 00:18:56,650
basis set extrapolation but based on

348
00:19:05,590 --> 00:19:02,150
not-so-good geometries but in this case

349
00:19:08,770 --> 00:19:05,600
we have a lot of borderline compounds

350
00:19:10,780 --> 00:19:08,780
that are in the limits of the reactants

351
00:19:13,120 --> 00:19:10,790
energy so we needed something very

352
00:19:15,610 --> 00:19:13,130
precise in the case of cyano methylamine

353
00:19:29,610 --> 00:19:15,620
everything was below so we just thought

354
00:19:36,640 --> 00:19:33,730
hello nice dog and on a curiosity do you

355
00:19:39,400 --> 00:19:36,650
know in what kind of environment they

356
00:19:42,490 --> 00:19:39,410
calculated abundances from your motto

357
00:19:43,740 --> 00:19:42,500
agree with the observed nope yeah it's

358
00:19:46,930 --> 00:19:43,750
in the paper

359
00:19:47,920 --> 00:19:46,940
their papers about that it's inside but

360
00:19:55,000 --> 00:19:47,930
I don't remember

361
00:19:58,570 --> 00:19:55,010
frankly it's alright anybody else with a

362
00:19:59,490 --> 00:19:58,580
quick question okay then let's thank our