A first principles approach to optimal control

《A first principles approach to optimal control 》由会员上传分享，免费在线阅读，更多相关内容在学术论文-天天文库。

1、TheorChemAcc(2006)116:148159DOI10.1007/s00214-005-0035-7REGULARARTICLELeticiaGonzález·JürgenFullAfirstprinciplesapproachtooptimalcontrolReceived:6April2005/Accepted:26October2005/Publishedonline:2December2005©Springer-Verlag2005AbstractThisarticleshowsthatbyusingabinitioorfirstisreshaping

2、quickly.Accordingtotheprevailingexperimentsprinciplecalculationsitispossibletoobtainreliableingre-andbasedontheavailabletheoreticalsimulations,itisnat-dientsneededtosimulatepump-probeandoptimalcontroluraltopredictthatthepathofquantumcontrolwillprovideexperiments.Ourexperimentalchallenge

3、istoelucidatetheexcitingscientificknowledgeandinnovativetechnologyinreactionmechanismbehindanoptimalpulsetailoredtomax-thenearfuture.imizeionizationinthesystemCpMn(CO)3,whileavoidingIntheframeoftraditionalchemistryonecanthinkofCOdissociation.StartingfromMRCI/CASSCFpotentialen-achievingth

4、ermodynamicorkineticcontrol.ThermodynamicergycurvescalculatedalongtherelevantCOfragmentationcontroliswellestablishedtotheextentthatvariablesliketem-channel,weusetheresultingMRCIwavefunctiontoesti-perature,pressureorconcentrationcaninfluencethecoursematenon-adiabaticcouplings,aswellasneut

5、ral-to-neutralofareaction;kineticcontrolisalsowellmasteredbyusingandneutral-to-ionicdipolecouplings.Thestate-of-the-artcatalyststhatcanreducethereactionbarrierofthedesiredpotentialsandcouplingsservetoperformwavepacketpropa-reactivechannel.Thesetools,however,donotaccessthegationswhichsim

6、ulatethefemtosecondpump-probespectramicroscopicbehaviorofachemicalreaction.thatexplainthefeaturesshownintheexperimentaloptimalWiththeadventofphotochemistry,lightemergedasapulse.powerfultooltosteerreactions.Controlmaybeachievedbyexcitingthesystemtopotentialenergysurfaces(PESs)whereKeywor

7、dsOrganometallics·Multiconfigurationalmeth-thefreeenergybetweenreactantsandproductsisdifferentods·Reactiondynamics·Femtochemistry·Optimalfromtheonegivenintheelectronicgroundstate.Kineticcon-controltrolcanbeaccomplishedsurpassingthereactionbarriersbymeansofappropriatephoto-excita