Molecular Ion Formation by Photoinduced Electron Transfer at the

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Letter

Molecular Ion Formation by Photo-Induced Electron Transfer at the Tetracyanoquinodimethane/Au(111) Interface David Gerbert, and Petra Tegeder J. Phys. Chem. Lett., Just Accepted Manuscript • DOI: 10.1021/acs.jpclett.7b01897 • Publication Date (Web): 12 Sep 2017 Downloaded from http://pubs.acs.org on September 14, 2017

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The Journal of Physical Chemistry Letters

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hn

e-

!! """ #$! $ %" ! "&' ! " "" $"(

) *" "$$* "+! +$"

%! + ! " * %" ," - "$ $$"( ."!" " $ ! " ! !%$+ - "$ $$" $ + !!"' !$! $*"" ! / - $+* """ $$* !! " " !! +/ -+ - $ !%"(

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89 :; -( 89 " 3& 1 %$* ! %" +$ " -"

! " $ ,* EA < (= > " +$ +$$ $

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%$ """ "- * ( +$ % !" %"

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) " "+$$ !"1 !! "- - "- " 1 ""! & =



10 IPS m = 1.2 ± 0.2

a)

q = 1.0±0.1 ML

SS‘ m = 1.9 ± 0.1 EFinal - EF [eV]

2PPE Intensity [normalized]

9 8 7

UMO m = 1.2 ± 0.1 HOMO m = 2.0 ± 0.1

IPS1

FS m = 0.1 ± 0.2

6 4.0

4.2 4.4 4.6 4.8 Photon Energy [eV]

5.0

SS‘

5

6

b)

hn = 4.79 eV 4.61 eV 4.42 eV 4.30 eV 4.19 eV

UMO

s ure eat MO df an HO d-b FS + +

7 8 9 E Final - EF [eV]

10


q = 1.0±0.1 ML increasing hn = 4.75 eV photon dose IPS1 FS HOMO

es

tur

ea

df

an

d-b

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

5

6

SS‘ UMO

7 8 9 E Final - E F [eV]

10

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B $" 1 !

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q = 1.0±0.1 ML hn = 4.52 eV


a)

IPS1+SS‘

before illumination (F B ) after illumination (FA ) increasing annealing temperature (FC (T))

s ture fea FS + and d-b OMO +H UMO

5

6

7 8 E Final - E F [eV]

9

b) ln[ln(FB -FA )-ln(FC (T)-FA )]

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

0 -2 -4 -6

q = 1.0±0.1 ML hn = 4.52 eV EA= 43±11 meV

-8 4

6 8 -3 -1 1/T [10 K ]

10

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DF 0.30 = eV

5.72 eV

4.45 eV

F = 5.50 eV

E i -EF

EVac

3.71 eV

FS

= DF eV 5 6 -0. 5.10 eV 1 IPS UMO

hn kBT

EF

EBind -EF

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

SS

-0.26 eV

SS’

HOMO -2.48 eV

Au(111)

1 ML TCNQ

= B$ " - 06 89:; $$" !! &3 - " ! +$$* "+$! 13 ' &$ "" - +$$ !! "" C!( !"" +$ " &$$ " !"( ;!!$$*' " " % 1 -$$* %"1$ +$ %' & " %* $3$*( 0%' 89 " $' "*++ +$$ & !$ ++ ! !"1" 2 !" +* ; "-( ; + -+ " !" " + $! 4 " $$* -%1$( +' + " - 89 &$! "$ - "- " ! !$* ; "- " "$! "*' 1 " & -! ??G " """! 1* $$+ ( )"!' & " !! "- 1 ""1$ - 1"%! C"( ; $ "- -+ ; "1" ! +$$ " % &$! #$ " - &3 -( % " $* +"1$' " +$ % $! !* - " + $ & &3 - !"( 8 489:; - " ??G " -!' & " 1! -$ "-' ((' " - %$* ! ""(


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Page 9 of 19

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$*/ !! $ "- + !$' & 74! "" ! -+! !" ! * !! +"+"( ;" - +$$* %! ' & "! &3 - - "+$ " 7% 1+3 - "" - "+$! ( Φ " - - !" " !! #+$$* - - !C " ( ( &3 - " " - - !" np ' +1 - " -$$&" "*+ 1% & "" Φ = 5.20 ± 0.05 > ! "" " %$ - Φ = 5.85 ± 0.05 >( ) 1 4! 1* "+$ + #$ " - Φ = Φ + ΔΦ exp( σ · np )

& " "! !+ C% "" " σ( 8 - " 1% ( > % &3 - %$" - ! > -!' ((' &3 - +"! - hν < ( > !" " ( > " ( ( )- " "" &" -$$* %"1$' & & 1 !"" "( 5&%' "" " "" & " * $" 10−21 +2 - " ( >( A" 1! %* - " !+ "" "" - $$&" " !& $"" 1 !$* # ""( 1 !"$*" " * !! - "" ""( " $ 4.25 ± 0.05 > " ! "" " #1" #$$* " ,* & " *( +"' 06 489:; !! &3 - "- " 1"%!( E! -$ !! $ "-' " - %$%! +$$ " " 1 %* -

4.25 ± 0.05 >

1%

EF (

A-$*' & ! 1"% 89 !%!

$ " " * ( ;" - $ " -+ 6A0

" 1% ' 1"% - +$$ $ "" B + 1 ! %" &% - %$( 5&%' #$$* " "" " &



Work Function [eV]

a) 5.8 TCNQ/Au(111) q = 1.0±0.1 ML

5.6

hn = 4.42 eV -23 2 s = 5.5±0.2 10 cm hn = 4.52 eV -22 2 s = 1.2±0.1 10 cm hn = 4.79 eV -22 2 s = 8.8±0.1 10 cm hn = 4.86 eV -22 2 s = 7.7±0.2 10 cm

5.4 5.2 0

2 4 6 22 -2 Photon Dose [10 cm ]

b) 10 Cross Section [10-22cm2 ]

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60

Page 10 of 19

8 6

TCNQ/Au(111) q = 1.0±0.1 ML F4TCNQ/Au(111) q = 1.0±0.1 ML

4 2 0 2.5 3.0 3.5 4.0 4.5 5.0 Photon Energy [eV]

D3 - & " !" ! $$+ 4! & #$ - ! 7 !+ C% "" ""

σ ( 1 * !! - C% "" "" - 06 89:; ( +" !! C " -! - 06 489:; ( " * " &!" $ - +$$ " 1* $" " ""( $ &$! 1 - " ! +$$ " (( 50 6A0 "1" +!! ! ""' & (( $" -+ $! "- " "$* $ ! +$$ "( !' & " * $ - $"' & " & ! +$$ $%$ $! ! ( >' "$!


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" $$* ! " 11$* - -+ - % "$! 1 !( ; 489:; - +$$" $!* %$* ! - !"' - $ "- " -"1$( ;" "+$$* "& "+ ' & "" -$$& """ 1 ""1$ - %"1$ &3 - " 89:; - 6 #" & " - hν>( > $!" $ $ - ! +$$ " % $ "- -+ +$$ "1"( ; $& +" ! % " "1$ ! +" $3$* !$! -+ "1" " 13 "- - $" " """!( 8 $ -

n

< ) ? -$$&! 1* "- +$$

" +* $" ""1$ " - % -+(

$" 1!

1* "+$$ $ 1' & 1 - EA < =± +>( D 1$% "1$/ - % " "! 1* " $ - +$$( " + - - % " ! " !" "$" &3 - " " %$( ; "+$ +"' % " !* % 13 "- - $" +$ & " !$* -$$&! 1* ! &3 - 13 " $ %$( ) "++*' & !+"! - 89:; - "- " ' &$ A> $ #" !! "1" +!! "- -+ +$ ! 89 !%! $ "( " $! - %$* ! 89 +$$" ! !$* ! " - &3 -( 1* &3 - - 89:; "*"+ 1 "$* ! "" 1 "1" %$ 1* $$+ & A> $ & "1$"" & $ ""1$" - 89 +$$" - #+$ " !% !! $ F $* A> $ ""( $$*' "!* $$"" !! "- """ : -" $ - " $ +$$" % 1 "!! ! !-* -$ "- " 1"" - &3 - %$" !+! +"" #+"(



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E hn > 4.25 eV

hot e -

EA 4.25 eV

EF

Au(111)

TCNQ

?+ "! " 89:; - $! %"1$ &3 - "( 5 $ !! ! "- -+ +$$ "1" ! +$$ " ! +$$* %! 13 "- - $"(

"+$ 89 +$$" & %! -+ C" $$ $! + - 390 I ! !"! ; "$ *"$ $! + + & &" %"$* $! 1* "%$ " ;+ ' + + ! $ *$" 800 I' 30 + ( J4! +$* % &" "! 1* ", !" + ! "1"7 $ " 370 I' & $!" !" - +$ $*" " 1 -$$&! 1* + ++! !" J " " -+ ( ?+$ " &$$ " J ! $ %+ +1 1" "" -

B #+" & -+!

5.3 · 10−11 +1(

&

+"" B #+" & -+! $7! + " " & &" #$$* !"1! $"&( ) ! "+$-* +" -

B " 3 !C " " !"$*! " -

- 4$ " * 1% + $%$ B

= 0 '

B − B

=

B − Φ( "

" " &3 - Φ "!" " - "!* ! $& * C ( $$*' B $$&" %" - 1' ! "


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&$$ " ! $ ""( "% ""+ &" %! 1* "!* * !! - " - !$" " E-"( ) ! % $ " - $$+! 89:; -'

B +

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+ ++! !" +"+"' & +"" ! - 1 ; "-(

! 1* + E" ! J $$1% " ?. F . " -$$* 3&$!!( J(( 3&$!" 4$ " -+ 5!$1 ! ?$ - !+$ *""(

?-' 8( ?(K ?+$&/' 6(K 5' ;( L(K D!$' ( !! B$ "- -+ ! $*+ .3+"-$$( + ' !,' M (

=



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E1$' )(K .3' .( ;(K I+' ( >( ?$ D$$! 1 81 !? 8+ "" " 6 5%" ;""+1$"

!! "- )"(

-) .) ' %/' M =(

= 6+' >(K ?$' 0(K .$F' J(K .N!"' L( 6(K $' L( !! ! E+1 J*+" 0!$ J:; " - ?$ $$ ;$" ; $$ 9+ +$ +( 0) -) ) +() ' % /' M (

I' 6( B(K 6' I(K ' ( I(K ;$$!-' 0(K > J*' E( (K 5' L( ( 0$M +&3 0$" " +$ ?""( ) ) ' %% ' M(

!' ( $$* ! +$$* )!! 0$$ ?& """ 0$ ?-"( 0) )1 ( ) . ' 2' = (

1' ;( (K D' ?( (K )%' L( (K ;%"' ;( L(K ."' L( (K ?! !' L( (K /*1&"3' .( ;( ?&" - ?-" ! J%"( -) .) '

!' ==M=(

J6+' J( 0( +(( . 3( +( ((( K ?' K M (

"' ?( E( A17" ! 6& " B$ ;$" $"( ' 2 ,' M (

?%' E( ( $3 ." - $" ?$ $$"( + ' "" ' =M =(

' 0( ;(K B+*' I(K 5"3&' O(K D' D(K J$' B( J(K 6%' J( 5(K 5 .$$' ;( D( ?$ $$ B,* 1$" %" ( (

((( 1

- ( ' !' =M=(


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;!+"' J( 0(K ."' 6(K !"*' ( B(K ' ?(K /' (K I' ( E(K I +' ( >(K 61+' 0(K 6!"*' ?(K 0"' E( ;(K $(' "- 8"$ ?"( 0 ) ) 4 ' %&/'

M

(

6!"+' ( J(K P' @( O( !! B$ "- 0$$ 0$ ) -"( ) ) ' %&#' M=(

= P' @( O(K O' 9(K 0&$' 0( "- B#" ?+ ! ?-" ! )-"( -) ) ) ' 2 ' M(

0' ( 6( ;( A!"! )-$ B$ ? ! "- ; B$" "%( 0) ) ) 5) ' "' =M=(

L$13%' ;( B(K D$$!' ;( (K "' L( E(K ' D( 6(K ?' 8(K 1' E(K I3' 6( (K D$$+"' I( L(K 6' I(K E""3*' ( L(K P' @( O( 5 "- B#" ? + 6+ - ? J:; )-" %$"( .) ' % '

M=(

I' 8(K ' J(K D1' E( 6(K .Q&' 8(K D' .(K D3' 0(K 6"' (K 5 $' )( >(K .' D( E! )!! J! ! ?- - $+" A$%$ +"" ?"*( 6 +( ' "$%' M(

D"1*' J(K D' 8(K 6"%*F' O(K I"+' )(K "' ;( 8(K ' J(K .$' L(K >"%' B(K J&1' ( ;( E! )!! J+" - 0$ 0$$ ." * '' ' +*$ =' ! )) ( - ) +3)

+) ' !!' = M=(

D3+' J(K 0*' 0(K E' (K D$-' 0(K ?R$' L( !! D3 0!4" ! BC $ ?"*( - ) ) 5) ' %&"' =(



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Page 16 of 19

0!*' E( L(K ?$3' D( E( )F . 5" ;"" 0$$* $+"( 0) 0) -) ) ' 22' =M= (

"' ( (K A1' (K D' O(K ' E(K ' ?( 6(K ;$+S' 0(K TF' J(K $3' 0(K $$' L( 0(K 6' 8(K $(' "- )!! ?$ E +" . ?!" - :0$ )-"( ) ' ' =M= (

DR3$' (K )%' (K *$3' J(K ""' (K L' ( ;(K .$$%' 8( ;""+1$* - J ) 6*" 1* E - ;$3$ 5$!" & B$$ ''' * 7!+ 89 ( ) () ' 2/' M (

3' (K EF"' ( ;(K L' ?(K I$$*' ?( L(K ?+' ?( (K ?+' .( (K O' 0(K 03"*+%*' ( D3 + )" $ ;""+1$* - ?$* .!! 89 ) ; 0$$" ?$% ?-"( ) ) 4 ' $&' =(

= J$$ ' ;(K E$$' 0(K ?""' J(K L"' ( ?(K .-/' J(K J >' ;(K " ' ( & J+"$ ?$$ J ; ;""+1$" 0$ ) -" +! 1* ?- 0!! "-( ( ' ,' M =(

I' I(K ;33' I(K I*"' I(K ?3' I(K 8"' (K I+/' O(K 8"' (K ' O(K ?3' I( J+ - B$ ;,* - B$ ; 0$$"(

- - ' $!' = M==(

U!/ ' )(K 3' I( L(K "$' L( )( ? ! B$ 4 - *7!+ 6*" ; ?-( ) 0) .

+) '

//' M=(

O' 5(K 6' ?(K O' 9(' (! K D' 6( ;!" - ' 89 ! 89 ; ; B?0 ?!*( +) + 41 ) ' ! ' M (


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0S/' L( )(K ;1!' B(K $"' (K ' L( ?+$ 0$$:0$ )- 89:; ( ) ) ( 78 ' 2,' M (

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