Ultra-Broadband Dielectric and Optical Kerr-Effect Study of the Ionic

Subscriber access provided by Indiana University

Article

An Ultra-Broadband Dielectric and Optical Kerr-Effect Study of the Ionic Liquids Ethyl- and Propylammonium Nitrate Thomas Sonnleitner, David Andrew Turton, Glenn Hefter, Alex Ortner, Stefan Waselikowski, Markus Walther, Klaas Wynne, and Richard Buchner J. Phys. Chem. B, Just Accepted Manuscript • Publication Date (Web): 19 Jun 2014 Downloaded from http://pubs.acs.org on June 24, 2014

Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a free service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are accessible to all readers and citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts.

The Journal of Physical Chemistry B is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties.

Page 1 of 49

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

The Journal of Physical Chemistry

!

† ‡

¶

§ §

§ ‡ ! "!

∗ †

!"#" $ % $& $& $'( )** + , - - ./0/ 1'2" 0 , - 3, 0 4& 5 6 '"# 5 $

!"#$%$ &! ‡ ' & & &() *++ , ¶ - - ./0/ 1(2$ 0 § - 3 0!4 ! 5 6"($% 5 & ∗

†

ACS Paragon Plus Environment


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

! " ! # # $%% &'( )% *'( "+ , - ., -/ + α 0 +

! 0 ! !

! ! !# ## 1 / # + "! + " !# " / 2 ! 3 '" !" #3 " " / * # + + " + "! /

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

# $

# (


Page 2 of 49

Page 3 of 49

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-/*+ 3 10/23 1

# # + 33 4 $ % # #

#$

5

6./6 7 75'

8' $

9

/

2

95

-./ # 4 : #&

-./ ;3

? ≤ ϑ@ A ≤ B3

(? A ( %*= = %*=%'6$ %

-./

εs $ % # 95 -./

* #$ *# #& # $ 9 9

/

'9%

#

$ /

-./ & $ % 2- '5 # %*=%'6 95 # # = $

.

-./ = $ % C



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 4 of 49

∼(33 8*= 3 %*= > ? ≤ ϑ@ A ≤ D? '5 ./ # 3 -./ (? A$ .

+

'5 -./ ./ 3 -./ 2- '5 # $

$

%# -./ # $ % + # # # = - /

# '5 2- $ 9

-./ >EFG *

εˆ(ν) = ε (ν) − iε (ν)

$

%

ε (ν) # εs = limν→0 ε (ν) + ε∞ = limν→∞ ε (ν)$ %

ε (ν)

# E(t) K $ ' # . -BCD;! L /#& . = L/. # # K B?3F3-3(3 3?3 3$( ≤ ν @

SOKE (t) ∝

1 d Πxy (t)Πxy (0) kB T dt

C

# kB ! =J T $ %# 2- # -./$ 9 A 86--' # B33 # B N (3 FD 8*=$ % # B3 G (3 G # # = $ 9 # # ±3$

A 2 '/$ .

& # ±3$ A # $ . D33 # ?3 3$CC ; #

/

(?3 8*=$

9 #

+ A ,67 # ∼ # #& $ % # # 9

+ 2- $

' ρ # ? A -./ ? A ./ D? A 3 A . (33 8*= ≤ ν ≤ 3 %*= ? D? A 9 $ ( C ; $ 2- ./ #$

# $$ + $ % #

= + $ %

$ % # + εˆ(ν) 2- SOKE (ν) #

F˜j (ν) Sj >

y=

n

Sj · F˜j (ν) + y∞

F

j=1

# y = εˆ(ν) P y∞ = ε∞ '5 y = SOKE (ν) P y∞ = 0 2- $ # 33 2 -./ ? A D? A 3 A $ ! & H +$ # = # $ *#

= + '5 2- &

$

#

$ ! +

# #& $

% ) Q +

= # $ 9 $ 6

# #$ % '5

# +



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 12 of 49

0.05 ν/THz 1 9 $ ( R D # $ 9 # ( #

# '5 2- # ν 0.5 A' W A W '*21 W γlib = 5 %*=

ν0,DHO2 = 7.7 %*= 9 $ 6 $ % -./ + '5 ./ 9 $ D$ % % 6? -./ '*21 '

./ (? A$ ! & + A' W '*21 W + νG1

C3


Page 31 of 49

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


DR SG1 # T 9 $ E $ % # #

$ 9 * * #& $ . # # T 9 $ E

# $ SG1 SG3 SG2 # T 9 $ E

$ 6 # * #$

?/ ' H

(B !] A$ 9$ N$H ! #)& $

- > . EFC$

: > ?/ ( H

. EFB$

;


- >


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 42 of 49

(E 9& A$ N$H - N$ '$H %& .$ . 5 6 8 8 6 8 & 2 - 6 $

8/ / /

4224 ''6

CER

?;$

C3 6& 6$H ! 5$ ' L 0 (FB$ ? C B$ ? 1 - A (EB$ ? . 6 A A A A A $

8/ / :/

42&& 21 ;E;;R;E;E$

C - / n2 ! 8 $ 8/ % /

4224 !' CEFR; C$

CF 9 N$ '$

? , H

;(

4 > /# [& EB3$


Page 43 of 49

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


CB . A$ .$ 5 A S6 @9 $

8/ 9 / %

&55& '!''!!

CRC $

CE 6 N$ .$H 4 - . N $ / 4/

8/ /

42&4 ! C3C;RC3CB$

?B / # 5 A ' ταDR + # DR α & τα,max ; 5$ BF$

?E 6 [$H *$ ' 5 A 6 5 6 ' 5% $ 3(BR

8/ / / ;

4221 ''(

3CB$

D3 '$H 6 =^

/ / / /

4225 ''

(;?(R(;?B$ DC ! N$H *= *$H ! 5$ ' 5 . - 6 $ $ 5 >( (> (>( - $

/ /

&554

1

; / ;$/

;(;R ;C($

D; 6 %$ . A % ' A $

&575 '2 ;CFR;;E$

D? % # μeﬀ μapp ./

# ;?



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 46 of 49

& #

H K /*+ 3 $ DD * $ .$H 8 6$ 5$ =5 , = 5 . $

8/ / / ;

4221 ''(

(EFDR (EB;$

DF 9& # %$H 6 %$H 4 N$H * [$H = 4$H ! 5$ 5 # ' #9 5 6 * ! $ / 4/

422/

2

/

EFB3($

DB 4& $H N$H L] $ # ' = 56 ' 4 9 2 - 8 >

. 5 % 8 $

/ / / /

4224 #

( ;;R( ??$ DE ! 9$ N$H = %$ .$ 5 6 > 2 8 $ / /

8/

&584 21 ; CR;(?$

F3 Z *$ 5$ % ' 2 A *2 2 '2 2 9 5 5 $

8/ -/ % /

&55/ !2" E?R

;$

F A -$ 4$H 8 8$ 6 ' ' 2 - ' ' %5 6& 6 8 > . - A $

8/ -/ 4=/

&551 66

RCD$

F( 9$H 8$H 6

$H 8 .$H , ' $ / ;

8/ /

42&2 ''# E;33RE; ($

F? . [$H % [$ #9 5 6 4 $

0

4222 (61 ;3 R; ($

FD

ν0,G3 ./ $ %

K = K $

Ultra-Broadband Dielectric and Optical Kerr-Effect Study of the Ionic

Recommend Documents