Probing the chiroptical response of a single molecule

被引：203

作者：

Hassey, Ruthanne ^{[1
]}

Swain, Ellen J. ^{[1
]}

Hammer, Nathan I. ^{[1
]}

Venkataraman, Dhandapani ^{[1
]}

Barnes, Michael D. ^{[1
]}

机构：

[1] Univ Massachusetts, Dept Chem, Amherst, MA 01003 USA

来源：

SCIENCE | 2006年 / 314卷 / 5804期

关键词：

D O I：

10.1126/science.1134231

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Chirally sensitive measurement techniques have generally been restricted to bulk samples. Here, we report the observation of fluorescence-detected circular dichroism (FDCD) from single (bridged-triarylamine) helicene molecules by using an excitation wavelength ( 457 nanometers) in the vicinity of an electronic transition that shows circular dichroism in bulk samples. The distributions of dissymmetry ( g) parameters by analysis of signals from pure M- and P-type diastereomers are almost perfect mirror images of one another, each spanning a range of both positive and negative values. In addition, we observe a well-defined structure in the histogram of dissymmetry parameters suggestive of specific molecular orientations at the polymer interface. These single-molecule results highlight strong intrinsic circular dichroism responses that can be obscured by cancellation effects in ensemble measurements of a randomly oriented bulk sample.

引用

页码：1437 / 1439

页数：3

共 24 条

[1] Single molecule physics and chemistry [J].

Bai, CL ;

Wang, C ;

Xie, XS ;

Wolynes, PG .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1999, 96 (20) :11075-11076

[2] Imaging three-dimensional single molecule orientations [J].

Bartko, AP ;

Dickson, RM .

JOURNAL OF PHYSICAL CHEMISTRY B, 1999, 103 (51) :11237-11241

[3] Three-dimensional single molecule rotational diffusion in glassy state polymer films [J].

Bartko, AP ;

Xu, KW ;

Dickson, RM .

PHYSICAL REVIEW LETTERS, 2002, 89 (02) :261011-261014

[4]

Berova N., 2000, Circular Dichroism: Principles and Applications

[5] Measurement of the radiative and nonradiative decay rates of single CdSe nanocrystals through a controlled modification of their spontaneous emission [J].

Brokmann, X ;

Coolen, L ;

Dahan, M ;

Hermier, JP .

PHYSICAL REVIEW LETTERS, 2004, 93 (10) :107403-1

[6] Circularly polarized light generated by photoexcitation of luminophores in glassy liquid-crystal films [J].

Chen, SH ;

Katsis, D ;

Schmid, AW ;

Mastrangelo, JC ;

Tsutsui, T ;

Blanton, TN .

NATURE, 1999, 397 (6719) :506-508

[7] Circular dichroism imaging microscopy: Application to enantiomorphous twinning in biaxial crystals of 1,8-dihydroxyanthraquinone [J].

Claborn, K ;

Puklin-Faucher, E ;

Kurimoto, M ;

Kaminsky, W ;

Kahr, B .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (48) :14825-14831

[8] Amplification of chirality in two-dimensional enantiomorphous lattices [J].

Fasel, R ;

Parschau, M ;

Ernst, KH .

NATURE, 2006, 439 (7075) :449-452

[9] Circularly polarized luminescence from bridged triarylamine helicenes [J].

Field, JE ;

Muller, G ;

Riehl, JP ;

Venkataraman, D .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (39) :11808-11809

[10] Bridged triarylamines: A new class of heterohelicenes [J].

Field, JE ;

Hill, TJ ;

Venkataraman, D .

JOURNAL OF ORGANIC CHEMISTRY, 2003, 68 (16) :6071-6078

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