Single-molecule pump-probe detection resolves ultrafast pathways in individual and coupled quantum systems -: art. no. 078302

被引:64
作者
van Dijk, EMHP [1 ]
Hernando, J [1 ]
García-López, JJ [1 ]
Crego-Calama, M [1 ]
Reinhoudt, DN [1 ]
Kuipers, L [1 ]
García-Parajó, MF [1 ]
van Hulst, NF [1 ]
机构
[1] Univ Twente, Appl Opt Grp, MESA Inst Nanotechnol, NL-7500 AE Enschede, Netherlands
关键词
D O I
10.1103/PhysRevLett.94.078302
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
We report the first experimental study of individual molecules with femtosecond time resolution using a novel ultrafast single-molecule pump-probe method. A wide range of relaxation times from below 100 up to 400 fs is found, revealing energy redistribution over different vibrational modes and phonon coupling to the nanoenvironment. Addressing quantum-coupled molecules we find longer decay times, pointing towards inhibited intramolecular decay due to delocalized excitation. Interestingly, each individual system shows discrete jumps in femtosecond response, reflecting sudden breakup of the coupled superradiant state.
引用
收藏
页数:4
相关论文
共 29 条
[11]  
KASHA M, 1991, BASIC LIFE SCI, V58, P231
[12]   Absolute optical cross section of individual fluorescent molecules [J].
Kastrup, L ;
Hell, SW .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2004, 43 (48) :6646-6649
[13]   Single-molecule optics [J].
Kulzer, F ;
Orrit, M .
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, 2004, 55 :585-611
[14]   Coherent electronic coupling versus localization in individual molecular dimers -: art. no. 103001 [J].
Lippitz, M ;
Hübner, CG ;
Christ, T ;
Eichner, H ;
Bordat, P ;
Herrmann, A ;
Müllen, K ;
Basché, T .
PHYSICAL REVIEW LETTERS, 2004, 92 (10) :103001-1
[15]   ENERGY TRANSFER IN MOLECULAR CRYSTALS AND IN DOUBLE MOLECULES [J].
MCCLURE, DS .
CANADIAN JOURNAL OF CHEMISTRY-REVUE CANADIENNE DE CHIMIE, 1958, 36 (01) :59-71
[16]   Illuminating single molecules in condensed matter [J].
Moerner, WE ;
Orrit, M .
SCIENCE, 1999, 283 (5408) :1670-+
[17]   FEMTOSECOND NON-MARKOVIAN OPTICAL-DYNAMICS IN SOLUTION [J].
NIBBERING, ETJ ;
WIERSMA, DA ;
DUPPEN, K .
PHYSICAL REVIEW LETTERS, 1991, 66 (19) :2464-2467
[18]   FEMTOSECOND RELAXATION DYNAMICS OF LARGE MOLECULES [J].
ROSKER, MJ ;
WISE, FW ;
TANG, CL .
PHYSICAL REVIEW LETTERS, 1986, 57 (03) :321-324
[19]   TEMPERATURE-DEPENDENT SUPERRADIANT DECAY OF EXCITONS IN SMALL AGGREGATES [J].
SPANO, FC ;
KUKLINSKI, JR ;
MUKAMEL, S .
PHYSICAL REVIEW LETTERS, 1990, 65 (02) :211-214
[20]   Intrinsic conformer jumps observed by single molecule spectroscopy in real time [J].
Stracke, F ;
Blum, C ;
Becker, S ;
Müllen, K ;
Meixner, AJ .
CHEMICAL PHYSICS LETTERS, 2000, 325 (1-3) :196-202