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

来源：

PHYSICAL REVIEW LETTERS | 2005年 / 94卷 / 07期

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

页数：4

共 29 条

[1] MOLECULAR THEORY OF NONPOLAR SOLVATION DYNAMICS [J].

BAGCHI, B .

JOURNAL OF CHEMICAL PHYSICS, 1994, 100 (09) :6658-6664

[2] Exciton delocalization and initial dephasing dynamics of purple bacterial LH2 [J].

Book, LD ;

Ostafin, AE ;

Ponomarenko, N ;

Norris, JR ;

Scherer, NF .

JOURNAL OF PHYSICAL CHEMISTRY B, 2000, 104 (34) :8295-8307

[3] Focal spots of size λ/23 open up far-field florescence microscopy at 33 nm axial resolution -: art. no. 163901 [J].

Dyba, M ;

Hell, SW .

PHYSICAL REVIEW LETTERS, 2002, 88 (16) :4-163901

[4] Probing photoinduced intersystem crossing by two-color, double resonance single molecule spectroscopy [J].

English, DS ;

Harbron, EJ ;

Barbara, PF .

JOURNAL OF PHYSICAL CHEMISTRY A, 2000, 104 (40) :9057-9061

[5] TEMPERATURE-DEPENDENT ULTRAFAST SOLVATION DYNAMICS IN A COMPLETELY NONPOLAR SYSTEM [J].

FOURKAS, JT ;

BERG, M .

JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (10) :7773-7785

[6] Coherent nonlinear optical response of single quantum dots studied by ultrafast near-field spectroscopy [J].

Guenther, T ;

Lienau, C ;

Elsaesser, T ;

Glanemann, M ;

Axt, VM ;

Kuhn, T ;

Eshlaghi, S ;

Wieck, AD .

PHYSICAL REVIEW LETTERS, 2002, 89 (05) :057401/1-057401/4

[7] Non-Markovian dynamics of the vibrations of ions in water from femtosecond infrared three-pulse photon echoes [J].

Hamm, P ;

Lim, M ;

Hochstrasser, RM .

PHYSICAL REVIEW LETTERS, 1998, 81 (24) :5326-5329

[8] Quantum control of energy flow in light harvesting [J].

Herek, JL ;

Wohlleben, W ;

Cogdell, RJ ;

Zeidler, D ;

Motzkus, M .

NATURE, 2002, 417 (6888) :533-535

[9] Excitonic behavior of rhodamine dimers:: A single-molecule study [J].

Hernando, J ;

van der Schaaf, M ;

van Dijk, EMHP ;

Sauer, M ;

García-Parajó, MF ;

van Hulst, NF .

JOURNAL OF PHYSICAL CHEMISTRY A, 2003, 107 (01) :43-52

[10] Nanometer resolution and coherent optical dipole coupling of two individual molecules [J].

Hettich, C ;

Schmitt, C ;

Zitzmann, J ;

Kühn, S ;

Gerhardt, I ;

Sandoghdar, V .

SCIENCE, 2002, 298 (5592) :385-389

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