Atomic-Scale Dynamics Probed by Photon Correlations

Rosławska, Anna; Leon, Christopher C.; Grewal, Abhishek; Merino, Pablo; Kuhnke, Klaus; Kern, Klaus

doi:10.1021/acsnano.0c03704

Cited by 18 publications

(22 citation statements)

References 81 publications

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“…Employing STM-induced luminescence (STML) 16 in contrast provides a specific selectivity to processes that result in photon emission, in particular to electroluminescence of molecular emitters [16][17][18][19][20][21][22][23][24][25] , including charged species 17,18 . Thanks to time-resolved single-photon detectors, the STML signal can be probed with sub-4 nanosecond temporal resolution 22,23,26 , albeit limited to local point measurements. In our work, we map the electroluminescence in the time-domain and record optical nanometer-nanosecond snapshots of light emitted by single defects in thin organic films that light up within a few nanoseconds after pulsed electronic excitation.…”

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confidence: 99%

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Gigahertz Frame Rate Imaging of Charge-Injection Dynamics in a Molecular Light Source

et al. 2021

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Light sources on the scale of single molecules can be addressed and characterized on their proper subnanometer scale by scanning tunneling microscopy induced luminescence (STML). Such a source can be driven by defined short charge pulses while the luminescence is detected with sub-nanosecond resolution. We introduce an approach to concurrently image the molecular emitter, which is based on an individual defect, with its local environment along with its luminescence dynamics at a resolution of a billion frames per second. The observed dynamics can be assigned to the single electron capture occurring in the low-nanosecond regime. While the emitter's location on the surface remains fixed, the scanning of

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confidence: 99%

“…Its rate can be obtained by fitting the transient to a kinetic model describing the sequence shown in Fig. 1b 25,26 . In Fig.…”

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Gigahertz Frame Rate Imaging of Charge-Injection Dynamics in a Molecular Light Source

et al. 2021

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“…The resulting light emission signal can be temporally monitored. 12 , 14 , 37 − 41 We observe irreversible changes in the plasmonic properties of the junction as well as light intensity fluctuations on the temporal scale of seconds, both of which are correlated with the transport properties of a single-atom contact. Our results agree with theoretical predictions 23 , 28 and show that minute changes in the atomic structure at or near the junction substantially modify the properties of the plasmonic antenna.…”

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confidence: 91%

Atomic-Scale Structural Fluctuations of a Plasmonic Cavity

et al. 2021

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Optical spectromicroscopies, which can reach atomic resolution due to plasmonic enhancement, are perturbed by spontaneous intensity modifications. Here, we study such fluctuations in plasmonic electroluminescence at the single-atom limit profiting from the precision of a low-temperature scanning tunneling microscope. First, we investigate the influence of a controlled single-atom transfer from the tip to the sample on the plasmonic properties of the junction. Next, we form a well-defined atomic contact of several quanta of conductance. In contact, we observe changes of the electroluminescence intensity that can be assigned to spontaneous modifications of electronic conductance, plasmonic excitation, and optical antenna properties all originating from minute atomic rearrangements at or near the contact. Our observations are relevant for the understanding of processes leading to spontaneous intensity variations in plasmon-enhanced atomic-scale spectroscopies such as intensity blinking in picocavities.

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“…Second-order correlation measurement performs excellent potential as an atomic-scale dynamics probe in light-matter interactions at the nanoscale 1 . This measurement provides unique access to characterizing the dynamics of some critical physical processes, such as the charge transport 2 , molecular motion 3 , and quantum properties of light fields [4][5][6][7][8][9][10][11][12] .…”

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confidence: 99%

Jitter-calibrated second-order correlation measurement of low-repetition-rate pulsed excitation

Gong¹,

Wu²,

Guo³

et al. 2022

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We report a new technique for the realization of second-order correlation (g 2 (τ )) measurement under low-repetition-rate pulsed excitation (1 kHz), with timing jitter calibrated to restore lateral g 2 (τ ) curves and determine g 2 (0). We use CdSe nanowire (NW) laser to demonstrate the jitter-calibrated g 2 (τ ) measurement, where g 2 (0) evolution shows the laser emission transition process. The exciting pulses are split into reference and excitation channels, which enables the jitter calibration when the exciting pulses have significant timing jitter and low repetition rate. After using the reference signals to calibrate and rearrange the single-photon signals, lateral g 2 (τ ) curves can be entirely restored, and g 2 (0) evolution is demonstrated from our method.

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Atomic-Scale Dynamics Probed by Photon Correlations

Cited by 18 publications

References 81 publications

Gigahertz Frame Rate Imaging of Charge-Injection Dynamics in a Molecular Light Source

Gigahertz Frame Rate Imaging of Charge-Injection Dynamics in a Molecular Light Source

Atomic-Scale Structural Fluctuations of a Plasmonic Cavity

Jitter-calibrated second-order correlation measurement of low-repetition-rate pulsed excitation

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