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We present a rapid-scanning approach to fluorescence-detected two-dimensional electronic spectroscopy that combines acousto-optic phase-modulation with digital lock-in detection. The approach shifts the signal detection window to suppress…

Two-dimensional electronic spectroscopy provides information on coupling and energy transfer between excited states on ultrafast timescales. Only recently, incoherent fluorescence detection has made it possible to combine this method with…

Optics · Physics 2025-05-14 Sanchayeeta Jana , Simon Durst , Lucas Ludwig , Markus Lippitz

Ultra-fast and multi-dimensional spectroscopy gives a powerful looking glass into the dynamics of molecular systems. In particular two-dimensional electronic spectroscopy (2DES) provides a probe of coherence and the flow of energy within…

Quantum Physics · Physics 2021-03-31 André Anda , Jared H. Cole

We present a variation of two-dimensional electronic spectroscopy that is capable of mapping spatially-varying differences in electronic couplings using a correlated map of excitation and detection frequencies, with sensitivity orders of…

We demonstrate an approach to two-dimensional electronic spectroscopy (2DES) that combines the benefits of shot-to-shot detection at high-repetition rates with the simplicity of a broadband white light continuum input and conventional…

Optics · Physics 2023-10-03 Asha S. Thomas , Vivek N. Bhat , Vivek Tiwari

A major limitation of transient optical spectroscopy is that relatively high laser fluences are required to enable broadband, multichannel detection with acceptable signal-to-noise levels. Under typical experimental conditions, many…

Optics · Physics 2023-05-03 Siedah J. Hall , Peter J. Budden , Anne Zats , Matthew Y. Sfeir

We perform a beat-frequency-resolved analysis for two-dimensional electronic spectroscopy using a high-speed and stable 2D electronic spectrometer and few-cycle visible laser pulses to disentangle the vibrational coherences in an artificial…

Real-time monitoring of dynamic biological processes in the body is critical to understanding disease progression and treatment response. This data, for instance, can help address the lower than 50% response rates to cancer immunotherapy.…

We present a widefield two-dimensional electronic spectroscopy microscope (2DESM) that integrates multidimensional coherent spectroscopy with optical imaging, enabling femtosecond temporal and micrometer spatial resolution. The broadband…

High-speed multiplex imaging of fluorescent probes is limited by a combination of spectral resolution, sensitivity, high cost and low light throughput of detectors, and filters. In this work, we present a hyperspectral detection system…

Single-molecule fluorescence spectroscopy is a powerful method that avoids ensemble averaging, but its temporal resolution is limited by the fluorescence lifetime to nanoseconds at most. At the ensemble level, two-dimensional spectroscopy…

Optics · Physics 2024-10-11 Sanchayeeta Jana , Simon Durst , Markus Lippitz

Vibrational coherences in ultrafast pump-probe (PP) and 2D electronic spectroscopy (2DES) provide insight into the excited state dynamics of molecules. Femtosecond coherence spectra (FCS) and 2D beat maps yield information about…

Chemical Physics · Physics 2024-06-07 Dale Green , Giovanni Bressan , Ismael A. Heisler , Stephen R. Meech , Garth A. Jones

We demonstrate a femtosecond pump-probe spectrometer which utilizes a white light supercontinuum as input, and relies on mutual synchronization of acousto-optical chopper, pump-probe delay stage and the CCD camera to record shot-to-shot…

Chemical Physics · Physics 2022-12-27 Vivek N. Bhat , Asha S. Thomas , Vivek Tiwari

Fluorescence Correlation Spectroscopy (FCS) is widely used to detect and quantify diffusion processes at the molecular level. The molecules of which diffusion is studied are marked with fluorescent dyes. It is commonly maintained that this…

Biological Physics · Physics 2018-06-12 Mathias Lechelon , Marco Pettini

Two-dimensional (2D) fluorescence-excitation (2D-FLEX) spectroscopy is a recently proposed nonlinear femtosecond technique for the detection of photoinduced dynamics. The method records a time-resolved fluorescence signal in its excitation-…

Chemical Physics · Physics 2024-06-24 Sebastian V. Pios , Maxim F. Gelin , Luis Vasquez , Jürgen Hauer , Lipeng Chen

Recent work applying multidimentional coherent electronic spectroscopy at dilute samples in the gas phase is reviewed. The development of refined phase-cycling approaches with improved sensitivity has opened-up new opportunities to probe…

Atomic and Molecular Clusters · Physics 2019-09-12 Lukas Bruder , Ulrich Bangert , Marcel Binz , Daniel Uhl , Frank Stienkemeier

Future experiments of nuclear and particle physics are moving towards the high luminosity regime, in order to access suppressed processes like rare B decays or exotic charmonium resonances. In this scenario, high rate capability is a key…

Instrumentation and Detectors · Physics 2015-02-18 M. Cardinali , O. Corell , M. I. Ferretti Bondy , M. Hoek , W. Lauth , C. Rosner , C. Sfienti , M. Thiel

The ability to perform broadband optical spectroscopy with sub-diffraction-limit resolution is highly sought-after for a wide range of critical applications. However, sophisticated tip-enhanced techniques are currently required to achieve…

Vacuum birefringence is one of the most striking predictions of strong field quantum electrodynamics: Probe photons traversing a strong field region can indirectly sense the applied "pump" electromagnetic field via quantum fluctuations of…

High Energy Physics - Phenomenology · Physics 2016-07-08 Felix Karbstein , Chantal Sundqvist

Optically-active spin qubits have emerged as powerful quantum sensors capable of nanoscale magnetometry, yet conventional coherent sensing approaches are ultimately limited by the coherence time of the sensor, typically precluding detection…

Quantum Physics · Physics 2025-10-10 Nicole Voce , Paul Stevenson
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