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Background-free fluorescence detection in multidimensional electronic spectroscopy promises high sensitivity compared to conventional approaches. Here we explore the sensitivity limits of multidimensional electronic spectroscopy. We present…

Chemical Physics · Physics 2022-10-18 Amitav Sahu , Vivek N. Bhat , Sanjoy Patra , Vivek Tiwari

Fluorescence-detected Fourier transform (FT) spectroscopy is a technique in which the relative paths of an optical interferometer are controlled to excite a material sample, and the ensuing fluorescence is detected as a function of the…

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

The development of a multiple-channel lock-in optical spectrometer (LIOS) is presented, which enables parallel phase-sensitive detection at the output of an optical spectrometer. The light intensity from a spectrally broad source is…

Other Condensed Matter · Physics 2009-11-10 P. S. Fodor , S. Rothenberger , J. Levy

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

We describe an experiment to measure the emitted real-time electric field from an ultrafast third-order nonlinear optical interaction in molecules, using a phase-tracked spectral interferometry scheme. By combining a software lock-in…

Optics · Physics 2025-03-11 Siddhant Pandey , Francis Walz , Niranjan Shivaram

We show that the modulation of the phases of the laser beams of ultra-short pulses leads to modulation of the two photon fluorescence intensity. The phase modulation technique when used in multi-photon microscopy can improve the signal to…

Optics · Physics 2015-03-12 Khadga Jung Karki , Mohammed Abdellah , Tonu Pullerits

We report a new method of two-pathway coherent control using three narrow-band cw laser sources, phase locked in an optical phase-lock loop, to maintain the high degree of optical coherence required for the coherent control process. In…

Atomic Physics · Physics 2026-01-16 Jonah A. Quirk , Carol E. Tanner , D. S. Elliott

We demonstrate an optical frequency analysis method using the Fourier transform of detection times of fluorescence photons emitted from a single trapped 40Ca+ ion. The response of the detected photon rate to the relative laser frequency…

Recent theoretical studies in quantum spectroscopy have emphasized the potential of non-classical correlations in entangled photon pairs for selectively targeting specific nonlinear optical processes in nonlinear optical responses. However,…

Chemical Physics · Physics 2026-04-21 Yuta Fujihashi , Ozora Iso , Ryosuke Shimizu , Akihito Ishizaki

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

Fluorescence microscopy is a powerful tool for imaging biological samples with molecular specificity. In contrast, phase microscopy provides label-free measurement of the sample's refractive index (RI), which is an intrinsic optical…

Optics · Physics 2022-01-26 Yi Xue , David Ren , Laura Waller

We propose a method to observe phase-dependent spectra in resonance fluorescence, employing a two-level atom driven by a strong coherent field and a weak, amplitude-fluctuating field. The spectra are similar to those which occur in a…

Quantum Physics · Physics 2009-10-31 Peng Zhou , S. Swain

We demonstrate a two-dimensional time-domain spectroscopy method to extract amplitude and phase modifications of excited atomic states caused by the interaction with ultrashort laser pulses. The technique is based on Fourier analysis of the…

Atomic Physics · Physics 2015-06-19 Alexander Blättermann , Christian Ott , Andreas Kaldun , Thomas Ding , Thomas Pfeifer

We calculate the utility of high-frequency squeezed-state enhanced two-frequency interferometry for low-frequency phase measurement. To use the high-frequency sidebands of the squeezed light, a two-frequency intense laser is used in the…

Quantum Physics · Physics 2015-05-27 Zehui Zhai , Jiangrui Gao

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

This is the first in a series of two papers investigating the effect of electron-phonon coupling in two-dimensional Fourier transformed electronic spectroscopy. We present a series of one- and two-dimensional nonlinear spectroscopic…

As optical two-dimensional coherent spectroscopy (2DCS) is extended to a broader range of applications, it is critical to improve the detection sensitivity of optical 2DCS. We developed a fast phase-cycling scheme in a non-collinear optical…

How atoms and electrons in a molecule move during a chemical reaction and how rapidly energy is transferred to or from the surroundings can be studied with flashes of laser light. However, despite prolonged efforts to develop various…

Chemical Physics · Physics 2022-01-05 JunWoo Kim , Jonggu Jeon , Tai Hyun Yoon , Minhaeng Cho

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…

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