An official website of the United States government
The electronic and nuclear dynamics inside molecules are essential for chemical reactions, where different pathways typically unfold on ultrafast timescales. Extreme ultraviolet (XUV) light pulses generated by free-electron lasers (FELs) allow atomic-site and electronic-state selectivity, triggering specific molecular dynamics while providing femtosecond resolution. Yet, time-resolved experiments are either blind to neutral fragments or limited by the spectral bandwidth of FEL pulses. Here, we combine a broadband XUV probe pulse from high-order harmonic generation with an FEL pump pulse to observe dissociation pathways leading to fragments in different quantum states. We temporally resolve the dissociation of a specific O2+state into two competing channels by measuring the resonances of ionic and neutral fragments. This scheme can be applied to investigate convoluted dynamics in larger molecules relevant to diverse science fields.
more »
« less
Time‐Resolved Second‐Order Coherence Characterization of Broadband Metallic Nanolasers
Abstract High‐bandwidth metallic coaxial nanolasers are of high interest to investigate laser physics such as thresholdless coherence transitions, and have a large variety of promising applications enabled by their ultrasmall size and large spectral bandwidth. Optical coherence properties are commonly characterized in Hanbury‐Brown and Twiss experiments. However, those are difficult to perform in broadband lasers when the coherence time is an order of magnitude shorter than the temporal resolution of the single‐photon detectors, thus requiring significant spectral filtering. This paper demonstrates a new approach in investigating the temporal dynamics of the photon statistics associated with the nanolaser emission, obtained without the requirement of spectral filtering. While optically pumping the nanolasers with nanosecond pulses, time‐resolved second‐order coherence properties are evaluated over the time duration of the pump pulse. Coherence transitions from thermal emission to lasing are observed in the gathered time‐resolved photon statistics, linked to the temporal change in optical power of the nanosecond pump pulses. As nanolasers show better performance for the pulsed pumping scheme, the temporal envelope modulation of these pulses results in varying degrees of coherence within the nanolaser pulse envelope. This approach can also be readily applied to characterize a large variety of broadband lasers.
more »
« less
- PAR ID:
- 10360077
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Laser & Photonics Reviews
- Volume:
- 15
- Issue:
- 11
- ISSN:
- 1863-8880
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Generating wavelength-tunable picosecond laser pulses from an ultrafast laser source is essential for femtosecond stimulated Raman scattering (FSRS) measurements. Etalon filters produce narrowband (picosecond) pulses with an asymmetric temporal profile that is ideal for stimulated resonance Raman excitation. However, direct spectral filtering of femtosecond laser pulses is typically limited to the laser’s fundamental and harmonic frequencies due to very low transmission of broad bandwidth pulses through an etalon. Here, we show that a single etalon filter (15 cm−1 bandwidth; 172 cm−1 free spectral range) provides an efficient and tunable option for generating Raman pump pulses over a wide range of wavelengths when used in combination with an optical parametric amplifier and a second harmonic generation (SHG) crystal that has an appropriate phase-matching bandwidth for partial spectral compression before the etalon. Tuning the SHG wavelength to match individual transmission lines of the etalon filter gives asymmetric picosecond pump pulses over a range of 460–650 nm. Importantly, the SHG crystal length determines the temporal rise time of the filtered pulse, which is an important property for reducing background and increasing Raman signals compared with symmetric pulses having the same total energy. We examine the wavelength-dependent trade-off between spectral narrowing via SHG and the asymmetric pulse shape after transmission through the etalon. This approach provides a relatively simple and efficient method to generate tunable pump pulses with the optimum temporal profile for resonance-enhanced FSRS measurements across the visible region of the spectrum.more » « less
-
Time-resolved photoelectron spectroscopy (TRPES) signals that monitor the relaxation of the RNA base uracil upon optical excitation are simulated. Distinguishable signatures of coherence dynamics at conical intersections are identified, with temporal and spectral resolutions determined by the duration of the ionizing probe pulse. The frequency resolution of the technique, either directly provided by the signal or retrieved at the data-processing stage, can magnify the contribution from molecular coherences, enabling the extraction of most valuable information about the nonadiabatic molecular dynamics. The predicted coherence signatures in TRPES could be experimentally observed with existing ultrashort pulses from high-order harmonic generation or free-electron lasers.more » « less
-
The ongoing miniaturization of semiconductor lasers has enabled ultra-low threshold devices and even provided a path to approach thresholdless lasing with linear input-output characteristics. Such nanoscale lasers have initiated a discourse on the origin of the physical mechanisms involved and their boundaries, such as the required photon number, the importance of optimized light confinement in a resonator and mode-density enhancement. Here, we investigate high-β metal-clad coaxial nanolasers, which facilitate thresholdless lasing. We experimentally and theoretically investigate both the conventional lasing characteristics, as well as the photon statistics of the emitted light. While the former lacks adequate information to determine the threshold to coherent radiation, the latter reveals a finite threshold pump power. Our work clearly highlights an important and often misunderstood aspect of high-β lasers, namely that a thresholdless laser does have a finite threshold pump power and must not be confused with a hypothetical zero threshold laser.more » « less
-
We demonstrate fluorescence-detected two-dimensional electronic spectroscopy (F-2DES) with a broadband, continuum probe pulse pair in the pump-probe geometry. The approach combines a pump pulse pair generated by an acousto-optic pulse-shaper with precise control of the relative pump pulse phase and time delay with a broadband, continuum probe pulse pair created using the Translating Wedge-based Identical pulses eNcoding System (TWINS). The continuum probe expands the spectral range of the detection axis and lengthens the waiting times that can be accessed in comparison to implementations of F-2DES using a single pulse-shaper. We employ phase-cycling of the pump pulse pair and take advantage of the separation of signals in the frequency domain to isolate rephasing and non-rephasing signals and optimize the signal-to-noise ratio. As proof of principle, we demonstrate broadband F-2DES on a laser dye and bacteriochlorophylla.more » « less
