Optical spectroscopy is the determination of a material's properties by measuring how much light it reflects or transmits. Pump-probe spectroscopy consists of first using a short, intense laser-pulse to perturb the material--for instance by exciting electrons or phonons--and then measuring the small changes in reflectivity brought about by this perturbation. As the electrons and phonons relax back to their initial states, on time scales from femtoseconds to nanoseconds, the reflectivity recovers its initial value.
Pump-probe spectroscopy is "ultrafast" because its time-resolution is determined only by the length of the "pump" pulse that initially perturbs the sample and of the later "probe" pulse whose reflectivity is measured. The Weber lab uses optical pulses with a duration of 70 fs (FWHM).
A material's ultrafast behavior depends on the energy of the pump photons, which determines the initial energy of photoexcited electrons. In the Weber lab, we use 1.5-eV (800-nm) photons produced by a Ti:Sapph laser operating at a repetition rate of 80 MHz. Working with collaborators, we also do experiments using mid-infrared pump photons, which correspond to the energy of Dirac electrons in topological materials.
The probe photons also matter: if the probe consists of X-ray or ultraviolet photons, then instead of time-resolved reflectivity an experiment may time-resolve diffracted X-rays (determining atoms' instantaneous positions) or photoemitted electrons (determining the electrons' instantaneous energy-vs-momentum dispersion). The Weber lab is using these and other elaborations of the pump-probe technique, described below.
Image: A schematic representation of a pump-probe experiment. The Titanium:Sapphire laser produces short pulses of 800-nm light, which is split into pump and probe pulses at the beamsplitter (dashed line).
Because X-rays are short-wavelength electromagnetic waves, they needn't travel in straight lines, but instead can be diffracted (bent) by atoms. When X-rays diffract off of the regular lattice of atoms in a solid, they interfere to form a characteristic pattern of bright spots. From a careful analysis of these spots one can reconstruct the atoms' positions.
If the X-rays come in a sufficiently short monochromatic pulse, then ultrafast X-ray diffraction is possible: the atoms' positions can be timed to precision better than 100 fs, allowing an ultrafast measure of their motion. Such pulses are produced by X-ray "free-electron lasers" (XFELs), large facilities of which just five have been built, beginning in 2009.
The Weber lab seeks to use ultrafast X-ray diffraction to measure coherent phonons--the rapid, in-sync oscillation of atomic positions that can occur after exciting a material with a short laser pulse. As part of our project on optical control of topological materials (see Research Topics), we are exploring coherent phonons in SrMnSb2 and other Dirac and Weyl semimetals. It is predicted that, when a coherent phonon causes the atoms to move far enough, it may rapidly and reversibly change these materials' electronic properties.
Image: Weber-lab researcher J. Matthew Kim (SCU 2019) at SACLA, the XFEL in Japan. Also shown: the goniometer, which positions and rotates samples for XRD experiments, and collaborator Samuel Teitelbaum.
Particles' random thermal motion tends to take them away from regions of high density and into regions where they are less dense, a process known as diffusion. (The famous Brownian motion is an example of diffusion.) A particle's diffusivity depends on both its speed and how frequently it suffers collisions, so a measurement of diffusivity can provide valuable microscopic insight into particles' motion. Transient-grating (TG) spectroscopy allows measurement of the diffusivity of photoexcited species like electrons, holes, phonons, or electrons' spins.
TG spectroscopy is a variation on optical pump-probe spectroscopy, in which a sample is photoexcited by two pump pulses arriving simultaneously and obliquely. Where the pulses overlap, their interference gives rise to a sinusoidal pattern of bright and dark regions and a corresponding sinusoidal pattern in the population of photoexcited electrons--the eponymous "grating." As the electrons diffuse, they tend to lower the grating's peaks and fill in its valleys, reducing the grating's overall modulation. The rate at which the grating decays thus encodes information about the electrons' diffusivity.
TG spectroscopy is particularly useful in semiconductor spintronics (see Research Topics), because a simple variation in the experiment allows the excitation and measurement of a grating of the electrons' spin-orientation.
Image: A representation of a transient grating's time-evolution, from a highly-corrugated distribution of electrons at t=0 to a spatially smooth distribution at later time. The grating's gradual smoothing results from the electrons' diffusion. In the Weber lab, grating spacings as short as 1 micron are possible.
National Science Foundation “RUI: Using coherent phonons for ultrafast control of the Dirac node SrMnSb2.” January 2020 - present.
National Science Foundation “RUI: Conductivity, diffusion, and dispersion of photoexcited Dirac fermions in cadmium arsenide.” September 2015 - August 2019.
National Science Foundation “RUI: Measurement of density of states of (Ga,Mn)As and diffusion of photoinduced order by ultrafast transient-grating spectroscopy.” July 2011 - June 2015.
Research Corporation “Ferromagnetic exchange in Ga1-xMnxAs: microscopic, time-resolved study by transient-grating spectroscopy.” January 2009 - December 2010.
Additional support over the years has come from Santa Clara University.
Email: cweber@scu.edu
Phone: 408-554-7869
Office: SCDI, room 2311M (2nd floor, southeast corner)
Lab: SCDI, rooms 1106 & 1108 (1st floor, north wing)
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Mailing address: Department of Physics // Santa Clara University // 500 El Camino Real // Santa Clara, CA 95053-0315 U.S.A.