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Phase-corrected time-domain terahertz spectroscopy in reflection geometry
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0009-0006-9686-5456
2025 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Terahertz time-domain spectroscopy (THz-TDS) is a reliable technique used for studying the complex optical properties of materials. Its frequency range makes it suitable for detecting low-energy collective excitations such as phonons, magnons, and plasmons. THz-TDS in transmission geometry has gained much attention over the years. However, despite the need for exploring reflective samples, the advancement of THz-TDS in reflection geometry has faced several obstacles, mainly due to its strict requirement for sub-micron precision in the placement of the sample and reference. Here, we demonstrate a technique for measuring samples in reflection geometry using THz-TDS which involves systematically resolving the alignment issue by first isolating and correcting sources of error in the experimental setup. We then use a novel and robust phase correction method to detect and rectify the remaining misplacement with nanometer precision. This provides us with precise values for the phase of the THz pulse, which in turn allows us to accurately compute the complex optical properties of different types of materials. We use well-known bulk semiconducting samples such as Si and InSb to validate the reliability of our technique. The experimental results of incident angle and polarization-dependent measurements are shown along with the retrieved complex refractive index of these samples. This method immensely simplifies the procedure for obtaining the optical properties of samples in the THz range.

We extend this technique to temperature-dependent measurements and, through a series of additional steps, present a method for studying SrTiO3, a material with strong temperature-dependent spectral features in the THz range. By combining the phase correction method with a novel self-referencing approach, we successfully extract the optical properties of SrTiO3 without the requirement of a reference measurement. These techniques collectively provide a robust and accessible approach for spectroscopic studies of materials in the THz range and can be applied without the requirement of expensive, high-precision equipment. We anticipate that these techniques will be used to study a wide variety of materials with collective excitations in the THz range.

Place, publisher, year, edition, pages
Stockholm: Department of Physics, Stockholm University , 2025. , p. 80
Keywords [en]
Terahertz, reflection, THz spectroscopy, phase, InSb, SrTiO3, phonons
National Category
Condensed Matter Physics Atom and Molecular Physics and Optics
Research subject
Physics
Identifiers
URN: urn:nbn:se:su:diva-240118ISBN: 978-91-8107-142-9 (print)ISBN: 978-91-8107-143-6 (electronic)OAI: oai:DiVA.org:su-240118DiVA, id: diva2:1941486
Public defence
2025-04-15, Lärosal 7, Hus 2, Plan 2, Campus Albano, Greta Arwidssons Väg 30, and online via zoom, Stockholm, 10:00 (English)
Opponent
Supervisors
Available from: 2025-03-21 Created: 2025-02-28 Last updated: 2025-03-14Bibliographically approved
List of papers
1. Near-zero-index behavior in indium antimonide revealed by phase-corrected terahertz reflection spectroscopy
Open this publication in new window or tab >>Near-zero-index behavior in indium antimonide revealed by phase-corrected terahertz reflection spectroscopy
(English)Manuscript (preprint) (Other academic)
Abstract [en]

We developed a phase correction method for broadband terahertz time-domain spectroscopy in reflection geometry, which allows us to obtain quantitative and accurate values for the complex refractive index of materials. The process is analytical, based on the Kramers-Kronig relations, and does not require any computationally intensive algorithms. We validate it by extracting the refractive index of silicon, obtaining the nominal value with an accuracy better than 2.5% over the 0.25–3.5 THz range, and better than 0.6% in the 1–2 THz range. We use the method to experimentally observe that an undoped InSb crystal shows a refractive index of n < 1 between 1 and 2 THz, in proximity to the plasma frequency of the material where, the amplitude of the group velocity goes as low as 0.08c.

National Category
Physical Sciences
Identifiers
urn:nbn:se:su:diva-240143 (URN)
Available from: 2025-03-03 Created: 2025-03-03 Last updated: 2025-03-03
2. Robust phase correction techniques for terahertz time-domain reflection spectroscopy
Open this publication in new window or tab >>Robust phase correction techniques for terahertz time-domain reflection spectroscopy
(English)Manuscript (preprint) (Other academic)
Abstract [en]

We introduce a systematic approach that enables two robust methods for performing terahertz time-domain spectroscopy in reflection geometry. Using the Kramers-Kronig relations in connection to accurate experimental measurements of the amplitude of the terahertz electric field, we show how the correct phase of the same field can be retrieved, even in the case of partly misaligned measurements. Our technique allows to accurately estimate the optical properties of in principle any material that reflects terahertz radiation. We demonstrate the accuracy of our approach by extracting the complex refractive index of InSb, a material with a strong plasma resonance in the low-terahertz range. Our technique applies to arbitrary incidence angles and polarization states.

National Category
Physical Sciences
Identifiers
urn:nbn:se:su:diva-240144 (URN)
Available from: 2025-03-03 Created: 2025-03-03 Last updated: 2025-03-03
3. Self-Reference Method for Phonon Mode Characterization in the Terahertz Regime Using Time-Domain Reflection Spectroscopy
Open this publication in new window or tab >>Self-Reference Method for Phonon Mode Characterization in the Terahertz Regime Using Time-Domain Reflection Spectroscopy
(English)Manuscript (preprint) (Other academic)
National Category
Physical Sciences
Identifiers
urn:nbn:se:su:diva-240145 (URN)
Available from: 2025-03-03 Created: 2025-03-03 Last updated: 2025-03-03

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